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Review

Behavior of microplastics and plastic film residues in the soil environment: A

critical review

Qi Ruimin, Davey L. Jones, Li Zhen, Liu Qin, Yan Changrong

PII: S0048-9697(19)34713-8
DOI: https://doi.org/10.1016/j.scitotenv.2019.134722
Reference: STOTEN 134722

To appear in: Science of the Total Environment

Received Date: 18 July 2019

Revised Date: 23 September 2019
Accepted Date: 27 September 2019

Please cite this article as: Q. Ruimin, D.L. Jones, L. Zhen, L. Qin, Y. Changrong, Behavior of microplastics and
plastic film residues in the soil environment: A critical review, Science of the Total Environment (2019), doi: https://
doi.org/10.1016/j.scitotenv.2019.134722

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Behavior of microplastics and plastic film
residues in the soil environment: A critical
review

Qi Ruimina, Davey L. Jonesb,c, Li Zhena, Liu Qina, Yan Changronga,*

aInstitute of Environment and Sustainable Development in Agriculture, Chinese

Academy of Agricultural Sciences, Beijing 100081, P.R. China/Key Laboratory of

Prevention and Control of Residual Pollution in Agricultural Film, Ministry of

Agriculture and Rural Affairs, Beijing 100081, P.R. China

bSchool of Natural Sciences, Bangor University, Bangor, Gwynedd, LL57 2UW, UK

cSoilsWest, UWA School of Agriculture and Environment, The University of Western

Australia, Perth, WA 6009, Australia

* Corresponding author. E-mail address: [email protected] (Yan Changrong).

Postal address:

Institute of Environment and Sustainable Development in Agriculture, Chinese Academy of

Agricultural Sciences, Beijing 100081, P.R. China/Key Laboratory of Prevention and Control of

Residual Pollution in Agricultural Film, Ministry of Agriculture and Rural Affairs, Beijing 100081,

P.R. China

Tel.: +86-10-82106018; fax: +86-10-82106018

E-mail address: [email protected] (Yan Changrong)

Behavior of microplastics and plastic film
residues in the soil environment: A critical
review
Qi Ruimina, Davey L. Jonesb,c, Li Zhena, Liu Qina, Yan Changronga,*

aInstitute of Environment and Sustainable Development in Agriculture, Chinese

Academy of Agricultural Sciences, Beijing 100081, P.R. China/Key Laboratory of

Prevention and Control of Residual Pollution in Agricultural Film, Ministry of

Agriculture and Rural Affairs, Beijing 100081, P.R. China

bSchool of Natural Sciences, Bangor University, Bangor, Gwynedd, LL57 2UW, UK

cSoilsWest, UWA School of Agriculture and Environment, The University of Western

Australia, Perth, WA 6009, Australia

* Corresponding author. E-mail address: [email protected] (Yan Changrong).

Abstract: It is now widely acknowledged that microplastic pollution represents one of the greatest

anthropogenically mediated threats to Earth-system functioning. In freshwater and marine

ecosystems the presence of large amounts of microplastic appears almost ubiquitous, with frequent

reports of negative impacts on aquatic health. In contrast, however, the impact of plastic in terrestrial

environments remains poorly understood. In agroecosystems, microplastics (particles < 5 mm) can

enter the soil environment either directly (e.g. from biosolids application, irrigation water,

atmospheric deposition), or indirectly through the in situ degradation of large pieces of plastic (e.g.

from plastic mulch films). Although we have encouraged the use of plastics over the last 50 years

in agriculture to promote greater resource use efficiency and food security, the legacy of this is that

many soils are now contaminated with large amounts of plastic residue (ca. 50-250 kg ha-1). Due to
difficulties in separating and quantifying plastic particles from soil, our knowledge of their

behaviour, fate and potential to transfer to other receptors (e.g. surface and groundwater, air) and

enter the human food chain remains poor. This information, however, is critical for evaluating the

risk of soil-borne microplastic pollution. In this critical review, we systematically summarize (i) the

distribution and migration of microplastics in soils, (ii) highlight the separation, extraction, and

identification methods for monitoring microplastics in soils, (iii) discuss the ecological effects and

pollution mechanisms of soil microplastics, (iv) propose mitigation strategies to help prevent and

reduce microplastic pollution, and (v) identify the most important future challenges in soil

microplastics research.

Keywords: Environmental risk, Nanoplastics, Soil heath, Mulching film, Plasticizer.

1. Introduction
Microplastics have often been defined as particles smaller than 5 mm in size. These mainly

originate from tiny plastic particles (such as abrasives in detergents and cosmetics) that are released

directly into the environment, or indirectly from the degradation of large piece plastics (such as

plastic film, household garbage, atmospheric deposition, and vehicle emissions) (Andrady, 2011;

Cole et al., 2011; Gesamp, 2015). Microplastics are now recognized as an important environmental

pollutant, being almost ubiquitous in the atmosphere, water, soil, and other environmental media.

Due to their small particle size and very slow biodegradation rate they can be easily absorbed by

organisms and subsequently transported through food webs (Horton et al., 2017a; Hurley and

Nizzetto, 2018; Liu et al., 2018; Rillig, 2012). In addition, they may act as a vector for other

contaminants (e.g. human pathogens, organic pollutants, heavy metals). For these reasons,

microplastic pollution was recently listed as one of the top 10 environmental problems by the United
Nations Environment Programme (UNEP, 2014). Consequently, plastic pollution is now considered

to be a major factor responsible for the global decline in biodiversity and represents a major threat

to the Earth-system functioning and human health (Gall and Thompson, 2015).

Microplastics are emerging pollutants that have been extensively detected in aquatic

ecosystems, especially oceans. However, there is a knowledge gap regarding microplastic pollution

in agricultural soils and terrestrial ecosystems (Horton et al., 2017a; Huerta Lwanga et al., 2016).

We surveyed the publications related to microplastic contaminants in the Scopus database

(https://www.scopus.com/) using the keywords “microplastic or microplastics” in combination with

“terrestrial or soil” and “sediment, beach, or sludge” and “water, river, lake, sea, ocean, or marine.”

