Water Research 134 (2018) 341e352

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Water Research
journal homepage: www.elsevier.com/locate/watres

Review

Advances in concrete materials for sewer systems affected by

microbial induced concrete corrosion: A review
Cyrill Grengg a, *, Florian Mittermayr b, Neven Ukrainczyk c, Günther Koraimann d,
Sabine Kienesberger d, e, Martin Dietzel a
a
Institute of Applied Geosciences, Graz University of Technology, Rechbauerstraße 12, 8010, Graz, Austria
b
Institute of Technology and Testing of Building Materials, Graz University of Technology, Inffeldgasse 24, 8010, Graz, Austria
c €t Darmstadt, Franziska-Braun-Straße 3, 64287, Darmstadt, Germany
Institute of Construction and Building Materials, Technische Universita
d
Institute of Molecular Biosciences, University of Graz, Humboldstraße 50, 8010, Graz, Austria
e
BioTechMed-Graz, Mozartgasse 12/II, 8010, Graz, Austria

a r t i c l e i n f o a b s t r a c t

Article history: Microbial induced concrete corrosion (MICC) is recognized as one of the main degradation mechanisms
Received 19 September 2017 of subsurface infrastructure worldwide, raising the demand for sustainable construction materials in
Received in revised form corrosive environments. This review aims to summarize the key research progress acquired during the
17 January 2018
last decade regarding the understanding of MICC reaction mechanisms and the development of durable
Accepted 18 January 2018
Available online 6 February 2018
materials from an interdisciplinary perspective. Special focus was laid on aspects governing concrete -
micoorganisms interaction since being the central process steering biogenic acid corrosion. The insuf-
ficient knowledge regarding the latter is proposed as a central reason for insufficient progress in tailored
Keywords:
Sustainable construction
material development for aggressive wastewater systems. To date no cement-based material exists,
Microbiological corrosion suitable to withstand the aggressive conditions related to MICC over its entire service life. Research is in
Concrete particular needed on the impact of physiochemical material parameters on microbial community
Microorganism interactions structure, growth characteristics and limitations within individual concrete speciation. Herein an
Geopolymers interdisciplinary approach is presented by combining results from material sciences, microbiology,
Antimicrobial agents mineralogy and hydrochemistry to stimulate the development of novel and sustainable materials and
Acid corrosion mitigation strategies for MICC. For instance, the application of antibacteriostatic agents is introduced as
an effective instrument to limit microbial growth on concrete surfaces in aggressive sewer environments.
Additionally, geopolymer concretes are introduced as highly resistent in acid environments, thus rep-
resenting a possible green alternative to conventional cement-based construction materials.
© 2018 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 342
2. Characteristics of wastewater environments inducing MICC . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 343
3. Effect of concrete characteristics on MICC . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 345
4. Geopolymer technology for wastewater applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 347
5. Antimicrobial agents . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 349
6. Conclusions and outlook . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 350
Acknowledgment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 350
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 350

* Corresponding author. Institute of Applied Geosciences, Graz University of

Technology, Rechbauerstraße 12, A-8010, Graz, Austria.
E-mail address: [email protected] (C. Grengg).

https://doi.org/10.1016/j.watres.2018.01.043
0043-1354/© 2018 Elsevier Ltd. All rights reserved.
342 C. Grengg et al. / Water Research 134 (2018) 341e352

1. Introduction situ testing have shown that significant durability variations exist
between different types of concrete subjected to MICC. Neverthe-
The efficient, safe and cost-effective collection and transport of less, none of the so far tested materials can entirely resist this
wastewater is a key criterion maintaining expected sanitary stan- biogenic acid attack. All materials failed to reach their projected
dards of modern society (Hvitved-Jacobsen et al., 2013). Especially operating life time (Alexander et al., 2013; De Belie et al., 2004;
in developing countries insufficient operating or lacking waste- Girardi et al., 2010; Goyns and Alexander, 2014; Herisson et al.,
water networks can lead to the spread of infectious diseases and 2013). Reasons for this failure may originate from insufficient
the contamination of drinking water (Hvitved-Jacobsen et al., knowledge on the initial processes leading to microbial coloniza-
2002). Microbial induced concrete corrosion (MICC) has been tion of construction materials in heterogenous wastewater envi-
recognized as one of the main processes for degradation of concrete ronments. While Li et al. (2017) have recently summarized the
based wastewater networks worldwide, increasingly triggering existing knowledge on microbial community structures of acido-
high economic expenses, as well as severe health and environ- philic bacteria associated with MICC, little is known about initial
mental concerns (Herisson et al., 2017; Islander et al., 1991; Jiang microbial colonization of concrete structures in sewer systems.
et al., 2016; Li et al., 2017; O'Connell et al., 2010; Peyre Lavigne Moreover, it is lagerly unknown how biofilms develop, which or-
et al., 2016). Typical damages of concrete elements from different ganisms typically compose these communities, how dynamic they
sewer systems caused by MICC are shown in Fig. 1. Annual reha- are over time, and how they interact with the applied concretes.
bilitation costs were estimated to reach over V450 million in Ger- Vise versa, the role of specific physical and chemical concrete
many (Berger et al., 2016) and £85 million in the UK, while the USA properties on microbial growth, subsequent corrosion initiation,
needs to spend around $390 billion within the next 20 years, in and propagation still needs further research. A general description
order to keep the existing wastewater infrastructure operational of biofilm characteristics together with the central physiochemical
(Gutierrez-Padilla et al., 2010). Additionally, hazardous gas pro- aspects of concrete are described in Fig. 2.
duction of mainly hydrogen sulfide (H2S) and carbon dioxide (CO2), To gain a better overview on the multifacetted phenomenona of
but also methane (CH4), ammonia (NH3) and other volatile organic MICC, this review aims to compile the key research findings in the
compounds (VOCs) associated with MICC, represent a severe health field of MICC during the last decade from an interdisciplinary
risk for community workers and wastewater system operators perspective, intertwining advances in concrete materials with
(Gutierrez et al., 2014, 2008; World Health Organisation, 2000). microbiological and hydro(geo)chemical related aspects. This
MICC is a complex process. To efficiently study MICC, an interdis- contribution emphasizes the central role of specific physical and
ciplinary approach that brings together the fields of civil and chemical concrete properties on MICC initiation and propagation,
chemical engineering (material scientists), microbiology, miner- allowing adhesion of microbial cells, microbial growth and subse-
alogy, hydro(geo)chemistry as well as environmental sciences is quent biofilm development. These properties are likely key factors
desired. Intensive research within segregate research areas has for MICC and are central for further research advances and the
produced a wide spectrum of data and hypothesis. To further development of durable materials. Moreover, we summarize po-
promote the emergance of innovations for sustainable building tential additives, such as antimicrobial agents applicable in MICC
material design in wastewater infrastructure efficient cooperation environments. In addition, possible advantages of geopolymer
between scientist from the before mentioned areas is required. concretes, being cement free alternatives, compared to conven-
While the fundamental corrosion processes have been intensly tional cement based building materials, such as Portland cement
investigated (Islander et al., 1991; Jiang et al., 2014a; Ling et al., (OPC) and calcium aluminate cement (CAC) based concretes, are
2015), to date no sustainable product is available, which meets discussed. Due to their acid resistance (Pacheco-Torgal et al., 2014),
the long term requirements in such extremely aggressive and cor- innovative geopolymer technology could represent a significant
rosive sewer environments. Extensive laboratory research and in- step towards the development of sustainable materials for MICC

