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Duis-Coors2016 Article MicroplasticsInTheAquaticAndTe

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Duis and Coors Environ Sci Eur (2016) 28:2

DOI 10.1186/s12302-015-0069-y

REVIEW Open Access

Microplastics in the aquatic


and terrestrial environment: sources (with
a specific focus on personal care products),
fate and effects
Karen Duis*  and Anja Coors

Abstract 
Due to the widespread use and durability of synthetic polymers, plastic debris occurs in the environment worldwide.
In the present work, information on sources and fate of microplastic particles in the aquatic and terrestrial environ‑
ment, and on their uptake and effects, mainly in aquatic organisms, is reviewed. Microplastics in the environment
originate from a variety of sources. Quantitative information on the relevance of these sources is generally lacking,
but first estimates indicate that abrasion and fragmentation of larger plastic items and materials containing synthetic
polymers are likely to be most relevant. Microplastics are ingested and, mostly, excreted rapidly by numerous aquatic
organisms. So far, there is no clear evidence of bioaccumulation or biomagnification. In laboratory studies, the inges‑
tion of large amounts of microplastics mainly led to a lower food uptake and, consequently, reduced energy reserves
and effects on other physiological functions. Based on the evaluated data, the lowest microplastic concentrations
affecting marine organisms exposed via water are much higher than levels measured in marine water. In lugworms
exposed via sediment, effects were observed at microplastic levels that were higher than those in subtidal sediments
but in the same range as maximum levels in beach sediments. Hydrophobic contaminants are enriched on microplas‑
tics, but the available experimental results and modelling approaches indicate that the transfer of sorbed pollutants
by microplastics is not likely to contribute significantly to bioaccumulation of these pollutants. Prior to being able to
comprehensively assess possible environmental risks caused by microplastics a number of knowledge gaps need to
be filled. However, in view of the persistence of microplastics in the environment, the high concentrations measured
at some environmental sites and the prospective of strongly increasing concentrations, the release of plastics into the
environment should be reduced in a broad and global effort regardless of a proof of an environmental risk.
Keywords:  Plastic debris, Environmental concern, Persistence, Personal care products,
Cosmetic products, Microplastic

Introduction large production volumes and the durability of plastics,


World production of plastics (i.e. synthetic organic it is not surprising that plastics are found in the environ-
polymers) has strongly expanded during the last dec- ment. Initially, scientific and public attention focused on
ades, from 1.7 million t in 1950 to 299 million t in 2013. larger plastic debris. However, the occurrence of small
While the amount of plastics produced in Europe has plastic particles in the marine environment was already
been relatively constant in the last 10  years, world plas- described in the early 1970s [3, 4]. During the last few
tic production continues to increase [1, 2]. In view of the years, microplastics in the environment have received
increasing attention and are now an emerging area of
research [5–8].
*Correspondence: k‑[email protected]
ECT Oekotoxikologie GmbH, Böttgerstr. 2‑14, 65439 Flörsheim/Main,
Most commonly, microplastics have been defined as
Germany synthetic organic polymer particles with a size (or, more

© 2016 Duis and Coors. This article is distributed under the terms of the Creative Commons Attribution 4.0 International License
(http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium,
provided you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license,
and indicate if changes were made.
Duis and Coors Environ Sci Eur (2016) 28:2 Page 2 of 25

specifically, largest dimension)  <5  mm [6, 8–11]. The the sampling nets was most commonly 300–390 µm [11].
majority of definitions do not include a lower size limit. The sampling method has a strong influence on the study
In view of the definition of nanoscale (1–100  nm [12]), results, especially concerning the smallest microplastics,
the term microplastics is used in this review for solid which require a sufficiently small mesh width or bulk
synthetic organic polymer particles with a size between sampling, depending on their size [21].
100  nm and 5  mm. In studies on the occurrence in the Samples from subtidal sediments are taken with sedi-
environment, the upper size limit of the sampled plastics ment sampling equipment, e.g. grab samplers [6, 11,
is not always indicated. In such cases, the term micro- 22]. For coastal sediments, direct sampling of visually
plastics is used, if it can be assumed that the sampled identified microplastics (e.g. by hand or using twee-
plastic items are in the size range mentioned above. In zers) has been used. This method can be employed to
cases where sampling included microplastics, but the sample larger microplastics such as plastic resin pel-
upper size limit of the sampled plastics is somewhat lets (typical diameter: 3.5  mm [23]) from the surface of
above 5 mm (e.g. 10 mm) the term ‘small plastic items’ is sandy beaches. However, it is not suitable for sampling
employed. Plastic items larger than 5 mm are designated microplastics that do not have a characteristic shape, are
as macroplastics. smaller than plastic resin pellets or are mixed with other
In the present work, currently available information debris [6, 11]. In these cases, bulk sampling is required
on sources, fate and occurrence of microplastics in the to avoid an underrepresentation of small microplastics.
aquatic and terrestrial environment, on their uptake by As the distribution of microplastics on beaches is often
aquatic and terrestrial organisms and possible effects on heterogeneous, attention needs to be paid to sample size,
these organisms is critically evaluated. replication and the location of the sampling sites on the
Recently, considerable public attention has focused beach [8].
on microplastics particles from personal care products,
which was mainly triggered by reports in news media. Sample processing
Therefore, a specific focus is placed on the contribution To recover microplastics from bulk or volume-reduced
of microplastics from personal care products (defined water samples, a sieving or filtration step is commonly
and regulated as cosmetic products in the EU [13]) to the used. Alternatively, microplastics have been collected
overall pollution of the environment with microplastics. from the surface of the water sample using tweezers. Yet,
An effort was made to report, as far as possible, numer- there is a high likelihood of bias when visually collecting
ical concentrations of microplastics for studies on occur- microplastics [11, 24]: the lowest particle size in studies,
rence, uptake and effects. Plastic products may contain in which sieves were used, was smaller than in studies, in
a number of additives including plasticisers, stabilisers, which particles were visually collected from the samples
flame retardants, pigments and antimicrobials [14–16]. [11].
Potential effects of these additives, which have been dis- Sieving and, especially, density separation are used to
cussed elsewhere (e.g. [17]), are not addressed in this extract microplastics from bulk sediment samples. Plas-
review. tic particles usually have a much lower specific weight
(Table  1) than sediments (typically 2.65  g/cm3 [11]).
Methods to sample, process and analyse When sediment samples are mixed with salt solution of
microplastics in the environment an appropriate density, sediment settles at the bottom,
A number of methods to sample, isolate, characterise, while microplastics can be collected from the surface [6,
identify and quantify microplastics have been devel- 11, 25]. Examples of such salt solutions are concentrated
oped for water and sediment. In the following sections, sodium chloride (density: 1.2  g/cm3), sodium polytung-
the most relevant methods are briefly presented. In view state (1.4 g/cm3), sodium iodide (1.6–1.8 g/cm3) and zinc
of the comprehensive review of Hidalgo-Ruz et  al. [11] chloride (1.5–1.7 g/cm3) [6, 26–29]. To separate all plas-
and available guidance on monitoring of marine litter tic resin types from the sediment, salt solutions with a
including microplastics [6], emphasis is placed on recent density  ≥1.45  g/cm3 have been recommended [26, 29].
developments. Several devices are available for density separation [26–
28]. The resultant salt solution is subjected to sieving or
Sampling filtration.
While in some cases bulk water samples were taken (e.g. To separate microplastics from other material recov-
[18]), volume-reduced sampling methods have gener- ered by the abovementioned sieving, filtration or density
ally been employed to sample microplastics from water: separation procedures, visual sorting has in most cases
neuston nets for the sea surface layer, and zooplankton been used. However, visual differentiation of microplastic
nets for sub-surface water [6, 11, 19, 20]. Mesh width of particles from other debris or grains of sand is difficult
Duis and Coors Environ Sci Eur (2016) 28:2 Page 3 of 25

Table 1  Densities of plastic materials that are often found were not confirmed to be plastics [11]. Using scanning
in the aquatic environment electron microscopy combined with energy dispersive
Plastic class Abbreviation Density X-ray spectroscopy (SEM–EDS), Eriksen al. [41] showed
(g/cm3)a,b that numerous particles, which had been visually identi-
fied as microplastics, were aluminium silicates from coal
Expanded polystyrene (styrofoam) EPS 0.01–0.04
ash and coal fly ash. Consequently, further analyses are
Low-density polyethylene LDPE 0.89–0.93
required (1) to unequivocally identify microplastics and
High-density polyethylene HDPE 0.94–0.98
(2) to obtain information on their resin composition [6,
Polypropylene PP 0.83–0.92
8, 11, 24, 30, 40, 41]. The use of infrared (IR) and Raman
Polyethylene terephthalate PET 0.96–1.45
spectroscopy has been highly recommended for this pur-
Polyamide (nylon) PA 1.02–1.16
pose [11, 30]. In EC [6], it is suggested that all particles
Polystyrene PS 1.04–1.1
with a size between 20 and 100  µm and 5–10  % of the
Polymethyl methacrylate (acrylic) PMMA 1.09–1.20
particles with a size between 100  µm and 5  mm should
Polyvinylchloride PVC 1.16–1.58
be further analysed by IR or Raman spectroscopy. Infra-
Polycarbonate PC 1.20–1.22
red spectrophotometry and FT-IR are probably the most
Polyurethane PU 1.2
commonly used method to identify the chemical compo-
Alkyd – 1.24–2.10
sition of microplastics. If coupled with microscopy they
Polyester PES 1.24–2.3
can be used to identify microplastics with a size >20 µm
Polytetrafluoroethylene PTFE 2.1–2.3
[6, 11, 30, 31]. Raman spectroscopy combined with
a
  Note that densities of plastic items can be modified by additives and microscopy has a higher resolution (approx. 1–2  µm
environmental processes such as weathering and fouling
b
[26, 30, 42]). Several other methods such as pyrolysis–
  Based on [11, 16, 25, 109]
gas chromatography combined with mass spectrometry
(Pyr-GC/MS), high temperature gel-permeation chro-
and only suitable for microplastics larger than approx. matography (HT-GPC) with IR detection, SEM–EDS
1  mm [6, 11, 22, 30]. Transparent or white particles and thermoextraction and -desorption coupled with GC/
require careful differentiation methods, e.g. examination MS [24, 41, 43–45] have been developed. With Pyr-GC/
under high magnification using a fluorescence micro- MS, both the polymer composition of microplastics and
scope to confirm the absence of cellular structures [11, organic additives (e.g. antioxidants and plasticisers) can
30]. be analysed simultaneously [24, 43].
Recently, methods for chemical and enzymatic clean- The abundance of microplastics is commonly indicated
up have been developed. Treatment of samples with as numerical or mass concentration: (1) for the sea sur-
chemicals (e.g. 30–35  % H2O2, 20  % HCl, 30  % NaOH), face layer as number or weight of items per area, (2) for
partly combined with increased temperatures, has been the water column as number or weight of items per vol-
used to remove organic material and calcified structures. ume and (3) for sediments as number or weight of items
However, chemical treatment may lead to a partial or per sediment area or sediment weight, referring to sedi-
complete degradation of microplastics [24, 26, 28, 31– ment wet (ww) or dry weight (dw) (see also Additional
33]. For this reason, digestion with enzymes (proteinase, file  1: Tables S1, S2). Due to the non-standardised units
cellulase, lipase and chitinase) has been recommended of quantification, the comparison of different studies can
to separate microplastics from organic material [31, 32]. be very difficult [11, 29, 46]. It has therefore been sug-
Chemical (e.g. 69 % HNO3, 10 % KOH, 30 % H2O2) and gested that all studies should provide sufficient informa-
enzymatic (proteinase) methods have also been used to tion to allow converting units, e.g. from items per area
extract microplastics from tissues of aquatic organisms to items per volume [11]. Preferably, both numerical and
and from the digestive tract content of fish [32–39]. mass concentration should be indicated [8].

