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Dynamic coupling of ferrihydrite transformation and associated arsenic desorption/redistribution mediated by sulfate-reducing bacteria

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Journal of Environmental Sciences 2024年第1期135卷 39-50页

作者： Wenjing Zhou Huiyan Zhu Shiwen Hu Bowei Zhang Kun Gao zhi dang Chongxuan Liu State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control School of Environmental Science and EngineeringSouthern University of Science and TechnologyShenzhen 518055China The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationSouth China University of TechnologyGuangzhou 510006China

Sulfate-reducing bacteria play an important role in the geochemistry of iron(oxyhydr)oxide and arsenic(As)in natural environments;however,the associated reaction processes are yet to be fully understood.In this study,batch experiments coupled with geochemical,spectroscopic,microscopic,and thermodynamic analyses were conducted to investigate the dynamic coupling of ferrihydrite transformation and the associated As desorption/redistribution mediated by Desulfovibrio vulgaris(D.vulgaris).The results indicated that D.vulgaris could induce ferrihydrite transformation via S^(2-)-driven and direct reduction processes.In the absence of SO_(4)^(2-),D.vulgaris directly reduced ferrihydrite,and As desorption and re-sorption occurred simultaneously during the partial transformation of ferrihydrite to magnetite.The increase in SO_(4)^(2-)loading promoted the S^(2-)-driven reduction of ferrihydrite and accelerated the subsequent mineralogical transformation.In the low and medium SO_(4)^(2-)treatments,ferrihydrite was completely transformed to a mixture of magnetite and mackinawite,which increased the fraction of As in the residual phase and stabilized As.In the high SO_(4)^(2-)treatment,although the replacement of ferrihydrite by only mackinawite also increased the fraction of As in the residual phase,22.1%of the total As was released into the solution due to the poor adsorption affinity of As to mackinawite and the conversion of As^(5+)to As^(3+).The mechanisms of ferrihydrite reduction,mineralogy transformation,and As mobilization and redistribution mediated by sulfate-reducing bacteria are closely related to the surrounding SO_(4)^(2-)loadings.These results advance our understanding of the biogeochemical behavior of Fe,S,and As,and are helpful for the risk assessment and remediation of As contamination.

关键词： Sulfate-reducing bacteria Arsenic Ferrihydrite Transformation Redistribution

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Fe(Ⅱ)-mediated transformation of schwertmannite associated with calcium from acid mine drainage treatment

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Journal of Environmental Sciences 2023年第4期126卷 612-620页

作者： Cong Fan Chuling Guo Wei Chen Guining Lu Yu Shen zhi dang National Research Base of Intelligent Manufacturing Service Chongqing Technology and Business UniversityChongqing 400067China School of Environment and Energy South China University of TechnologyGuangzhou 510006China The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationSouth China University of TechnologyGuangzhou 510006China Chongqing Key Laboratory of Environmental Materials and Remediation Technologies Chongqing University of Arts and SciencesChongqing 402160China

Schwertmannite is an important Fe(Ⅲ)-oxyhydroxysulfate in acid mine drainage (AMD) polluted areas and its stability depends on surrounding environmental factors and previously bound elements.The treatment and neutralization of AMD normally involve the use of lime,which leads to the discharge of abundant Ca in the mining area.Such an environmental disturbance brings up an important and less considered problem of how the reductive transformation of schwertmannite associated with coexisting Ca occurred.Here,the Fe(Ⅱ)-mediated transformation of Ca-adsorbed schwertmannite and subsequent Ca repartitioning behaviors were investigated.Results showed that adsorbed Ca had a weak inhibitory effect on Fe(Ⅱ)-mediated schwertmannite transformation.Release of SO_(4)2-and SEM images both indicated that transformation rates of schwertmannite decreased under the influence of adsorbed Ca.XRD patterns indicated that adsorbed Ca altered schwertmannite transformation pathways and product compositions upon treatment with 0.4 mmol/L Fe(Ⅱ).The end products of Sch notably contained both goethite and lepidocrocite;however,transformation products of SchCa only contained goethite all along.Approximately 33.5%of the surface adsorbed-Ca was released into solution within 6 hr after Fe(Ⅱ) injection.Aqueous Ca behaved in a“first release and then im-mobilization”manner,which indicated dissolution and secondary mineralization drove Ca migration during the Fe(Ⅱ)-mediated transformation of SchCa.Adsorbed Ca blocked the surface sites for subsequent Fe(Ⅱ) adsorption,limited the Fe(Ⅱ)-Fe(Ⅲ) ETAE,and decreased the transformation rates.This work sheds light on the complex geochemical behavior of schwertmannite under the influences of environmental perturbations in AMD environments.

