腐殖酸对好氧颗粒污泥系统的调控机理研究——以石墨烯和氧化石墨烯产生的毒性影响为例

张明, 冯雪丽, 时文歆, 张冰

中国环境科学 ›› 2025, Vol. 45 ›› Issue (4) : 1995-2007.

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中国环境科学 ›› 2025, Vol. 45 ›› Issue (4) : 1995-2007.
水污染与控制

腐殖酸对好氧颗粒污泥系统的调控机理研究——以石墨烯和氧化石墨烯产生的毒性影响为例

  • 张明, 冯雪丽, 时文歆, 张冰
作者信息 +

The regulatory mechanism of humic acid on aerobic granular sludge under prolonged exposure to graphene and oxide grapheme

  • ZHANG Ming, FENG Xue-li, SHI Wen-xin, ZHANG Bing
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文章历史 +

摘要

以受纳米材料石墨烯(G)和氧化石墨烯(GO)长期胁迫作用下的好氧颗粒污泥系统(AGS)为研究对象,探究投加适量腐殖酸(HA)对AGS理化特性和污染物处理性能的缓解作用及其机理.研究表明:经过适量浓度的HA (10.0mg/L)处理后,实验组R2(1.0mg/L G)和R3(1.0mg/L GO)中AGS的理化特性与系统的处理性能均得到了明显改善.其中,在整个实验期间(第0~75d),R3系统内的AGS平均粒径由1224.1μm增加至1407.5μm,R2系统内的AGS平均粒径由1313.0μm增加至1461.3μm.AGS理化特性的提升使得R2和R3系统内总氮去除率分别上升了2.3%和7.6%.通过投加HA,R2和R3系统内观察到活性氧含量、乳酸脱氢酶活性、过氧化氢酶活性和超氧化物歧化酶活性均出现明显降低,这是由于HA可以与细胞内积累的活性氧相结合,进而降低G和GO胁迫下生物体内产生的氧化应激水平.此外,HA的引入减少了AGS中胞外聚合物(EPS)的过量分泌,并降低了EPS中芳香类蛋白质和酪氨酸类物质的含量,使得AGS呈现出更加致密紧凑的颗粒结构.最后,分析G和GO在HA投加前后Zeta电位的变化情况,结果表明投加适量HA提高了G和GO的初始电势值,增强了G/GO与微生物之间的排斥力作用,减少了微生物与G/GO之间的直接接触,进而有效缓解了G和GO对AGS微生物产生的毒性影响.

Abstract

This study aimed to investigate the mitigating effect and regulatory mechanism of humic acid (HA) on the physicochemical properties and pollutant treatment performance of aerobic granular sludge (AGS) under prolonged stress induced by graphene (G) and oxide graphene (GO). The results demonstrated that the optimal dosage of HA (10mg/L) significantly enhanced the physicochemical characteristics of AGS, and improved the pollutant treatment performance of the AGS reactor (R2 (1.0mg/L G) and R3 (1.0mg/L GO)). At the 75th day, in R3, there was an obviously increase in average particle size of AGS from 1224.1μm to 1407.5μm, while in R2it increased from 1313.0μm to 1461.3μm. Simultaneously, the enhancement of AGS physicochemical properties led to a respective increase of 2.3% and 7.6% in TN removal efficiency for R2 and R3. The introduction of HA resulted in a significant reduction in the levels of reactive oxygen species (ROS), lactate dehydrogenase activity, catalase activity, and superoxide dismutase activity in R2 and R3. This suggested that HA can effectively bind with accumulated ROS within cells to further mitigate oxidative stress levels induced by G and GO. The addition of HA also effectively alleviated the excessive secretion of extracellular polymeric substances (EPS) in AGS, resulting in a decrease in the content of aromatic proteins and tyrosine-like substances within EPS. Consequently, this led to a more compact and denser AGS particle structure in R2 and R3. Ultimately, the changes in Zeta potential of G and GO (before and after the addition of HA) indicate that the incorporation of HA can enhance the initial potential values of G and GO, thereby augmenting the repulsive effect between G/GO and microorganisms, reducing direct contact between microorganisms and G/GO, thus effectively mitigating the toxic effects exerted by G and GO on microorganisms.