Identification and quantification Lower size limit of the sampled microplastics


Characteristics such as density and colour have been used The lower size limit of microplastics sampled in the envi-
to identify the polymer type of microplastics. However, ronment is obviously determined by the sampling and
these characteristics can be affected by weathering. As processing methods. Microplastics larger than 300  µm
mentioned above, non-plastic microparticles and micro- were sampled in most cases from seawater and micro-
fibers may be wrongly classified as microplastics [11, 30, plastics larger than 500  µm from sediment [11]. When
40]. When analysing microparticles, which had been vis- density separation with a subsequent filtration step is
ually classified as microplastics, with Fourier transform used, smaller particles can be retrieved from sediment.
infrared spectroscopy (FT-IR), up to 70 % of the particles The smallest microplastics sampled from sediment had
Duis and Coors Environ Sci Eur (2016) 28:2 Page 4 of 25

a diameter of 1  µm. With current state-of-the-art tech- Primary microplastics


niques it is most likely not possible to representatively Microplastic particles are used as exfoliants in certain
sample and unequivocally identify microplastics with a product segments of specific personal care products,
size below 1–2 µm [11, 26]. such as hand cleaners, facial cleaners and toothpaste
[51]. In the US patent for skin cleaners containing plas-
Quality control tic microparticles, polyolefin particles with a size of
Given that microplastics research is still in a relatively 74–420 µm and an amorphous shape without sharp edges
early stage, inter-laboratory comparisons of protocols for were described as appropriate for use as exfoliants [52].
sampling, processing and analysis and certified reference The used polyolefins include polyethylene (PE), polypro-
materials are lacking [6, 8, 29, 37]. There is little informa- pylene (PP) and polystyrene (PS; for abbreviations for the
tion on the recovery rates of different sampling and pro- plastic resins see also Table 1). Gouin et al. [53] estimated
cessing methods [26]. Especially small microplastics have that in 2012, approx. 6  % of the liquid skin cleaning
a strong tendency to adsorb to surfaces. Therefore, care products marketed in the European Union, Norway and
has to be taken to avoid overlooking particles that adhere Switzerland contained microplastics. Based on a survey
to the devices used to collect and process samples [11, conducted by Cosmetics Europe, PE accounted for 93 %
26]. of the microplastics used in skin cleaning products in
A further important issue is potential contamination these countries in 2012. The products typically contained
of samples by particles originating e.g. from the cloth- between 0.05 and 12  % of microplastic particles, with
ing of workers, the used equipment and the ambient air. the size of most particles ranging from 450 to 800  µm
As far as possible, such contamination has to be reduced [53]. When analysing skin cleaners, spherical particles
[6, 11, 26, 34, 47]. It has also been suggested that samples (mostly with a rough surface), threads and irregularly
should be processed in cleanrooms or cleanroom cabi- shaped particles consisting of PE and PS, and mainly hav-
nets and that procedural controls should be included to ing a blue or white colour were identified [45, 51, 54–56].
verify contamination during sample processing [6, 11, 28, Microplastics are also used in medical applications, e.g.
47–49]. in dentist tooth polish, and as carriers to deliver active
pharmaceutical agents [51, 57]. After use, microplastics
Summary: methods to sample, process and analyse from personal care products and such medical products
microplastics in the environment can reach the environment via wastewater.
Appropriate sampling, extraction and identification Microplastics are also used in drilling fluids for oil
methods are required to representatively sample and and gas exploration and in industrial abrasives, i.e. for
unequivocally identify microplastics in the environment. air-blasting to remove paint from metal surfaces and for
Visual sampling and sorting of small particles (<0.5–1.0 cleaning different types of engines [55, 57–59]. Industrial
mm) and visual identification of microplastics are not abrasives contain e.g. acrylic, PS, melamine, polyester
considered reliable, since particles may be overlooked or (PES) and poly allyl diglycol carbonate microplastics [41].
wrongly classified as microplastics. Quality controls have If not used in closed systems and disposed properly, they
to be included to verify the efficiency of the used meth- can end up in the environment [57].
ods and the absence of background contamination. Raw materials used for the fabrication of plastic prod-
ucts (pre-production plastics), namely plastic resin pel-
Sources of microplastics and routes of entry lets or flakes and plastic powder or fluff, are another
into the environment important source of primary microplastics. They can
Microplastics found in the environment are a very het- reach the environment after accidental loss during trans-
erogeneous group of particles differing in size, shape, port or with run-off from processing facilities, i.e. often
chemical composition and specific density that originate as a result of improper handling. Similarly, residues from
from a variety of different sources. The following two plastic processing factories and regranulate produced
sections provide an overview of sources of primary and during plastic recycling can end up in the environment
secondary microplastics in the environment (see also [9, 25, 58–62]. Concentrations of plastic resin pellets in
Table  2). Primary microplastics are commonly defined the environment were high from the 1970s to the 1990s
as microplastics produced (and released to the environ- [63, 64]. Highest concentrations of pre-production pel-
ment) in a micro-size range; secondary microplastics lets (up to 100,000 pellets/m of beach) were often found
result from the fragmentation of larger plastic materials on beaches close to plastic producing or processing
[8, 50]. sites [29, 60, 61]. In subsequent years, concentrations
Duis and Coors Environ Sci Eur (2016) 28:2 Page 5 of 25

Table 2  Overview of sources for primary and secondary microplastics in the environment

Primary microplastics
 Specific personal care products containing microplastics as exfoliants/abrasives
 Specific medical applications (e.g. dentist tooth polish)
 Drilling fluids for oil and gas exploration
 Industrial abrasives
 Pre-production plastics, production scrap, plastic regranulate: accidental losses, run-off from processing facilities
Secondary microplastics
 General littering, dumping of plastic waste
 Losses of waste during waste collection, from landfill sites and recycling facilities
 Losses of plastic materials during natural disasters
 Plastic mulching
 Synthetic polymer particles used to improve soil quality and as composting additive
 Abrasion/release of fibres from synthetic textiles
 Release of fibres from hygiene products
 Abrasion from car tyres
 Paints based on synthetic polymers (ship paints, other protective paints, house paint, road paint): abrasion during use and paint removal, spills, illegal
dumping
 Abrasion from other plastic materials (e.g. household plastics)
 Plastic items in organic waste
 Plastic coated or laminated paper: losses in paper recycling facilities
 Material lost or discarded from fishing vessels and aquaculture facilities
 Material lost or discarded from merchant ships (including lost cargo), recreational boats, oil and gas platforms
Based on [9, 21, 25, 31, 53, 55, 57, 58, 60, 61, 70, 72, 75, 77–79, 81]

of pre-production plastics in the environment gener- addition, large amounts of plastic debris can enter the
ally declined, probably due to improved practice during marine environment during natural disasters such as
handling [63, 65, 66]. Still, high concentrations have been hurricanes, tsunamis and strong sea [18, 74, 75].
found in some studies close to production facilities ([67– Low-density polyethylene (LDPE) films, which are
69]; see also section “Occurrence of microplastics in the used in large volumes to protect agricultural crops, sup-
aquatic and terrestrial environment”). press weeds, increase temperature and retain irrigation
water in the soil (‘plastic mulching’), are a further rele-
Macroplastics as sources of secondary microplastics vant source of microplastics in the environment. If these
Since secondary microplastics are generated when larger thin plastic foils embrittle, the fragments can end up in
plastic materials fragment, sources of macroplastics and the soil [72, 76, 77]. Synthetic polymer particles, such as

romull®) and polyurethane (PU) foam, are also used in


their routes of entry into the environment are considered expanded PS flakes with a size of approx. 5–15 mm (Sty-
in this section. It has been estimated that about 75–90 %
of the plastic debris in the marine environment originates horticulture to improve soil quality and as composting
from land-based and about 10–25  % from ocean-based additive [78, 79].
sources [25, 70]. General littering, dumping of plastic Moreover, synthetic textiles are an important source of
waste and loss from inappropriately managed landfill microplastics. In 2013, 54.4 million  t of synthetic fibres
sites and during waste collection are assumed to be the were produced worldwide with PES (44.6 million t) being
most important routes of entry of plastic materials into the dominant fibre type [80]. Browne et al. [81] quantified
the environment. Windblown litter is also lost from recy- the number of fibres released when washing PES blan-
cling facilities [60, 70–72]. In this context, it should be kets, fleeces and shirts in domestic washing machines. The
noted that a large percentage of the produced plastics is washing machine effluent contained approx. 120 (blanket)
used for packaging, i.e. for products with a short service to 300 fibres (fleece) per L. Overall, >1900 fibres were given
life [1]. In industrialised countries, waste that is depos- off from the evaluated PES fleece during a single wash. Syn-
ited in landfills is usually covered regularly with soil or thetic textile fibres are also released to air and dust, either
a synthetic material, and the landfill is surrounded by a during normal use [57] or during tumble drying [77]. In
fence to prevent that debris is blown away. However, in addition, synthetic fibres are released from hygiene prod-
developing regions this is often not the case [71–73]. In ucts, e.g. if improperly disposed into wastewater [31].
Duis and Coors Environ Sci Eur (2016) 28:2 Page 6 of 25

A number of other sources of microplastics in the envi- of microplastics originating from such products is not
ronment have been identified. Abrasion from car tyres typical enough to allow an identification of their source.
has been considered as very relevant [46, 57]. In addition, Effluents of two Australian WWTPs with tertiary
many ship paints and other protective paints contain syn- treatment contained on average 1 microplastic item/L
thetic polymers, e.g. alkyds, poly(acrylate/styrene), PU as identified by FT-IR. Polyester, acrylic and polyam-
and epoxy resins. Microplastics may be released by spills ide (PA) fibres were most frequently found [81]. Higher
during application of the paint, by abrasion during use of numbers were found in effluents from a German munici-
the painted product and during paint removal [21, 57]. pal WWTP (on average 33 granules/L, 24 fragments/L
Microplastics are also released as a consequence of abra- and 24 fibres/L [88]) and from three Dutch WWTPs (on
sion from other plastic materials such as household plas- average 55 microplastics/L [89]). However, in these two
tics [31, 57]. studies microplastics were only identified by visual analy-
Ocean-based sources of marine litter include material sis. In a Dutch pilot study, Leslie et  al. [90] investigated
lost or discarded from fishing vessels, aquaculture facili- microplastic concentrations in influent and effluent of a
ties, merchant ships, recreational boats, offshore oil or WWTP. With approx. 200 items/L in the WWTP influ-
gas platforms and during military activities. Cargo lost ent and 20 items/L in the effluent of the activated sludge
from merchant ships may lead to a significant input of treatment, removal efficiency of the WWTP was approx.
plastics into the marine environment [25, 58, 60, 72, 82]. 90  %. A preliminary study was also performed in the
Although dumping of plastic wastes at sea is prohibited central WWTP of St. Petersburg (Russia). Presumptive
since 1988, there are indications that plastic waste from a microplastic particles and fibres were identified by light
considerable number of vessels has still been dumped at microscopy. Approximately 95  % of fibres and particles
sea—mainly due to economic reasons [46, 58, 83]. present in WWTP influent were removed during waste-
water treatment. The WWPT effluent contained on aver-
Fate of microplastics in wastewater treatment age 16 textile fibres, 7 coloured particles and 125 black
plants particles/L [91].
Primary and secondary microplastics as well as macro- A more comprehensive study was performed by Mint-
plastics may enter the environment through wastewa- enig et  al. [31] for 12 German WWTPs. Microplastics
ter. During the primary (mechanical) treatment step (0.02–5 mm) were analysed in WWTP effluents (sampled
in wastewater treatment plants (WWTPs), coarse sus- before final filtration, where present) and sewage sludge.
pended or floating solids are removed from the wastewa- Microplastics were identified by FT-IR or micro-FT-IR.
ter by screens or sieves. Sand and other heavy particles In the WWTP effluents, 0.08–8.9 microplastic particles
are retained in sand traps; floating material is removed with a size <500 µm were detected per L. Particles with
in grease separators [84]. Coarse screens have openings a whitish/transparent colour and an irregular and, partly,
of approx. 20–50  mm, intermediate screens of approx. foil-like form were most common. The most frequently
10–20  mm and fine screens of approx. 2–10  mm [84, detected polymers were PE, polyvinyl alcohol, PES, PS
85]. Such screens are suitable for removing macroplas- and PA. The number of microplastic particles  >500  µm
tics from wastewater [72, 86, 87], while they will—based ranged from 0 to 0.05 per L of effluent. Again, most par-
on the opening sizes mentioned above—not be able to ticles had an irregular, partly foil-like shape. PE and PP
capture smaller microplastics. Still, microplastics may were the most frequently found polymers. Plastic fibre
be captured, if other materials are clogging the screens. content of the effluents ranged from 0.1 to 4.8 fibres/L.
Mintenig et al. [31] suggested that buoyant microplastics Effluent from one WWTP equipped with a final filtration
may be removed in the grease separating step. Micro- step was also sampled after filtration. Filtration removed
plastics with a high density such as PU can be expected all microplastic particles >500 µm, 93 % of the microplas-
to sediment and, thus, to be captured in the sand trap or tic particles <500 µm and 98 % of the microplastic fibres.
with the sludge. Sewage sludge contained 1041–24,129 microplastic par-
To date, only relatively few (often preliminary) stud- ticles/kg dw (fibre content was not analysed). Since single
ies are available on the effectivity of WWTPs to remove samples were investigated for each WWTP and matrix
microplastics from wastewater, and on microplastic levels and small subsamples were evaluated for sludge, Mint-
in WWTP effluents and sludge. In none of these studies, enig et al. [31] point out that their results should be con-
personal care products were unambiguously identified as sidered as indicative values.
source of the detected microplastics. This is due to the Size and form of microplastic fibres in sewage sludge
facts that (a)  microplastics used in personal care prod- can be affected during sludge stabilisation, e.g. as a con-
ucts mostly consist of PE [53], the most widely used plas- sequence of mechanical mixing, increased temperature
tic resin [2], and (b) the often amorphous, irregular form and increased pH [92, 93]. Sewage sludge is incinerated,
Duis and Coors Environ Sci Eur (2016) 28:2 Page 7 of 25