Fig. 1. Examples of typical deterioration symptoms within systems affected by microbial induced concrete corrosion. Pictures A, B and D were taken in concrete manholes following
power mains, while pictures C and E display damages within wastewater catchment basins.
 C. Grengg et al. / Water Research 134 (2018) 341e352 343

Fig. 2. A framework to understand the main characteristics of biofilms (left side) and physiochemical concrete parameters (right side).

endangered environments. organic molecules); and (v) the multiphase (i.e. gas, liquid and
solid), flow characteristics and retention times of the wastewater
2. Characteristics of wastewater environments inducing MICC (Hvitved-Jacobsen et al., 2013, 2002). Gaseous hydrogen sulfide
(H2S) is formed together with carbon dioxide (CO2), methane (CH4)
MICC can be described as a sequence of biogenic controlled and other VOCs and is partly degassing into the atmosphere of the
sulfate reduction and re-oxidation. Initial sulfide production occurs wastewater piping system, wastewater treatment plants and/or
within the sludge and sediment layers, deposited along the inner pumping stations. The liberation of those volatile components is
surfaces of the piping system, favoring corners and turns, areas governed by changes in the surrounding gas pressure, pH, tem-
with long retention times of the wastewater and low abrasive perature and wastewater turbulences. Intensified gas liberation is
forces. With decreasing oxygen and nitrate concentrations due to favored by transition chutes after power mains and gravity
ongoing fermentation processes, dissimilatory sulfate respiration is wastewater system sections with turns and hydraulic drops
initiated by different strains of sulfate reducing bacteria (SRB), e.g. (Grengg et al., 2016, 2015; Hvitved-Jacobsen et al., 2013; Hvitved-
Desulfovibrio and Desulfomaculum (Barton and Fauque, 2009) Jacobsen and Vollertsen, 2005). Via gaseous diffusion, H2S and
(Fig. 3). Accordingly, sulfides are formed as a side product of CO2 dissolve and accumulate in the moist pore space of the con-
anaerobic oxidation of organic carbon, whereas sulfate is used as an crete (Yuan et al., 2015). Islander at al. (1991) first summarized the
external electron acceptor in the absence of oxygen and nitrate fundamental processes within the aerobic sequence of MICC, pro-
(Jensen, 2009; Jensen et al., 2011). The concentration and chemical posing a 3-step corrosion model (Fig. 4). Since concrete is an
speciation of the produced sulfides is controlled by: (i) tempera- initially strongly alkaline, porous and multiphase material, with an
ture; (ii) pH of the wastewater; (iii) concentration of oxidized sulfur initial pore solution of around pH 13 (Alexander et al., 2013;
compounds in the wastewater; (iv) the biodegradability and Vollpracht et al., 2015), the first stage of corrosion is dominated
composition of the organic matter present (e.g. complex or small by abiotic acid-base reactions. Thereby, the pH reduction of

Fig. 3. Schematic description of the microbial processes occurring within sludge and sediment layers of sewer pipes with decreasing redox potential. Initial fermentation processes
are causing the transformation of complex organic molecules (COM) into low molecule organics (LMO) accompanied by CO2 production. LMO are thereupon consumed during the
sulfate respiration of sulfate-reducing bacteria, as well as during the methanogenesis of methane-producing bacteria under strongly anaerobic conditions, resulting in the pro-
duction of sulfide species (H2S, HS
and S2
), methane (CH4) and CO2 (modified and extended after Grengg et al., 2015).
344 C. Grengg et al. / Water Research 134 (2018) 341e352

1 2 3
Stages abiotic dominated biotic dominated
acid-base reaction oxidation reactions
acid-base reactions/ chemical corrosion chemical + mechanical corrosion
Mineralogical

carbonation
aspects

- cement (Ca(OH)2) - cement (C-S-H-phases, - cement (C-S-H-phases,

Ca(OH)2) Ca(OH)2)
+ sulfate salts (Gp, Ett,
Anh, Bas) - silicatic/carbonate aggregates
+ sulfate salts (Gp, Anh, Bas, Ett*)
+ calcium carbonate + sulfate salts (Gp, Anh, Bas, Ett*)

