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lable at ScienceDirect Journal of Cleaner Production 247 (2020) 119495 Contents lists avai Journal of Cleaner Production journal homepage: www.elsevier .com/locate/ jc lepro Review Feasibility of alternative sewage sludge treatment methods from a lifecycle assessment (LCA) perspective Soon Kay Teoh a, Loretta Y. Li b, * a National Environment Agency, 40 Scotts Road, Singapore, 228231, Singapore b Department of Civil Engineering, University of British Columbia, 6250 Applied Science Lane, Vancouver, B.C, V6T 1Z4, Canada a r t i c l e i n f o Article history: Received 26 June 2019 Received in revised form 8 October 2019 Accepted 27 November 2019 Available online 29 November 2019 Handling editor. Prof. Jiri Jaromir Kleme�s Keywords: Sewage sludge treatment Lifecycle assessment (LCA) Environmental pollutants Toxicity potentials Decision-making score * Corresponding author. E-mail address: lli@civil.ubc.ca (L.Y. Li). https://doi.org/10.1016/j.jclepro.2019.119495 0959-6526/© 2019 The Authors. Published by Elsevier a b s t r a c t Sewage sludge treatment and disposal are critical global issues, with concerns including sludge volume/ weight, release of pollutants, and other environmental impacts. This study develops a semi-quantitative assessment methodology for selecting appropriate sludge treatment options on the basis of a lifecycle assessment approach. Variousbiological, chemical, thermal, and thermo-chemical sludge treatmentmethods described in the literature are reviewedand evaluatedholistically byadopting the developedmethodology to determine their comparative effectiveness in reducing sludge volume/weight and environmental impacts. Anaerobic digestion, pyrolysis, and supercritical water oxidation are found to be the best-performing treat- ment methods. They are not only more effective in reducing sludge volume/weight and pollutants but also have lower global warming and toxicity potential compared to most of the other methods reviewed. The potential for adverse environmental effects remains owing to the release of pollutants when the products of sludge treatment are utilised, e.g. as soil amendments or fuel. This necessitates further investigation to explore the toxicity impacts of a wider array of emerging pollutants from a lifecycle perspective as well as further development of sludge treatment methods to overcome the drawbacks of existing methods. © 2019 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/). Contents 1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2 2. Approach and methodology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3 2.1. Feasibility assessment approach . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3 2.2. Methodology for assessing effectiveness and environmental impact . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3 2.3. Five-point scale scoring system . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4 3. Results and discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5 3.1. Effectiveness in reducing sludge volume/weight . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5 3.2. Effectiveness in reducing, removing, or stabilising pollutants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6 3.3. Global warming potential (GWP) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9 3.3.1. Effects of end-use and final disposal . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9 3.3.2. Net energy/fuel consumption/substitution . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12 3.4. Toxicity potentials (TPs) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13 4. Overall assessment and limitations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15 5. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 Funding . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 Supplementary data . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/). http://creativecommons.org/licenses/by-nc-nd/4.0/ mailto:lli@civil.ubc.ca http://crossmark.crossref.org/dialog/?doi=10.1016/j.jclepro.2019.119495&domain=pdf www.sciencedirect.com/science/journal/09596526 http://www.elsevier.com/locate/jclepro https://doi.org/10.1016/j.jclepro.2019.119495 http://creativecommons.org/licenses/by-nc-nd/4.0/ https://doi.org/10.1016/j.jclepro.2019.119495 Abbreviations AETP aquatic ecotoxicity potential ARDP abiotic resource depletion potential ASR automotive shredder residue BDE-209 decabromodiphenyl ether COD chemical oxygen demand DEHP diethylhexyl phthalate DEET N,N-Diethyl-meta-toluamide/N,N-Diethyl-3- methylbenzamide EP eutrophication potential ETP ecotoxicity potential GWP global warming potential HTP human toxicity potential LAS linear alkyl-benzene sulphonates LCA lifecycle assessment PAH polycyclic aromatic hydrocarbonPBDE polybrominated diphenyl ether PCB polychlorinated biphenyl PCDD/F polychlorinated dibenzo-p-dioxin and dibenzofuran PFOA perfluorooctanoic acid PFOS perfluorooctanesulphonate/sulphonic acid PPCP pharmaceuticals and personal care products RDF refuse-derived fuel SSRI selective serotonin re-uptake inhibitors SCWO supercritical water oxidation SWG supercritical water gasification TCLP toxicity characteristic leaching procedure TETP terrestrial ecotoxicity potential TP toxicity potential TSS total suspended solids TEQ toxic equivalent VOC volatile organic compound VS volatile solids VSS volatile suspended solids S.K. Teoh, L.Y. Li / Journal of Cleaner Production 247 (2020) 1194952 1. Introduction Population growth, urbanisation, industrialisation, and inade- quate wastewater management practices are resulting in critical unresolved challenges in municipal wastewater management. The increased adoption of secondary and tertiary wastewater treatment in recent decades has led to the emergence of twomajor challenges. First, the conventional activated sludge process, which is the most widely used biological process in secondary wastewater treatment (Wei et al., 2003), produces large amounts of excess sludge. Total sludge production in China showed an average annual growth of 13% from 2007 to 2013 (Yang et al., 2015). 6.25 million tonnes of dry solids were produced in China in 2013, while 13.8 million tonnes of dry sludge per year was captured during wastewater treatment in the United States (Seiple et al., 2017). The European Commission (2008) estimated that sewage sludge production in the European Union (EU) would amount to about 12 million tonnes of dry solids per year by 2020. The treatment and disposal of sludge is expensive, accounting for up to 60% of the total cost of wastewater treatment (Horan, 1990; Di Iaconi et al., 2017). The use of landfilling for final disposal has declined owing to the lack of available land, although ash from sludge incineration is generally destined for landfills because of its high heavy metal content (Wei et al., 2003). Similarly, land application of treated sludge has become increasingly restricted owing to environmental concerns regarding legacy or recalcitrant pollutants in the sludge (Aparicio et al., 2009; Alvarenga et al., 2017). These pollutants include heavy metals and organic pollutants, such as pharmaceuticals and personal care products, hormones, pesticides (Margot et al., 2015), persistent organic pollutants (POPs) (Hamid and Li, 2016), and emerging pollutants, e.g. phthalates and phenolics (H€ohne and Püttmann, 2008; Gao and Wen, 2016). In the EU, the extent of use of land- filling as a sludge disposal method declined from 15% in 2005 to 7% in 2015 and that of agricultural application decreased from 43% in 2005 to 28% in 2015, while that of sludge incineration increased from 21% to 38% over the same period (Gutjahr andMüller-Schaper, 2018). Second, conventional secondary wastewater treatment pro- cesses are known to play a key role in the environmental cycling of pollutants (Hamid and Li, 2016). Although conventional wastewater treatment removes substantial proportions of volatile and biodegradable pollutants, and although it is not designed or optimised for such purposes (Clara et al., 2007; Mailler et al., 2014a, 2015), hydrophilic or refractory organic compounds remain in the treated wastewater at ng/Lemg/L levels (Loos et al., 2013). A more severe problem may be encountered in the case of treated sewage sludge, in which pollutants with low aqueous solubility, high hy- drophobicity, and limited biodegradability persist. For example, over 60%e90% of the total polybrominated diphenyl ethers (PBDEs) detected in influent wastewater accumulates in sewage sludge in wastewater treatment plants (North, 2004; Song et al., 2006; Deng et al., 2015). Table SIe1 provides a summary of the pollutants typically contained in sludge. Therefore, there is an urgent need for treatment methods that not only reduce sludge quantities but also remove, stabilise, or reduce the pollutants found in the sludge. The choice of such methods requires holistic assessment, often involving a difficult decision-making process that weighs competing concerns, such as effectiveness and environmental impact. The importance of considering the technical and environmental sustainability of so- lutions has been recognised (Moe and Gangarosa, 2009), alongwith other factors such as cost, especially in less developed economies. In their assessment of progress towards achieving the United Na- tions (UN) Millennium Development Goal (MDG) of doubling ac- cess to sanitation facilities, UNICEF and World Health Organization (WHO), 2015 reported that despite some progress, large disparities in access to such facilities remain