disposed of in landfills or used to fertilise agricultural material reaching the marine environment [25]. Given
land [93], i.e. can represent a source of microplastics for the large amount of macroplastics entering the environ-
the terrestrial environment. Microplastics may remain ment, it is generally assumed that most microplastics in
in the soil, be mobilised and distributed by wind, or be the environment are secondary microplastics, i.e. a result
transported with surface run-off to the aquatic environ- of weathering of larger plastic debris [11, 25]. However,
ment [31, 77, 94, 95]. When sewage sludge is disposed fragmentation rates of macroplastics are largely unknown
into oceans, microplastics directly reach the aquatic [57, 59, 99]. As a result, no quantitative information is
environment. In most industrialised countries, ocean dis- available on the relative contribution of primary and sec-
posal of sewage sludge is prohibited. However, in some ondary microplastics to the overall amount of microplas-
countries sewage sludge is still disposed at sea [96]. tics in the environment [50].
During heavy rainfall events, sewer overflow may A first estimate of the relative contribution of micro-
occur, i.e. untreated wastewater may reach the environ- plastics from personal care products to the plastic debris
ment. Sewer overflow events have been assumed to be entering the North Sea has been provided by Gouin et al.
relevant with regard to the entry of microplastics into [53]. Based on sales data for liquid skin cleaning prod-
the environment [46, 72]. Furthermore, untreated sewage ucts and the estimates that (a) 6  % of liquid skin clean-
is in many regions of the world directly discharged into ers contains microplastic particles and (b) these products
the receiving waters [82]. In the OECD countries, waste- contain 10  % of microplastics, a mean annual amount
water of approx. 80 % of the population is discharged to of 4130  t of microplastic particles was derived for the
WWTPs [97]. However, worldwide only about 15–20  % European Union, Norway and Switzerland for 2012. This
of wastewater is treated [98]. value is consistent with the result of the previously men-
tioned survey of Cosmetics Europe (4360 t for the same
Relevance of different sources of microplastics region and year). For the countries in the watershed of
in the environment the North Sea (Norway, Denmark, Germany, Belgium,
In most cases, it is not possible to derive conclusions on The Netherlands, France, Switzerland, Czech Republic
the origin of microplastics when evaluating and charac- and the UK), annual use of microplastics in personal care
terising their occurrence in an environmental compart- products was estimated to be 2,300 t. Assuming removal
ment. So far, the contribution of specific sources has only of 90  % of the microplastics in WWTPs [90] and dis-
been identified for microplastics with a typical and dis- charge of all water from these countries to the North Sea,
tinct size and shape. Examples include pre-production microplastics from personal care products would consti-
plastic resin pellets, especially if released by localised tute approx. 1 % of the overall amount of marine debris
spills [60, 63, 99, 100], and styrofoam particles found that has been estimated to enter the North Sea each year
close to intensive aquaculture facilities, where styro- (20,000 t [106]). Since it is not specified how the amount
foam buoys and floats are used [8, 101, 102]. By contrast, of 20,000 t was estimated (see also [107]), the abovemen-
microplastics from personal care products lack such tioned information on the relative contribution of micro-
distinct characteristics that would allow an unequivocal plastics to the overall amount of plastic debris in the
identification of their source as has been discussed in the North Sea should be considered as a very rough estimate.
previous section. Sundt et al. [57] evaluated the most relevant sources for
Based on produced or consumed amounts, estimates direct release of microplastics to the Norwegian environ-
have been derived on the contribution of various sources ment. Such ‘primary sources’ of microplastics exclude
to the overall amount of microplastic debris in the envi- macroplastic litter, but include abrasion of microplastics
ronment. However, such estimates are hampered by the (e.g. from paints and tyres), i.e. are not confined to pri-
complexity of the sources of micro- and macroplastics, mary microplastics as defined in the present review. As
the lack of quantitative data on transport and fate in the far as possible, first estimates were provided for annually
environment (see next section), and the high geographic released amounts. These amounts are upstream or ‘start
variability of the relevance of different sources and intro- of the pipe’ amounts; transport processes are not consid-
duction routes, which is caused by differences in the ered. The estimated annually used amount of microplas-
infrastructure, especially with regard to waste manage- tics in personal care products (40 t) is in good agreement
ment [70, 72, 73, 99, 103]. with the estimate of Gouin et al. [53] for Norway (43 t).
Consequently, quantitative information on the con- According to Sundt et  al. [57] microplastics from per-
tribution of different sources to the overall amount of sonal care products account for approx. 0.5 % of all direct
macro- and, especially microplastics in the environment emissions of microplastics in Norway. Other sources
is generally lacking [8, 104, 105]. There are, e.g. no reli- such as losses of pre-production plastics during transport
able estimates of the percentage of plastic packaging and spills (approx. 5 %), abrasion from ship paints, other
Duis and Coors Environ Sci Eur (2016) 28:2 Page 8 of 25

protective paints, house and road paints (approx. 17 %), consumer plastic materials (including PE) are buoyant in
release of textile fibres during household and commercial seawater (Table 1). In aquatic environments, plastics are
laundry (approx. 8 %) and, especially, abrasion from tyres often colonised by a variety of organisms. This fouling
(approx. 54  %) were considered more relevant. Sundt can increase the density so that formerly buoyant items
et  al. [57] assumed that macroplastic litter substantially sink below the water surface. If other organisms graze on
contributes to the overall release of microplastics to the the foulants, density of a plastic item can decrease again
Norwegian environment. However, the available data so that it returns to the water surface [25, 71]. Erosion of
were not considered sufficient for deriving estimates of plastics may also change their specific density [66], and
this contribution. First estimates were only provided mixing of the upper water layer by wind may lead to sub-
for annual amounts of three types of macroplastic litter mersion of previously buoyant microplastics [19].
in Norway: plastic waste from fisheries and aquaculture Given that plastic is persistent (see below) it can be
(>1000  t), littered plastic bags (60  t) and macroplastics transported over long distances, depending on local
released during sewer overflow events (460 t). Estimates winds, ocean currents and geography of the coastline [11,
derived for Germany and Denmark also indicate that per- 71]. Floating plastic debris accumulates on beaches and
sonal care products are a minor source of microplastics in oceanic gyres, benthic debris on the sea bed in areas
in the environment and that other sources such as the with low circulation [9, 11, 71]. The transport of micro-
fragmentation of plastic debris and abrasion from tyres plastics in surface waters may differ from that of macro-
are more relevant [51, 59]. For Denmark, emissions of plastics, because smaller particles at the water surface
microplastics from personal care products to the aquatic are less exposed to wind. Distribution of microplastics
environment were estimated to account for 0.1 % of the may also be affected by particle aggregation and activity
overall emissions to the aquatic environment [51]. of animals [113, 114]. On beaches and in subtidal sedi-
Recently, a number of companies producing personal ments, microplastics can be covered by sediment [11]
care products have announced a phase-out of micro- and, hence be found at considerable depth [115].
plastic particles in their products. In addition, several So far, little is known on the transport of microplastics
US states have banned the manufacture and sale of per- within the terrestrial environment. Rillig [77] assumed
sonal care products containing microplastic particles [53, that terrestrial organisms such as earthworms and moles
57, 59, 108, 109]. It can thus be assumed that at least for contribute to the incorporation of micro- and macroplas-
Europe and the USA emissions from personal care prod- tic material into the soil.
ucts will decrease in the near future. However, the issue Disintegration of common polymers such as LDPE,
of microplastics in the environment will certainly not be high-density polyethylene (HDPE) and PP in the envi-
solved by these actions, since primary microplastics from ronment is mainly initiated by UV radiation. As a result
this source only contribute a small percentage based the of this photo-oxidative degradation, the plastic becomes
rough calculations mentioned above. brittle and fragments. Disintegration is facilitated by
increased temperatures, but reduced by stabilisers, low
Fate of macro‑ and microplastics temperature, low oxygen levels and by fouling or coverage
in the environment with water or sediment reducing exposure to UV radia-
Once released into the environment, plastic material can tion. Hence, photo-oxidative disintegration of plastics is
be transported by wind, washed from land to surface relatively effective on a beach surface, but extremely slow
waters during rainfall, especially with stormwater run- in the deep ocean [25, 71, 116] and for plastics buried in
off, and be transported in freshwater and seawater [61, beach sediment or soil [72, 82]. Water turbulences, wave
63, 72]. It is assumed that large rivers transport consider- action, physical abrasion and freeze–thaw cycles add to
able amounts of macro- and microplastics to the oceans, the disintegration of the plastics [116]. In addition, the
but few quantitative data are available [96, 110–112]. For boring activity of isopods substantially contributed to the
macroplastics, transport by wind to the oceans may be fragmentation of expanded polystyrene (EPS) floats used
significant, especially since approx. 50  % of the human in aquaculture facilities and docks [117]. Similarly, soil
population live within 80  km distance from the sea [9]. organisms that ingest plastic debris together with earth
Airborne transport might also be relevant for very small could contribute to the fragmentation of the plastics [77].
microplastics, which could e.g. be mobilised from uncov- During disintegration of the polymer matrix, particles
ered landfills [77]. of different sizes and shapes are formed [11, 71, 72]. Note
Fate in the aquatic environment depends on the den- that strongly weathered, brittle plastic material still con-
sity: plastics with a lower density than freshwater (approx. sists of polymers with a mean molecular weight of tens
1.0 g/cm3) or seawater (approx. 1.03 g/cm3) are buoyant, of thousands g/mol, which are not biodegraded to con-
those with a higher density are submerged [25]. Most siderable extent under relevant environmental (especially
Duis and Coors Environ Sci Eur (2016) 28:2 Page 9 of 25

