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Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

Postal Subscription Code 80-973

2018 Impact Factor: 3.883

Front. Environ. Sci. Eng.    2024, Vol. 18 Issue (12) : 149    https://doi.org/10.1007/s11783-024-1909-z
Syngas production and heavy metal dynamics during supercritical water gasification of sewage sludge
Mi Yan1, Shuai Liu1, Haihua Zhang2, Rendong Zheng3, Jintao Cui1, Dan Wang1, Dicka Ar Rahim1,4, Ekkachai Kanchanatip5()
1. Institute of Energy and Power Engineering, Zhejiang University of Technology, Hangzhou 310014, China
2. China Hangzhou Energy Group Co., Ltd., Hangzhou 310013, China
3. Hangzhou Linjiang Environmental Energy Co., Ltd., Hangzhou 310013, China
4. Department of Chemical Engineering, Bandung Institute of Technology, Bandung 40132, Indonesia
5. Department of Civil and Environmental Engineering, Faculty of Science and Engineering, Kasetsart University Chalermphrakiat Sakon Nakhon Province Campus, Sakon Nakhon 47000, Thailand
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Abstract

● The highest syngas yield of 10.9 mol/kg with 44.7% H2 concentration was achieved.

● The distribution of heavy metals with/without alkaline additives was investigated.

● Risk Assessment Code of heavy metals after SCWG reduced to less than 1%.

● Possible reaction pathways of heavy metals during SCWG of sludge were proposed.

The rising production of sewage sludge, characterized by high organic content and excessive heavy metals, necessitates an effective treatment method. This study investigated the production of syngas and the migration and transformation behavior of heavy metals such as Zn, Ni, Cr, Cu, and As during supercritical water gasification (SCWG) of sewage sludge. The experiments were conducted without or with alkaline additives at temperatures between 380 to 420 °C and retention time from 15 to 60 min. The results revealed that the highest syngas yield reached 10.9 mol/kg with an H2 concentration of 44.7% at 420 °C and 60 min. In this process, heavy metals were effectively immobilized and converted into a more stable form, whereas higher temperatures and longer retention time enhanced this effect. The introduction of alkaline additives (NaOH, KOH, Ca(OH)2, Na2CO3, and K2CO3) led to the redistribution of heavy metals, further promoting the stabilization of Zn, Cr, and Cu. An environmental risk assessment showed that SCWG could significantly lower the risk associated with heavy metals to a low or negligible level.