??? heterotrophic bacteria & fungi

Microbiological

carbonation H2S
aspects

Ca(OH)2+CO2 CaCO3+H2O E organic matter

chemical oxidation of H2S SO4

2-
CO2
thiosulfuric acid
polythionic acid chemoautotrophic bacteria
Environmental parameters

bacterial activity
H 2S
CO2 NSOB ASOB

RH Thiobacillus tioparus
Starkeya novella
Halothiobacillus neopolitanus
Thiobacillus intermedius
T°C Acidithiobacillus ferrooxidans
Acidithiobacillus thiooxidans
corrosion rate /acid generation pH

13 12 11 10 9 8 7 6 5 4 3 2 1 time

Fig. 4. Describes the main mineralogical and microbiological aspects of the aerobic part of MICC sequence, based on an adapted corrosion model of Islander et al. (1991). The initial
stage of corrosion is dominated by abiotic acid-base reaction resulting in carbonation and the formation of weak acids (thiosulfuric and polythionic acid). Within the biotic
dominated part of MICC, a succession of neutrophile sulfur oxidizing bacteria (NSOB) dominate the pore spaces of the concrete, producing sulfuric acid due to oxidation of reduced
sulfur species under humid conditions. Acidophil sulfur oxidizing bacteria (ASOB) dominate within the last stage of corrosion characterized by low pH and high corrosion rates (Ling
et al., 2015; Okabe et al., 2007). Changes in mineralogical compositions during the 3 stages of corrosion are indicated by þ (newly formed minerals) and e (dissolution and
mechanical corrosion of cementitious phases and aggregates). *Ett-Ettringite formation is limited to high pH areas (>10.7) such as the transition zone between non-corroded and
strongly affected concrete layers where alkaline conditions still dominate but sulfate rich pore fluids are already present. Uncertainties within the model, such as the impact of
bacteria within the initial pH reduction, the role of heterotrophs and fungi are highlighted in red. Abbreviations: Gp-Gypsum; Bas-Bassanite; Anh-Anhydrite. (For interpretation of
the references to colour in this figure legend, the reader is referred to the Web version of this article.)

concrete occurs due to carbonation and simultaneous attack of hydroxides and isochronal precipitation of expansive sulfate salts
thiosulfuric and polythionic acids produced by chemical oxidation such as gypsum (Gp), or ettringite (Ett), especially within the
of H2S (Roberts et al., 2002). Described pH reduction is potentially cement rich interfacial transition zones close to the aggregates.
controlled by physiochemical material properties steering abiotic Associated increase in pore pressure results in structural destabi-
oxidation of reduced sulfur species and associated precipitation of lization and crack formation (Grengg et al., 2015; Jiang et al., 2014b;
the latter. Oxidation products formed, such as elemental sulfur (S0) Mittermayr et al., 2015; Scrivener et al., 2004). The transition to the
or thiosulfate (S2O3), provide the energy source for successive biotic second stage of corrosion is marked by the colonization of various
acid production within the latter stages of corrosion (Grandclerc strains of neutrophilic sulfur oxidizing bacteria (NSOB) which adopt
et al., 2017; Sun et al., 2013). To what extend microbial activity the moist concrete surface and pore structure at pH around 9 to 9.5
contributes towards the initial pH neutralization of concrete is still (Islander et al., 1991; Joseph et al., 2012; Satoh et al., 2009; Vincke
under debate. Commonly, it is considered that due to strongly et al., 2000). A succession of at least 4 phylotypes of NSOB with
alkaline conditions present in concrete, the microbial occurrence decreasing pH is reported (Fig. 4). NSOB possess the ability to utilize
within this stage is limited (Joseph et al., 2012). Nevertheless, different sulfur compounds to form sulfuric acid (H2SO4) under
Okabe et al. (2007) reported four times higher pH declining rates on moist conditions (Gomez-Alvarez et al., 2012; Okabe et al., 2007).
the surface of concrete specimen than calculated considering Continued bacterial activity, associated with biogenic H2SO4 pro-
purely chemical neutralization reactions. Such a strong pH reduc- duction and corresponding acidification is causing dissolution of
tion was consequently related to diverse bacterial species (mainly the cementitious matrix and, if present, carbonatic aggregates,
heterotrophic halotolerant and neutrophilic) found on the con- together with neo-formation of sulfate salts and consequent mass
cretes surface. Generally, no loss of material occurs during this first loss of material. The newly formed mineral phases, precipitating
stage, but similar to conventional sulfate attack, the diffusion of from strongly oversaturated interstitial concrete pore solutions, are
sulfate rich pore fluids is triggering initial leaching of calcium rich dominated by expansive gypsum, bassanite (Bas) and anhydrite
 C. Grengg et al. / Water Research 134 (2018) 341e352 345