between the rich and the poor. Lack of access to sanitation and wastewater treatment facilities intensifies the above-mentioned challenges. The main objective of this review is to develop a semi- quantitative methodology to evaluate various existing methods for managing municipal wastewater sludge and reducing disposal impacts. In particular, this study aims to identify sludge treatment methods and assess their feasibility in terms of effectiveness and environmental impact. Feasibility is assessed in terms of four fac- tors, namely (i) effectiveness in reducing sludge volume/weight, (ii) effectiveness in reducing, removing, or stabilising pollutants, (iii) environmental impact based on lifecycle assessment (LCA) of global warming potential (GWP), and (iv) environmental impact based on LCA of toxicity potentials (TPs), including human toxicity, terrestrial S.K. Teoh, L.Y. Li / Journal of Cleaner Production 247 (2020) 119495 3 ecotoxicity, and aquatic ecotoxicity potentials (HTP, TETP, AETP). Effectiveness in reducing sludge volume/weight was chosen as one of the factors to determine feasibility because of the high cost of sludge treatment and disposal (Horan, 1990; Di Iaconi et al., 2017). Effectiveness in reducing, removing, or stabilising pollutants was also chosen owing to the risk of environmental cycling of pollutants arising from sludge disposal (Hamid and Li, 2016). We have also included environmental impact based on LCA of GWP and TPs, as LCA has been extensively used to quantify the environmental impact of sludge treatment processes (Hospido et al., 2005) and GWP and TPs have attracted considerable attention in such studies on sludge treatment and disposal. Based on a review of the data compiled from the literature, an assessment methodology is developed and used to define and evaluate effectiveness and environmental impact. In summary, this review contributes towards improving our understanding of the relative feasibility of various sludge management methods. In addition, the proposed assessment method will be a useful decision-making tool for selecting appropriate options for imple- mentation in a particular case. 2. Approach and methodology 2.1. Feasibility assessment approach Fig. 1 shows a diagrammatic representation of the approach adopted in this study. Previous research was broadly reviewed by collecting papers from the Web of Science website (http://apps. webofknowledge.com), as well as the ScienceDirect and Scopus databases. Multiple keywords related to the effectiveness and environmental impact of sludge treatment methods, such as “life- cycle assessment (LCA)”, “sludge treatment”, “sludge disposal”, “sludge volume reduction”, “pollutant reduction”, “environmental impact”, “global warming potential (GWP)”, and “toxicity potential (TP)”, were used as topic queries. A full list of keywords used is provided in Table SIe2. The collected papers were examined and included in the review if considered relevant. Papers citing or cited by each relevant paper collected using the topic queries were also included if they were considered appropriate. For the purposes of this review, sludge treatment methods were considered to consist of three steps (Fig. 2): (A)pre-treatment, (B) the actual treatment process, and (C) product end-use or disposal. Each step may incorporate one or more processes; in particular, the actual treatment step may incorporate one or more biological, chemical, thermal, or thermo-chemical treatment processes. Two important technical aims of the treatment process, in addition to those that are the focus of this review, are the elimination of Sewage sludge from secondary wastewater treatment Reduc on of sludge volume o Aims of Sludge Treatment Me Reduc on, removal, or stabili pollutants in sludge Fig. 1. Feasibility assessm pathogens remaining after the secondary treatment process and the recovery of materials or energy. Tertiary biological nutrient removal processes, which mainly aim to remove or recover nitro- gen and phosphorus, can be incorporated before the steps shown in Fig. 2, but they are beyond the scope of this review, even though they may offer some benefits. Other possible pre-treatments, such as ozonation before anaerobic digestion (Carballa et al., 2011), are also beyond the scope of this review. The benefits of material or energy recovery may be reflected in reduced environmental impact under LCA. 2.2. Methodology for assessing effectiveness and environmental impact Effectiveness is defined as the reported percentage reduction in sludge volume/weight, or pollutant mass or concentration, over the “conventional” process with which the treatment method was compared in the original study. Environmental impact is assessed via comparison with the re- sults of LCA conducted by the original researchers. Environmental LCA is a tool for comprehensively evaluating the environmental impacts of processes, services, or goods (collectively termed as products) throughout their lifecycles (Hospido et al., 2005), and it has been extensively used to quantify the environmental impact of sludge treatment processes. Evaluation using LCA is important for elucidating the overall impact of sludge treatment and thus facili- tating an examination of trade-offs by considering lifecycle im- pacts. For example, a certain sludge treatment method may be effective in reducing or stabilising certain pollutants, but it may produce other pollutants. LCA compares such relative effects across multiple treatment methods by using a common unit of measure- ment and is thus useful for measuring the overall impact. As the numerical magnitudes of LCA impact potentials (or category in- dicators) are determined to a large extent by the methodologies and assumptions adopted and by the geographical context, they are first assessed within the context of each study before comparisons are drawn across studies. Guine�e et al. (2001) identified several impact categories relevant to sludge treatment, such as GWP, TPs, abiotic resource depletion potential (ARDP), and eutrophication potential (EP). In our review, we assess only GWP and TPs, because they have attracted consid- erable attention in studies on the lifecycle environmental impacts of sludge treatment, possibly reflecting a greater overall concern with regard to these two factors. Further, the effectiveness of a sludge treatment method in reducing or stabilising pollutants is linked to the magnitude of its TPs. Although ARDP has been widely discussed in the scientific literature, it may be correlated with GWP (i) Effec veness r weight thods Feasibility Assessment Factors for Sludge Treatment Methods (ii) Environmental impact (LCA) (a) Sludge volume or weight reduc on (b) Reduc on, removal, or stabilisa on of pollutants (a) Global warming poten al (b) Toxicity poten als sa on of ent methodology. http://apps.webofknowledge.com http://apps.webofknowledge.com A. Pre-Treatment 1. Thickening Waste-ac vated sludge 2. Dewatering B2. Chemical Treatment 2. Incinera on 4. Mel ng 5. Pyrolysis 2 Incinera 1. Drying B1. Biological Treatment 1. Anaerobic diges on 2. Co-diges on C. End-use or Disposal 2. Land/agricultural applica on 3. Fuel 1. Landfill 4. Material 1 D i B3. Thermal/Thermo-chemical Treatment 1. Lime stabilisa on 7. Supercri cal water oxida on 8. Wet oxida on 3. Compos ng/aerobic diges on 4. Constructed wetlands 3. Co-incinera on 6. Gasifica on 9. Hydrothermal processes Fig. 2. Processes for recovery of material and energy from sludge. S.K. Teoh, L.Y. Li / Journal of Cleaner Production 247 (2020) 1194954 if non-renewable energy use results in greenhouse gas emissions that contribute significantly to the overall GWP. Other potentials have not been discussed extensively. It should be noted that the studies reviewed in this paper assess TPs from a lifecycle perspective. TPs, measured in units of reference chemicals, are calculated indices based on both the inherent toxicity of substances and their potential doses, and are used to weight emissions inventoried as part of an LCA (Hertwich et al., 2001). The potential dose of a chemical can be calculated using a generic fate and exposure model, which determines its distribution in a model environment and accounts for different exposure routes, such as inhalation, ingestion, and dermal contact with water and soil (Hertwich et al., 2001). The LCA-based TPs discussed in this review are thus defined differently from toxicities derived through toxicological risk assessments, which are based on hazard quotients and cancer risks (Volosin and Cardwell, 2002). Most original studies presented their LCA findings of impact potentials in graphical form, as plots of un-normalised, normalised, or weighted values. When actual numerical values were not available, the values were estimated as accurately as possible from these plots. Owing to the difficulty in making meaningful com- parisons across numerous normalisation or weighting methods, only un-normalised values were assessed and compared. As most studies investigated mid-point impacts (rather than end-point impacts), these impacts were considered. The majority of the original researchers selected one tonne of dry solids (t-DS) as the functional unit (FU). Un-normalised values are presented in the units of measurement used in the original studies; if possible, the units are converted into kg-CO2e/t-DS for GWP and kg-1,4-DCB-eq/ t-DS for TPs. 2.3. Five-point scale scoring system This study developed a scoring system based on a semi- quantitative Likert-type five-point scale (Cartmell et al., 2006) to assign