关键词： Acid mine drainage Schwertmannite Calcium Fe(II) Transformation

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Remediation performance and mechanisms of Cu and Cd contaminated water and soil using Mn/Al-layered double oxide-loaded biochar

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Journal of Environmental Sciences 2023年第3期125卷 593-602页

作者： Pengcheng Lin Hang Liu Hua Yin Minghan Zhu Haoyu Luo zhi dang School of Environment and Energy South China University of TechnologyGuangzhou 510006China Key Laboratory of Ministry of Education on Pollution Control and Ecosystem Restoration in Industry Clusters Guangzhou 510006China Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling Guangzhou 510006China

The combined pollution of heavy metals is ubiquitous worldwide.Mn/Al-layered double oxide-loaded crab shells biochar (LDO/BC) was prepared,so as to remediate the combined pollution of Cd and Cu in soil and water.The pristine and used LDO/BC were characterized and the results revealed that the layered double oxide was successfully loaded on crab shells biochar (BC) and metal element Ca in crab shells was beneficial to the formation of more regular layered and flake structure.The maximal adsorption capacity (Qm) of LDO/BC for aqueous Cu^(2+)and Cd^(2+)was 66.23 and 73.47 mg/g,respectively.LDO/BC and BC were used to remediate e-waste-contaminated soil for the first time and exhibited highly efficient performance.The extraction amount of Cu and Cd in the contaminated soil by diethylene triamine penta-acetic acid (DTPA) after treating with 5% LDO/BC was significantly reduced from 819.84 to 205.95 mg/kg (with passivation rate 74.8%) and 8.46 to 4.16 mg/kg(with passivation rate 50.8%),respectively,inferring that the bioavailability of heavy metals declined remarkably.The experimental result also suggested that after remediation by LDO/BC the exchangeable and weak acid soluble Cu and Cd in soil translated to reducible,residual and oxidizable fraction which are more stable state.Precipitation,complexation and ion exchange were proposed as the possible mechanisms for Cd and Cu removal.In general,these experiment results indicate that LDO/BC can be a potentially effective reagent for remediation of heavy metal contaminated water and soil.

关键词： Mn/Al-layered double oxide Biochar Cd and Cu combined pollution Adsorption Soil remediation

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Remediation of Cu and As contaminated water and soil utilizing biochar supported layered double hydroxide:Mechanisms and soil environment altering

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Journal of Environmental Sciences 2023年第4期126卷 275-286页

作者： Pengling Shao Hua Yin Yingchao Li Yuhao Cai Caiya Yan Yibo Yuan zhi dang School of Environment and Energy South China University of TechnologyGuangzhou 510006China Key Laboratory of Ministry of Education on Pollution Control and Ecosystem Restoration in Industry Clusters Guangzhou 510006China Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling Guangzhou 510006China

Preparing materials for simultaneous remediation of anionic and cationic heavy metals contamination has always been the focus of research. Herein a biochar supported FeMnMg layered double hydroxide(LDH) composites(LB) for simultaneous remediation of copper and arsenic contamination in water and soil has been assembled by a facile co-precipitation approach. Both adsorption isotherm and kinetics studies of heavy metals removal by LB were applied to look into the adsorption performance of adsorbents in water. Moreover, the adsorption mechanisms of Cu and As by LB were investigated, showing that Cu in aqueous solution was removed by the isomorphic substitution, precipitation and electrostatic adsorption while As was removed by complexation. In addition, the availability of Cu and As in the soil incubation experiments was reduced by 35.54%–63.00% and 8.39%–29.04%, respectively by using LB. Meanwhile, the addition of LB increased the activities of urease and sucrase by 93.78%–374.35% and 84.35%–520.04%, respectively, of which 1% of the dosage was the best. A phenomenon was found that the richness and structure of microbial community became vigorous within 1% dosage of LB, which indirectly enhanced the passivation and stabilization of heavy metals. These results indicated that the soil environment was significantly improved by LB. This research demonstrates that LB would be an imaginably forceful material for the remediation of anionic and cationic heavy metals in contaminated water and soil.