marine) conditions [25]. Based on the data available so of small plastic items for each 1°  ×  1° (latitude × lon-
far, mineralisation of plastics appears to be an extremely gitude) area. On the basis of these data, Law et  al. [20]
slow process [25, 116]. For example, sheets of LDPE, concluded that both mean and median numbers of small
HDPE and PP that had been immersed for 6  months in plastic items in the surface layer of the North Pacific gyre
sea water only lost 1.5–2.5 % (LDPE), 0.5–0.8 % (HDPE) increased by a factor of approx. 10 between 1972–1985
and 0.5–0.6  % (PP) of their initial weight [118]. Conse- and 2002–2012. It is controversially discussed if the
quently, estimates of the lifetime of plastics are in the increasing trend has continued since the 1990s [20, 65,
range of hundreds of years [9, 71]. It has therefore been 71, 128, 129]. Due to large spatial and temporal variabil-
assumed that all conventional plastic, which has entered ity in the concentrations of microplastics, it is difficult to
the environment, is still present in the environment, detect smaller increases [19]. High variability of the levels
either in an unfragmented or in a fragmented form [74]. of small plastic items at a smaller scale (i.e. within tens
of km) is caused by local wind-driven turbulences and
Occurrence of microplastics in the aquatic local circulation patterns [20]. Higher concentrations in
and terrestrial environment the sea surface layer are e.g. measured during low-wind
Marine environment conditions [19, 126]. Temporal variability can be high,
Triggered by the detection of unexpectedly high levels e.g. due to variations in oceanic circulations related to El
of microplastics in oceanic convergence zones (e.g. [3, Niño events [71, 99]. Due to the embrittlement and frag-
25, 119]), the occurrence of microplastics has mainly mentation of larger plastic items present in the oceans, it
been investigated in the marine environment (including has been predicted that the overall abundance of micro-
shorelines). Microplastics have been found in the oceans plastics will increase in the future [25, 71, 99, 120].
worldwide [71, 120], including remote regions such as In the following, an overview is provided of the con-
Antarctica and the deep sea [58, 121–124]. The distribu- centration ranges of microplastics in the marine environ-
tion of microplastics in the oceans is very heterogeneous. ment (including estuaries) that is based on the review of
High concentrations have been found close to indus- Hidalgo-Ruz et al. [11] and selected recent publications.
trial centres and metropolitan areas [22, 58, 110, 125], The compiled data shall primarily serve as background
in enclosed or semi-enclosed seas such as the Caribbean information when evaluating the environmental rel-
and the Mediterranean Sea and in gyres [8, 64, 71, 126]. evance of test concentrations in studies on uptake and
Clear increases in the abundance of microplastics in effects of microplastics. For this reason, main focus is
seawater have been found over larger temporal scales. placed on studies reporting numerical concentrations per
Thompson et  al. [127] evaluated archived plankton water volume, sediment weight or sediment volume. As
samples collected with continuous plankton recorders outlined above, most data on the occurrence of micro-
in the northeast Atlantic at 10  m depth. Samples were plastics in the marine environment have been obtained
examined microscopically and unusual fragments were using visual selection and often also visual identifica-
identified by FT-IR. The concentration of microplastics tion of microplastics [11]; the results of quality controls
significantly increased from the 1960s and 1970s (approx. are only reported in some cases (e.g. [49, 110, 123]).
0.01 items/m3) to the 1980s and 1990s (approx. 0.04–0.05 Although data obtained by visually selecting and/or iden-
items/m3). Based on published data and own investiga- tifying small microplastics should be considered with
tions using a manta trawl and visual identification of care, they provide a first impression on the abundance
microplastics Goldstein et  al. [128] evaluated temporal of microplastics in marine systems and were, thus, not
changes in microplastic levels in the surface layer of the excluded from the present review. However, an attempt
North Pacific gyre. They found that between 1972–1987 was made to especially include recent publications using
and 1999–2010 the median numerical concentration of state-of-the-art sampling, extraction and identification
microplastics had increased by a factor of approx. 140 techniques (see Additional file  1: Table S1 for informa-
(from 0.003 to 0.425 items/m3) and the median mass tion on the used methods).
concentration by a factor of 1000 (from 0.003 to 3  mg/ As most consumer plastics are at least initially buoy-
m3). Law et al. [20] re-analysed the temporal trend using ant in seawater, the abundance of microplastics in the
a combined dataset including the data of Goldstein et al. sea surface layer, the upper approx. 20  cm of the water
[128] and their own data obtained by sampling using column, was addressed in many studies. Buoyant micro-
neuston nets and visual identification of small plastic and macroplastics have been found to accumulate in
items (typically mm-sized; see Additional file  1: Table the North Atlantic, South Atlantic, North Pacific, South
S1). To reduce the bias, which is caused by an increased Pacific and Indian Ocean gyre [65, 119, 128–130]. In the
sampling frequency in areas with high plastic levels in North Pacific gyre, mean abundance of visually identified
recent years, they calculated average concentrations plastic items (0.33  items/m2, mostly fragments, plastic
Duis and Coors Environ Sci Eur (2016) 28:2 Page 10 of 25

films and fibres with a size <5 mm) in 3 out of 11 samples during flooding occurs less frequently. In sediments from
was found to be higher than plankton abundance [119]. a beach on the East Frisian Island Norderney (Germany),
Based on the review of Hidalgo-Ruz et  al. [11] and the levels of microplastic particles (<1 mm) were low (mean
evaluated recently published studies (Additional file  1: values: 1.7, 1.3 and 2.3 particles/kg sediment dw). Due to
Table S1), concentrations of microplastics in the sea sur- background contamination with fibres, fibre content of
face layer range from 0 to 12.3 items/m2 [20] and from 0 the sediment was not evaluated [49].
to approx. 8700 items/m3 (i.e. 8.7 items/L [11]). A much Much higher concentrations of microplastics (at
higher abundance of synthetic polymer particles was least 2 dimensions  <5  mm) were found on beaches of
found in the sea surface microlayer, i.e. the upper 1 mm three Canary Islands [133]. They ranged from 1 to 30
of the water column (Additional file  1: Table S1). Mean (Fuerteventura), <1–109 (Lanzarote) and <1–90 g/L sedi-
abundance was 195  items/L for paint particles, mainly ment (La Graciosa). Low microplastic levels were found
alkyd and poly(acrylate/styrene) polymers and 16 items/L on rocky shores and on beaches being completely sub-
for non-paint microplastics [21]. merged at high tide (i.e. offering no space for deposition
In the water column below the sea surface layer, con- of plastics). Highest levels were recorded on the north-
centrations of microplastics can be expected to be lower ern coasts, which are reached by currents likely to trans-
than at the water surface. According to the evaluation of port plastic debris. Carson et  al. [134] detected partly
Hidalgo-Ruz et  al. [11], concentrations of microplastics extremely high levels of small plastic particles (<10 mm)
in the water column ranged from 0.014 to 12.5  items/ on southern Hawaii, on two beaches located close to the
m3. Considerably higher concentrations were detected North Pacific subtropical convergent zone. Kamilo beach
in a recent study [18] in the north-eastern Pacific and sediment contained on average 1.3 % (w/w) of small plas-
close to the coast of British Columbia (Canada). Con- tic particles. More than 50 % of the particles were found
centrations of microplastics in seawater sampled from in the upper 5  cm of the sediment, which contained on
a depth of 4.5  m ranged from 8 to 9180  items/m3. They average 3.3 % (w/w) of small plastics (the maximum value
were lowest at offshore sites in the north-eastern Pacific was 30  %). At Waikapuna beach, mean plastic content
(mean: 279 items/m3) and higher at nearshore sites was 0.03 %. Again, most plastic occurred in the top 5 cm
(1710–7630 items/m3). Approx. 75 % of the microplastics of the beach, where plastic content was 0.1 %. The plas-
were fibres; the percentage of fibres increased near the tic particles analysed by FT-IR mainly consisted of PE
shores. As noted by the authors, fibre content was under- (85  %) and PP (14  %). Elevated concentrations of small
estimated: brightly coloured brittle fibres were observed plastic particles (mean: 805 items/m2) were also found
in most samples, but could not be quantified since they on beaches on the Easter Islands [101]. Lee et  al. [102]
were eliminated during acid digestion. High concentra- recorded high microplastic levels (mean values: 8205
tions of microplastics (0.5  mm to approx. 5  mm) were items/m2 before and 27,606 items/m2 after the rainy sea-
also found in the Yangtze estuary in China [131]. In water son) on South Korean beaches close to the estuary of the
samples collected at 1  m depth, the average concentra- Nakdong River, which flows through a densely populated
tion of microplastics was 4137 items/m3. metropolitan area.
Coastal and, especially, subtidal sediments appear to Microplastic levels in subtidal sediments from har-
be sinks for microplastics [89, 115, 123]. As pointed out bours, coastal and offshore areas of the Belgian conti-
by Hidalgo-Ruz et  al. [11] microplastic concentrations nental shelf were investigated by Claessens et  al. [110].
in sediments tend to be much higher than those in the Harbour sediments contained significantly more micro-
sea surface layer and in the water column. Microplastics plastics (mean: 167  items/kg sediment dw) than coastal
have been detected in coastal sediments (in most cases (92  items/kg sediment dw) and offshore sediments
beaches) around the world [81, 99]. At some sites, they (105  items/kg sediment dw). In harbour sediments,
accounted for 80 % of the intertidal plastic debris [132]. fibres accounted for 40  % of the microplastics, granules
Microplastic levels vary greatly between beaches. for 34  %, plastic films for 4  % and PS spheres for 22  %.
Claessens et al. [110] and Van Cauwenberghe et al. [105] Microplastics in coastal and offshore sediments consisted
evaluated microplastics (≤1  mm) on Belgian beaches. of 68 % fibres, 30 % granules and 2 % plastic films. High
Claessens et al. [110] recorded an average concentration concentrations in harbour sediments were thought to
of 93 items/kg sediment dw with plastic fibres accounting be related to local input and to the fact that the studied
for 88 % of the microplastics, granules for 7 % and plas- harbour areas were partly enclosed. The analysed fibres
tic films for 5  %. Van Cauwenberghe et  al. [105] found consisted of PA, polyvinyl alcohol and PP, the granules of
a mean concentration of 13  items/kg sediment dw. In PS, PE and PP. Concentrations of microplastics (<1 mm)
both studies, highest microplastic levels were observed in sediments sampled at approx. 1 m depth in the Lagoon
at the high tide line, where resuspension of particles of Venice (Italy) were studied by Vianello et  al. [22].
Duis and Coors Environ Sci Eur (2016) 28:2 Page 11 of 25