a relative numerical score to each of the four feasibility factors assessed. The scoring system enables decision-makers to holistically consider multiple feasibility concerns of the methods in a relatively simple manner. Methods that performwell are assigned positive scores, whereas those that perform poorly are assigned negative scores. The methods are scored against each feasibility factor on a scale of�2 (very negative) through 0 (neutral, or balance of negative and positive) toþ2 (very positive). As themagnitudes of volume/weight reduction, pollutant reduction, and LCA impact potentials often cannot be meaningfully compared across studies, scoring is based on comparisons between different sludge treat- ment methods within each reviewed study. For the LCA impact potentials, it should be noted that scores are given on the basis of the magnitude of the net rather than the gross impact potentials; for example, a better score is given to a treatment method with compensating factors that reduce an otherwise high GWP or toxicity to a negative impact potential, than to another treatment method with low GWP or toxicity without any compensating fac- tors. Semi-quantitative numerical scores for the two effectiveness S.K. Teoh, L.Y. Li / Journal of Cleaner Production 247 (2020) 119495 5 factors and for GWP and TPs are given according to the matrix shown in Table 1. The semi-quantitative scores are then converted into a single overall score for each treatment method by considering the four feasibility factors as a whole. A single overall score further aids decision-makers in feasibilityappraisal. The maximum potential overall score for any treatment method is þ2; conversely, the minimum is �2. Decision-makers can use the same scoring system and tailor it to their needs by assigning their ownweights according to what they consider important in their respective contexts. It should be noted that sensitivity analysis is beyond the scope of this paper, as only a few of the studies reviewed have included a thor- ough discussion on the sensitivity of their findings. Previous research has focused on the assessment of one or more feasibility concerns of a single sludge treatment method or com- binations of sludge treatment methods in various geographical contexts, as well as on the basis of various modifications spurred by environmental regulatory requirements. In this paper, we assess and review the findings of 67 studies published between 2000 and 2018, identified through a literature search. Tables SI-3 and SI-4 summarise these studies, while Table SIe5 summarises the func- tional units, lifecycle stages, and system boundaries considered in each study. It should be noted that the sludge treatmentmethods in Tables SI-3 and SI-4 include only methods within the boundaries of the systems assessed by the studies, whereas the process steps that occur outside the system boundaries are excluded from the table. Evaluating and comparing the findings facilitates elucidation of the trends in the effectiveness and environmental impacts of the sludge treatment methods, as observed and analysed across studies. The following sections discuss these trends as well as the relative feasibility of the various sludge treatment methods. 3. Results and discussion 3.1. Effectiveness in reducing sludge volume/weight Among biological treatment methods, anaerobic digestion is known to perform relatively well, resulting in substantial destruction of volatile solids (VS) and decrease in sludge dry weight. The typical range of values for VS destruction in mesophilic anaerobic digestion was reported to be 40%e50% (European Commission, 2001b). In a study to investigate the effect of adding Table 1 Assessment matrix for effectiveness and environmental impact. Score Effectiveness Sludge volume/weight reduction Pollutant reduction, removal, or s þ2 High volume/weight reduction relative to other sludge treatment methods High reduction, removal, or stabi range of organic pollutants and h relative to other sludge treatmen þ1 Moderate volume/weight reduction relative to other sludge treatment methods Moderate reduction, removal, or some pollutants relative to other methods 0 Little or no change in volume/weight relative to sludge that has not been treated with the method in question Little or no change or improveme concentrations, quantities, leacha destabilisation, or effects uncerta relative to sludge that has not bee method in question �1 Moderate increase in volume/weight relative to other sludge treatment methods Moderate increase in pollutant co quantities, leachability, or destab pollutants relative to other sludg methods �2 Large increase in volume/weight relative to other sludge treatment methods Large increase in pollutant conce quantities, leachability, or destab pollutants relative to other sludg methods crude glycerol on sludge digestion efficiency, it was found that, even without such addition, the sewage sludge dry weight decreased by around 20% within 6 days of reaction, while the VS destruction was around 11% (Kurahashi et al., 2017). Aerobic digestion and composting also achieve volume/weight reduction through moisture removal and partial conversion into gaseous products and heat. Salsabil et al. (2010) found that anaer- obic digestion slightly out-performed aerobic digestion in terms of the total suspended solids (TSS) removal yield for all scenarios investigated (i.e. with or without pre-treatment). The TSS removal yield for aerobic digestion was 57%e76% while that for anaerobic digestion was 66%e86%. Pre-treatment steps before biological treatment, such as ultrasound treatment and ozonation, promote solubilisation and lysis, thereby enhancing VS reduction (Salsabil et al., 2010); however, these technologies are beyond the scope of this review. Co-digestion with high-organic-content waste can improve the activity of micro-organisms owing to the higher volatile-to-total solids ratio (Kurahashi et al., 2017), leading to greater VS destruc- tion. In an investigation of the co-digestion of dewatered sewage sludge and food waste at various mixing ratios and solid retention times (SRT), Dai et al. (2013) found that an increase in the food waste ratio resulted in greater VS reduction. For example, at an SRT of 20 days, the VS reduction was 32.1 ± 1.1% for 100% dewatered sludge, but when food waste was added and mixed in at a sludge- to-food waste ratio of 2.4:1, the VS reduction improved to 45.5 ± 1.0%. At even higher food waste percentages (e.g. sludge-to- food waste ratio of 0.9:1), the VS reduction improved further (to 58.1 ± 0.8%). The main functions of lime stabilisation are the reduction of the microbial content of sludge and reduction of heavy metal avail- ability (Wong and Selvam, 2006). Lime stabilisation is included in this review owing to its ability to stabilise heavy metal leaching. The addition of lime does not lead to volume/weight reduction; instead, it increases the overall volume/weight of the sludge (dis- countingmoisture loss due to dewatering or drying). In terms of the typical amount of lime added to sewage sludge, the European Lime Association recommends addition of 50%e90% CaO per unit dry solids for 75 min to treat sludge at >55 �C and pH > 12, or the addition of 20%e40% CaO or equivalent Ca(OH)2 per unit dry solids for 3 months. A correspondingly large increase in weight can thus be expected. Furthermore, any high-pH leachate after landfill Environmental Impact (LCA Impact Category) tabilisation Global Warming Potential (GWP) Toxicity Potentials (TP) lisation for a wide eavy metals t methods Very low or negative GWP or TP relative to other sludge treatment methods stabilisation for sludge treatment Moderately low or negative GWP or TP relative to other sludge treatment methods nt in pollutant bility, or in or variable, n treated with the Average GWP or TP relative to other sludge treatment methods ncentrations, ilisation for some e treatment Moderately high GWP or TP relative to other sludge treatment methods ntrations, ilisation for many e treatment Very high GWP or TP relative to other sludge treatment methods S.K. Teoh, L.Y. Li / Journal of Cleaner Production 247 (2020) 1194956 disposal can produce an adverse environmental impact, necessi- tating additional control steps to bring the pH within environ- mental regulation limits (e.g. B.C. Reg. 63/88 O.C. 268/88). In general, thermo-chemical treatment methods are among the most effectivemethods for reducing sewage sludge volume/weight, particularly for high-temperature treatment, such as incineration, pyrolysis, and gasification processes. Incineration was reported to reduce the volume of the sludge cake by up to 96% to stabilised ash (Vesilind and Ramsey, 1996). Pyrolysis, which is the process of thermal degradation in an inert atmosphere generally occurring at a temperature range of 300e900 �C (or even higher), reduced the volume of sewage sludge at 5.2 wt% moisture by around 40%e50% to carbonaceous residues (Inguanzo et al., 2002). Hwang et al. (2007) found that the reductions of sewage sludge weight by py- rolysis and incineration were very similar, i.e. 63% and 62%, respectively. The principal stages of gasification, which converts carbonaceous content into combustible gas and ash in a net chemically reducing atmosphere, include drying, pyrolysis, oxida- tion, and reduction. Thus, while reliable estimates of volume reduction by gasification have not been uncovered in the literature review, they are expected to be similar to those achieved by pyrolysis. Hydrothermal carbonisation (~180e250 �C)and hydrothermal liquefaction (~250e400 �C) processes, which aim to recover solid carbonaceous fuel (i.e. hydrochar) and liquid bio-oil, respectively, appear to reduce sludge weight to a somewhat lower extent than incineration, pyrolysis, and gasification. Hydrothermal carbon- isation was reported to recover around 60% of the input solid mass in the form of hydrochar (He et al., 2013). With the addition of various organic and inorganic additives at 10 wt% to sewage sludge at a moisture content of 85 wt%, the quantity of solid residues from hydrothermal liquefaction was around 12.8e22.6 wt% of the total product weight (Qian et al., 2017). Sub/supercritical water gasifi- cation (�400 �C and >400 �C respectively) appears to generate a lower average proportion of solid residue compared to that generated by hydrothermal carbonisation and hydrothermal liquefaction, but this output seems to vary considerably. Li et al. (2012) reported that the amount of solid residue obtained in sub/ supercritical water gasification from completely dewatered sewage sludge (original moisture content estimated to be >80%) was around 68%e69% of the sludge dry weight (Li et al., 2012), while Zhang et al. (2010) reported solid residues of <30% of the original sludge dry weight by supercritical water gasification. Therefore, it should be noted that the amount of solid residue recovered from supercritical water gasification depends significantly on factors such as operating temperature and the physical and chemical characteristics of the sludge (Zhang et al., 2010). Both supercritical water oxidation (SCWO) and wet oxidation are expected to leave primarily inorganic residues, as the processes are reported to effectively oxidise organic matter primarily to carbon dioxide, water, and nitrogen (Svanstr€om et al., 2004, 2005; Houillon and Jolliet, 2005). The combined processes of supercritical water gasi- fication and SCWO were reported to reduce the weight of sludge solids to 3.5% of the initial weight (Qian et al., 2015). While numerical values for sludge volume/weight reduction for other thermal and thermo-chemical methods have not been un- covered in the literature review, some inferences can be drawn with regard to the extent of volume/weight reduction. In sludge melting, sludge is heated to 1200e1500 �C; at such temperatures, organic matter is burnt and the remaining inorganic matter be- comes a liquid, which solidifies into a glass-like slag upon cooling (Smith, 1992). As combustion temperatures are higher than incin- eration temperatures (leading to more complete combustion) and the slag is expected to be of higher density than incinerator ash, a greater volume reduction is attained than that in the case of incineration (Smith, 1992). Drying reduces the volume/weight contributed by the sludgemoisture content. Reductions by as much as >85 wt% dry solids may be required for certain applications, such as pre-treatment for pyrolysis or gasification (Spinosa et al., 2011) and land spreading (Lowe, 1995). However, because chemical conversion of solids to liquid or gaseous products does not occur to a significant extent, the extent of volume/weight reduction is ex- pected to be less than that for thermo-chemical treatment methods. Table 2 summarises the effectiveness of sludge treatment methods in reducing sludge volume/weight, as well as in reducing, removing, or stabilising pollutants, and it suggests scores based on their comparative effectiveness. Incineration, pyrolysis, and gasifi- cation, which involve the complete removal of moisture and partial conversion of solids into gaseous and/or liquid products, lead to the greatest volume/weight reduction and have the highest score (þ2). A score of þ2 is given for the combined process of SCWO and wet oxidation owing to the significant volume/weight reduction re- ported (Qian et al., 2015). These methods are followed closely by hydrothermal carbonisation, liquefaction, and sub/supercritical water gasification, which are given the same score of þ2. Digestion processes result in substantial destruction of the VS/TSS and decrease in the sludge dry weight, but they are given a slightly lower score (þ1), as they do not perform as well. A score of �2 is given to lime stabilisation owing to the large resultant increase in weight. 3.2. Effectiveness in reducing, removing, or stabilising pollutants Anaerobic digestion has been found to effectively degrade some pharmaceuticals and reduce the level of polychlorinated biphenyls (PCBs). However, there is some uncertainty regarding the fate of other organic pollutants, and anaerobic digestion is unable to biodegrade pollutants containing heavy metals. In particular, anaerobic digestion (both mesophilic and thermophilic) was found to be effective in reducing a range of pharmaceutical organics (including selective serotonin re-uptake inhibitors (SSRIs) and oestrogens/endocrine disruptors), with an average reduction of around 30% (Malmborg and Magn�er, 2015). Rosi�nska and Dąbrowska, 2014 found that anaerobic digestion could effectively biodegrade both highly and less brominated PCB congeners in digested sludge products. The test sludge mixture was enriched with PCB congeners 28, 52, 101, 118, 138, 153, and 180 to initial concentrations of 151.0e375.3 mg kg�1 dry matter. After 21 days, the PCB congener concentrations decreased to 45.3e48.5 mg kg�1 dry matter (with concentrations in the control staying nearly the same). However, it should be noted that 21 days were required for this decrease; after 7 days of digestion, the PCB congener concen- trations remained the same (150.2e374.1 mg kg�1 dry matter), while only partial degradation was attained after 14 days (to 67.9e231.8 mg kg�1 dry matter). This may pose problems if suffi- cient time is not allowed for less brominated congeners to degrade, as some of them (e.g. PCB-77, PCB-126, and PCB-169) are toxic (Ahlborg et al., 1994). On the other hand, the ability of anaerobic digestion to reduce other pollutants is less certain. Mailler et al. (2014b) investigated the fate of a wide range of pollutants in anaerobically digested sludge, including organotins, pesticides and herbicides, benzene- based products, volatile organic carbon compounds (VOCs), phe- nolics, diethylhexyl phthalate (DEHP), PBDEs, polycyclic aromatic hydrocarbons (PAHs), PCBs, and heavy metals. As heavy metals are not biodegradable or volatile, there was an increase in the heavy metal concentration in the final solid product compared to the input sludge, owing to the removal of the liquid matrix. The study reported that the biodegradation of most organotins was to the Table 2 Summary of effectiveness in volume/weight and pollutant reduction. Sludge Treatment Method Volume/Weight Reduction Effectiveness Score Pollutant Reduction Effectiveness Score Biological treatment Anaerobic digestion VS destruction ¼ 40%e50% (European Commission, 2001b) TSS removal yield ¼ 66%e86.2% (Salsabil et al., 2010) Sludge dry wt. reduction after 6 days ¼ 20% (Kurahashi et al., 2017) þ1 Pharmaceuticals ¼ 30% reduction (Malmborg and Magn�er, 2015) PCBs after 21 days ¼ 12%e32% of original concentration (Rosi�nska and Dąbrowska, 2014) Effects uncertain for other organic pollutants (Mailler et al., 2014b, 2017) No biodegradation of heavy metals þ1 Composting/aerobic digestion TSS removal yield ¼ 57%e76% (Salsabil et al., 2010) þ1 12 organic pollutants experienced mass reductions ranging from 13% to 89% (Poulsen and Bester, 2010) No biodegradation of heavy metals þ1 Constructed wetlands No data 0 Ibuprofen and caffeine reduction ¼ >80%; partial or poor removal of other organic pollutants (Zhu and Chen, 2014) No biodegradation of heavy metals 0 Chemical treatment Lime stabilisation Addition of 20%e40% or 50%e90% CaO or equivalent Ca(OH)2 per unit dry solids (European Lime Association), with corresponding volume/weight increase �2 Reduction of some heavy metals by 6%e23%, but no reduction of others. Dosages may be too high for land application(Wong and Selvam, 2006; Wong and Fang, 2000) None reported for organic pollutants 0 Thermal or thermo-chemical treatment Incineration Reduction of sludge cake by up to 96% (Vesilind and Ramsey, 1996) Weight reduction ¼ 62% (Hwang et al., 2007) þ2 Net formation of PCDD/Fs (Van Caneghem et al., 2010; Dai et al., 2014) Net destruction of dioxin-like PCBs, PCBs, and PAHs for sludge co-incinerated with other waste; (Van Caneghem et al., 2010) Heavy metals contained in solid residue (ash) 0 Pyrolysis Reduction of dry sludge (5.2 wt% moisture) by 35% e50% (Inguanzo et al., 2002) Weight reduction ¼ 63% (Hwang et al., 2007) þ2 Reduction of PCDD/Fs to <5 wt% of original (Dai et al., 2014) Reduced leaching of heavy metals from biochar, from 0.43% e88.87% to 0.09%e13.24% (Lu et al., 2016) Accumulation of 5%e20% of heavy metal content in bio-oil, with risk of exchange and leaching (Leng et al., 2015) þ1 Gasification Expected to be similar to pyrolysis þ2 Low rate of retention of metals (as low as 13.1% for Cd) on biochar when tested for leaching with 50% nitric acid (Marrero et al., 2004) 0 Hydrothermal carbonisation 60% of input solid mass in hydrochar (He et al., 2013) þ2 Leaching rates of Cu, Cd, Ni and Zn reduced from 2.04% e7.31% to 0.14%e2.30% after treatment (Huang et al., 2011). Zn leaching still above TCLP limit by 1.6e4.1 times (Yuan et al., 2015) Heavy metal distribution into bio-oil (5%e20%) poses risks for somemetals (Leng et al., 2015; Yuan et al., 2015; Li et al., 2012) Formation of small amounts of PAHs during gasification (Xu et al., 2013) þ1 Hydrothermal