Electrode loaded ferrihydrite enhances the performance of the soil microbial electrochemical system in the remediation of petroleum hydrocarbon-contaminated soil

YU Xin; ZHANG Xiao-lin; QU Yong-shuai; ZHONG Peng-ju; LU jia-jun; LI Xiao-jing

PDF(3327 KB)

China Environmental Science ›› 2026, Vol. 46 ›› Issue (3) : 1475-1485.

Electrode loaded ferrihydrite enhances the performance of the soil microbial electrochemical system in the remediation of petroleum hydrocarbon-contaminated soil

YU Xin¹, ZHANG Xiao-lin¹, QU Yong-shuai², ZHONG Peng-ju¹, LU jia-jun², LI Xiao-jing¹

Author information +

History +

Abstract

To investigate the enhanced effect of ferrihydrite-loaded electrodes on the degradation of organic pollutants in petroleum-contaminated soil using a Microbial Electrochemical System (MES), and to elucidate the underlying synergistic mechanisms, a single-chamber soil MES reactor was constructed. Using oil-contaminated soil as the experimental medium, we compared the performance of the original soil, the conventional electrode setup, and the ferrihydrite-loaded electrode setup. The system's effectiveness was evaluated through electrochemical analysis, assessment of soil carbon degradation and transformation, characterization of iron forms, and determination of enzyme activity. Results indicate that loading electrodes with ferrihydrite significantly improved the system's electrochemical performance, with cumulative charge output increasing by 18%. The carbon degradation capacity was also enhanced, with the total carbon degradation rate increasing by up to 11%, effectively promoting the transformation of recalcitrant carbon, such as humus, into more labile forms. Ferrihydrite facilitated the iron cycle, with iron ion content increasing by up to 28%, thereby enhancing the Fe(II)/Fe(III) redox cycling and strengthening the coupling between carbon and nitrogen transformations. Additionally, the bioelectric field accelerated the phase transformation of ferrihydrite into goethite and hematite. The presence of ferrihydrite stimulated microbial secretion of degradative enzymes, significantly increasing the activity of key enzymes involved in pollutant degradation. Mantel test results further reveal that dehydrogenase and polyphenol oxidase served as the primary drivers of carbon mineralization.

Key words

soil microbial electrochemical system / ferrihydrite / carbon degradation/transformation / iron cycle / oil-contaminated soil

Cite this article

EndNote

Ris (Procite)

Bibtex

Download Citations

YU Xin, ZHANG Xiao-lin, QU Yong-shuai, ZHONG Peng-ju, LU jia-jun, LI Xiao-jing. Electrode loaded ferrihydrite enhances the performance of the soil microbial electrochemical system in the remediation of petroleum hydrocarbon-contaminated soil[J]. China Environmental Science. 2026, 46(3): 1475-1485