关键词： Heavy metal Biochar supported layered double hydroxide composite Adsorption mechanism Soil remediation Microbial community

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Extracellular polymeric substance induces biogenesis of vivianite under inorganic phosphate-free conditions

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Journal of Environmental Sciences 2022年第10期34卷 115-124页

作者： Xinrui Hao Jie Tang Xiaoyun Yi Kun Gao Qian Yao Chunhua Feng Weilin Huang zhi dang School of Environment and Energy South China University of TechnologyGuangzhou 510006China The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationSouth China University of TechnologyGuangzhou 510006China Department of Environmental Science Rutgers UniversityNew BrunswickNJ 08901USA

Vivianite is often found in reducing environments rich in iron and phosphorus from organic debris degradation or phosphorus mineral dissolution. The formation of vivianite is essential to the geochemical cycling of phosphorus and iron elements in natural environments. In this study, extracellular polymeric substances(EPS) were selected as the source of phosphorus. Microcosm experiments were conducted to test the evolution of mineralogy during the reduction of polyferric sulfate flocs(PFS) by Shewanella oneidensis MR-1(S. oneidensis MR-1) at EPS concentrations of 0, 0.03, and 0.3 g/L. Vivianite was found to be the secondary mineral in EPS treatment when there was no phosphate in the media. The EPS DNA served as the phosphorus source and DNA-supplied phosphate could induce the formation of vivianite.EPS impedes PFS aggregation, contains redox proteins and stores electron shuttle, and thus greatly promotes the formation of minerals and enhances the reduction of Fe(Ⅲ). At EPS concentration of 0, 0.03, and 0.3 g/L, the produced HCl-extractable Fe(Ⅱ) was 107.9, 111.0,and 115.2 mg/L, respectively. However, when the microcosms remained unstirred, vivianite can be formed without the addition of EPS. In unstirred systems, the EPS secreted by S. oneidensis MR-1 could agglomerate at some areas, resulting in the formation of vivianite in the proximity of microbial cells. It was found that vivianite can be generated biogenetically by S. oneidensis MR-1 strain and EPS may play a key role in iron reduction and concentrating phosphorus in the oligotrophic ecosystems where quiescent conditions prevail.

关键词： Vivianite Phosphorous Extracellular polymeric substances Polyferric flocs Shewanella oneidensis MR-1

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Efficient removal of polybrominated diphenyl ethers from soil washing effluent by dummy molecular imprinted adsorbents: Selectivity and mechanisms

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Journal of Environmental Sciences 2023年第7期129卷 45-57页

作者： Yao Ma Jinfan Chen Xiaodong Du Chunsheng Xie Jiangmin Zhou Xueqin Tao zhi dang Guining Lu School of Environment and Energy South China University of TechnologyGuangzhou 510006China Guangdong Provincial Key Laboratory of Environmental Health and Land Resource Zhaoqing UniversityZhaoqing 526061China College of Life and Environmental Sciences Wenzhou UniversityWenzhou 325035China College of Resources and Environment Zhongkai University of Agriculture and EngineeringGuangzhou 510225China The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationGuangzhou 510006China Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling South China University of TechnologyGuangzhou 510006China

Surfactant enhanced elution is an effective method for removing hydrophobic organic pollutants from soils.The key to the development of leaching technology is selective removal of targeted pollutants in soil washing effluent and recycling of surfactant solutions.In this study,a molecular imprinting technique was applied to selectively sorb polybrominated diphenyl ethers(PBDEs)in soil washing effluent.The novel molecular imprinted polymers(MIPs)using different template molecules were synthesized by precipitation polymerization.Adsorption behaviors andmechanisms ofMIPs were studied through experiments and theoretical calculations.The results show that 4-bromo-4'-hydroxybiphenyl and toluene can be effective imprinting molecule for MIPs synthesis.The maximal adsorption capacity of selected dummy molecular imprinted polymer(D1-MIP)was 1032.36μmol/g,and that of part molecular imprinted polymer(P-MIP)was 981.13μmol/g.Their imprinting factors in 5 PBDEs adsorption ranged from 2.13 to 5.88,the recovery percentage of Triton X-100 can reach 99.09%,confirming the feasibility of reusing surfactant.Various PBDEs could be removed by MIPs,and Quantitative Structure Property Relationship analysis revealed that PBDEs’molecular volume,planarity,polarity,and hydrophobicity have major influences on their adsorption performance.DFT calculation revealed that Van derWaals force and hydrogen bonding played important roles during selective adsorption.These results can provide effective theoretical guidance for surfactant enhanced soil elution in practical engineering applications.