(Anh) (Grengg et al., 2015; Jiang et al., 2014b). The formation of and cementitious materials. Associated gaps in knowledge have to
secondary ettringite and associated internal cracking, as reported in be bridged by complementary research activities in order to
conventional sulfate attack on concrete, is unlikely within the develop sustainable materials and efficient mitigation strategies for
surface near, low pH areas due to its instability below pH 10.7 MICC environments (Gomez-Alvarez et al., 2012; Okabe et al., 2007;
(Gabrisova et al., 1991; Mittermayr et al., 2015). Additionally, con- Satoh et al., 2009).
crete standard regulations (e.g. EN-206-1) stipulate tri-calcium
aluminate (C3A) free (OPC) cement for concretes used in such 3. Effect of concrete characteristics on MICC
aggressive environments, thereby limiting the aluminum source
central for ettringite formation. Nevertheless, ettringite appearance To date no concrete product exists withstanding the aggressive
is reported in various studies (Jiang et al., 2015; Peyre Lavigne et al., MICC environments over its entire service life but also there is no
2016, 2015a,b). Presumably, secondary ettringite could form within standard regulation for concrete, which recognizes the processes
the transition zone between non-corroded and strongly affected responsible for this specific type of sulfate attack. Contrarily to the
concrete layers where alkaline conditions still dominate but sulfate conventional form of sulfate attack, where concrete degradation
rich pore fluids are already present. There, ettringite formation proceeds due to the interaction between sulfate rich fluids and the
could trigger initial crack formation, thereby actively enhancing concrete, MICC is controlled via the emission and transport of
concrete degradation. Depending on the concrete chemistry, the hazardous gases. Therefore, conventional exposition classes
formation of iron oxyhydroxides, e.g. lepidocrocite (g-FeO(OH)) defined by critical sulfate/acid concentrations within the interact-
and goethite (a-FeO(OH)), and iron hydrosulfates, such as para- ing fluids cannot address the requirements. On the other hand,
butlerite (Fe(SO4)(OH)∙2H2O) within the deterioration layers are researchers have described temperature, relative humidity (RH),
possible (Grengg et al., 2017; Jiang et al., 2014b). The third corrosion H2S and CO2 concentrations as the key environmental parameters
stage begins once a pH of ~4 is reached, as acidophil bacteria are in MICC (Pomeroy and Parkhurst, 1977; Jensen, 2009; Jiang et al.,
starting to dominate the biofilm, with Acidithiobacillus thiooxidans 2015; Nielsen et al., 2006; Okabe et al., 2007; Satoh et al., 2009;
being the most common one (Jiang et al., 2016; Li et al., 2017; Okabe Vollertsen et al., 2008), however variations in single parameters
et al., 2007; Satoh et al., 2009). While the central role of show relatively small effect on durability of investigated concretes.
A. thiooxidans is well described, little information exists regarding Jiang et al. (2015) for example observed a corrosion difference of
the contribution of other bacterial species. Especially the impact of only 10 months for an individually fixed corrosion level (surface
Acidithiobacillus ferrooxidans, a chemoautotrophic ASOB well precipitation of 1gS/m2) to be reached between specimens exposed
known from acid mine drainage environments (Osorio et al., 2013; to 50 and 5 ppm H2S. The expected service life for concrete based
Sugio et al., 1992; Valde s et al., 2008), on corrosion, which is often wastewater systems is up to 100 years, thus 10 months in durability
found within strongly deteriorated systems is under debate (Maeda variation appears insignificantly small. In contrast, large durability
et al., 1999; Yamanaka et al., 2002). While Okabe et al. (2007) re- variations are known to exist between different types of concretes
ported low abundances of the latter ones and consequently low subjected to MICC (Alexander et al., 2013; De Belie et al., 2004;
impact on corrosion processes within their sampling campaign, Girardi et al., 2010; Goyns and Alexander, 2014; Lors et al., 2017;
other studies emphasized their possible impact under suitable Herisson et al., 2013). For instance calcium aluminate cements
conditions (Grengg et al., 2017, 2015; Jiang et al., 2016). This last (CAC) with carbonate aggregates have shown to perform up to 6
stage of MICC is associated with massive loss of material, as re- times more effective than ordinary Portland cement (OPC) based
ported by corrosion rates of >10 mm/year (Grengg et al., 2015; Mori concretes within the same aggressive environments (Goyns and
et al., 1992) (Fig. 4). During the biotic cycle of MICC, the appearance Alexander, 2014; Kiliswa, 2016). Hence, it can be concluded that
and dominance of single SOB (both NSOB and ASOB) is controlled the specific interaction of microorganism with certain materials,
by pH, trophic properties and the ability to utilize different sulfur rather than different levels of other environmental parameters are
compounds, e.g. H2S, S0, S2O3 (Islander et al., 1991; Li et al., 2017). steering the degradation rates of concrete-based construction
Besides SOB, heterotrophic bacteria and fungi have been found in materials in wastewater applications. Accordingly, the prevention
biofilms observed in various deteriorated wastewater systems (Cho of the catalytic microbial growth within concrete is crucial for MICC
and Mori, 1995; Davis et al., 1998; Peyre Lavigne et al., 2015a,b; Nica mitigation. In depth knowledge of the physiochemical concrete
et al., 2000; Vincke et al., 2001; Okabe et al., 2007). The importance parameters and their impact regarding biofilm adhesion, biofilm
of fungi, algae, and lichens in colonization of stone and concrete development and microstructure form the basis for future devel-
buildings especially under extreme environmental conditions is opment of suitable concrete technology for sustainable wastewater
well documented and they are important in biofilm formation and systems. An overview of chemical and physical concrete parame-
stabilization (Flemming et al., 2016). If and how heterotrophs ters controlling MICC is summarized in Fig. 5. To date no systematic
contribute to the corrosion process in wastewater systems still re- study exists focusing on the latter subject matter from a combined
mains uncertain. However, Peyre Lavigne et al. (2015a,b) outlined microbiological and material sciences perspective.
the impact of heterotrophs on O2 mass transfer and their capability The impact of certain physicochemical concrete parameters on
to produce CO2 locally. Alternatively, they could limit the self- MICC initiation and propagation have been recognized from a
inhibition of growth of autotrophic bacteria by consumption of material sciences perspective (De Belie et al., 2004; Girardi et al.,
organic cell material of the latter. Both processes would stimulate 2010; Goyns and Alexander, 2014; Herisson et al., 2014a, 2014b).
autotrophic metabolic activities and associated acid production, Cement/concrete chemistry, water/binder (w/b) ratio or pore size
thus representing important aspects regarding the microbial cycle and distribution could be attributed to process relevant aspects,
during MICC progress. Scrutinizing of metabolic processes as well such as diffusion rates of H2S and CO2, water saturation and acid
as characterization of microbial communities contributing to bio- neutralization capacity, and were subsequently assigned to corro-
film structure is required to better understand the biotic stages of sion rates and material sustainability (Fig. 5). Especially the pore
MICC. Therefore, it is essential to quantify functional capabilities of size distribution and connectivity is central within all types of
heterotroph bacteria and fungi, especially since the contribution of diffusion based transport processes (Vincke et al., 2002). Accord-
the latter is still under debate (Valix and Shanmugarajah, 2015). ingly, new concrete formulations were designed which account for
Detailed knowledge on the metabolic interaction of these micro- those parameters, thereby achieving significant durability im-
organisms is crucial to decipher reactions between such biofilms provements (Herisson et al., 2017; Peyre Lavigne et al., 2015a,b). In
346 C. Grengg et al. / Water Research 134 (2018) 341e352