The literature retrieved included 1331 publications covering the period between 2004 and February

2019. Among these publications, 71% focused on marine environments, freshwater lakes, rivers,

and other aquatic ecosystems, 24% concentrated on sediments (from aquatic environments, beaches,

and sludge), and 5% were devoted to terrestrial ecosystems (Fig. 1). Since Rillig (2012) identified

the problem of microplastic pollution in the soil environment, increasing attention has been paid to

plastic pollution in soils and the potential dangers of soil microplastics (de Souza Machado et al.,

2018a; Horton et al., 2017b; Huerta Lwanga et al., 2016; Nizzetto et al., 2016b; Scheurer and

Bigalke, 2018; Yang et al., 2018; Zhang and Liu, 2018). The number of studies on microplastics

related to terrestrial ecosystems is increasing compared to a previous surveys, however, it is still

lagging behind work in aquatic habitats (Andrés Rodríguez-Seijo, 2018).

Globally, the most frequently polymers found in the soil environment are polyethylene and

polypropylene with lesser amounts of polyvinyl chloride and polyethylene terephthalate also present.

Although these plastic polymers are relatively simple in structure and may be relatively
environmentally benign, plastics may also contain a wide range of additives which may greatly

enhance their ecological toxicity (Koelmans et al., 2019). For example, plasticizers such as phthalic

acid esters (PAEs) represent a main additive of plastic films commonly used in agriculture and have

been implicated in the contamination of vegetables and fruits (He et al., 2014; Kong et al., 2012).

After entering the soil, macroplastic residues typically disintegrate into micro- and nano-plastics

and absorb a variety of heavy metals or release organic pollutants into the soil, especially PAEs,

which pose potential risks to soil biology and human health (Kasirajan and Ngouajio, 2012;

Steinmetz et al., 2016; Wang et al., 2013, 2016). Interestingly, however, the presence of

microplastics and PAEs have been reported in agricultural soils where microplastic-containing

fertilizers and agricultural plastics have never been used (Kong et al., 2012; Piehl et al., 2018). It is

still unclear therefore whether microplastics and PAEs in soil and crop products actually originate

from plastic mulching film and whether they pose an actual risk to soil organisms and soil quality.

It is necessary to systematically study the changes and safety of microplastics in soils where

plastic mulching film has been intensively used in agriculture. In this context, the main objectives

of this study were to (1) summarize the distribution and migration of microplastics in soils; (2)

highlight the separation, extraction, and identification methods for monitoring microplastics in soils;

(3) discuss the ecological effects and pollution mechanisms of soil microplastics; (4) identify

potential solutions to mitigate microplastic pollution; and (5) identify the future challenges in soil

microplastics research.

2. Classification and migration of microplastics in soil

2.1. Classification and source of microplastics in soil

Microplastics can be divided into primary microplastics and secondary microplastics based on
the original manufactured particle size. Primary microplastics mainly include plastic microbeads

and nanoparticles directly used in a variety of industrial processes, such as industrial detergents and

cosmetics. In addition, they may enter soil from atmospheric deposition (Allen et al., 2019).

Secondary microplastics originate from large plastic products that have broken down in situ (e.g.

plastic film residues, household garbage). This may occur at the soil surface in response to solar UV

irradiation or within the soil profile due to physical abrasion (abiotic) and biological attack (Andrady,

2011; Cole et al., 2011; Gesamp, 2015). The types of microplastics can be divided into fibers,

fragments, thin films, and particles depending on the plastic shape. Depending on the source, fibers

often represent the predominant form if they enter soil from biosolids or irrigation waters derived

from municipal wastewater (Jabeen et al., 2017; Liu et al., 2018). In contrast, the breakdown of

plastic mulch films leads to a predominance of heterogeneous fragments, while plastic coated

fertilisers leads to a predominance of thin films. Microplastics are further divided into small

microplastics (<1 mm), medium microplastics (1-3 mm), and large microplastics (3-5 mm)

according to their particle size (Andrady, 2011; Andrés Rodríguez-Seijo, 2018; Gesamp, 2015;

Horton et al., 2017a; Liu et al., 2018; Rillig, 2012). Nanoplastics are typically referred to as being

1-1000 µm in size, while picoplastics are <1 µm in size. The reason that categorizing microplastic

size is important is that it affects their potential for transport in soil and their potential to be taken

up by cells. For example, microplastics >150 µm are unlikely to be taken up by most plants and soil

organisms (with the exception of mesofauna) and are not thought to pose a risk to human health

(WHO, 2019). In contrast, nanoplastics are more likely to pose an environmental risk as they have

the potential to be taken into cells in a similar way to other nanoparticles (e.g. by endocytosis; Kuhn

et al., 2014). In the case of nanoparticles, the rate of uptake is known to be dependent on the size,
shape and surface chemistry of the material (Ma et al., 2013). Unfortunately, nanoplastics are rarely

quantified in soil and their uptake into plants and soil microorgansims has not been evaluated from

a risk assessment perspective. However, based on studies in marine systems we expect this exposure

route to be significant (Al-Sid-Cheikh et al., 2018).

The main sources of macro- and microplastics entering agricultural soils includes plastic mulch

films, municipal waste (e.g. municipal solid waste, compost), biosolids (sewage sludge and

anaerobic digestate), plastic-coated fertilizers and atmospheric deposition (Andrés Rodríguez-Seijo,

2018; Blasing and Amelung, 2018; Liu et al., 2018; McCormick et al., 2014; Nizzetto et al., 2016b).

Of these, agricultural films and compost application are the probably the most important (Blasing

and Amelung, 2018; Hurley and Nizzetto, 2018). Plastic mulching is an important technique used

to promote agricultural production in many regions of the world. Specifically, plastic mulches

greatly enhance water and nutrient resource efficiency as well as providing thermal insulation and

early planting and/or harvest cropping (Yin et al., 2014; Liu et al., 2019; Gao et al., 2019). In

addition, plastic mulch films may reduce soil erosion and reduce the disease burden of the crop and

allow the more efficient use of pesticides (Yan et al., 2010; Ruíz-Machuca et al., 2015). It is

therefore not surprising that the use of plastic mulch films has been widely promoted by industry

and agri-extension agencies to promote greater food security, sustainable food production and

improve livelihoods (Liu et al., 2014; Yan et al., 2014; Steinmetz et al., 2016). However, in the

long-term, the application of plastic film may cause serious pollution problems. One of the key

debates is therefore whether the short term gains from using plastic films to promote food security

outweigh the potential long-term risk to soil health. One of the major issues is that these films are

extremely thin (ca. 8-50 µm thick) making their physical extraction from soil at the end of the
growing season very difficult (Liu et al., 2013). In addition, there is a lack of recycling facilities

capable of handling soil-contaminated plastic making recovery from the soil uneconomic as well as

impractical. Inevitably, this has led to the progressive accumulation of large amounts of residual

film in farmland (Fig. 2). Aided by tillage, UV irradiation and biodegradation, this residual mulch

slowly fragments forming a continuum of macro, micro and nano plastics in soil (Ramos et al.,

2015; Steinmetz et al., 2016).