References

[1] Mohan S V, Chandrasekhar K. Self-induced bio-potential and graphite electron accepting conditions enhances petroleum sludge degradation in bio-electrochemical system with simultaneous power generation [J]. Bioresource Technology, 2011,102(20):9532-9541.
[2] Zhou Q, Sun F, Liu R. Joint chemical flushing of soils contaminated with petroleum hydrocarbons [J]. Environment International, 2005,31 (6):835-839.
[3] Kronenberg M, Trably E, Bernet N, et al. Biodegradation of polycyclic aromatic hydrocarbons: Using microbial bioelectrochemical systems to overcome an impasse [J]. Environmental Pollution, 2017,231:509- 523.
[4] Zhang T, Gannon S M, Nevin K P, et al. Stimulating the anaerobic degradation of aromatic hydrocarbons in contaminated sediments by providing an electrode as the electron acceptor [J]. Environmental Microbiology, 2010,12(4):1011-1020.
[5] Lu L, Huggins T, Jin S, et al. Microbial metabolism and community structure in response to bioelectrochemically enhanced remediation of petroleum hydrocarbon-contaminated soil [J]. Environmental Science and Technology, 2014,48(7):4021-4029.
[6] Wang X, Cai Z, Zhou Q, et al. Bioelectrochemical stimulation of petroleum hydrocarbon degradation in saline soil using U-tube microbial fuel cells [J]. Biotechnology and Bioengineering, 2012, 109(2):426-433.
[7] 赵晓东,李晓晶,赵鹏宇,等.土壤微生物电化学系统降解四环素的机理 [J]. 中国环境科学, 2021,41(2):778-786. Zhao X D, Li X J, Zhao P Y, et al. Mechanism of tetracycline degradation by soil microbial electrochemical systems [J]. Zhongguo Huanjing Kexue [J]. China Environmental Science, 2021,41(2): 778-786.
[8] 李瑞祥,李田,张晓林,等.微生物电化学技术在石油烃污染土壤修复中的应用研究进展 [J]. 中国环境科学, 2023,43(6):3042-3054. Li R X, Li T, Zhang X L, et al. Application and progress of microbial electrochemical technology in the remediation of petroleum contaminated soil [J]. China Environmental Science, 2023,43(6): 3042-3054.
[9] 朱丽君,王欢,李绍峰,等.水平碳纤维刷耦合生物电化学系统强化土壤中总石油烃降解及扩展作用半径 [J]. 环境工程, 2023,41(7): 159-165. Zhu L J, Wang H, Li S F, et al. Horizontal carbon fiber brush coupling bioelectrochemical system to strengthen total petroleum hydrocarbon degradation and expand influence radius [J]. Chinese Journal of Environmental Engineering, 2023,41(7):159-165.
[10] 刘诗彧,王荣昌,马翠香,等.氧化石墨烯与聚苯胺修饰阴极的微生物燃料电池电化学性能 [J]. 中国环境科学, 2019,39(9):3866-3871. Liu S H, Wang R C, Ma C X, et al. Electrochemical performance of microbial fuel cell with graphene oxide and polyaniline loaded cathode [J]. China Environmental Science, 2019,39(9):3866-3871.
[11] 郑飞,朱维晃,高昊翔.微生物还原石墨烯修饰碳毡电极的电化学特征 [J]. 中国环境科学, 2019,39(2):823-830. Zheng F, Zhu W H, Gao H X, et al. Electrochemical characteristics of microbe reduced graphene loaded carbon felt electrodes [J]. China Environmental Science, 2019,39(2):823-830.
[12] Qin X, Lu X, Cai T, et al. Magnetite-enhanced bioelectrochemical stimulation for biodegradation and biomethane production of waste activated sludge [J]. Science of The Total Environment, 2021,789: 147859.
[13] Vu M T, Noori M T, Min B. Conductive magnetite nanoparticles trigger syntrophic methane production in single chamber microbial electrochemical systems [J]. Bioresource Technology, 2020,296: 122265.
[14] Kato S, Hashimoto K, Watanabe K. Methanogenesis facilitated by electric syntrophy via (semi)conductive iron-oxide minerals [J]. Environmental Microbiology, 2012,14(7):1646-1654.
[15] Kato S, Hashimoto K, Watanabe K. Microbial interspecies electron transfer via electric currents through conductive minerals [J]. Proceedings of the National Academy of Sciences, 2012,109(25): 10042-10046.
[16] Hiemstra T. Surface and mineral structure of ferrihydrite [J]. Geochimica et Cosmochimica Acta, 2013,105:316-325.
[17] Usman M, Byrne J M, Chaudhary A, et al. Magnetite and green rust: synthesis, properties, and environmental applications of mixed-valent iron minerals [J]. Chemical Reviews, 2018,118(7):3251-3304.
[18] Jiao Y, Kappler A, Croal L R, et al. Isolation and characterization of a genetically tractable photoautotrophic Fe(II)-oxidizing bacterium, rhodopseudomonas palustris strain TIE-1 [J]. Appl Environ Microbiol, 2005,71:4487.
[19] Sakakibara M, Tanaka M, Takahashi Y, et al. Redistribution of Zn during transformation of ferrihydrite: Effects of initial Zn concentration [J]. Chemical Geology, 2019,522:121-134.
[20] Childs C W. Ferrihydrite: A review of structure, properties and occurrence in relation to soils [J]. Zeitschrift für Pflanzenernährung und Bodenkunde, 1992,155(5):441-448.
[21] Chen X, Han T, Miao X, et al. Ferrihydrite enhanced the electrogenic hydrocarbon degradation in soil microbial electrochemical remediation [J]. Chemical Engineering Journal, 2022,446:136901.
[22] He J, Yang C, Deng Y, et al. Mechanistic insights into the environmental fate of tetracycline affected by ferrihydrite: Adsorption versus degradation [J]. Science of The Total Environment, 2022,811: 152283.
[23] Schmidtmann J, Elagami H, Gilfedder B S, et al. Heteroaggregation of PS microplastic with ferrihydrite leads to rapid removal of microplastic particles from the water column [J]. Environmental Science: Processes & Impacts, 2022,24(10):1782-1789.
[24] Veronico L, Gentile L. Removal of pollutants by ferrihydrite nanoparticles combined with Brij L4self-assembled nanostructures [J]. ACS Applied Nano Materials, 2023,6(1):720-728.