Fig. 5. Displays an overview of differences in chemical and physical concrete parameters steering microorganism - cementitious material interactions. Different bioreceptivity of
concrete materials was attributed to chemical variations of the different mixing designs during concrete manufacturing and corresponding differences in chemical and physical
material properties.

this context the application of CAC cements has provided signifi- research is needed. Also, little is known about the impact of cement
cant advantages compared to conventional OPC based concretes chemistry on microbial growth characteristics. In this context,
according to standard regulations (e.g. EN 206-1) (Alexander et al., especially the role of Ca for the metabolic cycle of SOB is seen as
2008). This is attributed to i) CACs higher acid neutralization ca- fruitful avenue for future research. Kierek and Watnick (2003),
pacity (Kiliswa, 2016); ii) the formation of an aluminum hydroxide showed the Ca2þ dependency of biofilm development in seawater
gel under acid attack, which is stable above pH 4 and decreases containing mainly gram negative proteobacteria. Accordingly, Ca
porosity and associated ingress of aggressive species; and iii) could also occupy a key position regarding the metabolism of
possibly antibacteriostatic characteristics due to higher Al content phylogenetically similar SOB. Additionally, the influence of surface
(Herisson et al., 2017, 2014a; Valix et al., 2014). Nevertheless, to date conditions like surface roughness and texture, controlled by
a complete inhibition of corrosion could not be achieved. One chemical composition of mortar admixtures as well as the type of
reason for this is that hardly any concrete parameter has been curing applied, on bio-adhesion should be investigated in more
considered for its characteristics regarding biofilm adhesion, details in future studies. The application of possible surface treat-
composition and development. For example, the impact of total ments and sealing methods with focus on applicability in MICC
porosity and pore size distribution on diffusion of aggressive spe- environments should be substance of further research.
cies and water saturation capacity has been extensively studied in To date a variety of organic polymer based sealers are applied to
various applications (Page and Page, 2007). At the same time, in prevent the access of aggressive substances in wastewater net-
order to characterize its effect on biofilm development extended works (Valix and Shanmugarajah, 2015; Kaempfer and Berndt,
 C. Grengg et al. / Water Research 134 (2018) 341e352 347

1998). For instance, the “patch repair no-dig method” is widely

Geopolymer
used for rehabilitation of the concrete pipes where organic polymer
binders allow for rapid repair without pipe excavation or shrinkage
problems. The most widely used water repellent is silane and its
derivatives, e.g. silane-siloxane. While the use of polymer-modified H2O
H2 O
H2 O
Na+ H O
mortars and linings could potentially improve the durability of H2O
H2O
2

concrete sewer pipes in the latter aggressive environments

(Beeldens et al., 2001), its impact and interaction on and with mi-
croorganisms and on associated transformation of harmful gaseous H 2O
H2 O H2O Legend
K+
species is unknown. Presumably, the application of sealing H2O
H2O
H2O
Tetrahedron H2O +
Na
methods described, would potentially contribute towards H2O
H2O

+
H2O
Na
increased accumulations of toxic and odorous substances, e.g. H2S H2O
H2O
H2O

and VOCs, in the pipe atmospheres, eventually representing a po- Acid attack
tential harmful source for continuing operations of wastewater + 2H + Octahedron
OH- or O2-

networks.
Si4+ or Al3+

4. Geopolymer technology for wastewater applications

Geopolymer concretes (GPC) possibly have a great potential as a Degradated Geopolymer

new multi-functional material for the wastewater infrastructure
(Pacheco-Torgal et al., 2014). Due to their geopolymer characteris-
H+
H2O
H2O H2O
+
tics, they potentially combine positive properties of vitreous H2O
Na
H2O
H 2O