Levels of microplastics ranged from 672 to 2175 items/ a municipal WWTP on microplastic levels was dem-
kg sediment dw. They were higher in the inner area of onstrated in North Shore Channel (Chicago, USA).
the lagoon, where water currents were low (i.e. more Mean microplastic concentration in the surface layer
sedimentation occurred). Most microplastics consisted increased from 1.94 items/m3 upstream of the WWTP to
of PE (48  %) or PP (34  %). Irregularly shaped fragments 17.93 items/m3 downstream of the WWTP [139]. In sedi-
accounted for 86  % of all microplastics, fibres for 11  %, ments from St. Lawrence River (Canada), plastic granules
films for 2 % and pellets/granules for 1 %. with diameters of 0.4–2.2  mm and mainly grey or black
In an early study using polarised light microscopy and colour were detected. Based on their melting point, it
semi-quantitative evaluation, Habib et  al. [92] found was assumed that the granules consist of PE. Personal
that abundance and size of textile fibres in subtidal sedi- care products were mentioned as possible source. How-
ments decreased with increasing distance from a WWTP. ever, highest concentrations (136,926  items/m2) were
Browne et al. [81] sampled subtidal sediments from two found in the effluent canal of a nuclear power plant, while
sites, where sewage sludge had been disposed, and two concentrations at the other nine sampling sites ranged
reference sites (Additional file  1: Table S1). Although from 0 to 243 items/m2 [140]. This suggests that the gran-
disposal of sewage sludge had been stopped more than ules may originate from a source other than personal care
10  years before, the former disposal sites contained 4 products that remains to be identified.
times (North Sea) and 2.5 times (English Channel) more In a preliminary study of microplastic (0.3–5  mm)
microplastics than the reference site. levels in the surface layer of Lake Geneva (Switzer-
Microplastics were also detected in deep sea sedi- land), a microplastic concentration of 0.048  items/m2
ments, e.g. in the northeast North Atlantic and south- was derived [141]. A similar mean microplastic level
west Indian Ocean and in the Mediterranean Sea at water (0.091 items/m2) was determined in six lakes located (or
depths between 300 and 3500  m [123]. The sediments partly located) in Switzerland [138]. Fragments, foams,
contained 28–800 microplastics/L. Notably, exclusively films and fibres were dominant. Microplastics (0.355 to
fibres were found. Likewise, fibres were the dominant approx. 5 mm) were also analysed in three of the Great
type of microplastics found in sediments from the Kuril- Lakes: Lake Superior, Lake Huron and Lake Erie [41].
Kamchatka Trench (northwest Pacific) at water depths The mean concentration in the surface layer of these
of 4869–5766 m. In addition, paint chips and fragments lakes was 0.043 items/m2; 81 % of all microplastics had
were recorded. The microplastics did not only occur in a size  ≤1  mm. The highest microplastics levels (0.463
the upper 2 cm of the sediment, but also in deeper sedi- items/m2) were detected in Lake Erie, downstream of
ment layers [124]. the cities of Detroit, Cleveland and Erie. Fragments, pel-
lets and foams were found most frequently. The parti-
Freshwater environment cles also included green, blue and purple spheres, which
So far, there are only relatively few studies on microplas- had a similar size, shape, colour and elemental compo-
tics in the freshwater environment. These studies have sition as microbeads from facial cleansers analysed by
focused on larger rivers and lakes, while there are no data Eriksen et  al. [41]. However, more specific information
on the occurrence of microplastics in smaller streams or on the abundance of the coloured spheres in the surface
lakes [72, 95, 111]. layer from the Great Lakes is not provided. Only slightly
During a 2-year survey, Lechner et  al. [68] evaluated lower levels of microplastics (0.355  mm to approx.
the abundance of small plastic items (0.5–20 mm) in the 5 mm) were recorded in the surface layer of Lake Hov-
surface layer of River Danube between Vienna (Austria) sgol, a large mountain lake in northern Mongolia [103].
and Bratislava (Czech Republic). In 2010, mean concen- Fragments, films and lines/fibres were the dominant
tration of small plastic items was 0.938 items/m3; 86 % of items. The average microplastic concentration was
these items were pre-production plastics. In 2012, plastic 0.0203 items/m2. Around the lake, there is no industry,
abundance was much lower (0.055  items/m3); pre-pro- and population density is low. Free et al. [103] assumed
duction plastics accounted for 31  % of these items. The that the complete lack of a waste management system
high levels of pre-production plastics in 2010 were appar- (waste is burned, buried or dumped) and of wastewater
ently caused by leakages in the pipe system of a plastic treatment are the causes for the relatively high micro-
producer and by a strong rain event, during which pel- plastic levels. Microplastic concentrations were high-
lets were washed into the Danube [135–137]. Recently, est in the most populated and most touristic part of
a similar mean microplastic concentration (0.29  items/ the lake. A parallel survey of macroplastic showed that
m3) was derived for the surface layer of the River Rhône household plastics (plastic bottles and bags) and fishing
[138]. The microplastics mainly consisted of fragments gear were the dominant macroplastic items at the lake
(40  %), foams (37  %) and fibres (14  %). A clear effect of shores.
Duis and Coors Environ Sci Eur (2016) 28:2 Page 12 of 25

In sediments sampled at the shores of the rivers Rhine Uptake of microplastics by organisms in the
and Main in Germany, microplastic concentrations of environment and trophic transfer
228–3763 items/kg dw (River Rhine) and 786–1368 Due to their low size, microplastics are ingested by a
items/kg dw (River Main) were recorded with PE, PP and variety of species ranging from protozoans to marine
PS being the dominant polymers [112]. mammals [7, 75, 143, 144]. Their uptake depends on
Imhof et  al. [142] evaluated levels of microplastics properties such as size, shape, density and colour. For
(<5 mm) in sediment samples from two beaches of Lake instance, low-density (i.e. buoyant) microplastics are
Garda (Italy). Microplastic concentration was much ingested by pelagic filter feeders, high-density microplas-
higher at the northern (1108 items/m2) than at the south- tics by benthic deposit feeders [7, 132, 145]. Many filter
ern lake shore (108 items/m2). This difference was attrib- feeding and deposit feeding organisms are indiscriminate
uted to the prevailing wind direction and the resulting feeders: they capture food of a suitable size without fur-
water circulation. PS, PE and PP particles were most fre- ther selection [9]. The following four sections provide an
quently found. With regard to the smallest microplastics overview of uptake, translocation within the body, excre-
(<500  µm), PA and polyvinyl chloride (PVC) were also tion and trophic transfer of microplastics as investigated
relevant. Most particles were classified as fragments; in laboratory studies with aquatic organisms. Afterwards,
signs of degradation/fragmentation were identified by field studies with aquatic organisms and studies with ter-
SEM. At beaches of six lakes in Switzerland, microplastic restrial organisms are discussed.
levels ranged from 20 to 7200 items/m2. Foam, fragments
and fibres were found most frequently [138]. Uptake by aquatic organisms
In laboratory experiments, ingestion of microplastics has
Terrestrial environment been demonstrated for a number of marine invertebrates
Although microplastics obviously enter the terrestrial including ciliates, cnidarians, rotifers, annelids, copep-
environment (e.g. due to littering and application of sew- ods, cladocerans, amphipods, mysids, euphausiids, bar-
age sludge to land) and soils have been assumed to be a nacles, mussels and tunicates [8, 127, 145–147] and fish
sink for microplastics, there are only extremely few data [148]. For example, Lee et al. [149] investigated the uptake
on microplastic concentrations in the terrestrial envi- of nano- (50  nm) and microsized (0.5 and 6  µm) fluores-
ronment [71, 72, 77]. It was suggested to use synthetic cently labelled PS spheres by the copepod Tigriopus japoni-
fibres as indicators of previous sludge application to land cus. Copepods were exposed for 24  h to concentrations
[92, 93]. Using polarised light microscopy, Zubris and of 9.1  ×  1014 (50  nm), 9.1  ×  1011 (0.5  µm) and 5.3  ×  108
Richards [93] showed that up to 15  years after sludge items/L (6  µm). Spheres of all three sizes were detected
application, levels of plastic fibres in soil of a long-term in the gut of the copepods. In the marine amphipod
experimental field site clearly exceeded levels at control Allorchestes compressa, which had been exposed for 72  h
sites. to a very high concentration (100 g/L) of PE microplastics
(11–700  µm), on average 19 particles per amphipod were
Summary: occurrence of microplastics in the aquatic detected [150]. Ingestion of microplastics was also dem-
and terrestrial environment onstrated in larvae of the sea urchin Tripneustes gratilla
As a consequence of their persistence and long-range held for 5  d at concentrations of 103–3  ×  105 items/L of
transport, microplastics are ubiquitous in the marine fluorescent PE microspheres (10–45  µm). At the highest
environment. Notably, beaches (where extremely high concentration up to 31  % of sea urchin larvae contained
levels have been recorded at some cases) and subtidal microplastics in their stomachs, at the lowest concentration
sediments appear to be sinks for microplastics. Based on up to 5 % (on average 1–2 microspheres per larva; [151]).
first investigations, microplastic levels in large rivers and In addition to being ingested, small microplastics might
lakes are similar to those in the marine environment. The also be taken up via the gills [8]. For mussels, it has been
occurrence of microplastics in smaller streams and lakes suggested that uptake via the gill surface (endocytosis)
and, especially, in the terrestrial environment remains to may be relevant for smaller microplastics, while larger
be investigated. particles are taken up via the digestive system ([152], see
In aquatic environments, fibres, fragments, granules, next section for further details on this study). In shore
films and styrofoam particles are the most commonly crabs (Carcinus maenas) exposed to PS microspheres
found particle types, while PE, PP and PS are the most (8–10  µm), exclusively via the ventilation route, micro-
frequently found polymers. Due to the lack of distinct spheres were detected on the gill surface but not in the
characteristics, it is generally not feasible to unequivo- gill tissue [153].
cally identify personal care products as source of micro- Uptake of microplastics by freshwater organisms has so
plastics detected in the environment. far only been addressed in relatively few studies. As to be
Duis and Coors Environ Sci Eur (2016) 28:2 Page 13 of 25

expected, the available data show that microplastics are microparticles were detected on the gill surface and
also ingested by freshwater organisms. Fluorescent PS in blood lacunae of the gills, as well as in the intestine,
microparticles (1 µm) were ingested by protozoans (Par- digestive gland and connective tissue.
amecium sp.) and Daphnia sp. [144]. Nano- (20 nm) and In a very recent study, mullets (Mugil cephalus) were
microsized (1 µm) fluorescent carboxylated PS spheres held for 7 days in water containing 33.8 mg/L of PE or PS
were taken up by neonates and adults of Daphnia magna particles with a size of 0.1–1 mm (nearly 2500 particles/L
[154]. Ground fluorescent polymethyl methacrylate par- [33]). Microplastics were not only found in the gastroin-
ticles (approx. 30  µm) were ingested by D.  magna, the testinal tract (approx. 10 PE particles and 90 PS particles
ostracod Notodromas monacha, the amphipod Gam- per fish), but also in the liver of the fish (approx. 1–2 par-
marus pulex, the snail Potamopyrgus antipodarum and ticles per fish for both PE and PS).
the oligochaete Lumbriculus variegatus [142]. Thus, based on the results of laboratory experiments,
translocation from the intestinal tract to the circulatory
Transfer from the intestinal tract to the surrounding system or surrounding tissue depends on the size of the
tissue or circulatory system microplastics with an upper size limit for translocation
After ingestion, microplastics can remain in the diges- that appears to be specific for the species or taxonomic
tive tract, be excreted or absorbed from the digestive group.
tract into the body tissue [132, 145]. Lugworms (Areni-
cola marina) exposed to sediment containing pre-pro- Excretion by aquatic organisms
duction PS particles (400–1300  µm, 7.4  % of sediment In laboratory experiments, microplastics, which had
dw) ingested these microplastics. However, no trans- only entered the organisms’ intestinal tract, were gener-
location of the relatively large PS particles from the gut ally excreted within hours or few days. Rapid excretion of
to the tissue was recorded [155]. Hämer et  al. [156] fed microplastics was e.g. reported for the copepod Euryte-
marine isopods (Idotea emarginata) with food contain- mora affinis [147]. After 3  h exposure to fluorescent PE
ing fluorescent PS microspheres (10  µm), PS fragments spheres (10 µm; 2 × 106 items/L), 67 % of the copepods
(1–100  µm) or acrylic fibres (0.02–2.5  mm). Micro- had ingested microspheres. Following a 12 h post-expo-
plastics were detected in stomach and intestine, but sure, only 4  % of the copepods still contained micro-
not in the midgut where nutrients are resorbed. Pas- spheres. In marine amphipods (A.  compressa), most
sage of the microplastics to the midgut was most likely ingested PE microplastics were excreted within 2 d [150].
impeded by filter structures in the isopods’ proventricu- Sea urchin larvae (T.  gratilla) egested PE microspheres
lus. In D. magna, fluorescent-carboxylated PS nano- and (10–45 µm) within 7 h [151].
microspheres (20  nm and 1  µm diameter) were mainly In cases, where microplastics had translocated to the
observed in the gastrointestinal tract, but also in struc- circulatory system and/or the surrounding tissues, excre-
tures assumed to be oil storage droplets. It was concluded tion was also demonstrated, but was slower. In shore
that the PS spheres are able to cross the gut epithelium crabs (C.  maenas), concentrations of fluorescent PS
[154]. In shore crabs (C.  maenas), which were fed with microspheres (0.5  µm) in the haemolymph decreased
mussels (Mytilus edulis) pre-exposed to PS microspheres, from 24  h to 21  days post-exposure. Yet, on day  21 the
translocation from the intestinal tract to haemolymph, haemolymph still contained a few microspheres [157]. In
hepatopancreas, ovary and gills was demonstrated for mussels (M. edulis), fluorescent PS microspheres (3.0 and
microspheres with 0.5  µm diameter [157]. By contrast, 9.6  µm) were—despite excretion with the faeces—still
larger microspheres (8–10  µm diameter) were only detected in the haemolymph 48 d post-exposure [144].
detected in the intestine but not in the haemolymph of
shore crabs [153]. Trophic transfer
Browne et al. [145] kept mussels (M. edulis) for 3 h in Several laboratory studies have demonstrated that micro-
a suspension of fluorescent PS microspheres (3.0 and plastics are transferred in the food chain, i.e. from prey to
9.6 µm; 4.3 × 104 items/L). Microspheres were detected predator. Trophic transfer of fluorescent PS microspheres
in the haemolymph and inside the haemocytes. The (10 µm) from zooplankton to the mysid shrimp Mysis rel-
smaller microspheres occurred in significantly higher icta was observed by Setälä et al. [147]. M. relicta, which
abundance in the haemolymph than the larger ones. Von had been kept together with zooplankton (copepods and
Moos et al. [152] exposed mussels for 3–96 h to 2.5 g/L of polychaete larvae) pre-exposed for 12 h to microplastics,
HDPE fluff consisting of non-uniformly shaped particles contained PS microspheres in their stomach. Trophic
with a size between 0 and 80  µm. The concentration of transfer of microplastics from mussels (M.  edulis) to
HDPE fluff corresponds to approx. 2.7 × 107 to 3.6 × 107 shore crabs (C.  maenas) was shown for fluorescently
items/L (NR von Moos, personal communication). HDPE labelled PS microspheres with 0.5 µm [157] and 8–10 µm
Duis and Coors Environ Sci Eur (2016) 28:2 Page 14 of 25