关键词

Zeta电位 / 胞外聚合物 / 好氧颗粒污泥 / 石墨烯 / 氧化石墨烯 / 氧化应激反应

Key words

aerobic granular sludge (AGS) / extracellular polymeric substances (EPS) / graphene (G) / oxidative stress response / oxide graphene (GO) / Zeta potential

引用本文

导出引用
张明, 冯雪丽, 时文歆, 张冰. 腐殖酸对好氧颗粒污泥系统的调控机理研究——以石墨烯和氧化石墨烯产生的毒性影响为例[J]. 中国环境科学. 2025, 45(4): 1995-2007
ZHANG Ming, FENG Xue-li, SHI Wen-xin, ZHANG Bing. The regulatory mechanism of humic acid on aerobic granular sludge under prolonged exposure to graphene and oxide grapheme[J]. China Environmental Science. 2025, 45(4): 1995-2007
中图分类号: X703   

参考文献

[1] Adav S S, Lee D J, Show K Y, et al. Aerobic granular sludge:recent advances[J]. Biotechnol Advances, 2008,26(5):411-423.
[2] Nancharaiah Y V, Reddy G K K. Aerobic granular sludge technology:mechanisms of granulation and biotechnological applications[J]. Bioresource Technology, 2018,247:1128-1143.
[3] Chen J, Yu Z, Cheng P, et al. Microbial synergy achieving simultaneous nitrification-denitrification (SND) in salt-tolerant aerobic granular sludge[J]. Journal of Water Process Engineering, 2024,60:105138.
[4] Peng T, Wang Y, Wang J, et al. Effect of different forms and components of EPS on sludge aggregation during granulation process of aerobic granular sludge[J]. Chemosphere, 2022,303:135116.
[5] Barrios A C, Wang Y, Gilbertson L M, et al. Structure-property-toxicity relationships of graphene oxide:Role of surface chemistry on the mechanisms of interaction with bacteria[J]. Environmental Science& Technology, 2019,53(24):14679-14687.
[6] Han Y, Knightes C D, Bouchard D, et al. Simulating graphene oxide nanomaterial phototransformation and transport in surface water[J]. Environmental Science:Nano, 2019,6(1):180-194.
[7] Priyadharshini S D, Manikandan S, Kiruthiga R, et al. Graphene oxide-based nanomaterials for the treatment of pollutants in the aquatic environment:Recent trends and perspectives-A review[J]. Environmental Pollution, 2022,306:119377.
[8] Guo C, Wang Y, Luo Y, et al. Effect of graphene oxide on the bioactivities of nitrifying and denitrifying bacteria in aerobic granular sludge[J]. Ecotoxicology and Environmental Safety, 2018,156:287-293.
[9] Keller A A, Lazareva A. Predicted releases of engineered nanomaterials:from global to regional to local[J]. Environmental Science& Technology Letters, 2014,1(1):65-70.
[10] Kedves A, Sánta L, Balázs M, et al. Chronic responses of aerobic granules to the presence of graphene oxide in sequencing batch reactors[J]. Journal of hazardous materials, 2020,389:121905.
[11] Zhang M, Fu G, Shi W, et al. Microbial response to the chronic toxicity effect of graphene and graphene oxide nanomaterials within aerobic granular sludge systems[J]. Journal of Hazardous Materials, 2024:135350.
[12] Wei S, Li Z, Sun Y, et al. A comprehensive review on biomass humification:Recent advances in pathways, challenges, new applications, and perspectives[J]. Renewable and Sustainable Energy Reviews, 2022,170:112984.
[13] Yang F, Antonietti M. Artificial humic acids:sustainable materials against climate change[J]. Advanced Science, 2020,7(5):1902992.
[14] Zashikhin A V, Suvorova O N. Properties of Gold-Bearing Humic Acids[J]. Journal of Mining Science, 2023,59(2):311-319.
[15] Zhao J, Li Y, Cao X, et al. Humic acid mitigated toxicity of graphene-family materials to algae through reducing oxidative stress and heteroaggregation[J]. Environmental Science-Nano, 2019,6(6):1909-1920.
[16] Deng C, Gong J, Zeng G, et al. Graphene-cds nanocomposite inactivation performance toward escherichia coli in the presence of humic acid under visible light irradiation[J]. Chemical Engineering Journal, 2016,284:41-53.
[17] Zhang X, Sui M, Yan X, et al. Mitigation in the toxicity of graphene oxide nanosheets towards escherichia coli in the presence of humic acid[J]. Environmental Science-Processes& Impacts, 2016,18(6):744-750.
[18] 国家环境保护总局.《水和废水监测分析方法》编委会.水和废水监测分析方法(第四版)[M].北京:中国环境科学出版社, 2002. Ministry of Ecology and Environment of the People's Republic of China.Water and wastewater monitoring and analysis methods[M]. 4th ed. Beijing:China Environmental Science Press, 2002.
[19] Wang Z, Gao M, Wang Z, et al. Effect of salinity on extracellular polymeric substances of activated sludge from an anoxic-aerobic sequencing batch reactor[J]. Chemosphere, 2013,93(11):2789-2795.