liquefaction Solid residues around 12.8e22.6 wt% of total product weight (Qian et al., 2017) þ2 þ1 Sub/supercritical water gasification (SWG) Varies: Solid residues of around 68%e69% of dry weight of sludge (Li et al., 2012); <30% of original sludge dry weight (Zhang et al., 2010) þ2 þ1 Supercritical water oxidation (SCWO) Primarily inorganic residues Combined SWG and SCWO reduced weight to 3.5% of initial (Qian et al., 2015) No other numerical evidence uncovered þ1 95% destruction of COD and >95% destruction of wide range of organics in diesel fuel and waste landfill leachate contaminated soil (Williams and Onwudili, 2006; Zou et al., 2013) (Similar process application) Reduced leachability of Cr, Cu, Zn, and Fe by as much as 99% but increased leachability of Ni by 13 times (Zou et al., 2013) No relevant studies uncovered for sewage sludge þ1 Wet oxidation Primarily inorganic residues No numerical evidence uncovered for volume/ weight reduction þ1 Maximum COD destruction of 89% achieved for pulp and paper mill effluent treated by catalytic wet air oxidation (Garg et al., 2007) (similar process application) No relevant studies uncovered for wet oxidation of sewage sludge þ1 Melting Higher combustion temperature than incineration; glass-like slag with higher density than ash No numerical evidence uncovered for volume/ weight reduction þ1 Reduced leachability of wide range of heavy metals to very low amounts (�2.89 mg/L) (Idris and Saed, 2002) Dioxin production reported to be reduced (Hong et al., 2009) (no numerical evidence uncovered) þ1 Drying Reduces moisture by as much as 85e95 wt% dry solids (i.e. 5%e15% moisture) þ1 No studies uncovered 0 S.K. Teoh, L.Y. Li / Journal of Cleaner Production 247 (2020) 119495 7 same extent as that of dry matter, indicated by little or no change in the pollutant concentration before and after sludge digestion. It was found that most alkylphenols, DEHP, and BDE-209 were removed to a greater extent than dry matter. Up to 42% of the original dry matter was removed, whereas up to 40%e95% of nonylphenols, nonylphenol monoethoxylate, nonylphenol dieth- oxylate, octylphenol, DEHP, and BDE-209 were removed, leading to lower concentrations in the final solid product; however, the au- thors noted that BDE-209 may be biodegraded to less brominated congeners. Subsequently, Mailler et al. (2017) investigated the fate of pharmaceuticals, hormones, perfluorinated acids, linear alkylben- zene sulphonate, alkylphenols, phthalates, PAHs, PCBs, and other pollutants after anaerobic digestion. They found that the S.K. Teoh, L.Y. Li / Journal of Cleaner Production 247 (2020) 1194958 concentrations of some pharmaceuticals (e.g. azithromycin, dom- peridone, lidocaine, sulphamethoxazole, tramadol) decreased from 40 to 130 mg kg�1 dry matter to as low as undetectable levels after digestion, while those of perfluorinated acids (PFOA, PFOS) decreased as well (from 316 mg kg�1 dry matter to 49 mg kg�1 dry matter for PFOS). However, the concentrations of some other pharmaceuticals, most hormones, linear alkylbenzene sulphonate, alkylphenols, PAHs, DEHP, and PCBs were found to increase after digestion. For example, the concentration of DEHP increased from 41,500 mg kg�1 dry matter in raw sludge to 58,100 mg kg�1 dry matter in digested sludge, while those of nonylphenols, non- ylphenol monoethoxylate, and diethoxylate increased from 940 to 1720 mg kg�1 dry matter to 1300e4520 mg kg�1 dry matter. The authors attributed this increase in concentration to the greater removal of both drymatter andmoisture (i.e. a decrease in themass of the substrate). Considering the findings of the 2014 and 2017 studies together, the effect of anaerobic digestion on the concen- trations of alkylphenols and DEHP seems to be somewhat uncertain. Poulsen and Bester (2010) reported that composting under thermophilic conditions could reduce the concentrations of some organic pollutants found in sewage sludge. They investigated 12 pollutants, including soaps and detergents, plasticisers (including DEHP), flame retardants, and other chemicals. The concentrations and masses of all 12 pollutants decreased during composting (seven of whichwere statistically significant), withmass reductions of 13%e89%. For example, the mass of DEHP (initial concentration of 31,000 ng/g dry matter) was reported to decrease by 84% over 24 days. However, the authors noted that the final concentration of DEHP was still significantly higher than the EU environmental standards. By comparison, constructed sludge treatment wetlands are generally less effective in reducing, removing, or stabilising pol- lutants. Uggetti et al. (2011, 2012) found that constructed wetlands did not reduce heavy metal concentrations. Plant uptake was shown to remove some pharmaceuticals and personal care prod- ucts, such as ibuprofen and caffeine (Zhu and Chen, 2014), with reported removal efficiencies of >80%, whereas other pharmaceu- ticals were partially removed (e.g. DEET by 32.3%e78.4%, sulpha- methoxazole by 33.6%e41.6%) or not removed significantly (e.g. carbamazepine and diclofenac sodium salt by <30%) (Zhu and Chen, 2014). Lime stabilisation was found to reduce the leaching of heavy metals from dewatered sewage sludge. The concentrations of Ni, Cu, and Zn in the leachate decreased from 0.55mg/L, 2.42mg/L, and 1.09mg/L to 0.13mg/L,1.54mg/L, and 0.01mg/L, respectively, when the lime dosage was 10%, and to 0.09 mg/L, 1.04 mg/L, and 0.01 mg/ L, respectively, when the dosage was increased to 20% (Liu et al., 2012). This represents reductions of 84%, 57%, and >99% for Ni, Cu, and Zn, respectively, at 20% dosage. Wong and Selvam (2006) found that composting sewage sludge mixed with sawdust and amended with lime at 0.63% dry wt. for 100 days reduced Cu, Mn, and Ni from 176, 141, and 64.0 mg kg�1 dry wt. to 166, 130, and 59.4 mg kg�1 dry wt., respectively, representing a reduction of around 6%e7%. They did not find reductions for Pb and Zn. When the lime dosage was increased to 1.63% dry wt., Cu, Mn, Ni, Pb, and Zn decreased by 6%e23%. Previously, Wong and Fang (2000) recommended that the lime dosage should be kept below 1% dry wt. if land application was intended as the end-use, as higher dosages were likely to inhibit microbial activity during composting if the pH was high. Further, liming was reported to be inappropriate for Cr- and Mo-polluted soils because of the high mobilityof these metals in a neutral and weakly alkaline environment (Koptsik, 2014). Thus, liming as a method to stabilise heavy metals in sludge is not expected to be highly effective at dosages suitable for subsequent land application or universally for all heavy metals that may be present. During incineration, organic pollutants may undergo thermo- chemical conversion or destruction and be released primarily in stack gases. Several studies have shown that, in general, incinera- tion does not necessarily lead to the net destruction of organic pollutants. Dai et al. (2014) found that the incineration of wet sewage sludge at different temperatures (700e950 �C) produced 2 to 13 times as much toxic polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in gaseous emissions as the amount originally present in the untreated sludge. When sewage sludge was co-incinerated with various other waste types, such as auto- motive shredder residue (ASR) and refuse-derived fuel (RDF), it was observed that PCDD/Fs, dioxin-like PCBs, PCBs, and PAHs in the input waste were destroyed, whereas other PCDD/Fs, dioxin-like PCBs, PCBs, and PAHs were newly formed in the post-combustion zone (Van Caneghem et al., 2010, 2014), with the effect largely in- dependent of the input concentrations. Overall, Van Caneghem et al. (2010) reported net destruction of dioxin-like PCBs, PCBs, and PAHs, but net formation of PCDD/Fs for a mixture of 70% RDF and 30% sludge, with input/output mass ratios of 5e14, 1200e3,900, and 70e110 for dioxin-like PCBs, PCBs, and PAHs, respectively, and 0.03e0.1 for PCDD/Fs. For a mixture of 25% ASR, 25% RDF, and 50% sludge, net destruction of dioxin-like PCBs, PCBs, and PAHs (input/output mass ratios of 150e380, 4900e6,900, and 1000e8,200, respectively) was also reported, while the net change in the mass of PCDD/Fs was small (input/output mass ratio 0.95e3.35) (Van Caneghem et al., 2010). Jin et al. (2017) found that co-incineration of sludge and other waste with coal in cement kilns led to a net reduction of 70.4%e97.5% of PCBs in the flue gas compared to the input mass. Thus, the net destruction efficiency of organic pollutants by incineration appears to be high for dioxin-like PCBs, PCBs, and PAHs, but low for PCDD/Fs. Therefore, flue gas cleaning (or the use of inhibitors for dioxins (Zhan et al., 2016)) is necessary to further reduce organic pollutant emissions (Werther and Ogada, 1999). In the case of heavy metals and metalloids, which are not thermo- chemically destroyed during incineration, fly ash and bottom ash are the final sinks (Santos et al., 2013; Weibel et al., 2017), which complicates their recycling or disposal. Hoffman et al. (2016) found that sludge pyrolysis significantly reduces oestrogenicity by up to 95% in oestradiol equivalent at pyrolysis temperatures >400 �C. This reduction was considered to be due to the volatilisation of most oestrogens at such tempera- tures, followed either by partitioning to py-oil or py-gas, or thermal decomposition. Less than 5 wt% of 17 toxic PCDD/Fs originally present in untreated sewage sludge was reported to survive py- rolysis at temperatures of 400e600 �C, explained by distillation