ceramic pipes (acid, permeability and abrasion resistance) with

advanced performance of concrete pipes (low temperature mold- + H2O

ing, no dig repair, any pipe diameter possible), while overcoming H2O

H2O
K+
H2 O

H2O

their individual specific limitations at the same time (Ceramic: H +

H2O

brittle, small diameters, dig renewal, higher cost; Concrete: low

durability). Compared to existing concepts for concrete durability
based on neutralization by an inevitable dissolution of a sacrificial
layer thickness, of about 3e10 mm/year (Kiliswa, 2016), GPC exhibit
high acid resistance (Davidovits, 2015; Pacheco-Torgal et al., 2014; Fig. 6. Schematic structural description of geopolymer structure, together with the
Provis et al., 2015). Especially in combination with potential anti- potential degradation of the GP framework due to acid ingress, including ion exchange
microbial properties (see section 5), they may provide a much reactions between Hþ and charge compensating cations (Naþ, Kþ) and the dissolution
of tetrahedral Al from aluminosilicate framework (breaking of Si-O-Al bonds).
longer (stable) barrier against MICC, while acting as an implicit pipe
protection. Traditional, OPC cement-based materials are formed via
the cement hydration reactions to form mainly calcium hydroxide immobilization (Andrejkovicova et al., 2016; Pacheco-Torgal et al.,
(portlandite) and calcium silicate hydrates (C-S-H phases), whereas 2014). Although significant research efforts have already been done
GPC is produced by polycondensation of alumino-silicates. Thereby, so far on GPBs, there is no record of research evaluating the per-
alumina silicate materials (calcined clays, volcanic rocks, blast formance of GPB related to MICC environments, which considers
furnace slag (BFS), fly ash (FA)) are mixed with an alkaline reagent both, the cause and the resulting bio-chemical degradation from a
solutions, e.g. sodium or potassium soluble silicates, water and combined material and microbiological perspective. Therefore, it
stone aggregates to form a hardened concrete-like texture with should be emphasized here that GPC performance has not yet been
similar strength properties (Davidovits, 2013). GPC technology proven in MICC environments. Research so far covered only
avoids the formation of Ca-rich acid-dissolvable hydration prod- empirical GPC tests on acid resistance (Gao et al., 2013; Pacheco-
ucts, as so far present in all cement-based materials, as well as in Torgal et al., 2014). In this context, acid degradation of GPC de-
alkali activated Ca-rich binders, thereby exhibiting high acid pends on the concentration of the acid and can be described as
resistant properties (Provis and van Deventer, 2009). Geopolymer follows (Fig. 6; Table 1):
binders (GPB) build a three-dimensional network of [SiO4]4- and
[AlO4]5- tetrahedrons linked randomly by sharing oxygen atoms 1) ion exchange reaction between the penetrating acid protons
(Fig. 6). Thereby, the negative charge of the [AlO4]5- tetrahedron is (Hþ) and the charge compensating cations (Naþ or Kþ) of the
balanced by additional framework cations (Naþ, Kþ etc.). Possible geopolymer framework (Skv  ara et al., 2012; Ukrainczyk et al.,
chemical and mineralogical reactions of geopolymer binders (GPBs) 2016), along with
compared to different cement-based materials in aggressive biotic 2) dissolution of tetrahedral Al from the aluminosilicate frame-
controlled acidic environments are summarized in Table 1. While work by breaking of SieOeAl bonds and formation of water as a
the chemical resistance of cement-based concretes is based on the by-product, resulting in an increase in solution pH (neutraliza-
acid buffer capacity of their constituents and associated dissolution tion capacity), as well as
of the cementitious matrix and carbonate aggregates, GPB resis- 3) crystallization of zeolites causing some additional strength loss.
tance is governed by ion exchange reactions (absorption, leaching,
de-alumination and zeolite crystallization) and permeability The framework vacancies formed by Al dissolution are mostly
(Table 1). GPBs are considered as analogues of zeolites, due to their re-occupied by Si resulting in the formation of an imperfect
nano-structural similarity, but packed in an amorphous micro- (amorphous) highly siliceous framework that is relatively hard but
structure (Pacheco-Torgal et al., 2014), which enables them to have brittle. Such an undissolved corroded layer could effectively inhibit
analogous applications. Some examples include embodiment of the process of corrosion by acting as a barrier to the transport of
antimicrobial cation additives to sharply reduce bacterial coloni- acid protons as well as dissolved constituents if the shrinkage
zation (Hashimoto et al., 2015), as well as for toxic waste cracks due to the leaching of soluble constituents can be
348 C. Grengg et al. / Water Research 134 (2018) 341e352

Table 1
Comparison of the different binder types regarding compositional changes under acid attack, separating chemical dissolution and precipitation reactions. The cement
chemistry shorthand notation was used to describe the hydration products: C-CaO, A-Al2O3, H-H2O, S-SiO2.

Acid-Base Binder Types

Reactions
Ordinary Portland cement (OPC) Calcium aluminate cement (CAC) Low-Ca geopolymers (GP) Ca-rich geopolymers (GP)

Dissolution Unreacted cement; CAH10; Unreacted precursors; Unreacted precursors;

Ca(OH)2; C2AH8; Naþ/Kþ; Ca and Al from C-A-S-H;
Ca from C-S-H gel; C3AH6; Al and Si from GP gel Fe-phases;
Al-Fe-hydrates; AHx; Mg/Fe anionic clays
CaCO3 Fe-hydrates
Precipitation CaCO3; CaCO3; Carbonates; Sulfate salts (predominant Ca sulfates);
S0; AHx; Sulfate salts (predominant alkalines); Carbonates;
Sulfate salts Sulfate salts; S0 Zeolites; Zeolites;
S0 S0