[25] Li X, Wang X, Ren Z J, et al. Sand amendment enhances bioelectrochemical remediation of petroleum hydrocarbon contaminated soil [J]. Chemosphere, 2015,141:62-70.
[26] Li X, Wang X, Zhao Q, et al. Carbon fiber enhanced bioelectricity generation in soil microbial fuel cells [J]. Biosensors and Bioelectronics, 2016,85:135-141.
[27] Li X, Li Y, Zhang X, et al. Long-term effect of biochar amendment on the biodegradation of petroleum hydrocarbons in soil microbial fuel cells [J]. Science of The Total Environment, 2019,651:796-806.
[28] Yang S, Chang X, Pan Z. Effects of earthworms on soil enzyme activities and microbial communities of chlortetracycline- contaminated soils [J]. Journal of Agro-Environment Science, 2020,40(6):1268-1280.
[29] Zhao Y, Moore O W, Xiao K Q, et al. The role and fate of organic carbon during aging of ferrihydrite [J]. Geochimica et Cosmochimica Acta, 2022,335:339-355.
[30] Wang X, Tang C, Baldock J A, et al. Long-term effect of lime application on the chemical composition of soil organic carbon in acid soils varying in texture and liming history [J]. Biology and Fertility of Soils, 2016,52(3):295-306.
[31] Whittinghill K A, Hobbie S E. Effects of pH and calcium on soil organic matter dynamics in Alaskan tundra [J]. Biogeochemistry, 2012, 111(1):569-581.
[32] Wang D, Mai L, Yu Z, et al. Deciphering the bioavailability of dissolved organic matter in thermophilic compost and vermicompost at the molecular level [J]. Bioresource Technology, 2024,391:129947.
[33] Yang S, Wang K, Yu X, et al. Fulvic acid more facilitated the soil electron transfer than humic acid [J]. Journal of Hazardous Materials, 2024,469:134080.
[34] Du L, Liu Y, Hao Z, et al. Fertilization regime shifts the molecular diversity and chlorine reactivity of soil dissolved organic matter from tropical croplands [J]. Water Research, 2022,225:119106.
[35] Wang K, Yang S, Yu X, et al. Effect of microplastics on the degradation of tetracycline in a soil microbial electric field [J]. Journal of Hazardous Materials, 2023,460:132313.
[36] Wei W, Wang C, Shi X, et al. Multiple microplastics induced stress on anaerobic granular sludge and an effectively overcoming strategy using hydrochar [J]. Water Research, 2022,222:118895.
[37] Li S, Cao Y, Zhao Z, et al. Regulating secretion of extracellular polymeric substances through dosing magnetite and zerovalent iron nanoparticles to affect anaerobic digestion mode [J]. ACS Sustainable Chemistry & Engineering, 2019,7(10):9655-9662.
[38] Li S, Cao Y, Bi C, et al. Promoting electron transfer to enhance anaerobic treatment of azo dye wastewater with adding Fe(OH)₃ [J]. Bioresource Technology, 2017,245:138-144.
[39] Notini L, Thomasarrigo L K, Kaegi R, et al. Coexisting goethite promotes Fe(II)-catalyzed transformation of ferrihydrite to goethite [J]. Environmental Science & Technology, 2022,56(17):12723-12733.
[40] Yoon Y, Kim B, Cho M. Mineral transformation of poorly crystalline ferrihydrite to hematite and goethite facilitated by an acclimated microbial consortium in electrodes of soil microbial fuel cells [J]. Science of The Total Environment, 2023,902:166414.
[41] Schulz K, Wisawapipat W, Barmettler K, et al. Iron oxyhydroxide transformation in a flooded rice paddy field and the effect of adsorbed phosphate [J]. Environmental Science & Technology, 2024,58(24): 10601-10610.
[42] Zhuang L, Tang Z, Ma J, et al. Enhanced anaerobic biodegradation of benzoate under sulfate-reducing conditions with conductive iron- oxides in sediment of pearl river estuary [J]. Frontiers in Microbiology, 2019,10.
[43] Han T, Wang K, Rushimisha I E, et al. Influence of biocurrent self-generated by indigenous microorganisms on soil quality [J]. Chemosphere, 2022,307:135864.
[44] Han T, Chen X, Wang K, et al. Electron transfer by ion conductance in a soil bioelectric field [J]. Sustainable Energy Technologies and Assessments, 2023,55:102902.
[45] Chen X, Li X, Li Y, et al. Bioelectric field drives ion migration with the electricity generation and pollutant removal [J]. Environmental Technology & Innovation, 2021,24:101901.
[46] Zhang X, Xue W, Wang G, et al. Biogeochemical coupling of C/Fe in oil-polluted wetlands associated with iron reduction [J]. Communications Earth & Environment, 2025,6(1):77.
[47] Zhang X, Liu Y, Zhou Q, et al. Exogenous electroactive microbes regulate soil geochemical properties and microbial communities by enhancing the reduction and transformation of Fe(III) minerals [J]. Environmental Science & Technology, 2023,57(20):7743-7752.
[48] Subrahmanyam G, Shen J P, Liu Y R, et al. Effect of long-term industrial waste effluent pollution on soil enzyme activities and bacterial community composition [J]. Environmental Monitoring and Assessment, 2016,188(2):112.
[49] Okafor C D, Lanier K A, Petrov A S, et al. Iron mediates catalysis of nucleic acid processing enzymes: support for Fe(II) as a cofactor before the great oxidation event [J]. Nucleic Acids Research, 2017, 45(7):3634-3642.
[50] Burns R G. International conference: enzymes in the environment: activity, ecology and applications [J]. Soil Biology and Biochemistry, 2000,32(13):1815-1815.