The recycling of biosolids to land is widely advocated as a way of closing the nutrient cycling

loop as well as replenishing organic matter in highly intensive cropping systems (Singh and Agrawal,

2008; Sullivan et al. 2015). While it is known that biosolids may contain a range of metals and

organic pollutants (Smith, 2009; Semblante et al. 2015; Sharma et al. 2017), it is now becoming

evident that they may contain significant amounts of plastic pollution (Gatidou et al., 2019).

Typically, between 70 and 99% of the microplastics present in domestic wastewater are recovered

in the sludge fraction during water treatment (Carr et al., 2016) leading to microplastic

concentrations in sludge of 103 to 105 particles kg-1. Consequently, large amount of microplastics

will accumulate in the soil, particularly after repeated applications of sewage sludge to agricultural

land (Andrés Rodríguez-Seijo, 2018; Nizzetto et al., 2016b). One of the key debates is therefore

whether the effective recycling of nutrients and organic matter back to land via biosolids outweighs

the risk of plastic contamination.

Municipal solid waste landfills may also represent point sources of microplastic pollution

affecting the underlying soil and groundwater (Andrés Rodríguez-Seijo, 2018; Duis and Coors,

2016; Hopewell et al., 2009; Zubris and Richards, 2005). In the leachate fraction, microplastic

particles range from 100-1000 µm in size with a concentration of 1-25 particles l-1 (He et al., 2019).
As landfill leachate is rarely applied to agricultural land this probably represents a minor source of

contamination globally (Jones et al., 2006).

2.2. The distribution and migration of microplastics in soil

With the development of the plastics industry, the global production of plastics has rapidly

increased from 1.5 million tons in 1950 to 348 million tons in 2017 (Liu et al., 2018; Statista, 2018;

PlasticEurope, 2018). Since 1950, the total cumulative global production of plastic has been

estimated at ca.10 billion tonnes, of which 55% has been sent to landfill or discarded either on land

or in the oceans (Geyer et al., 2017; Roland Geye, 2017). At the global level, best estimates suggest

that approximately 80% of ocean plastics come from land-based sources (Li W.C. et al., 2016).

Although packaging represents the biggest consumer of plastic (ca. 150 million tonnes y-1), the

global consumption of plastics by agriculture is also significant at 8 million tonnes per year with an

estimated annual market value of $6 billion (Scarascia-Mugnozza et al., 2012). Of this,

approximately 427 and 300 thousand tons of plastic mulching are used each year to cover farmland

in Europe and North America, respectively (Nizzetto et al., 2016b, 2016c). China also represents

one of the largest producers and consumers of plastics in the world, accounting for around 30% of

global use. The use of agricultural film in China (including mulching film and greenhouse film) has

now reached up to 2.6 million tons y-1, of which mulching film accounts for 1.5 million tons

covering a total area of 18.4 million ha (Yan et al., 2014; China Statistical Yearbook, 2017). Using

an Autoregressive Integrated Moving Average model we have predicted the future amount and

coverage of plastic mulching film in China (Fig. 3). Our findings suggest that the use of plastic

mulching film will reach 1.99 million tons in 2020 and 2.28 million tons by 2025 (Fig. 3A). We

also predict that the area covered by mulching film in China will continue to increase, and will reach
21.0 million ha in 2020 and 23.4 million ha by 2025 (Fig. 3B). As it is impossible to completely

remove plastic films from soil, and the rate of degradation is very slow, this will inevitably lead to

a progressive accumulation of plastic in soil (Liu et al., 2014). An investigation of the major plastic

mulching film usage areas in China has shown that the most severe pollution occurred in cotton

fields in Xinjiang Province, with an average plastic film residue level in soil of 259 kg ha-1 and

maximum plastic film residue of 381 kg ha-1 in some areas (Yan et al., 2014). Large amounts of

macroplastic residues also inevitably leads to a significant accumulation of microplastics in

agricultural soils over time (Ramos et al., 2015; Steinmetz et al., 2016). In the case of biosolids,

assuming an average microplastics contamination of 104 particles kg-1 and a typical land application

rate of 1-15 t ha-1 y-1 this would add between 106 and 109 particles ha-1 y-1 leading to a topsoil

contamination level of ca. 4 to 150 particles/kg for each year of application. It is therefore not

surprising that contamination level of 670 fibers kg-1 have been reported in the topsoils from

European farmland (Barnes et al., 2009; Ren et al., 2018), and that microplastics have been detected

in 90% of Swiss floodplain soils (Scheurer and Bigalke, 2018). It should also be noted that the

abundance of microplastics in the terrestrial environment is much higher than that in marine

ecosystems (Horton et al., 2017a; Nizzetto et al., 2016b; van Sebille et al., 2015).

Many studies have documented the distribution and pollution mechanisms of microplastics in

coastal and marine environments (Bergmann et al., 2017; Cole et al., 2011), particularly in lakeside

and coastal areas where there is a high intensity of human activity (Duis and Coors, 2016; Horton

et al., 2017b; Jabeen et al., 2017; Wang et al., 2017; Zhou et al., 2018). However, there are few

studies on the distribution and migration of microplastics from agricultural soils into the wider

environment (de Souza Machado et al., 2018a; Zhou et al., 2018); several studies have shown that
the abundance of microplastics varies at different soil depths, reaching up to 7% by weight in highly

polluted topsoils (Fuller and Gautam, 2016; Liu et al., 2018). Liu et al. (2018) showed that

microplastics were found in both shallow and deep soils from a range of agricultural sites in China,

but that the abundance of microplastics in shallow soils was much higher than that in deep soils.