and dechlorination effects (Dai et al., 2014). The potential for leaching of heavy metals from biochar (the solid residue from the pyrolysis process) produced at a pyrolysis temperature of 500 �C was small, with the leaching ratios of Cd, Cr, Pb, Zn, and Cu in the range of <0.01e0.1, defined as the ratio of the leaching concentration to the metal content (Hwang et al., 2007). Lu et al. (2016) further found that the leaching rate from biochar, defined as the ratio of the leachable heavy metal to the total content of the heavy metal, was reduced after pyrolysis compared to the input sludge. For example, at a pyrolysis temperature of 500 �C and leachate pH of 5, the leaching rate decreased from 0.43%e88.87% to 0.06%e13.24% for a range of metals including Pb, Zn, Ni, Cd, As, Cu, and Cr (even though the retention rate, defined as the ratio of heavy metal quantities in biochar to that in sludge, exceeded 80%). On the other hand, Leng et al. (2015) found that 5%e20% of metals including Cu, Zn, Pb, Cd, Cr, Ni, V, Mn, Ba, Co, Ti, Sn, As, and Hg could be distributed in bio-oil, while Yuan et al. (2015) found that metals such as Zn, Ni, S.K. Teoh, L.Y. Li / Journal of Cleaner Production 247 (2020) 119495 9 and Cd were at risk of exchange and leaching from bio-oil, sug- gesting that bio-oils produced by pyrolysis from metal-rich biomass such as sewage sludge should be pre-treated or upgra- ded before utilisation. There are also mixed results regarding the effectiveness of gasification in reducing, removing, or stabilising pollutants. Heavy metals mainly accumulate in the final carbona- ceous residue. However, Marrero et al. (2004) demonstrated that low percentages of metals (ranging from 13.1 ± 14.1% for Cd to 61.2 ± 3.8% for As) were retained in the char from the gasifier after leaching with 50% nitric acid. The leaching rates of Cu, Cd, Ni, and Zn from liquefaction resi- dues were suppressed after hydrothermal liquefaction compared with untreated sewage sludge, from 2.04% to 7.31% in the untreated sludge to 0.14%e2.30% in the treated sludge (Huang et al., 2011). However, leachable Zn concentrations based on the toxicity char- acteristic leaching procedure (TCLP) were still above the US EPA threshold limit by 1.6e4.1 times. Leng et al. (2015) reported that heavy metals were distributed mainly into biochar, with around 5%e20% into bio-oil, when these products were obtained from sewage sludge liquefaction with ethanol or acetone; however, increasing the liquefaction temperature promotes distribution into bio-oil. Although heavy metals are distributed mainly into biochar, the significant amount of metals partitioned into bio-oil poses an environmental risk (Leng et al., 2015; Yuan et al., 2015). Using two risk assessment methods, Li et al. (2012) concluded that Cu, Zn, and Cd in solid residues obtained from supercritical water gasification of sludge pose a high risk in terms of eco-toxicity and bioavailability within soil, while the risks of Cr and Pb are minimised. With regard to organic pollutants, Xu et al. (2013) showed that PAHs were generated during supercritical water gasification and that a high reaction temperature, long reaction time, and low dry matter content favour the formation of mainly 4-ring PAHs in the solid residue. They also noted that the total amount of PAHs in the solid residue met the Canadian soil quality standard for commercial use. Although our literature review did not uncover studies that investigated the destruction of organic pollutants by the wet oxidation or SCWO of municipal sewage sludge, the effectiveness of such destruction has been examined for other substrates. Catalytic wet air oxidation, which is somewhat similar to wet oxidation, has been assessed to determine its effectiveness in destroying re- fractory organic pollutants in industrial wastewater effluents. Wet oxidation is the aqueous oxidation of thickened sludgewith oxygen at elevated temperature and pressure (e.g. 235 �C and 40 bar) (Houillon and Jolliet, 2005). It transforms organic matter primarily into carbon dioxide and water vapour, destroying organic pollut- ants in the process and producing a mineral residue to be disposed of (Houillon and Jolliet, 2005). Catalytic wet air oxidation involves the use of catalysts, such as noble metals, metal oxides, and mixed oxides, to oxidise organic pollutants into biodegradable in- termediates, carbon dioxide, water, and innocuous end products at elevated temperature (125e320 �C) and pressure (0.5e20 MPa) (Kim and Ihm, 2011). Using 5% CuO/95% activated carbon as a catalyst, a maximum chemical oxygen demand (COD) destruction of 89% was achieved for pulp and paper mill effluent treated by catalytic wet air oxidation at 443 K and 0.85MPa (Garg et al., 2007). Williams and Onwudili (2006) assessed the effect of SCWO on or- ganics in dieselfuel and waste landfill leachate. Organic species in diesel fuel spiked into the sandmatrix at concentrations of 4e20wt % were decomposed at 96.6%e99.8%. Furthermore, a wide range of organics in waste landfill leachate were reported to be destroyed at >99.99%. Zou et al. (2013) studied the destruction of organics and the stabilisation of Cr, Cu, Pb, Zn, Ni, and Fe by SCWO of tannery sludge, which has high concentrations of organics (up to 54.2 wt% dry matter) and chromium salts. The destruction efficiency of COD, measured as a surrogate for organic content, increased with the temperature, reaching ~95% at a process temperature of 500 �C and an oxygen-to-COD ratio of 3:1. As for heavy metals, Zou et al. (2013) suggested that these were concentrated in the solid ash residue owing to the poor solubility of inorganic compounds in supercrit- ical water. Concentrations of Cr, for example, were found to lie in the range of 9.33e11.21 wt% in ash compared to 4.71 wt% dry matter basis in tannery sludge. A reduction in the leachability of Cr (from 11.41 mg/L to 0.12 mg/L) was observed owing to SCWO at 400 �C at an oxidant ratio of 3:1. Similar trends were observed for Cu, Zn, and Fe. However, Ni experienced an increase in leachability, from 0.28 mg/L in raw sludge to 3.51 mg/L in the ash produced under the same oxidation conditions. Sludge melting has been shown to be a promising method for stabilising inorganic pollutants as well as avoiding the generation of additional organic pollutants during the process. Idris and Saed (2002) conducted leaching tests on melted ash from sludge incin- eration and showed that the quantities leached from the final product after melting treatment were extremely low compared to the standard limits, with the metal concentrations of As, Ba, Cd, Cr, Cu, Ni, and Pb ranging from undetectable amounts to 2.89 mg/L compared to the standard limits of 1.0e100.0 mg/L. Hong et al. (2009) reported sludge melting to be advantageous over incinera- tion, as dioxin production is reduced owing to crystallisation at high temperature. Table 2 shows the scores assigned for the comparative effec- tiveness of the treatment methods in reducing, removing, or sta- bilising pollutants. No sludge treatment method discussed in the literature is able to reduce, remove, or stabilise pollutants comprehensively. As such, the highest score awarded was þ1 for methods that perform well. These include the following: (1) anaerobic digestion and composting, which effectively degrade at least some organic pollutants (but have no effect on heavy metals); (2) pyrolysis, which effectively degrades at least some organic pollutants and reduces heavy metal leaching, but some problems persist; (3) hydrothermal processes, which reduce heavy metal leaching and show limited organic pollutant destruction; and (4) wet oxidation, SCWO, and sludge melting, which show some effectiveness in destroying organics and reducing metal leach- ability. Methods that are moderately effective in reducing pollutant levels, such as constructed wetlands, incineration, and gasification, were assigned a score of 0. 3.3. Global warming potential (GWP) Two factors are observed to exert a clear influence on the GWP of sludge treatment methods: (1) end-use and final disposal methods of treated sludge, (2) overall or net energy/fuel con- sumption/substitution. Table 3 summarises the effects of these factors and suggests scores based on the methodology described in Table 1. Fig. SI-3 graphically summarises un-normalised GWPs of sludge treatment methods, as determined by the studies reviewed (unit conversion was performed as required). 