Keywords Sludge      Heavy metal      Immobilization      Supercritical water gasification      Environmental risk assessment     
Corresponding Author(s): Ekkachai Kanchanatip   
Issue Date: 08 October 2024
 Cite this article:   
Mi Yan,Shuai Liu,Haihua Zhang, et al. Syngas production and heavy metal dynamics during supercritical water gasification of sewage sludge[J]. Front. Environ. Sci. Eng., 2024, 18(12): 149.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-024-1909-z
https://academic.hep.com.cn/fese/EN/Y2024/V18/I12/149
Analysis Value
Proximate analysis (wt%, dry basis)
 Volatile matter 45.9
 Ash 49.4
 Fixed carbon 4.7
Ultimate analysis (wt%, dry ash-free basis)
 C 49.1
 H 7.2
 N 8.5
 S 3.0
 O* 32.2
Tab.1  Proximate and ultimate analysis of sludge sample
Compound Content (wt%)
Zn 0.058
Ni 0.003
Cr 0.034
Cu 0.013
As 0.002
Tab.2  Heavy metals in the raw sewage sludge (dry basis)
Fig.1  Schematic diagram of the SCWG system.
Symbol Mass of sludge (g) Mass of deionized water (g) Reaction temperature ( °C) Retention time (min)
S1 10 90 380 60
S2 10 90 400 15
S3 10 90 400 30
S4 10 90 400 60
S5 10 90 420 60
Tab.3  Details of the experimental conditions
Fig.2  Effect of reaction temperature (380–420 °C) and retention time (15–60 min) on (a) HE, CE, syngas yield and (b) syngas composition.
Fig.3  Mass balance of heavy metals during SCWG of sludge at different conditions. (a) Zn, (b) Ni, (c) Cr, (d) Cu, (e) As.
Fig.4  Heavy metals speciation distribution during SCWG of sludge under different conditions. (a) Zn, (b) Ni, (c) Cr, (d) Cu, and (e) As.
Fig.5  Effect of alkaline additives on the speciation distribution of heavy metals, (a) Zn; (b) Ni; (c) Cr; (d) Cu; (e) As.
Fig.6  RAC assessment of heavy metals. (a) RAC indices of raw sludge and solid residues after SCWG, (b) RAC indices with the addition of alkaline metals (400 °C, 60 min).
Fig.7  Transformation pathways of heavy metals (X = Zn, Ni, Cr, Cu, and As, and n represents the valence state of the heavy metals element).
1 E Adar, M Ince, M S Bilgili. (2020). Supercritical water gasification of sewage sludge by continuous flow tubular reactor: a pilot scale study. Chemical Engineering Journal, 391: 123499
https://doi.org/10.1016/j.cej.2019.123499
2 Z A S Bairq, R D Li, Y L Li, H X Gao, T Sema, W C Teng, S Kumar, Z W Liang. (2018). New advancement perspectives of chloride additives on enhanced heavy metals removal and phosphorus fixation during thermal processing of sewage sludge. Journal of Cleaner Production, 188: 185–194
https://doi.org/10.1016/j.jclepro.2018.03.276
3 W Bühler, E Dinjus, H J Ederer, A Kruse, C Mas. (2002). Ionic reactions and pyrolysis of glycerol as competing reaction pathways in near- and supercritical water. Journal of Supercritical Fluids, 22(1): 37–53
https://doi.org/10.1016/S0896-8446(01)00105-X
4 G Chen, J Andries, Z Luo, H Spliethoff. (2003). Biomass pyrolysis/gasification for product gas production: the overall investigation of parametric effects. Energy Conversion and Management, 44(11): 1875–1884
https://doi.org/10.1016/S0196-8904(02)00188-7
5 G Chen, X Yang, S Chen, Y Dong, L Cui, Y Zhang, P Wang, X Zhao, C Ma. (2017). Transformation of heavy metals in lignite during supercritical water gasification. Applied Energy, 187: 272–280
https://doi.org/10.1016/j.apenergy.2016.11.054
6 Y Chen, L Yi, W Wei, H Jin, L Guo. (2022). Hydrogen production by sewage sludge gasification in supercritical water with high heating rate batch reactor. Energy, 238: 121740
https://doi.org/10.1016/j.energy.2021.121740
7 J Cui, X Wen, F Chen, M Yan, D Hantoko. (2023). Migration of nitrogen and phosphorus during supercritical water gasification of sewage sludge: effect of alkaline additives. Fuel Processing Technology, 245: 107727
https://doi.org/10.1016/j.fuproc.2023.107727
8 A Ding, R R Zhang, H H Ngo, X He, J Ma, J Nan, G B Li. (2021). Life cycle assessment of sewage sludge treatment and disposal based on nutrient and energy recovery: a review. Science of the Total Environment, 769: 144451
https://doi.org/10.1016/j.scitotenv.2020.144451
9 Y R Fang, S Li, Y Zhang, G H Xie. (2019). Spatio-temporal distribution of sewage sludge, its methane production potential, and a greenhouse gas emissions analysis. Journal of Cleaner Production, 238: 117895
https://doi.org/10.1016/j.jclepro.2019.117895
10 M Gabarrón, R Zornoza, S Martínez-Martínez, V A Muñoz, A Faz, J A Acosta. (2019). Effect of land use and soil properties in the feasibility of two sequential extraction procedures for metals fractionation. Chemosphere, 218: 266–272