Soil is not only a sink of microplastics, but may also represent a source of microplastics to

groundwater and the aquatic environment (Fig. 4). This risk of loss is expected to be much greater

in agricultural soils with artificial drainage, large amounts of macropores and when surface runoff

occurs. Currently, microplastic contamination of groundwaters are low but have shown to reach

levels of 12 particles l-1 suggesting that transfer does occur (Panno et al., 2019). However, it is likely

that this contamination may also be derived from human-derived wastewater (e.g. septic tanks)

rather than from agricultural plastics. Microplastics can be also transferred directly through the soil

via bioturbation (Rillig, 2012; Rillig et al., 2017b), tillage operations (Liu et al., 2018), and water

infiltration (Lou et al., 2018). In addition, losses from soil may occur via wind erosion, surface

runoff or during crop offtake (Zhang et al., 2018b). Microplastics can also be transported and

dispersed by soil animals and livestock, either through attaching to the outside of the organism or

through transfer from ingestion and defecation (Cao et al., 2017; Rillig et al., 2017b). Microplastics

can also be transferred to aquatic ecosystems by surface runoff (Blasing and Amelung, 2018;

Brodhagen et al., 2015; Hurley and Nizzetto, 2018; Kyrikou and Briassoulis, 2007; Steinmetz et al.,

2016). The migration of microplastics through surface runoff is related to the particle size and

density of the microplastic. The bulk density of common plastics typically varies from 910-970 kg

m-3 depending on the nature of the material. Therefore plastics without much soil mineral

contamination (density of 2650 kg m-3) readily float. In addition, the migration is easier for smaller
particles as there is less likelihood of physical trapping in the soil matrix or surface vegetation

(Nizzetto et al., 2016a; Li et al., 2019). Additionally, the shape, type, and surface characteristics of

microplastics are also important factors which are likely to affect their migration in soils. Thus, it is

vital to further study the weathering process, adsorption capacity, and migration of microplastics,

especially those with a particle size < 1 mm (Zhou et al., 2018). These studies will not only be

beneficial to understanding the distribution and migration of microplastics in marine and terrestrial

ecosystems, but also provide an important reference for protection and governance of marine,

freshwater and terrestrial ecosystems. Given the numerous potential ways in which microplastics

can move in soil, it is also critically important that we determine the quantitative importance of each

pathway. This will enable the better parameterization of risk models and also the implementation of

more targeted monitoring and mitigation programmes.

3. Separation and detection of microplastics in soil

Separation of microplastics, especially nanoplastic, from the soil environment is more complex

than from aquatic ecosystems owing to the complexity of the soil environment and characteristics

of microplastics (Alimi et al., 2018; Hurley and Nizzetto, 2018). Despite efforts to establish

effective analytical procedures (Gigault et al., 2016; Velzeboer et al., 2014), the comparative

analysis of microplastics in different components of the Earth system remains challenging as no

unified standard methods exist for microplastic separation and identification (Song et al., 2015;

Tagg et al., 2015).

In accordance with methods for separating microplastics from marine sediments and aquatic

environments, microplastic separation from soil can be divided into the process of microplastics

extraction and impurity removal. Microplastics extraction methods for soils includes: (1) air
flotation; (2) heating (3-5 s at 130°C); and (3) density suspension. Notable problems with these

approaches, however, include: (i) the recovery rate is often not reproducible and the extraction

efficiency is low; (ii) it is difficult to capture the high degree of spatial heterogeneity in soil plastic

contamination; (iii) current methods are not designed to capture nano- and picoplastic particles; (iv)

the heating method is not feasible for large numbers of samples and cannot readily detect the

quantity and size of microplastics, which is not suitable for the analysis of samples in complex

environments; (v) the density suspension method is a common method to extract microplastics from

sediment and sludge, but its suitability in soil remains to be validated. One of the major challenges

is the removal of other contaminants from the samples (e.g. organic matter). Impurity removal

methods include: (1) acid digestion; (2) alkali digestion; (3) enzyme digestion, and (4) chemical

oxidation. The problems with these approaches include: (i) some plastics react with strong acids or

alkali; (ii) enzymatic digestion is not feasible for large numbers of samples and/or large-volume

samples, due to prohibitive costs and is very poor at removing stable organic matter; (iii) the impact

of wet oxidation on microplastics and the potential to inadvertently remove co-contaminants (e.g.

plasticizers) remains to be verified.

A major consideration in microplastic research is the robust collection of the samples from the

field. It is recommended that collection of samples in plastic materials be avoided where possible

to minimize contamination (Koelmans et al., 2019). In addition, contamination of samples in the

laboratory due to airborne polymer particles and fibres has been described as a major problem in

microplastic analysis (Torre et al., 2016). Further, adequate negative controls (blanks) should be

included to demonstrate absence of contamination during sample processing (e.g. during sieving,

filtration, digestion, transfer and analytical identification steps; Hermsen et al., 2018). In addition,
the recovery of pure microplastics of different sizes (i.e. reference standard, positive control) added

to the samples should be used to validate plastic recovery.

The development of techniques for extraction and analysis of microplastics from soil media is

in its infancy. Extraction using density suspension and the removal of organic matter on the surface

of microplastics using a suitable oxidizer solution are the most commonly used methods for

separating microplastics from soils (Liu et al., 2018; Nuelle et al., 2014; Qiu et al., 2016; Thompson

et al., 2004; Zhang et al., 2018b). According to the methods for separation of microplastics from

marine sediments and aquatic environments, a saturated sodium chloride solution, sodium

polytungstate solution, or seawater can be used for density separation of plastic particles from soils

(Scheurer and Bigalke, 2018). Sodium iodide and zinc chloride solutions are also commonly used

density suspensions (Claessens et al., 2013; Corcoran et al., 2015; Fok and Cheung, 2015). However,

different types of microplastics have different densities, and other interfering substances can be

easily suspended in high density liquids, while some types of microplastics cannot be suspended in

low density solutions. Zhang et al. (2018b) used pure water to float polyethylene and polypropylene

microplastics (density 0.90 to 0.96 g cm-3) from soils, however, this necessitates removal of mineral

contaminants. Theoretically therefore, to improve the extraction efficiency of microplastics,

suspension of different concentrations can be used to extract different types of microplastics from

soil samples step-by-step. Nuelle et al. (2014) used an air-induced overflow method to extract

microplastics from soil samples using a low-density suspension solution first, and then used a high-

density solution for the subsequent flotation step. The extraction efficiency, which was dependent

on the shape, size, and source of microplastics in the whole procedure, reached up to 91%-99%.