3.3.1. Effects of end-use and final disposal In general, the end-use and final disposal methods for biologi- cally or chemically treated sludge differ from those of thermally or thermo-chemically treated sludge. Most scenarios for biologically or chemically treated sludge examined in studies considered land or agricultural application as the end-use, with only a small number considering landfilling or other end-uses (Table SIe6). Land or agricultural application of treated sludge affects the GWP in several ways. (1) As a soil amendment, treated sludge may reduce the GWP by offsetting the need for fertilisers and avoiding emissions related to their production, transport, spreading, and anaerobic degradation (i.e. biogeochemical emissions). (2) As a soil Table 3 Summary of net global warming potential. Sludge Treatment Method End-Use/Disposal Energy/Fuel Consumption/Substitution References Score Biological treatment AD Landfill Partial use of biogas from AD for heat and/or power generation (Poulsen and Hansen, 2003; Brown et al., 2010); None (Peters and Rowley, 2009) Poulsen and Hansen (2003) Peters and Rowley (2009) Brown et al. (2010) �1 AD Agricultural application None Peters and Lundie (2001) Hospido et al. (2005) 0 AD Agricultural application Partial use of biogas from AD for heat and/or power generation Poulsen and Hansen (2003) Murray et al. (2008) Brown et al. (2010) þ1 AD Agricultural application Use of biogas from AD for power generation Peters and Lundie (2001) þ2 AD þ composting Agricultural application Partial use of biogas from AD for heat and/or power generation Poulsen and Hansen (2003) 0 Composting Agricultural application None Liu et al. (2013) 0 Chemical treatment Lime stabilisation Landfill None Houillon and Jolliet (2005) �2 Lime stabilisation Agricultural application None Peters and Lundie (2001) Houillon and Jolliet (2005) Murray et al. (2008) Peters and Rowley (2009) �1 Thermal or thermo-chemical treatment Drying Agricultural application None Peters and Rowley (2009) �2 Drying Fuel for cement kiln firing Partially replace coal Peters and Rowley (2009) þ2 Incineration Ash landfilled None Hospido et al. (2005) 0 Pyrolysis (w/pre-drying) Fuel/raw material Use of syngas only Hospido et al. (2005) �1 Pyrolysis (w/pre-drying) Fuel/raw material Use of syngas, char, tar Hospido et al. (2005) 0 Pyrolysis Fuel/substitute for fertiliser Use of bio-oil for heat and power generation Use of bio-char to replace fertiliser Cao and Pawłowski (2013) þ1 SCWO Land Excess heat used for district heating Johansson et al. (2008) þ1 Combinations of treatment methods AD þ co-incineration Fuel/additive for cement kiln firing/production Partial use of biogas from AD for heat and power generation Partially replace cement kiln primary fuel mix Poulsen and Hansen (2003) þ2 AD þ co-incineration Fuel in MSW incinerator Ash landfilled Partial use of biogas from AD for heat and power generation Heat and power generation from MSW co- incineration Poulsen and Hansen (2003) þ1 AD þ drying Agricultural application None Peters and Lundie (2001) Peters and Rowley (2009) �2 AD þ drying Agricultural application Use of biogas from AD to power dryers Peters and Lundie (2001) þ1 AD þ drying Fuel for cement kiln firing Partially replace coal Peters and Rowley (2009) þ2 AD þ drying þ co-incineration Fuel in MSW incinerator Ash landfilled Partial use of biogas from AD for heat and power generation Heat and power generation from MSW co- incineration Poulsen and Hansen (2003) þ2 AD þ pyrolysis Fuel/substitute for fertiliser Use of biogas for heat and power generation and to replace diesel Use of bio-oil for heat and power generation Use of bio-char to replace fertiliser Cao and Pawłowski (2013) þ2 Drying þ composting Agricultural application None Murray et al. (2008) �1 Abbreviations: AD ¼ anaerobic digestion; MSW ¼ municipal solid waste; SCWO ¼ super-critical water oxidation. S.K. Teoh, L.Y. Li / Journal of Cleaner Production 247 (2020) 11949510 amendment, treated sludge may also reduce the GWP by seques- tering soil carbon. (3) Land application of treated sludge may in- crease the GWP owing to the release of methane and nitrous oxide following anaerobic degradation in the soil (Johansson et al., 2008; Brown et al., 2010). The relative magnitudes of these factors determine the overall contribution to theGWP. Table SIe6 summarises how the above-mentioned factors were assessed in the studies, with detailed analyses of their effects. Most studies considered only two out of the three factors (i.e. carbon sequestration was not considered). There is some debate as to whether carbon sequestration by the addition of organic matter to soil should be included in LCA studies (Peters and Rowley, 2009), partly because the management of soils may not maintain the carbon store over the time scale used for GWP assessment (100 years). Consequently, soil carbon sequestration has been dis- counted by some studies. Emission factors vary widely across studies, with ranges of 0.02e6.3 kg CH4/t-DS and 0.00011e1.80 kg N2O/t-DS for methane and nitrous oxide emissions owing to the degradation of treated sludge in soil, and 50e328 kg CO2/t-DS avoided owing to fertiliser offset. Fig. 3 shows the effects of the main factors influencing the GWP arising from land application of treated sludge (fertiliser offset, methane and nitrous oxide emissions due to anaerobic degradation in soil, carbon sequestration), compared with the GWP of other factors not associated with land application. The values are plotted from the studies listed in Table SIe6, which have conducted such an assessment and published values for comparison. Fig. 3 shows that fertiliser offset, methane, and nitrous oxide emissions due to anaerobic degradation in soil, and carbon sequestration can all be significant factors contributing towards the overall GWP in land application end-uses. However, because the estimates vary across studies (as seen in Fig. 3), it is difficult to draw wider inferences as to how significant these factors may be in determining the overall GWP. We examine the findings of two studies that considered all three factors (Table SIe6). In the first of these studies, Brown et al. (2010) AD (lime) Lime (agri.) Lime (lf.) AD + SCWO (land) Comp. (low) Comp. (high) AD (no lime) Lime AD (fer lizer) AD (no fer lizer) AD Comp. Co-AD + comp. Comp. -2000 -1000 0 1000 2000 3000 4000 GW P (k g- CO 2e /t -D S) Dry. + comp. Houillon and Jolliet, 2005 Johansson et al., 2008 Murray et al., 2008 Brown et al., 2010 Carballa et al., 2011 Liu et al., 2013 Righi et al., 2013 Usapein and Chavalparit, 2017 GWP due to carbon sequestra on GWP due to fer liser avoidance GWP due to release of methane and nitrous oxide following land applica on GWP due to other factors Fig. 3. Contribution to GWP by Factors due to Land Application of Treated Sludge Note: Findings from studies are plotted in chronological order of study. Abbreviations: AD (fertiliser; no fertiliser; lime; no lime) ¼ anaerobic digestion (with replacement of fertiliser by treated sludge; without replacement of fertiliser by treated sludge; with lime addition; without lime addition); Co-AD ¼ co-digestion (anaerobic) with organic fraction of municipal solid waste; Comp. (low; high) ¼ composting (low estimate for methane and nitrous oxide release; high estimate for methane and nitrousoxide release); Dry. ¼ drying; Lime (agri.; lf.) ¼ lime stabilisation (with agricultural application as the end-use; with landfill disposal); SCWO (land) ¼ supercritical water oxidation with land application as the end-use. S.K. Teoh, L.Y. Li / Journal of Cleaner Production 247 (2020) 119495 11 applied a greenhouse gas calculator tool (Biosolids Emissions Assessment Model, BEAM), developed for the Canadian Council of Ministers of the Environment (CCME) using data from peer- reviewed literature and municipalities, to nine scenarios in Can- ada. The modelling approach incorporated a critical assumption that nitrous oxide emissions from treated sludge applied on land are equivalent in magnitude to those from the synthetic fertilisers replaced. Thus, in the model, if treated sludge replaced fertilisers, credits from fertiliser offset and carbon sequestration accrued without any increase in the GWP owing to additional nitrous oxide emissions. If treated sludge did not replace fertilisers, only credits from carbon sequestration accrued, which was accompanied by an increase in the GWP owing to additional nitrous oxide emissions. Fig. 3 compares these two end-use possibilities (replacement vs. no replacement of fertilisers) for the scenario in British Columbia that involved anaerobic digestion, followed by land application of the treated product. In the second study that considered all three factors (Liu et al., 2013), the authors examined the effect of composting followed by land application of the treated product (which replaced the fertil- iser) in one scenario. Fig. 3 shows the GWP for this scenario. Similar to Brown et al. (2010), Liu et al. (2013) excluded greenhouse gas emissions from sludge application in soil, noting that no significant differences were found between emissions from treated sludge and those from the replaced fertilisers. The authors noted that the overall GWP could be further decreased by 45% if carbon seques- tration was considered, based on findings by other authors (including Peters and Rowley (2009) and Brown et al. (2010)). Some studies listed in Table SIe3 (Houillon and Jolliet (2005); Johansson et al. (2008); Carballa et al. (2011); Mills et al. (2014); Usapein and Chavalparit (2017)) did not adopt the same reasoning as Brown et al. (2010) and Liu et al. (2013) in assuming that nitrous oxide emissions from treated sludge applied on land are equivalent in magnitude to those from the synthetic fertilisers replaced. This deviation from the assumption made by Brown et al. (2010) and Liu et al. (2013) may significantly affect the GWP estimates, as can be seen in Fig. 3 for Johansson et al. (2008). Johansson et al. (2008) emphasised the benefits of SCWO in eliminating biogeochemical emissions. In this scenario, fertiliser avoidance accounted for nearly 10% of all GWP contributions, and together with the use of biogas in district heating, reduced the overall GWP to a negative value. Johansson et al. (2008) also noted considerable uncertainty in the magnitude of biogeochemical emissions from the land application of sludge treated by anaerobic digestion, as can be seen from the considerable differences between high and low estimates. Two studies listed in Table SIe6 (Peters and Rowley (2009); Mills et al. (2014)) were not plotted in Fig. 3, as their published findings did not