diameter [153]. So far, it is not known if microplas- identification of the particles as microplastic was possi-
tics biomagnify, i.e. if concentrations in the organisms ble. The authors assumed that this might be due to effects
increase at higher trophic level [158]. of the digestion procedure on the plastic matrix. Similar
microplastic concentrations were reported for M. edulis
Field studies with aquatic organisms collected at the French, Belgian and Dutch North Sea
The uptake of microplastics has also been investigated in coast [122], and slightly lower levels for Mediterranean
a number of field studies, mainly with marine organisms. mussels (Mytilus galloprovincialis) sampled in the estuar-
Note that in these studies no differentiation between ies of the rivers Tagus (Portugal) and Po (Italy) and in the
direct ingestion of microplastics and uptake with the Ebro delta (Spain [37]). A.  marina from the French and
food (i.e. trophic transfer) is possible. Belgian North Sea coast contained on average 1.2 micro-
Desforges et  al. [36] analysed microplastics in two plastic particles/g tissue [122].
zooplankton species, the copepod Neocalanus cristatus Plastic concentrations in the gut of small (up to 10 cm
and the euphausiid Euphausia pacifica, sampled in the standard length) pelagic fish in the North Pacific gyre
Northeast Pacific. On average, 0.03 microplastic items/ were studied by Boerger et al. [160]. Fish from six species
individual were found in N. cristatus, 0.06 in E. pacifica. were caught with manta trawls. Approx. 35 % of the fish
Goldstein and Goodwin [159] evaluated plastic inges- had plastic particles (on average 2 items) in their stom-
tion by gooseneck barnacles (Lepas anatifera, Lepas ach. Most of the ingested plastics were fragments (94 %)
pacifica, Lepas sp.), rafting organisms attached to floating and had a size of 1.0–2.8 mm. Lusher et al. [161] evalu-
substrates at the sea surface. Gooseneck barnacles were ated the plastic content in the gastrointestinal tract of 5
sampled from floating debris in the North Pacific gyre; pelagic and 5 demersal fish species caught in the English
microplastics in their stomachs and intestines were iden- Channel. All items, which were not classified as natu-
tified visually. Due to the possibility of airborne contami- ral prey of the fish, were analysed by FT-IR. Items con-
nation, fine microfibers were not considered. A subset of sisting of plastic or the semi-synthetic fibre rayon were
microplastic particles was analysed by Raman spectrom- found in 37 % of the analysed fish (on average 1.9 items/
etry. Microplastics were found in 34  % of the barnacles, fish). There was no significant difference in the number
with most barnacles having ≤5 particles in their intesti- of ingested items between pelagic and demersal species.
nal tract. Nearly all (99 %) particles were degraded frag- The ingested material mainly consisted of fibres (68  %),
ments (median diameter: 1.4  mm). No blockage of the fragments (16  %) and beads (12  %); 92  % of the items
stomach or intestine was recorded. Analysis by Raman were smaller than 5  mm, with particles of 1.0–2.0  mm
spectrometry revealed that 58  % of the particles con- size being most common. More than half of the items
sisted of PE, 5 % of PP and 1 % of PS (polymer type of the (58 %) were identified as rayon, 36 % as PA, 5 % as PES,
remaining particles could not be analysed). 1 % as PS, 0.3 % as PE and 0.3 % as acrylic. Polymers with
Van Cauwenberghe and Janssen [38] investigated levels a lower density were predominantly detected in pelagic
of microplastics in cultured mussels (M.  edulis) reared fish species, those with a higher density in demersal spe-
in the North Sea and Pacific oyster (Crassostrea gigas) cies. Microplastic particles (0.2–5 mm; due to the possi-
reared in the Atlantic. Mussels were either analysed bility of airborne contamination fibres were not included
directly for their microplastic content or kept for 3 days in in the evaluation) were found in the intestinal tracts of 5
filtered artificial seawater to allow clearing of the gut. Soft out of 7 fish species sampled in the North Sea. Overall,
tissues were digested in concentrated nitric acid, boiled, 2.6  % of the fish had ingested microplastics [34]. In an
diluted with deionised water and filtered (5 µm). Micro- analysis of the microplastic content in the gastrointesti-
plastics were identified microscopically, and a subset was nal tract of fish from five commercially used species sam-
analysed by micro-Raman-spectrometry. Samples were pled in the Adriatic Sea, microplastic items were found in
processed in a laminar flow cabinet; procedural controls 28 % of the fish (1–2 items/fish [33]).
were free of microplastics. In M. edulis, 0.36 microparti- Plastic items, including microplastics, have also been
cles per g soft tissue ww were detected without depura- shown to be ingested by seabirds and marine mammals.
tion. After the depuration period, 0.24 items/g soft tissue For instance, plastic content in the stomach of dead,
ww were found. In C.  gigas, 0.47 items/g soft tissue ww beach-washed northern fulmars (Fulmarus glacialis) is
were found before and 0.35 items/g tissue ww after depu- monitored in the context of the OSPAR ecological qual-
ration. As discussed by Van Cauwenberghe and Janssen ity objective for marine litter stating that less than 10 %
[38] tissue digestion by nitric acid and boiling may have of northern fulmars should have >0.1 g plastic particles
led to destruction of smaller microplastics and, hence, in their stomachs [162]. Fulmar stomachs were shown to
to an underestimation of microplastic levels in the mus- contain macro- and microplastics. However, the latter
sels. With micro-Raman-spectrometry, no unambiguous were not quantified separately [163, 164]. Microplastics
Duis and Coors Environ Sci Eur (2016) 28:2 Page 15 of 25

and small macroplastics (0.5–30 mm) were detected in Physical effects of microplastics


the scats (faeces) of fur seals (Arctocephalus tropicalis, Macroplastics physically affect marine organisms. Espe-
Arctocephalus gazella) on Macquarie Islands, between cially for air-breathing animals, entanglement may result
New Zealand and Antarctica [165]. Plastic particles in death. The ingestion of macroplastic items may reduce
were collected visually and analysed by SEM and FT-IR. the amount of consumed food and, consequently, the
Most scats contained 1 plastic item; particles mainly organisms’ fitness. Macroplastics can also block the intes-
consisted of PE and had a size between 2 and 5 mm. tinal tract and cause internal injuries [58, 75, 169–171]. It
Microplastics were also found in the digestive tract of has been assumed that microplastics cause similar effects
a whale (Mesoplodon mirus) stranded on the Irish coast in smaller organisms, mainly with regard to the physical
[166]. obstruction of feeding and digestion [6, 7, 71, 75]. Sharp-
Little information is available on the uptake of micro- edged microplastics may injure gill tissues and the intes-
plastics by freshwater organisms in the field. In a prelimi- tinal tract [7, 144]. In the following, the available data on
nary study, Sanchez et al. [167] examined wild gudgeons physical effects of microplastics on aquatic organisms are
(Gobio gobio), caught in French streams. The digestive summarised (see also Additional file 1: Table S3). While
tract of the fish was analysed visually for microplastics. studies dealing exclusively with effects of nanoplastics
Based on first results, 12  % of the gudgeons had micro- were not considered, results of comparative studies of
plastics in their intestine. The abundance of microplastics nano- and microplastics have been included.
increased with the anthropogenic impact on the rivers.
While no microplastics were found in the intestine of Physical effects of microplastics on marine organisms
fish captured at three sites characterised by a low anthro- To date, most studies were performed with marine inver-
pogenic influence, the highest percentage of fish with tebrates. In larvae of the sea urchin T.  gratilla exposed
microplastics in their intestine (approx. 20–30  %) was for 5  days to fluorescent PE microspheres (10–45  µm,
recorded at two sites in urban areas. 103–3  ×  105 items/L), effects were only observed at the
highest tested concentration. Body width was signifi-
Uptake and excretion by terrestrial organisms cantly lower than in the control; survival was reduced to
Very little information is available on the uptake of approx. 50 % of the control level, but this effect was not
microplastics by terrestrial organisms. Ugolini et al. [168] significant [151].
performed a laboratory study with the sand hopper Tali- In the marine copepod Centropages typicus, a 24-h
trus saltator, an amphipod inhabiting sandy coasts. In exposure to concentrations  ≥7  ×  106 items/L of fluo-
T. saltator, which had been fed with dry fish food mixed rescent PS microspheres (7.3  µm) led to significantly
with 10 % (w/w) of PE microspheres (10–45 µm), inges- reduced ingestion of algae [146]. Similarly, Calanus
tion of the microspheres was demonstrated. Within helgolandicus exposed for 24  h to PS spheres (20  µm,
24 h most microspheres were excreted, within a week all 7.5  ×  104 items/L) ingested 11  % less algae than the
microspheres. controls. In addition, exposed copepods preferentially
ingested smaller algae. During a 6-day exposure of C. hel-
Summary: uptake and trophic transfer golandicus to the same type and concentration of PS
A wide variety of aquatic organisms have been shown spheres, egg production was not significantly affected,
to ingest microplastics. In most cases, particles were but egg size was reduced during the second half of expo-
only detected in the intestinal tract and excreted rapidly. sure. This effect was attributed to energy depletion [172].
Translocation from the intestinal tract to the circulatory In 96-h acute tests, survival of adults and nauplii of the
system or surrounding tissues was observed in some spe- copepod T. japonicus was not affected by nano- (50 nm)
cies for very small microplastics. In field studies, micro- and microsized (0.5 and 6 µm) PS spheres at concentra-
plastics were ingested, but the ingested quantities were tions up to 1.1 × 1015 (50 nm), 1.1 × 1012 (0.5 µm) and
low. Microplastics are transferred in the food chain. Yet 6.6 × 108 items/L (6 µm). Chronic effects of these three
so far, there are no data demonstrating their bioaccumu- sizes of PS spheres were studied in a two-generation test
lation or biomagnification. with T. japonicus. The nanosized (50 nm) spheres led to
a significant reduction in survival of the first (F0) and the
Effects of microplastics on the environment second generation (F1) at concentrations  ≥4.6  ×  1012
Microplastics may have very different types of effects items/L. In F0 and F1, the development from nauplius
on the environment: they may physically (mechanically) to copepodid was delayed at 4.6  ×  1012 items/L (see
affect organisms, act as vectors for hydrophobic pollut- also Additional file 1: Table S3). For both sizes of micro-
ants and as substrates for organisms, and affect sediment spheres, the pattern of toxicity was different. The 0.5-µm
properties. microspheres caused an increased development time
Duis and Coors Environ Sci Eur (2016) 28:2 Page 16 of 25