It is more difficult to extract microplastics from soil environments than from aquatic
ecosystems because the surface of soil microplastics often develop biofilms that absorb impurities,

such as mineral particles and organic matter. These impurities need to be removed for further studies.

Solutions of acid (e.g. HCl, HNO3, H2SO4), base (e.g. KOH, NaOH) and oxidants (e.g. KMnO4,

H2O2) in isolation or combination have all been used to remove surface impurities (Liu et al., 2018;

Qiu et al., 2016). It was reported that a 35% H2O2 solution was more conducive to the removal of

biological organic matter than 37% HCl and 20%, 30%, 40%, and 50% NaOH (Nuelle et al., 2014).

Tagg et al. (2015) showed that a 30% H2O2 solution could not only effectively remove organic

matter, but also improve the filtration efficiency, which is beneficial to identifying different types

of microplastics by Fourier transform infrared spectrometry (FTIR). Cole et al. (2014) found that

enzymatic digestion was a more effective method for the removal of organic impurities compared

with acid or alkali digestion. Unfortunately, there is no uniform standard to remove organic

impurities from the surface of microplastics.

The main identification methods of microplastics include visual screening, stereoscopic

microscopy, scanning electron microscopy (SEM), FTIR, and Raman spectroscopy. In the

assessment process, FTIR and Raman spectroscopy have been applied for qualitative assessments,

while microscopy, including SEM, has been used for the quantification of microplastics (Qiu et al.,

2016; Scheurer and Bigalke, 2018; Song et al., 2015; Zhou et al., 2018). The visual method is also

used to detect microplastics, but it is difficult to identify small plastic particles, and underestimation

or overestimation of the abundance of microplastics in the ecological environment is likely to occur

(Song et al., 2015; Shim et al., 2017).

4. Impact of microplastics on soil ecosystems

4.1. Impact of microplastics on the soil structure

A loss of soil structure commonly occurs when large amounts of macroplastics are present in

the soil. This is deleterious as it reduces the infiltration of rainwater and irrigation water, negatively

affects the soil’s water holding capacity and may induce anoxia (Liu et al., 2014). It has also been

reported that residual plastic mulch film damages the structure of soil aggregates and reduces soil

aeration and water permeability, thereby reducing root growth and overall plant productivity (Jiang

et al., 2017; Zeng et al., 2013; Zhang et al., 2018a). In contrast to macroplastics, there are relatively

few reports on the relationship between microplastics and the soil structure and aggregates (Zhang

and Liu, 2018), and no studies have clearly shown the influence of microplastics on soil structure.

Further studies are required to determine where microplastics are physically located in the soil

matrix and how this affects their fate and behaviour.

4.2. Effect of microplastics on soil physical and chemical properties

Several studies have reported that microplastics have a negative impact on soil organic carbon

(C) and nitrogen (N) cycling, soil microbial activity, and nutrient transfer (Cao et al., 2017; Liu et

al., 2017; Rillig, 2012, 2018; Rillig et al., 2017b). Liu et al. (2017) showed that the addition of

microplastics can stimulate soil enzyme activities and the accumulation of soluble nutrients in soil.

In addition, plastic mulch residues inadvertently contribute to increasing the size of the stable soil

organic C pool. At a typical plastic contamination level of 5-25 kg ha-1 y-1, this equates to a C

addition rate of ca. 4-20 kg C ha-1 y-1. It should be noted that this is low in comparison to rates of

organic C loss from most intensive agricultural systems and therefore should not be viewed in a

positive light. Hodson et al. (2017) found that microplastics can improve the bioavailability of zinc
and increase the contact between earthworms and zinc as a medium, but little is known about the

potential risk to earthworms. In addition, the underpinning mechanisms responsible for this increase

in micronutrient bioavailability remain unknown.

In agriculture, measurements of soil physical and chemical quality indicators have been used

as indicators to evaluate the advantages and disadvantages of agricultural plastics. In some cases,

plastic mulch films improve specific soil quality indicators whilst in others a decline is apparent

(Jiang et al., 2017; Liu et al., 2014; Steinmetz et al., 2016). As no integrated soil quality assessment

system currently exists it remains difficult to ascertain whether the benefits of plastic mulches

outweighs the potential disadvantages (Sarmiento et al., 2018). Some studies have concluded that

residual plastic accumulation negatively impacts on the soil’s physicochemical properties and will

subsequently lead to unsustainable farmland use and environmental damage (Andrés Rodríguez-

Seijo, 2018). However, rarely are critical limits for excessive microplastic contamination defined

(i.e. tipping points) at which these negative impacts are observed. This makes it difficult to evaluate

the spatial scale of the problem, give guidance on microplastic loading rates and predict the carrying

capacity of agroecosystems. Ramos et al. (2015) found that plastic residues can accumulate

pesticides from soil leading to changes in the soil habitat. Several studies have also indicated that

the soil microbial biomass C and N contents significantly decrease with an increasing amount of

film residues (Moreno and Moreno, 2008; Wang et al., 2016). It is necessary to confirm whether the

abovementioned results were caused by the plastic residues themselves, their intrinsic primary

pollutant load (e.g. plasticizers) or secondary pollutant load (e.g. pesticides). In addition, it is

necessary to differentiate between the potential toxic effects of the macroplastic vs. microplastic

components. Consequently, the evidence base on the impact of plastics on many soil properties is
somewhat contradictory and often incomplete. In addition, the focus of previous research has not

been on soil function and has not taken an ecosystem services approach. Thus our ability to evaluate

their impact on soil health remains very difficult. Another major issue is that the results are not put

into a wider context. For example, it is difficult to assess whether the observed changes in soil

quality due to microplastics are any different from other waste materials commonly added to land

(e.g. biochar, manure, sludges).