minimized. Thus, compared to the neutralization capacity, achieved Upon acid attack, the Meþ will be gradually released according
by dissolution of hydration products, the permeability of the to the cation-exchange reaction (Equation (2)), keeping them
acidified GPC layers governs the rate of further ingress of acids. enclosed (minimizing leaching and therefore environmental
Many studies have demonstrated that geopolymers exhibit better problems), but allowing the interaction with microorganisms.
acid attack resistance than Portland cement (Kwasny et al., 2016; Another mechanism for metal incorporation in GP structures con-
Pacheco-Torgal et al., 2014; Provis et al., 2015; Bakaharev, 2005). siders the amphoteric behavior of metals, which in alkaline envi-
The low initial permeability of alkali-activated slag specimens, ronments creates hydroxide aquocomplexes (e.g. [Zn(OH)4]2-) that
along with the low Ca/Si ratio typical in Ca-rich geopolymer are potentially strongly (covalently) incorporated in the geo-
binders, results in a sound layer of aluminosilicate gel even after polymer structure.
decalcification (Provis et al., 2015; Lloyd et al., 2012). Gao et al. Additionally, GPC can add to the pressing need for innovative
(2013) investigated acid resistance of metakaolin, i.e. very low green construction materials, which contributes towards a reduc-
calcium based GPB exposed to 0.01M HCl (pH ¼ 2) for 28 days. High tion of the CO2 footprint associated with cement production. GPB
content of potassium was leached out (exchanged by Hþ) but the raw material production (Metakaolin (MK) and water-glass) cradle
XRD, electron microscopy and mechanical tests showed that the to gate CO2 embodiment is about 70% (Davidovits, 2015) of OPC-
binder network structure remained practically intact still showing based binders and 82% of raw material extraction (Kwasny et al.,
excellent binding properties. In this context, in depth knowledge of 2016). Moreover, the MK production requires much less capital
GPB solubility is central to evaluate the permeability and acid investment in plant and equipment, than cement production. CO2
resistance of GPB based materials. However, predicting the extent emissions for MK production depend on clay purity and crystal-
of dissolution reactions of zeolites, and even more so of GPB, has so linity, calcination and transport to the production site. Recent de-
far been impeded by insufficient thermodynamic data which could velopments include optimized K-based waterglass for improved
not entirely consider the large variations in Si/Al proportions, and workability and efflorescence over Na-based ones, MK sub-
H2O and cation contents. Another aspect controlling the chemical stitutions, and alternative cost-effective waterglass production
resistance of GPCs in aggressive environments is the intrinsic from reuse of SF (Silica fume) and RHA (Rice Husk Ash) (Tchakoute 
ordering present within aluminosilicate gel (Gao et al., 2013; et al., 2016). Partial replacement of MK by reuse of waste materials
Pacheco-Torgal et al., 2014). Accordingly, additional aluminum in (e.g. fly ash (FA), waste FCC catalyst; MK from paper sludge waste
metakaolin-based geopolymer cements might favor their resis- ash, kaolin sludge waste), may enable further decrease of GPC CO2
tance against acid attack (cross-linking gel property) as well as embodiment and cost reduction, as well as improvement in
presumably the biological anergic state. workability and thus reduction in waterglass requirement, while
The nano-structural similarity of GPB with zeolites enables GPB maintaining optimal mechanical properties and durability. More-
to have analogous applications as a carrier of antimicrobial cations over, expected increased durability of GP based products for MICC-
(see in detail section 5), particularly due to their cation-exchange resistant infrastructure, or durable repair mortars, will lower
properties. The potential mechanism of metal ions (Meþ) interac- maintenance cost and result in decreasing overall CO2 embodiment
tion with GPB is proposed in the following equations: for the concrete structure.
Described properties clearly demonstrate the general applica-
½Si
O
Al
O:: :

Kþ þ Meþ 4½Si
O
Al
O:::
bility potential of GPC for wastewater applications. Additionally,
the incorporation of antimicrobial agents into the GPC structure

Meþ þ Kþ
could contribute towards further increase in its MICC resistance
(1) (Hashimoto et al., 2015). Nevertheless, more research, especially
regarding GPC-biofilm interaction is needed in order to verify GPC
½Si
O
Al
O:::

Meþ þ Hþ 4½Si
O
Al
O:::
long-term performance, to characterize possible limitations and to
validate suitable antimicrobial additives.

Hþ þ Meþ (2)
Although having a high potential, GPC applications are not a
The incorporation of Meþ within the geopolymer (GP) network, common practice yet. Lack of data on durability performances and
according to cation-exchange reaction (Equation (1)), can be per- standardization makes the field use of GPC difficult (Provis et al.,
formed in two ways (Hashimoto et al., 2015; Pacheco-Torgal et al., 2015). Cation exchange property of geopolymers have also a
2014): negative effect, e.g. alkalies leach out from geopolymer materials
and form alkali-carbonates (and alkali sulfides in MICC environ-
ments) on the concrete surface, known as efflorescence (Skv  a ra
1) During GP synthesis by addition of metal salts during mixing in
a fresh state; and/or et al., 2012; Pacheco-Torgal et al., 2014). The leaching of alkalis is
2) impregnation of hardened GP with a solution of metal cations. also lowering the pH inside the geopolymer, eventually posing
 C. Grengg et al. / Water Research 134 (2018) 341e352 349