(both from nauplius to copepodite and from nauplius to In a water/sediment study, lugworms (A. marina) were
adult) and a reduced survival of the F1 at the highest con- exposed for 28 days to sediment containing unplasticised
centration (9.1 × 1010 items/L). The 6-µm microspheres, PVC (uPVC) granules (mean size: 130  µm; 5, 10 and
for which the highest concentration contained 5.2 × 107 50  g uPVC/kg sediment ww). During the first 2  weeks
items/L, had no effect on survival and development of of exposure, feeding rate of lugworms was significantly
both copepod generations. However, microspheres of reduced at 50  g/kg  sediment ww. However, during the
both sizes significantly reduced fecundity of the F0 and third and fourth week of exposure, feeding rate in the
the F1 at all tested concentrations, i.e. the lowest observed controls decreased to levels close to those observed at
effect concentration (LOEC) was ≤4.6 × 108 items/L for 50 g/kg ww. No clear effect on feeding was seen at 5 and
the 0.5 µm spheres and ≤2.6 × 105 items/L for the 6 µm 10 g/kg ww. Phagocytic activity of coelomic fluid was sig-
spheres. The effects on fecundity may have been a conse- nificantly increased at 5 and 50, but not at 10  g/kg  ww.
quence of a reduced quantity of ingested food associated At 10 and 50  g/kg  ww, total available energy reserves
to the presence of larger amounts of ingested micro- were significantly lower than in the controls. Yet, weight
spheres [149]. It is well known that reduced growth often of the uPVC exposed worms at the end of the experi-
leads to a reduced fecundity [173–175]. ment did not significantly differ from the control value.
In juveniles of the marine isopod I.  emarginata fed In a second experiment, A. marina was exposed for 51 h
for 6–7  weeks (2  moult cycles) with agar-based food to 50  g  uPVC/kg  ww. The frequency of egestion events
containing seaweed powder and fluorescent micro- (evaluated during the last 3  h of exposure) was signifi-
spheres (10 µm, approx. 12 items/mg food), PS fragments cantly reduced at 50  g/kg  ww. In a further experiment,
(1–100  µm, 20 fragments/mg food) or acrylic fibres lugworms were exposed for 7 days to sediment with 10,
(0.02–2.5  mm, 0.3  mg/g food), no significant effects on 50 and 100  g silica/kg  ww. Since exposure to silica did
survival, growth and duration of the intermoult period not significantly affect the number of faecal casts, the
were recorded [156]. reduced organic content did not appear to be the cause
Mussels (M. edulis) were exposed for 3 h to fluorescent for the reduced feeding activity. It was assumed that the
PS microspheres (3.0 and 9.6 µm, 4.3 × 104 items/L) and reduced egestion frequency of the worms at 50 g uPVC/
then transferred to control water. Effects on their feed- kg  ww might be due to a lower feeding activity or a
ing rate, and on haemocyte viability, phagocytic activ- reduced uptake efficiency, possibly caused by reduced
ity of the haemocytes and ability of the haemocytes to adhesion of uPVC particles (as compared to sediment) to
cope with oxidative stress were evaluated 3–48  days the feeding apparatus of A. marina [177].
after transfer to control water. Neither the 3.0  µm nor In a recent 14-days water/sediment test with A. marina
the 9.6 µm microspheres had any significant effect on the exposed to PS microspheres (1.1  ×  105 items/kg sedi-
evaluated endpoints [145]. Von Moos et al. [152] exposed ment) with diameters of 10, 30 and 90 µm, protein con-
M.  edulis for 3–96  h to 2.5  g/L (approx. 2.7  ×  107 to tent of the exposed lugworms was significantly increased,
3.6 × 107 items/L, see above) of HDPE fluff (0–80 µm). In but the overall energy budget was not affected [39]. The
exposed mussels, granulocytoma formation (indicating shorter exposure duration and the more regular form of
an inflammatory response) was significantly increased, the microplastics in this study [39] have probably con-
and lysosomal membrane stability was significantly tributed to the difference between the results of the two
reduced. No effects were recorded on the condition water/sediment studies. In addition, the LOEC of 10 g/
index, the neutral lipid content and the accumulation of kg  sediment ww obtained in the 28-days test [177] cor-
lipofuscin (a biomarker of oxidative stress) in the diges- responds to a numerical concentration of roughly
tive tract. A 14-day exposure of M. edulis to PS micro- 8  ×  105  items/kg sediment ww (see Additional file  1:
spheres (1.1 × 105 items/L) with diameters of 10, 30 and Table S3), i.e. a higher concentration than used in the
90  µm led to a significant increase in energy consump- 14-days test [39].
tion, but did not significantly affect the overall energy
budget of the mussels [39]. Physical effects of microplastics on freshwater organisms
Acute effects of PE microspheres (1–5  µm) were So far, very few data are available on effects of micro-
studied in juveniles of common goby (Pomatoschistus plastics on freshwater organisms. Rochman et  al. [178,
microps). After 96  h exposure to two concentrations of 179] performed a study with Japanese medaka (Ory-
microspheres (18.4 and 184  µg/L), acetylcholinesterase zias latipes) to evaluate the uptake of contaminants
activity was significantly reduced (to approx. 80 % of the from microplastics into fish and resultant effects (see
control level), while survival and other biomarkers (see next section). This study included a treatment with vir-
Additional file 1: Table S3) were not affected [176]. gin microplastics (pre-production LDPE pellets ground
Duis and Coors Environ Sci Eur (2016) 28:2 Page 17 of 25

to <500 µm). Fish were fed for 2 months at a rate of 2 % phenanthrene reached much higher equilibrium con-
bodyweight per day with a diet containing 10  % (w/w) centrations on PE than on PP and PVC granules (200–
virgin microplastics. This diet was prepared by reducing 250 µm): distribution coefficients (Kd) are 38,100 L/kg for
the dextrin content of the food and, instead, adding the PE, 2190  L/kg for PP and 1650  L/kg for PVC. These Kd
microplastics. Consequently, it had a lower energy den- values are much higher than those for sorption of phen-
sity than the control diet. An appropriate negative con- anthrene to two sediments (19 and 135 L/kg). However,
trol receiving food with the same energy density as the when normalising distribution coefficients to the organic
fish exposed to microplastics would have been desir- carbon content of plastics and sediments (i.e. when com-
able (see e.g. [180]) but was not included. Survival of the paring KOC rather than Kd values), differences between
fish receiving the microplastics-containing diet was not plastics and sediments are strongly reduced. The KOC for
affected. However, 46 % of these fish exhibited severe gly- sorption of phenanthrene to PE granules (44,500  L/kg)
cogen depletion in the liver. This effect, which was not is by a factor of 2–4 higher than those for the sediments
observed in the controls, was most likely caused by the (10,400 and 20,100 L/kg), while the KOC values for PP and
reduced energy content of the microplastics-contain- PVC granules (2560 and 4340 L/kg) are lower than those
ing food. Following exposure to microplastics, the inci- derived for the sediments [182]. For PCBs, Velzeboer
dence of fatty vacuolar degeneration in medaka liver was et al. [183] also found a similar magnitude of sorption to
slightly increased, while gonad histology was not affected. microplastics (PE microspheres of 10–180 µm size) and
The microplastic treatment had no significant effect on sediment organic matter.
expression of cyp1a, vitellogenin  I and oestrogen recep-
tor α in male and female fish, and on expression of cho- Transport of pollutants sorbed to microplastics
riogenin  H in male fish. In female fish, choriogenin  H Since microplastics can be transported over long dis-
expression was significantly reduced after 2  months tances, it has been proposed that they may function as
exposure, an effect interpreted by Rochman et  al. [179] vectors for sorbed hydrophobic pollutants. Such pollut-
as early warning sign of endocrine disruption. However, ants might e.g. be transported to remote sites as the Arc-
in view of the lower energy density of the microplastics- tic [121, 182]. The relevance of marine plastics (including
containing food it appears likely that the reduced chori- both micro- and macroplastics) as transport vectors for
ogenin expression is an effect of the glycogen depletion PCBs, PBDEs and perfluorooctanoic acid (PFOA) to the
described above, i.e. should not be considered as endo- Arctic was evaluated by Zarfl and Matthies [121]. Based
crine disruption as defined in [181]. Unfortunately, Roch- on estimated amounts of plastics and pollutants in the
man et al. [178, 179] do not provide any information on oceans, sorption of the pollutants to plastics, and ocean
effects of the microplastics treatment on fish growth. current velocities they derived a rough estimate of plas-
tic-mediated mass fluxes of PCBs, PBDEs and PFOA.
Summary: physical effects of microplastics These mass fluxes were by factors of 103–106 lower than
Physical effects on marine organisms were shown to mass fluxes via atmospheric transport and transport with
occur at high concentrations of microplastics. The water. Therefore, it was concluded that for most sub-
observed effects appear to be mainly due to the inges- stances, plastics are no relevant vectors for transport to
tion of microplastics leading to a reduced uptake of food, the Arctic. Yet, plastic-mediated transport might increase
which in turn results in lower energy reserves and asso- the mobility of highly hydrophobic substances, which are
ciated effects on other physiological functions. Studies due to their sorption to sediment quickly removed from
on possible toxic effects of microplastics on freshwater the water column.
organisms are scarce, effects on terrestrial biota have so
far not been investigated [72, 77]. Uptake of pollutants sorbed to microplastics
and resultant effects
Microplastics as vectors for pollutants Given that (1) concentrations of pollutants on microplas-
Sorption of pollutants to microplastics tics can be several orders of magnitude higher than in the
Hydrophobic organic pollutants sorb to microplastics, surrounding water and (2) microplastics are ingested by
which are hydrophobic and have a large surface to vol- a wide variety of organisms, it has been postulated that
ume ratio. There is clear evidence that contaminants such microplastics may lead to an increased uptake of pol-
as hexachlorinated hexanes, polycyclic aromatic hydro- lutants by aquatic organisms (see e.g. [25]). Such an
carbons (PAHs), polychlorinated biphenyls (PCBs) and uptake requires desorption of the contaminants in the
polybrominated diphenyl ethers (PBDEs) are enriched on organisms. Addition of the digestive surfactant sodium
microplastics [11, 14, 56, 62, 71]. Sorption and desorp- taurocholate was shown to enhance desorption of phen-
tion processes depend on the polymer type. For instance, anthrene from PE, PP and PVC microplastics [182].
Duis and Coors Environ Sci Eur (2016) 28:2 Page 18 of 25