4.3. Impact of microplastics on soil organisms and plants

Based on the negative impacts of plastic pollution on marine organisms, there is increasing

focus on the dangers of microplastics to soil organisms (Cao et al., 2017; Chae and An, 2018; Huerta

Lwanga et al., 2016, 2017a,b; Rillig et al., 2017b). Mesofauna (e.g. earthworms, mites, collembola)

are known to be vital in maintaining soil quality, however, intensive agricultural systems typically

lead to a loss in mesofaunal abundance (George et al., 2017). Consequently, a further loss of these

keystone organisms by plastics could represent a major threat to long-term agroecosystem

functioning. Huerta Lwanga et al. (2016) studied the survival and fitness of earthworms exposed to

microplastics in litter at concentrations of 7%, 28%, 45%, and 60% dry weight. After incubation for

60 d, the earthworms in the 28%, 45%, and 60% microplastic conditions in the litter had a higher

mortality rate and significantly lower growth rate compared with those of the control and 7%

treatment. The research also confirmed the concentration-transport and size-selection mechanisms

of microplastics, which may have important implications for the fate and risk of microplastics in

terrestrial ecosystems. It should be noted, however, that the concentrations of plastic used in those

studies were 1000-fold higher than seen in most plastic-contaminated agricultural soils. Cao et al.

(2017) stated that a low soil microplastic concentration (<0.5%) has little impact on earthworms,
but when the microplastic concentration rose to 1% and 2%, it significantly inhibited the growth of

earthworms and increased their mortality. The adverse effects of microplastics on soil organisms

may be mainly caused by the significant accumulation of microplastics in the gut and stomach of

organisms, which can damage their immune systems and affect their feeding behavior and

development. Studies in marine organisms indicate that organic pollutants sorbed to microplastics,

however, do not readily transfer to the host (Bakir et al., 2016; Ziccardi et al., 2016), albeit this

xenobiotic exposure route still needs testing in soil organisms. Bandopadhyay et al. (2018) indicted

that biodegradable plastic mulches affect soil microbial communities indirectly by changing the soil

microclimate, soil physical structure and through the addition of contaminants adhering to the film

fragments. Given the high degree of functional redundancy and diversity within the soil microbial

community, it is highly likely that plastic mulch films will affect the composition of the microbial

community as it will create new ecological niches within the soil. What is critical, however, for

future studies is whether microplastics negatively affect keystone microbial species that are

fundamental to the delivery of key soil functions (e.g. nitrifiers, arbuscular mycorrhizas) or whether

they increase the prevalence of disease causing organisms (e.g. plant and animal pathogens).

Agricultural plants are known to take up a range of nanoparticles and consequently it is likely

that microplastics may enter the food chain through this route (Jassby et al., 2019). Li et al. (2019)

has reported that polystyrene microplastics (0.2 µm) can be absorbed and enriched in the root of

raw vegetables, and migrate from the root to the shoots. A comparison of microplastics transported

from the soil to the edible parts of the plant versus that deposited directly onto the shoots from

atmospheric deposition or wastewater irrigation remains unknown. Based on current evidence it is

unlikely that this exposure pathway constitutes a major risk to human health or other parts of the
food chain (Mateos-Cardenas et al., 2019). Qi et al. (2018) indicated that the microplastics derived

from starch-based plastic mulching film showed stronger negative effects on wheat growth

compared to polyethylene. This may be ascribed to the biodegradable plastic being composed of

44.6% polyethylene terephthalate and 18.3% polybutylene terephthalate, or more likely to shifts in

microbial communities or starch-induced N immobilization in the soil. The mechanisms by which

macro- and micro-plastic contamination in soil affects plant growth remains largely unknown and

further work is required to explore this for a wide range of crop plants, especially for edible root

crops.

4.4. Influence of microplastics on the groundwater environment

Some studies have indicated that microplastics in marine environments originate from

terrestrial ecosystems (Horton et al., 2017b; Luo et al., 2018; Wagner, 2014). Soil microplastics can

be transported from land to the groundwater environment via long-distance movement, such as

animal disturbance, surface runoff, and water infiltration (Blasing and Amelung, 2018; Brodhagen

et al., 2015; Hurley and Nizzetto, 2018; Kyrikou and Briassoulis, 2007; Steinmetz et al., 2016),

thereby affecting the underground aquatic environment and even disturbing the marine ecosystem.

There are scarce reports on the effects of microplastics on the groundwater environment (Chae and

An, 2018), even though studies on the marine environment widely exist (McCormick et al., 2014;

Zettler et al., 2013).

5. Soil microplastics and phthalic acid esters

One of the key challenges in microplastic research is separating the environmental effects of

the plastic polymer from primary and secondary contaminants present in the plastic. Plastic mulch

films contain large amounts of phthalate esters (PAEs) which can be released into the soil. As they
are endocrine disrupting chemicals, PAEs are often known as “environmental hormones,” and have

the potential to severely impair human health owing to their reproductive toxicity, developmental

toxicity, carcinogenicity, and other toxic responses, particularly if there is prolonged exposure (He

et al., 2014; Kong et al., 2012). Six of these PAEs (namely, butyl benzyl phthalate (BBP), di-(2-

ethylhexyl) phthalate (DEHP), dimethyl phthalate (DMP), diethyl phthalate (DEP), di-n-butyl

phthalate (DBP), and di-n-octyl phthalate (DOP)) found in mulch films are listed as environmental

priority pollutants by the United States Environmental Protection Agency (USEPA, 2013).

Concentrations of PAEs in soil exposed to much films have been found in the range 1.8 to 3.5 mg kg-

1 (Shi et al., 2019). In addition, di-n-butyl phthalate (DBP) and di-(2-ethylhexyl) phthalate (DEHP)

were found to be highly enriched in grain samples in the same study (4-12 mg kg-1). Consequently,

PAEs not only have negative effects on soil properties, but also accumulate in the food chain,

thereby posing a major threat to ecosystem and human health. In order to avoid this threat, it is

particularly important to reduce and eliminate the sources of PAEs and offset the existing pollution

of PAEs in the environment (He et al., 2014). Microbial degradation is one of the most important

methods to remove PAEs in the environment, but it cannot completely remove PAEs from soil or

aqueous solutions in the short term (Zhang et al., 2007). It is therefore vital that we reduce or prohibit

the use of PAEs in industrial processes where there is an appreciable environmental risk.