[20] Dubios M, Gilles K A, Hamilton J K, et al. Colorimetric method for determination of sugar and related substances[J]. Analytical Chemistry, 1956,28:250-256.
[21] Baghoth S A, Sharma S K, Amy G L. Tracking natural organic matter (nom) in a drinking water treatment plant using fluorescence excitation-emission matrices and parafac[J]. Water Research, 2011, 45(2):797-809.
[22] 余华荣.基于微生物群体感应猝灭的MBR膜污染控制研究[D].哈尔滨:哈尔滨工业大学, 2015. Yu H. Research on membrane fouling control in MBR based on microbial quorum quenching[D]. Harbin:Harbin institute of technology, 2015.
[23] Kuo-Dahab W C, Stauch-White K, Butler C S, et al. Investigation of the fate and dynamics of extracellular polymeric substances (EPS) during sludge-based photogranulation under hydrostatic conditions[J]. Environmental Science& Technology, 2018,52(18):10462-10471.
[24] Huang S, Zhang B, Cui F, et al. Mechanisms underlying the detrimental impact of micro (nano) plastics on the stability of aerobic granular sludge:Interactions between micro (nano) plastics and extracellular polymeric substances[J]. Journal of Hazardous Materials, 2024:135512.
[25] Lu C, Yuan C, Zhu T, et al. Effect of humic acid on the single-stage nitrogen removal using anammox and partial nitritation (snap) process:Performance and bacterial communities[J]. Journal of Environmental Chemical Engineering, 2021,9(6):106680.
[26] Caluwé M, Dobbeleers T, D'aes J, et al. Formation of aerobic granular sludge during the treatment of petrochemical wastewater[J]. Bioresource Technology, 2017,238:559-567.
[27] Huang B C, Li G F, Ren Z Q, et al. Light-Driven electron uptake from nonfermentative organic matter to expedite nitrogen dissimilation by chemolithotrophic anammox consortia[J]. Environmental Science& Technology, 2023,57(34):12732-12740.
[28] Li Y Q, Zhao B H, Zhang Y Q, et al. Insight into response mechanism of aerobic granular sludge to combined nanoparticle stress:Nitrogen removal, microbial community and heavy metal resistance genes[J]. Chemical Engineering Journal, 2024,496:154327.
[29] Chen M, Yin J, Liang Y, et al. Oxidative stress and immunotoxicity induced by graphene oxide in zebrafish[J]. Aquatic Toxicology, 2016, 174:54-60.
[30] Elahinik A, de Clercq F, Pabst M, et al. Effects of salinity on glycerol conversion and biological phosphorus removal by aerobic granular sludge[J]. Water Research, 2024,257:121737.
[31] Meng F, Huang W, Liu D, et al. Application of aerobic granules-continuous flow reactor for saline wastewater treatment:Granular stability, lipid production and symbiotic relationship between bacteria and algae[J]. Bioresource Technology, 2020,295:122291.
[32] Zhang B, Huang S, Wu L, et al. Micro (nano) plastic size and concentration co-differentiate the treatment performance and toxicity mechanism in aerobic granular sludge systems[J]. Chemical Engineering Journal, 2023,457:141212.
[33] He C, He P, Yang H, et al. Impact of zero-valent iron nanoparticles on the activity of anaerobic granular sludge:From macroscopic to microcosmic investigation[J]. Water Research, 2017,127:32-40.
[34] Zhang L, Feng X, Zhu N, et al. Role of extracellular protein in the formation and stability of aerobic granules[J]. Enzyme and Microbial Technology, 2007,41(5):551-557.
[35] Chabaliná Domínguez L, Pastor Rodríguez M, Prats, et al. Characterization of soluble and bound eps obtained from 2submerged membrane bioreactors by 3D-EEM and hpsec[J]. Talanta, 2013,115:706-712.
[36] Yin Y, Sun J, Liu F, et al. Effect of nitrogen deficiency on the stability of aerobic granular sludge[J]. Bioresource Technology, 2018,275:307-313.
[37] Zhang M, Xu Y, Xiao K Q, et al. Characterising soil extracellular polymeric substances (EPS) by application of spectral-chemometrics and deconstruction of the extraction process[J]. Chemical Geology, 2023,618:121271.
[38] Zhou M R, Qu J B, Li Peng, et al. The"Cluster-Regression"COD prediction model of distributed rural sewage based on three-dimensional fluorescence spectrum and ultraviolet-visible absorption spectrum[J]. Spectroscopy and Spectral Analysis, 2022,42(7):2113-2119.
[39] Chen Y, Ren C, Ouyang S, et al. Mitigation in multiple effects of graphene oxide toxicity in zebrafish embryogenesis driven by humic acid[J]. Environmental Science& Technology, 2015,49(16):10147-10154.

基金

国家自然科学基金资助项目(52370029,52270025)

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