Similar results were obtained by Bakir et  al. [184] for choriogenin  H and oestrogen receptor  α was slightly
various organic pollutants sorbed to PE and PVC micro- lower than in fish fed with virgin microplastics and signif-
plastics. Several studies have demonstrated that con- icantly lower than in the control fish. These effects were
taminants, which had been sorbed to microplastics, are considered as indicators of endocrine disruption [179],
transferred to organisms ingesting these microplastics. but are most likely related to the observed energy deple-
For instance, nonylphenol and phenanthrene that had tion. In this context, it is of note that reduced vitellogenin
been sorbed to PVC microplastics were detected in the levels can only be interpreted as indicator for endocrine
tissue of A. marina exposed for 10 days to these micro- activity, if there is no systemic toxicity [186].
plastics [185].
Besseling et  al. [155] exposed A. marina for 28 d to Relevance of microplastics as vector for pollutants
sediment contaminated with low PCB concentrations As outlined above, there is clear evidence that hydro-
(5.28  µg PCBs/kg dw)—either alone or in combination phobic contaminants are enriched on microplastics and
with pre-production PS particles (400–1300  µm; 0.074, transferred to organisms ingesting these microplastics.
0.74 and 7.4  % of sediment dw) previously equilibrated However, it has been questioned, if the transport of
for 6 weeks with the sediment. In the presence of 0.074 % sorbed pollutants by microplastics is a relevant factor
PS particles, PCB concentrations in A.  marina were by contributing to accumulation and adverse effects in the
a factor of approx. 1.1–1.5 higher than in PCB-contam- environment, i.e. if microplastics transport pollutants in
inated sediment without microplastics. At 0.74 and 7.4 % sufficiently high concentrations to biota [99, 187]. In this
PS particles, PCB concentrations in the worms were context, the contribution of the uptake via microplastics
lower than with 0.074 % PS, but remained in most cases to the total uptake of a pollutant (including uptake via
above levels in the PCB-contaminated sediment without integument, gills and food) has to be considered. Since
microplastics. The authors concluded that PS micropar- microplastics are in most cases excreted by the organ-
ticles had a relatively limited effect on uptake of PCBs by isms that have ingested them, desorption rates of the
A.  marina. Feeding activity of the lugworms decreased pollutants from the microplastics in the intestinal tract
with increasing microplastics content. Worms in all are important. Modelling approaches have been used to
treatments lost weight, and weight loss increased with assess the relative contribution of microplastics as vec-
increasing microplastics concentration. It was suggested tors to the overall uptake of hydrophobic organic pollut-
that ingestion of the relatively large microplastic parti- ants by A. marina [187, 188] and piscivorous fish [104].
cles might have led to physical stress. In addition, organic Koelmans et  al. [187, 188] developed a biodynamic
matter content of the sediment was reduced in the pres- model for PCB accumulation by A.  marina in an envi-
ence of microplastics, i.e. the worms had to ingest larger ronment containing PS and PE microparticles. Differ-
amounts of sediment. ent uptake processes and desorption in the intestinal
Rochman et  al. [178, 179] performed a two-month tract were considered. Bioaccumulation of various PCBs
experiment with adult medaka (O. latipes) that received was modelled in the presence of three concentra-
control food, or food containing virgin microplastics (see tions (0.1, 1 and 10  % of sediment dw) of microplastics
previous section) or contaminated (‘marine’) microplas- (approx. 1  mm) and in the absence of microplastics. PS
tics. The latter were prepared by exposing pre-produc- microparticles had no significant effect on bioaccumula-
tion LDPE pellets for 3  months at a marine site. Pellets tion of PCBs in lugworms. For PE, the model predicted
were then ground to  <500  µm and incorporated into a decrease in steady-state bioaccumulation for PCBs
fish food. The diets containing microplastics (10 % w/w) with log KOW values  >5–6. When tissue concentrations
had a lower energy density than the control diet. At the increase to levels typical for substances with such high
end of exposure, levels of PAHs, PCBs and PBDEs in KOW, the gradient between concentrations in tissue and
fish that had received marine microplastics were higher on the ingested PE microparticles may become negative.
than in the control and in the virgin microplastic treat- Consequently, PCBs may be resorbed to the microplas-
ment. Marine microplastics had no significant effect on tics, i.e. bioaccumulation is attenuated. Based on these
survival and expression of cyp1a. However, they caused results, Koelmans et  al. [187] concluded that the con-
more pronounced histopathological changes in the liver tribution of microplastics to bioaccumulation can be
than virgin microplastics: 74  % of the fish exposed to assumed to be not very relevant.
marine microplastics exhibited severe glycogen depletion Similar results were obtained by Gouin et al. [104] with
(virgin microplastics: 46  %), 47  % fatty vacuolar degen- two modelling approaches. Using an equilibrium parti-
eration (virgin microplastics: 29  %) and 11  % single cell tioning model significant (>1  %) partitioning to plastics
necrosis (virgin microplastics: 0 %). In female medaka fed was only predicted for environments with very high plastic
with marine microplastics, the expression of vitellogenin, concentration and limited natural organic matter. Based
Duis and Coors Environ Sci Eur (2016) 28:2 Page 19 of 25

on the steady-state food-web component of the bioac- of plastic particles was higher than mean grain size of the
cumulation model of Arnot and Gobas [189], into which sediment. At 15.9 and 29.4 % (w/w) plastics, water perme-
10 % PE microplastics were included as additional compo- ability was significantly increased. With increasing plastic
nent of the diet, a reduced bioaccumulation was obtained content, sediments warmed more slowly. A 16 % decrease
for substances with log KOW values between 5.5 and 6.5. in heat transfer was recorded at the highest plastic con-
As outlined above, this reduction is due to the high affin- centration. Possible implications of such effects on physi-
ity of the microplastics to the pollutants, which prevents cal properties of sediments remain to be investigated.
transfer of the pollutants to the fish. Gouin et  al. [104]
concluded that microplastics have a limited relevance as Do microplastics cause environmental risks?
vector for the transfer of hydrophobic pollutants to fish. A In the context of risk assessment, polymers are—given
number of uncertainties were identified, which include the their high molecular weight—generally considered as
effects of fouling on sorption of pollutants to microplas- being of low concern. It is of note that, for this reason,
tics, gut retention times of microplastics and uptake rates registration and evaluation of polymers under REACH
of microplastics into the tissue of an organism. is usually not required unless triggered by certain addi-
tives [15]. As a first estimate of possible concern for the
Microplastics as substrates for organisms environment, the highest measured levels of microplas-
Many marine organisms live attached to debris [190, tics in the environment, which were identified based on
191]. Due to plastics, the amount of floating debris in Hidalgo-Ruz et  al. [11] and selected recent publications
the oceans has greatly increased [190]. This is most rel- (Additional file  1: Table S1), are compared to the con-
evant in the open ocean, where only very limited float- centrations of microplastics, which were shown to cause
ing substrate is available [128, 192]. Plastic debris is physical effects in laboratory tests. In the surface layer
often colonised by microorganisms and—depending on and the water column of the oceans, maximum concen-
its size—also by larger organisms. PE microplastics and trations of 9 [11] and 10 items/L [18], respectively, were
small macroplastics collected in the surface layer of the found. These concentrations are by a factor of approx. 104
North Atlantic were colonised by a variety of organisms lower than the acute LOEC of 3 × 105 items/L [151] and
including bacteria, cyanobacteria, diatoms, ciliates and the chronic LOEC of ≤2.6 × 105 items/L [149] obtained
radiolaria [191]. Bryozoans were identified on 3–5  mm- for marine invertebrates exposed via the water phase.
sized microplastics sampled in the surface layer at differ- Note that in the chronic test [149] a clear effect was
ent sites around Australia [193]. Microplastic particles observed at the lowest tested concentration (Additional
are also used as oviposition sites by the sea skater Halo- file  1: Table S3), i.e. significant effects may be caused at
bates, an insect living at the sea/air interface in the open a lower microplastic level. The highest microplastic con-
ocean [128, 192]. The strong increase in microplastics centrations measured in subtidal sediments, 2175 items/
in the North Pacific gyre, which was observed between kg dw in the lagoon of Venice [22] and 3600  items/kg
1972–1987 and 1999–2010, was associated with a con- dw in the Rhine estuary [89], are lower than the LOEC
siderable increase in the number of eggs, juveniles and of 10  g/kg sediment ww (1  %  w/w [177]) derived in a
adults of Halobates sericeus. Possible effects of the water/sediment test with marine polychaetes, which
increased abundance of H. sericeus on other species have corresponds to a numerical concentration of roughly
so far not been investigated [128]. 106 items/kg sediment dw (Additional file 1: Table S3). In
Given that plastics can be transported over long dis- beach sediments, maximum levels of 109 g microplastic
tances, they may contribute to the dispersal of species items/L (on the Canary Island Lanzarote [134]) and 30 %
[75, 190]. This includes invasive species [190] and species (w/w) small plastic particles (in the upper layer of Kamilo
causing harmful algal blooms [194]. Due to their low size, beach, Hawaii [133]) were determined. These values are
microplastics may especially facilitate transport of micro- higher than the LOEC obtained in the water/sediment
organisms (including pathogens) and other very small test mentioned above (no toxicity data for organisms
organism. So far, it is not known if the transport of spe- inhabiting beaches are available).
cies with microplastics has any significant effect on spe- It should be noted that to date only relatively few stud-
cies assemblages [158, 195]. ies are available on the effects of microplastics in marine
organisms and even fewer on those in freshwater organ-
Effects of microplastics on sediment properties isms. In several cases, only single concentrations were
Carson et al. [134] used artificially constructed beach sed- tested and threshold concentrations, below which no
iment cores containing 1.5, 7.3, 15.9 and 29.4 % (w/w) of significant effects are observed in the respective test
small plastic particles (<10  mm) to investigate effects on organisms, were not determined (Additional file 1: Table
water permeability and heat transfer. Notably, mean size S3). Effects on terrestrial organisms have so far not been
Duis and Coors Environ Sci Eur (2016) 28:2 Page 20 of 25

studied at all. Furthermore, microplastics are a very het- the overall amount of microplastics in the environment is
erogeneous group of particles differing e.g. in size, shape, of minor relevance. Abrasion and fragmentation of larger
chemical composition and specific density. Little is plastic items and of materials containing synthetic poly-
known on the influence of these factors on the effects of mers have been considered as much more relevant.
microplastics [196]. Based on the evaluated data, the lowest concentrations
In addition, there are a number of knowledge gaps eliciting adverse effects in aquatic organisms exposed
concerning fate and occurrence of microplastics in the via the water are by a factor of approx. 104 higher than
environment. Little information is available on fragmen- maximum microplastic concentrations found in marine
tation and degradation rates of macro- and microplastics. waters. The effect concentration in a water/sediment test
Due to methodological limitations, size distributions in with lugworms is higher than microplastic levels meas-
the environment are only partly known, especially with ured in subtidal sediments but in the same range as high-
regard to the smallest microplastics and nanoplastics est levels recorded in beach sediments.
[8, 11, 99, 196]. While there are many studies on micro- Before we are able to perform a comprehensive assess-
plastic abundance in the marine environment, data on ment of possible environmental risks caused by micro-
the occurrence of microplastics in freshwater systems plastics, a number of data gaps (e.g. fate and effects in
are limited. Information on possible hotspots and sinks freshwater and soil, and size distributions in all envi-
is missing [97]. For the terrestrial environment, there are ronmental compartments) need to be filled and avail-
nearly no data on the occurrence of microplastics. These able environmental risk assessment procedures have to
data gaps need to be filled prior to being able to perform be adapted. However, given that (1) very high concen-
a comprehensive assessment of possible environmental trations of microplastics have already been observed at
risks caused by microplastics. some sites (especially in sediments and on beaches), (2)
Moreover, a number of possible effects of microplas- plastics are extremely persistent in the environment, (3)
tics on the environment are not covered by current envi- microplastics in the environment originate from a mul-
ronmental risk assessment procedures, which have been titude of sources and (4) the abundance of microplastic
developed for chemical substances. These include poten- is expected to further increase due to fragmentation of
tial effects on sediment properties, and the function of the macroplastic present in the environment, strategies
microplastics as vector for the transport of pollutants, should be developed to address the issue of nano-, micro-
invasive species or pathogens. Assessment factors, which and macroplastics in the environment on a broad and
have been derived for the environmental risk assessment global basis in order to avoid exceeding critical environ-
of chemicals, may not be appropriate for microplas- mental threshold concentrations.
tics. For these reasons, assessing possible environmen-
tal risks caused by microplastics is not straightforward. Additional file
An approach that enables a comprehensive assessment
of possible environmental risks caused by microplastics Additional file 1: Table S1. Overview of ranges and mean or median
values (underlined) of concentrations of microplastics (or, where specified,
remains to be developed [14, 97]. As suggested by Syberg small plastic particles) in the marine environment based on Hidalgo-Ruz
et  al. [196], such an approach should build on frame- et al. [11] and selected recent publication. Table S2. Overview of ranges
works, which have been developed for assessing environ- and mean or median values (underlined) of concentrations of microplas‑
tics (or, where specified, small plastic particles) in the freshwater environ‑
mental risks of nanomaterials and mixtures. ment. Table S3. Overview of effect concentrations derived in ecotoxicity
It should be pointed out that based on available infor- tests with aquatic organisms exposed to microplastics.
mation microplastics are extremely persistent. For this
reason and due to the fragmentation of macroplastic
Authors’ contributions
debris, which is abundant in the environment, concentra- KD developed the concept for the literature review, performed literature
tions of microplastics in the environment will increase search and evaluation and drafted the manuscript. AC contributed to devel‑
at least as long as the release of plastics to the environ- oping the concept for the review, discussing the main findings and amending
the draft manuscript. Both authors read and approved the final manuscript.
ment is not stopped [8, 25, 99]. In this context, the high
concentrations in coastal sediments, which have been
recorded at some sites [133, 134], are of specific concern. Acknowledgements
The authors would like to thank M. Weil (ECT) for valuable comments on
the manuscript. The present study was funded by the German Cosmetic,
Conclusions Toiletry, Perfumery and Detergent Association (IKW). The opinions and views
As a result of the widespread use of plastics there are expressed in this manuscript do not necessarily reflect those of the IKW.
a great number of sources of primary and secondary Competing interests
microplastics in the environment. First estimates indi- The present study was funded by the German Cosmetic, Toiletry, Perfumery
cate that the contribution of personal care products to and Detergent Association (IKW).
Duis and Coors Environ Sci Eur (2016) 28:2 Page 21 of 25

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