It has been reported that PAEs can reduce microbial activity by inhibiting soil respiration and

enzyme activity (Guo et al., 2010; Xie et al., 2009). Additionally, PAEs can also affect soil

invertebrates, such as earthworms (Chen et al., 2004). Studies have shown that plastic film residues

can readily release PAEs into soil (He et al., 2014; Wang et al., 2013; Wang et al., 2016) and that

these toxic compounds may change the behavior of organic pesticides in soils (Ramos et al., 2015),
inhibit enzyme activities (He et al., 2014; Wang et al., 2009; Xie et al., 2010; Zhou et al., 2005) and

alter soil microbial communities (Chen et al., 2013; Wang et al., 2016). Thus, they may pose a

potential danger to soil functioning (Kasirajan and Ngouajio, 2012; Steinmetz et al., 2016).

Worryingly, Wang et al. (2016) have shown that the content of PAEs in soil continues to accumulate

with the repeated application of plastic mulch. This suggests that PAEs are relatively recalcitrant in

soil and may pose a long-term risk. However, it is unclear whether PAEs in soil and crop products

actually originate from plastic films or from another source (Duis and Coors, 2016; Lambert and

Wagner, 2016; Rillig, 2012; Wang et al., 2016). For example, DBP may exist in the atmosphere at

concentrations of 3-59 ng m-3 while in aquatic environments it can be present at concentrations of

1-30 ng l-1 (Xie et al., 2005; Wang et al., 2008). There is therefore a clear need to determine the

source-partitioning of PAE in agricultural systems. In addition, it is known that PAE removal from

soil can be stimulated by the addition of organic materials in the laboratory (e.g. compost; Chang et

al., 2009), however, this still needs testing under realistic conditions in the field to facilitate the

design of effective mitigation strategies.

6. How to solve microplastic pollution

Microplastics, which are stable and non-degradable, will quasi-permanently remain in the

environment, and thereby pose a long-term risk to ecosystems (Horton et al., 2017b; Hurley and

Nizzetto, 2018; Liu et al., 2018). An important measure to reduce microplastic pollution in soil is

to minimize or avoid using plastics within food production systems. Plastic mulching film, as an

important microplastic source in agriculture soils, yet it is indispensable in agricultural production.

These films increase crop yields by more than 30%, thereby making a great contribution to the

security of agricultural products in countries like China (Fan et al., 2017). Li X.L. et al. (2016)
indicated that the use of agricultural film led to 42.3% greater water use efficiency. Give that water

supplies are dwindling in soil countries and becoming more uncertain with climate change, it is

unlikely that the use of plastic mulch films will stop (van Ittersum et al., 2013).

Thus, reasonable usage and forced recycling of traditional polyethylene mulch films represents

a promising solution to reduce plastic pollution in agriculture. The government and relevant

departments should also strictly control the entry of low grade plastic film (i.e. high contaminant

load) from entering the market. Additionally, we should also promote the multi-year use of

agricultural plastic films.

The use of bioplastic, which is a material that can be partially or completely degraded by

microorganisms, is an important direction for the plastic industry and agricultural development. The

use of biodegradable especially bio-based mulching film is becoming another significant method to

solve the problem of plastic film residue and microplastic pollution at source. However, compared

to polyethylene film, biodegradable mulch films (especially those which are bio-based) have

significant limiting factors for large-scale application owing to their lower mechanical strength,

higher cost and greater C footprint associated with production. In the future, it is necessary to reduce

the production cost, improve the properties of these products, and optimize raw materials and

control degradation time of biodegradable plastic mulching film.

7. Conclusions and perspectives for future work

As an emerging research field, microplastic pollution in terrestrial ecosystems is gaining

increasing scientific and media attention due to the long-term threat to agroecosystem functioning,

food security and human health. The study of microplastics in soil has proven more difficult than in

aquatic ecosystems owing to difficulties in separating plastics from the soil matrix. It is clear from
current evidence, however, that a comprehensive mechanistic investigation of the properties and

behavior of microplastics in agricultural soils is urgently required. Without this, it will not be

possible to evaluate the true risk that microplastics pose to the environment and also will prevent

the formulation of effective legislation and policies which enable the safeguarding of human health

and help protect the soil and wider environment. Based on the current evidence we have identified

12 priorities for future research:

(1) Standardization of microplastic separation and detection methods. Standardization

of techniques and methodologies is vital for the quantitative comparison of microplastics in different

environments and for the assessment of their potential risks. This also needs to incorporate good

quality assurance (QA) procedures to avoid contamination from other sources. Microplastics may

decompose or degrade into nanoplastics, which can be ingested in large quantities by marine or

terrestrial organisms, thereby posing a serious threat to the organismal and ecosystem health. Hence,

it is not only necessary to identify and standardize the separation and identification methods for

microplastics, but also to explore and establish methods for the separation, detection and pollutant

load assessment of nanoplastics to better understand their ecological significance.

(2) Microplastics and soil aggregates. Soil aggregates, as the most basic structural unit of

soil and the foundation of soil fertility, are an important site for soil organic matter decomposition

and accumulation, nutrient transfer, and transformation. The study of the spatial distribution and

behavior of microplastics within soil aggregates in both top and subsoils will be vital in predicting

the likelihood of transport, uptake and transformation within the soil profile.

(3) Microplastics, heavy metals and organic pollutants. Microplastics, which have a large

specific surface area, strong adsorptivity, and strong hydrophobicity, can sorb large amounts of
heavy metals, organic pollutants, and pathogens from soil. Research on the sorption/desorption

relationships of heavy metal ions and pesticides with microplastics is needed. In addition, the role

of plastic biofilms on the retention of plant and animal pathogens is required. This information will

greatly inform the likely risk of these pollutants to be transported in soil as well as their potential

for long term accumulation in soil, biotransformation and bioaccumulation.

(4) Microplastics and plasticizers. Plasticizers, especially phthalic acid esters (PAEs), are

now widespread contaminants in agricultural soils and can negatively affect soil enzyme activity,

microbial diversity, crop yield, and crop quality. Knowledge of plasticizer concentrations in soil

remains fundamental to undertaking holistic risk assessments for microplastics in soils. Work is

therefore needed to study the behaviour of PAEs in residual agricultural film (macroplastics) and

microplastics in a range of soil types and under a wide range of conditions. We also need to evaluate

the extent to which PAEs can affect soil food webs and enter the human food chain.