provide related numerical details. The GWP of the application of sludge on land was not consid- ered at all in two studies. Suh and Rousseaux (2002) investigated scenarios in France involving the anaerobic digestion, composting, lime stabilisation, or incineration of sludge, followed by either land application or landfilling. The effect of sludge degradation into landfill gas was considered, but the effect of degradation after land application was not considered. Xu et al. (2014) studied, within their system boundary, various anaerobic digestion configurations in China as well as their end-uses, including agricultural applica- tion, incineration, and landfilling. For the agricultural application end-use, the authors considered the toxicity of leaching of metals into the soil but not the GWP owing to anaerobic degradation of the sludge in soil. Some discrepancies in themethodologies adopted by the above- S.K. Teoh, L.Y. Li / Journal of Cleaner Production 247 (2020) 11949512 mentioned studies in determining the GWP are also apparent. The considered range of emissions due to land spreading differs across studies. Johansson et al. (2008) considered both methane and nitrous oxide emissions, while Houillon and Jolliet (2005), Brown et al. (2010), and Carballa et al. (2011) did not, with Houillon and Jolliet (2005) citing “a lack of available data”. This may not be sig- nificant if the same amounts of avoided emissions from fertiliser offset are netted off (Brown et al., 2010; Liu et al., 2013), but some uncertainty still remains as to whether artificial fertilisers and biosolidsproduce similar amounts of methane and nitrous oxide emissions, particularly with varying rates of biosolid application (Chiaradia et al., 2009). The choice of the system boundary can also lead to differences in the apparent significance of the factors associated with land spreading. Johansson et al. (2008) considered only processes after anaerobic digestion (e.g. transport, machine loading, storage, and spreading of treated sludge in one of their scenarios). Thus, potentially significant emissions from anaerobic digestion were not factored into their overall GWP comparison. On the other hand, Houillon and Jolliet (2005) included the liming process in their study, which produced a significant GWP owing to drying and liming, leading to a smaller percentage impact from fertiliser offset and biogeochemical emissions. Thus, the differences in the choice of system boundaries explain why findings cannot easily be compared across studies. In order to make sense of the findings, it is useful to first assess trends within a study examining multiple treatment options before further comparing them with trends in other studies. End-uses or final disposal methods for thermally/thermo- chemically treated sludge differ from those of chemically or bio- logically treated sludge. Of the studies reviewed, only drying/pas- teurisation, SCWO, and wet oxidation processes led to land/ AD (Malabar) AD (alternate) AD + dry. (alternate) Lime (North Head) AD (Bondi) AD + co- inc. (cement) AD + co-inc. (MSW) AD + inc. AD (agri.) AD + comp. AD -5000 -4000 -3000 -2000 -1000 0 1000 2000 3000 4000 5000 GW P (k g- CO 2e /t - t/h Wk( noitp musnoC ygrenEte Nro)SD -D S) Peters and Lundie, 2001 Poulsen and Hansen, 2003 Hosp GWP (kg CO2e/t-DS) Net Energy Consump Fig. 4. GWP and Net Energy Consumption. Note: Findings from studies are plotted in chronological order of study. Abbreviations: AD (agri.; alternate; Bondi; Malabar) ¼ anaerobic digestion (with agricultura facility); Comp. ¼ composting; Co-inc. (cement; MSW) ¼ co-incineration (with cement k cement) ¼ drying (with agricultural application end-use; with end-use as cement kiln fue facility); Pyr. (partial reuse; full reuse) ¼ pyrolysis (with partial reuse of products (syngas) agricultural application. This is not unusual, as drying/pasteurisa- tion has been used primarily to remove pathogens from sludge, so that the product may be suitable for land/agricultural application (European Commission, 2001b). SCWO and wet oxidation produce inert outputs that can be safely spread on land without adverse effects, and no GWP was reported to be associated with land spreading (Svanstr€om et al., 2004; Johansson et al., 2008). Residues from sludge incineration or co-incineration are usually landfilled. The studies surveyed in this review did not report GWP associated with such landfilling. Pyrolyzed/gasified sludge is incorporated into fuel products, leading to eventual fuel/energy substitution. Simi- larly, the contribution to GWP due to fuel use for drying and incineration dominated the study by Brown et al. (2010). The effect of fuel/energy consumption/substitution on GWP is explored in the following section. 3.3.2. Net energy/fuel consumption/substitution Energy consumption by processes such as material transport, electricity use, or fuel use in sludge drying or combustion usually results in an increase in the GWP (e.g. if the energy replaced is non- renewable). Conversely, substituting energy generated from sludge treatment for use in the treatment process or elsewhere, or substituting sludge or sludge treatment products as fuel to offset the use of other fuels, usually results in a decrease in the GWP (e.g. if the fuel replaced is non-renewable). Fig. 4 compares the GWP with the net energy consumption for five studies that conducted such an analysis. For the same sludge treatment method (e.g. anaerobic digestion), Fig. 4 shows that the GWP can be either positive or negative depending on the choice of LCA methods, system boundaries, inventory analysis, and other parameters. Therefore, comparison of relative magnitudes is only meaningful Inc. Pyr. (full reuse) Pyr. (par al reuse) Dry. (cement) AD + dry. (cement) AD AD + comp. Lime AD + dry. (agri.) Dry. (agri.) AD + pyr. Pyr. ido et al., 2005 Peters and Rowley, 2009 Cao and Pawłowski, 2013 on (kWh/t-DS) l application end-use; alternate scenario; process at Bondi facility; process at Malabar iln primary fuel mix;with municipal solid waste); Comp. ¼ composting; Dry. (agri.; l); Inc. ¼ incineration; Lime (North Head) ¼ lime stabilisation (process at North Head ; with full reuse of products (syngas, char, tar)). S.K. Teoh, L.Y. Li / Journal of Cleaner Production 247 (2020) 119495 13 within studies. Fig. 4 shows a clear trend of the GWP increasing with the net energy consumption across the studies. For example, in the study by Peters and Lundie (2001), lime stabilisation at the North Head plant in Sydney, Australia, resulted in a lower GWP compared to anaerobic digestion at the Bondi plant, but a higher GWP compared to anaerobic digestion at the Malabar plant. This was due to the use of biogas for power generation at Malabar (resulting in a negative GWP of around �200 kg CO2e/t-DS), but not at Bondi, where it was flared. Anaerobic digestion and drying as alternative process for North Head resulted in a lower GWP compared to lime stabilisation (by 45%) if the biogas from the digesters was used to power the dryers, but a higher GWP (by 10%) if natural gas was used instead. Thus, biogas generation and use are important in lowering the GWP of anaerobic digestion. In a study by Poulsen and Hansen (2003), alternative scenarios incorporating co-incineration in the Aalborg municipality, Denmark, were found to have the lowest GWP owing to the greatest substitution of energy and resources. In both py- rolysis scenarios examined by Cao and Pawłowski (2013), avoidance of greenhouse gas emissions due to bioenergy production (bio-oil in both scenarios; biogas in the scenario with anaerobic digestion), together with biochar substitution of the fertiliser, resulted in a net GWP offset. By assessing the findings of these studies as a whole, we can see that energy or fuel substitution plays an important role in reducing the GWP for energy-intensive thermal and thermo-chemical pro- cesses, such as drying, incineration, and pyrolysis, as well as for anaerobic digestion. For example, in the study by Cao and Pawłowski (2013), sludge pre-drying was the most energy- consumptive process, accounting for 53.1% and 81.8% of the total energy consumption for scenarios with and without anaerobic digestion, respectively. Anaerobic digestion, when incorporated, accounted for 34.8% of the total energy consumption. The pyrolysis process itself was less energy-consumptive than anaerobic diges- tion, accounting for 8.5% of the total energy consumption for the scenario incorporating anaerobic digestion. The contribution to the GWP also followed the same order: the drying operation was the largest GWP contributor, followed by anaerobic digestion and py- rolysis. The combined contribution of the other processes, such as dewatering and transport, accounted for <10% of the total GWP in both scenarios. The effect of transport on GWP was significant only for non- thermal/thermo-chemical processes, such as lime stabilisation and, at times, anaerobic digestion. For instance, in the study by Peters and Lundie (2001), transport of limed sludge by truck from North Head for a distance of 250 kmwas a significant contributor to both energy consumption and GWP, accounting for >50% of both total energy consumption and total GWP. By contrast, transport of dry sludge from North Head in the alternative scenario accounted for <20% of the total GWP, because of weight reduction due to a lower moisture content. 3.4. Toxicity potentials (TPs) LCAs of toxicity potentials arising from sludge treatment have, by and large,
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