https://doi.org/10.1016/j.chemosphere.2018.11.114
11 D Hantoko, E Antoni, M Kanchanatip, Z Yan, Z Weng, Y Gao. (2019). Assessment of sewage sludge gasification in supercritical water for H2-rich syngas production. Process Safety and Environmental Protection, 131: 63–72
https://doi.org/10.1016/j.psep.2019.08.035
12 J Jia, J Bai, R Xiao, S Tian, D Wang, W Wang, G Zhang, H Cui, Q Zhao. (2022). Fractionation, source, and ecological risk assessment of heavy metals in cropland soils across a 100-year reclamation chronosequence in an estuary, South China. Science of the Total Environment, 807: 151725
https://doi.org/10.1016/j.scitotenv.2021.151725
13 C S Lee, A V Conradie, E Lester. (2021). Review of supercritical water gasification with lignocellulosic real biomass as the feedstocks: process parameters, biomass composition, catalyst development, reactor design and its challenges. Chemical Engineering Journal, 415: 128837
https://doi.org/10.1016/j.cej.2021.128837
14 L Leng, S Leng, J Chen, X Yuan, J Li, K Li, Y Wang, W Zhou. (2018). The migration and transformation behavior of heavy metals during co-liquefaction of municipal sewage sludge and lignocellulosic biomass. Bioresource Technology, 259: 156–163
https://doi.org/10.1016/j.biortech.2018.03.019
15 B Li, S Ding, H Fan, Y Ren. (2021). Experimental investigation into the effect of pyrolysis on chemical forms of heavy metals in sewage sludge biochar (SSB), with brief ecological risk assessment. Materials, 14(2): 447
https://doi.org/10.3390/ma14020447
16 C X Li, J Li, S Y Xie, G Y Zhang, L J Pan, R M Wang, G Wang, X F Pan, Y Wang, I Angelidaki. (2022a). Enhancement of heavy metal immobilization in sewage sludge biochar by combining alkaline hydrothermal treatment and pyrolysis. Journal of Cleaner Production, 369: 133325
https://doi.org/10.1016/j.jclepro.2022.133325
17 D Li, R Shan, L Jiang, J Gu, Y Zhang, H Yuan, Y Chen. (2022b). A review on the migration and transformation of heavy metals in the process of sludge pyrolysis. Resources, Conservation and Recycling, 185: 106452
https://doi.org/10.1016/j.resconrec.2022.106452
18 H Li, Y Jin, R Mahar, Z Wang, Y Nie. (2008). Effects and model of alkaline waste activated sludge treatment. Bioresource Technology, 99(11): 5140–5144
https://doi.org/10.1016/j.biortech.2007.09.019
19 L Li, W Cao, G Wang, P Peng, S Liu, H Jin, W Wei, L Guo. (2022c). Experimental and kinetic study of heavy metals transformation in supercritical water gasification of oily sludge. Journal of Cleaner Production, 373: 133898
https://doi.org/10.1016/j.jclepro.2022.133898
20 L Li, X Li, W Cao. (2023). An experimental and thermodynamic equilibrium investigation of heavy metals transformation in supercritical water gasification of oily sludge. Journal of Environmental Management, 348: 119365
https://doi.org/10.1016/j.jenvman.2023.119365
21 Q Li, Z Zhong, H Du, X Zheng, B Zhang, B Jin. (2022d). Co-pyrolysis of sludge and kaolin/zeolite in a rotary kiln: analysis of stabilizing heavy metals. Frontiers of Environmental Science & Engineering, 16(7): 85
https://doi.org/10.1007/s11783-021-1488-1
22 Y Liang, D Xu, P Feng, B Hao, Y Guo, S Wang, J J Klemes. (2021). Municipal sewage sludge incineration and its air pollution control. Journal of Cleaner Production, 295: 126456
https://doi.org/10.1016/j.jclepro.2021.126456
23 Y Lin, D Wang, S Wu, C Wang. (2009). Alkali pretreatment enhances biogas production in the anaerobic digestion of pulp and paper sludge. Journal of Hazardous Materials, 170(1): 366–373
https://doi.org/10.1016/j.jhazmat.2009.04.086
24 L Liu, L Huang, R Huang, H Lin, D Wang. (2021a). Immobilization of heavy metals in biochar derived from co-pyrolysis of sewage sludge and calcium sulfate. Journal of Hazardous Materials, 403: 123648
https://doi.org/10.1016/j.jhazmat.2020.123648
25 M Liu, X Han, C Q Liu, L Guo, H Ding, Y Lang. (2021b). Differences in the spectroscopic characteristics of wetland dissolved organic matter binding with Fe3+, Cu2+, Cd2+, Cr3+ and Zn2+. Science of the Total Environment, 800: 149476
https://doi.org/10.1016/j.scitotenv.2021.149476
26 Y F Lu, H E Allen. (2002). Characterization of copper complexation with natural dissolved organic matter (DOM)-link to acidic moieties of DOM and competition by Ca and Mg. Water Research, 36(20): 5083–5101
https://doi.org/10.1016/S0043-1354(02)00240-3
27 R Muangrat, J A Onwudili, P T Williams. (2010). Influence of alkali catalysts on the production of hydrogen-rich gas from the hydrothermal gasification of food processing waste. Applied Catalysis B: Environmental, 100(3−4): 440–449