(5) Long-term fate of plastics in soil and their legacy. Vast areas of the world’s agricultural

land are now contaminated with plastics. While it is widely acknowledged that we should gradually

transition from using non-renewable plastics to more bio-based plastics within agriculture, the

legacy of these conventional plastics is likely to remain for hundreds of years. Consequently, we

need to better understand the rates by which macroplastics fragment into micro- and nano-plastics

over time and whether problems will still exist even when renewable mulch films are in use.

(6) Microplastic tipping points. At present, no critical limits for microplastic pollution in

soil have been determined. This limits our ability to be able to quantify the present and future degree

of environmental damage caused by microplastic pollution. Consequently, more ecotoxicological

dose-response studies are required in which a broad range of soil functions are assessed. This should
also focus on the behaviour of keystone organisms which regulate critical functions in soil.

(7) The use of appropriate quality control in microplastic experiments. In many respects,

there are great similarities between research looking at the impact of biochar and microplastics on

soil quality. In the former, it is now widely recognized that a standard set of measurements are

needed to characterize the biochar used in experiments to allow comparison between studies.

Biochar is known to vary greatly depending on origin and this has been shown to greatly affect how

it affects the plant-soil-microbial system. Microplastics also vary in size, shape, composition,

crystallinity, impurity/contaminant load and consequently a standard set of reporting criteria should

be developed to facilitate inter-study comparisons.

(8) Representative soil conditions and unbiased reporting. Many previous studies on the

impact of microplastics on the soil ecosystems have used extremely high doses which do not reflect

real world conditions. These are not useful from a risk assessment perspective. In addition, the

studies using excessive doses has led to misinterpretation and over-sensationalization of the results

by the media. It is important that researchers provide a balanced opinion and place the results in a

wider context when reporting.

(9) Longer-term field trials. Most controlled studies using microplastics have been

performed in the laboratory over a period of weeks or months, however, this only provides an initial

snapshot of the response. It is important therefore that controlled trials are set up which allow the

longer-term impact of microplastics to be evaluated. These should preferably be performed at the

field scale with sufficient replication and the appropriate controls. Field-scale trials will also

improve our understanding of how UV weathering of plastics affects its persistence in soil.

(10) Cleaning-up plastic pollution in soil using bio- and phyto-remediation. A range of
microorganisms have been isolated from soils and waters which possess the ability to degrade

plastic polymers. These are normally present at low abundance suggesting that their realized niche

in soil is small. Although bio-inoculants typically have low rates of persistence in soil, there is a

need to look at the potential to inoculate soils with these organisms to facilitate plastic

depolymerization. In addition, it is clearly possible to genetically modify plants and associated

symbionts to produce exoenzymes (e.g. PETase and MHETase) which can degrade plastic residues.

(11) Comparison of the impact of macro- and microplastics. It is still unclear whether

micro- and nano-plastics are more environmentally damaging than macroplastics. More work is

therefore needed to directly compare these different size fractions. In addition, the effect of

microplastics are typically only compared against an unamended control sample. The use of a

negative control (e.g. addition of inert quartz sand) or a positive control (e.g. compost, biochar)

could be used to better contextualize any changes observed following the addition of microplastics.

(12) Microplastic modelling at the field and landscape scale. It is widely reported that

many microplastics entering the ocean are derived from the land. The role of agriculture and plastic

much films in particular in this transfer process remains unknown. More landscape-level monitoring

studies are therefore needed where source apportionment can be made between the different

microplastic sources and sinks. This will be greatly aided by soil profile-based models which can

predict the long-term movement and persistence of microplastics in soil.

In conclusion, microplastics are becoming almost ubiquitous in soils and they are likely to

increase in abundance for the foreseeable-future. Based on their recalcitrance, it is also likely that

they will still be present in soil for generations to come. Therefore, it is necessary and urgent that

we prohibit the addition of microplastic particles to cosmetics, detergents, and other industrial
products which may enter soil via biosolids and irrigation water. It is also important that we continue

to develop more environmentally friendly biodegradable mulches to replace conventional plastic

films. Plastic has proved to be vital in the green revolution, however, we need a second green

revolution in which mulch films are truly biodegradable and which leave no toxic, visible or

distinguishable residues following degradation. These products will ensure that we are able to

maintain the sustainable development of agricultural systems and restore soil health.

Acknowledgments
This work was supported by the Zero-Waste Agricultural Mulch Films for Crops in China project

(Newton Fund: Newton UK-China Agritech Challenge 2017; No. 2017YFE0121900), National

Natural Science Foundation of China General Program (No. 31871575), Science and Technology

Innovation Project of CAAS (2018-2020) and the UK Global Challenges Research Fund (BU2019).

We gratefully acknowledge the anonymous reviewers for their valuable comments on our

manuscript.

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Figure legends:

Fig. 1 Global scientific publications on microplastic pollution after the concept of microplastic was
first proposed by Richard C. Thompson in 2004. The bars represent the annual number of papers

published in each research area from 2004 to February of 2019 (Scopus database).

Fig. 2 Large amount of plastic mulching film residues in farmland in China. A and B show recycled
film residues, while C and D show residual film in agricultural soils. The photos were taken in
Gansu Province by Yan Changrong in 2018.

Fig. 3 Past and future prediction of the application of plastic mulching film to agricultural land in
China according to the Autoregressive Integrated Moving Average model. A and B indicate the

amount and coverage areas of plastic mulching film, respectively.

Fig. 4 Schematic showing the main sources and fates of microplastics in the environment. Notes:
MPs represents microplastics; BB represents bioturbation; WI represents water infiltration; AM

represents agricultural management; and SR represents surface runoff.

Fig. 1

400
Terrestrial
350 Sediment
Aquatic
300
Number of publications

250

200

150

100

50

0
20
20
20
20
20
20
20
20
20
20
20
20
20
20
20
20
04
05
06
07
08
09
10
11
12
13
14
15
16
17
18
19
Year

Fig. 2
Fig. 3
Fig. 4

Highlights
1. Micro- and nano-plastics in agricultural soils represents a major environmental threat.

2. Standard methods for microplastic separation and detection are urgently needed.

3. Microplastics affect agroecosystem functioning by accumulating heavy metals or organic

contaminants.

4. Plasticizers represent a major source of pollution within microplastics.

5. Adoption of biodegradable films will help reduce soil microplastic accumulation.