threats to initiate corrosion of steel reinforcement. Alkali hydroxide Contrarily, higher Fe concentration could be positively correlated to
solutions and soluble silicate solutions with SiO2/Na2O molar ratios bacterial activity of A. ferrooxidans and associated acid production
smaller than 1.45 are considered hazardous, which limits the field (Grengg et al., 2017, 2015; Maeda et al., 1999). Diverse studies have
application of geopolymer mixes using such solutions. As the already demonstrated the bacteriostatic effects of different (heavy)
superplasticizer concept for cement dispersion and reducing water metal ions described on the growth of relevant SOBs in various
content in mix designs does not work on geopolymers, new design environments (Ezaka and Anyanwu, 2011; Navarro et al., 2013;
strategies are needed to lower the amounts of activator solutions as Orell et al., 2013) (Table 2). For instance, Navarro et al. (2013)
well as water content for producing denser microstructures determined the minimum inhibitory concentration of Cu, As, Zn,
without impairing fresh concrete rheological properties. The Cd and Ni for different strains of acidophilic bacteria associated
guarantee for no alkali-silica reaction degradation requires again a with a certain relevance regarding biomining, including two strains
low calcium content (Pacheco-Torgal et al., 2014). Shrinkage and of A. caldus and A. ferrooxidans. At the same time, Orell et al. (2013)
creep of geopolymer materials is yet particularly under-explored investigated the tolerance of thermoacidophilic crenarchaeon, used
but an important topic to be studied as well. in high-temperature bioleaching processes, regarding Cd and Cu
concentrations. Negishi et al. (2005) were able to inhibit the growth
5. Antimicrobial agents of five strains of SOB, including A. thiooxidans, completely by the
addition of 50 mM of sodium tungstate to the nutrient solution. In
The successful use of antimicrobial agents has been documented the process, tungsten was bound to the cell structure, thereby
in various applications, ranging from environmental studies inhibiting the activity of the sulfur oxidase of the bacteria and co-
investigating the tolerance of (heavy) metals on Fe(III)-reducing depending cell growth. In a further step 0.075 wt. % calcium
microbial communities in soils (Burkhardt et al., 2011), to the tungstate was added to Portland cement bars and outsourced to a
antimicrobial function of copper coatings in the public sectors (Wei wastewater system with mean H2S concentrations of 28 ppm. Sig-
et al., 2014). Within recent years, antimicrobial additives have also nificant decrease in weight loss for the calcium tungstate bearing
been increasingly used in conventional concretes (Vincke et al., mortars could be observed, demonstrating the inhibitory effect of
2001). For instance Alum et al. (2008) studied different antimi- W on the growth of SOBs present. At the same time a bacteriostatic
crobial formulations containing FA, silica fume (SF), ZnO, Cu-slag, impact of Al on microbial growth is proposed as one of the reasons
ammonium and bromide. They demonstrated by field and labora- for higher durability of CAC-based materials observed in MICC
tory tests that concrete mixtures containing 10% ZnO had compa- environments (Herisson et al., 2017, 2013). Alternatively, the
rable antimicrobial properties similar to commercial biocides. application of zeolites exchanged with Meþ could provide a
Accordingly, bacteriostatic characteristics of (heavy) metal ions promising substitute for concretes suitable for aggressive waste-
could provide novel, sustainable and economic answers to many water systems (Inoue et al., 2002; Kaali et al., 2011; Zhang et al.,
aspects of biodeterioration, but especially for MICC environments 2009). Kaali et al. (2011) investigated the influence of Agþ, Zn2þ
(Gu et al., 2011). A summary of the relevant studies on the effects of and Cu2þ exchanged zeolite on antimicrobial and long term in vitro
potential antimicrobial agents in MICC relevant settings is pre- stability of medical grade polyether polyurethane, finding that the
sented in Table 2. binary Cu/Zn system had the same bacteriostatic efficiency as the
The toxic effect of (heavy) metal ions (Meþ) on bacteria is based single silver systems. The synergetic effect was explained by
on Meþ reactions with the negatively charged cell walls of bacteria different toxic mechanisms within the cell initiated by the indi-
and associated formation of complex compounds within the bac- vidual metal cation. Accordingly, they concluded that zeolites
terial membrane. These reactions are suggested to inhibit life exchanged with metal cations exhibit a high potential technology
essential activity of sensitive enzymes, as well as to disturb the to enhance antimicrobial properties of materials. Alternatively,
osmotic stability of the cell, resulting in the leakage of intracellular Hashimoto et al. (2015) have shown that the antimicrobial activity
constituents (Nies, 1999). The inhibitory efficiency and applicability of metakaolin GP's against fungi hyphae could be significantly
of Meþ on microbial growth in MICC environments is based on their increased by the incorporation of copper ions into the GP structure,
solubility (and/or ion exchange) function under acid attack condi- due to immersing the latter in a 0.1 M copper chloride solution for
tions, their affinity to sulfur, their interaction with microbiological 24 h. In both contexts, the antimicrobial mechanism of metal cation
populations, as well as on their geochemical abundances (Nies, loaded zeolites is based on cation exchange reactions, during which
1999). Therefore, the range of Meþ, possibly eligible as antimicro- the inorganic molecular sieves trap the antibacterial metals,
bial agents for wastewater networks can be limited to Al, Fe, Mo, keeping them enclosed and thus minimizing leaching and associ-
Mn, Zn, Ni, Cu, V, Co, W and Cr. Since Fe and Mn are always present ated environmental problems, but allowing the interaction with
in significant concentrations within concrete admixtures, they are microorganisms (as explained in detail within the section on
not seen as decisive for achieving the desired bacteriostatic effects. Geopolymers).

Table 2
Summary of relevant studies describing the effects of Meþ, utilized as antimicrobial agents in various applications, with special focus on relevant bacterial species such as SOB.

Setup Material Metal addition Conclusion/Effect Reference

in situ experiments OPC Ni Significant inhibitory effects on different strains of neutrophile bacteria (Negishi et al., 2005)
in situ experiments OPC CaWO4, Ni Complete inhibition of growth of 5 differentstrains of Acidithiobacillus spp. from (Negishi et al., 2005)
concentrations >50 mM
laboratory testing OPC Ni, W, ZnSiF6 Suppressed growth of diverse SOBs (Kim et al., 2009)
field and laboratory OPC ZnO, Cu-slag, Br, Mixtures containing 10% ZnO had similar bacteriostatic properties as commercial biocides. (Alum et al., 2008)
testing NH4
laboratory testing MK GP Cu Suppressed growth of oyster mushrooms (Hashimoto et al.,
2015)
laboratory testing GP Ag 99% mortality for gram positive/negative bacteria (Adak et al., 2015)
laboratory testing Zeolites Ag, Zn, Cu Binary Cu/Zn same bacteriostatic efficiency as Ag (Kaali et al., 2011)
laboratory testing PPC Cu 95% mortality of E. coli after 4 h contact (Delgado et al., 2011)

GP…geopolymer; MK GP...metakaolin geopolymer; OPC…ordinary Portland cement; PPC...polypropylene composites.

350 C. Grengg et al. / Water Research 134 (2018) 341e352

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