https://doi.org/10.1016/j.apcatb.2010.08.019
28 S Nanda, A K Dalai, J A Kozinski. (2016). Supercritical water gasification of timothy grass as an energy crop in the presence of alkali carbonate and hydroxide catalysts. Biomass and Bioenergy, 95: 378–387
https://doi.org/10.1016/j.biombioe.2016.05.023
29 J A Okolie, S Nanda, A K Dalai, J A Kozinski. (2021). Techno-economic evaluation and sensitivity analysis of a conceptual design for supercritical water gasification of soybean straw to produce hydrogen. Bioresource Technology, 331: 125005
https://doi.org/10.1016/j.biortech.2021.125005
30 L M Quan, H Kamyab, A Yuzir, V Ashokkumar, S E Hosseini, B Balasubramanian, I Kirpichnikova. (2022). Review of the application of gasification and combustion technology and waste-to-energy technologies in sewage sludge treatment. Fuel, 316: 123199
https://doi.org/10.1016/j.fuel.2022.123199
31 W Su, M Zhao, Y Xing, H Ma, P Liu, X Li, H Zhang, Y Wu, C Xia. (2022). Supercritical water gasification of hyperaccumulators for hydrogen production and heavy metal immobilization with alkali metal catalysts. Environmental Research, 214: 114093
https://doi.org/10.1016/j.envres.2022.114093
32 J Sun, H Feng, J Kou, H Jin, Y Chen, L Guo. (2021). Experimental investigation on carbon microstructure for coal gasification in supercritical water. Fuel, 306: 121675
https://doi.org/10.1016/j.fuel.2021.121675
33 W Tang, L Sun, L Shu, C Wang. (2020). Evaluating heavy metal contamination of riverine sediment cores in different land-use areas. Frontiers of Environmental Science & Engineering, 14(6): 104
https://doi.org/10.1007/s11783-020-1283-4
34 C Wang, C Wu, U Hornung, W Zhu, N Dahmen. (2021a). Suppression of tar and char formation in supercritical water gasification of sewage sludge by additive addition. Chemosphere, 262: 128412
https://doi.org/10.1016/j.chemosphere.2020.128412
35 Y Wang, Y Tang, R Li, X Guo, J P Hurley, R B Finkelman. (2021b). Measurements of the leachability of potentially hazardous trace elements from solid coal gasification wastes in China. Science of the Total Environment, 759: 143463
https://doi.org/10.1016/j.scitotenv.2020.143463
36 Y Wang, Y Zhu, Z Liu, L Wang, D Xu, C Fang, S Wang. (2019). Catalytic performances of Ni-based catalysts on supercritical water gasification of phenol solution and coal-gasification wastewater. International Journal of Hydrogen Energy, 44(7): 3470–3480
https://doi.org/10.1016/j.ijhydene.2018.08.218
37 N Wei, D H Xu, B T Hao, S W Guo, Y Guo, S Z Wang. (2021). Chemical reactions of organic compounds in supercritical water gasification and oxidation. Water Research, 190: 116634
https://doi.org/10.1016/j.watres.2020.116634
38 D Xu, L Liu, N Wei, Y Guo, S Wang, Z Wu, P Duan. (2019). Catalytic supercritical water gasification of aqueous phase directly derived from microalgae hydrothermal liquefaction. International Journal of Hydrogen Energy, 44(48): 26181–26192
https://doi.org/10.1016/j.ijhydene.2019.08.106
39 M Yan, J Cui, T Li, H Feng, D Hantoko, E Kanchanatip. (2023). Transformation and distribution of nitrogen and phosphorus in sewage sludge during supercritical water gasification. Fuel, 332: 125918
https://doi.org/10.1016/j.fuel.2022.125918
40 M Yan, H Y Feng, R D Zheng, C M Yu, D Hantoko, Z H Zhou, Y Zhang, E Kanchanatip. (2021). Sulfur conversion and distribution during supercritical water gasification of sewage sludge. Journal of the Energy Institute, 95: 61–68
https://doi.org/10.1016/j.joei.2021.01.002
41 G Yang, G Zhang, H Wang. (2015). Current state of sludge production, management, treatment and disposal in China. Water Research, 78: 60–73
https://doi.org/10.1016/j.watres.2015.04.002
42 J Yu, L Sun, J Xiang, S Hu, S Su, J Qiu. (2012). Vaporization of heavy metals during thermal treatment of model solid waste in a fluidized bed incinerator. Chemosphere, 86(11): 1122–1126
https://doi.org/10.1016/j.chemosphere.2011.12.010
43 B Zhou, W Wu, X Li, R Dai, Z Wang. (2023). A state-of-the-art review on anaerobic digestion of sewage sludge based on microbial abundance: correlations among microbiota, performance and process parameters. Critical Reviews in Environmental Science and Technology, 54(15): 1093–1116
https://doi.org/10.1080/10643389.2023.2292972
44 W Z Zhou, X G Chen, Y Wang, N Tuersun, M Ismail, C Cheng, Z N Li, Q Song, Y Q Wang, C Y Ma. (2021). Anaerobic co-digestion of textile dyeing sludge: digestion efficiency and heavy metal stability. Science of the Total Environment, 801: 149722
https://doi.org/10.1016/j.scitotenv.2021.149722
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