关键词： Molecular imprinting Selective adsorption Polybrominated diphenyl ethers Triton X-100 DFT calculation

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A binder-free electrode for efficient H_(2)O_(2) formation and Fe2+ regeneration and its application to an electro-Fenton process for removing organics in iron-laden acid wastewater

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Chinese Chemical Letters 2022年第2期33卷 920-925页

作者： Ziliang Wei Haolin Xu Zhenchao Lei Xiaoyun Yi Chunhua Feng zhi dang The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationSchool of Environment and EnergySouth China University of TechnologyGuangzhou 510006China

The electro-Fenton process,with its capacity for in-situ H_(2)O_(2)formation and Fe^(2+)regeneration,is a strik-ing alternative to the traditional chemical-Fenton process.However,the frequent requirement of extra binders for electrode fabrication leads to low catalyst utilization,a complex fabrication process,and weak conductivity.Herein,a three-dimensional(3D)porous electrode was fabricated in-situ on a Ni foam(NF)substrate integrated with nitrogen-doped carbon nanotubes(N@C)derived from carbonization of zeolitic imidazolate framework-8(ZIF-8)without any binder.The resulting 900/N@C-NF cathode(synthesized at 900℃)was high in surface area,N content,and degree of graphitization,achieved high performance of H_(2)O_(2)production(2.58 mg L^(−1)h^(−1)H_(2)O_(2)/mg catalyst)at-0.7 V(vs.SCE),and enabled prompt regeneration of Fe^(2+).The electro-Fenton system equipped with the 900/N@C-NF cathode was effective in removing a diverse range of organic pollutants,including rhodamine B(Rh B),phenol,bisphenol A(BPA),nitroben-zene(NB),and Cu-ethylenediaminetetraacetic acid(EDTA),and signiﬁcantly attenuating the concentration of chemical oxygen demand(COD)in the real acid wastewater,exhibiting superior activity and stability.This binder-free and self-supporting electro-Fenton cathode was thus shown to be an attractive candidate for application to wastewater treatment,particularly those rich in organics,acids,and Fe^(3+)/Fe^(2+).

关键词： Binder-free electrode Oxygen reduction reaction N-doped carbon nanotubes Fe^(2+)regeneration Acid wastewater treatment

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Accumulation, transportation, and distribution of tetracycline and cadmium in rice

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Journal of Environmental Sciences 2023年第4期126卷 58-69页

作者： Chunfeng He Jini Zhou Chen Yang zhiyi Song Junheng He Ziqing Huang Yurong Deng Jinling Wang Yu Xiong zhi dang College of Environment and Energy South China University of TechnologyGuangzhou 510006China The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationGuangzhou 510006China Department of Environmental Sciences The State University of New JerseyRutgers UniversityNew BrunswickNJ 08901USA Guangdong Institute of Ecological Environment and Soil Guangzhou 510650China

Co-exposure to heavy metal and antibiotic pollution might result in complexation and synergistic interactions,affecting rice growth and further exacerbating pollutant enrichment.Therefore,our study sought to clarify the influence of different Tetracycline (TC) and Cadmium(Cd) concentration ratios (both alone and combined) on rice growth,pollutant accumulation,and transportation during the tillering stage in hydroponic system.Surprisingly,our findings indicated that the interaction between TC and Cd could alleviate the toxic effects of TC/Cd on aerial rice structures and decrease pollutant burdens during root elongation.In contrast,TC and Cd synergistically promoted the accumulation of TC/Cd in rice roots.However,their interaction increased the accumulation of TC in roots while decreasing the accumulation of Cd when the toxicant doses increased.The strong affinity of rice to Cd promoted its upward transport from the roots,whereas the toxic effects of TC reduced TC transport.Therefore,the combined toxicity of the two pollutants inhibited their upward transport.Additionally,a low concentration of TC promoted the accumulation of Cd in rice mainly in the root tip.Furthermore,a certain dose of TC promoted the upward migration of Cd from the root tip.Laser ablation-inductively coupled plasma mass spectrometry demonstrated that Cd mainly accumulated in the epidermis and stele of the root,whereas Fe mainly accumulated in the epidermis,which inhibited the absorption and accumulation of Cd by the rice roots through the generation of a Fe plaque.Our findings thus provide insights into the effects of TC and Cd co-exposure on rice growth.

关键词： Laser ablation-inductively coupled plasma mass spectrometry Tetracycline Cadmium Accumulation Distribution

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Co-metabolic and biochar-promoted biodegradation of mixed PAHs by highly efficient microbial consortium QY1

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Journal of Environmental Sciences 2021年第9期33卷 65-76页

作者： Min Li Hua Yin Minghan Zhu Yuanyuan Yu Guining Lu zhi dang Key Laboratory of Ministry of Education on Pollution Control and Ecosystem Restoration in Industry Clusters School of Environment and EnergySouth China University of TechnologyGuangdong 510006China Guangdong Provincial Key Laboratory of Petrochemical Pollution Processes and Control School of Environmental Science and EngineeringGuangdong University of Petrochemical TechnologyGuangdong 525000China

Polycyclic aromatic hydrocarbons(PAHs), typical representatives of the persistent organic pollutants(POPs), have become ubiquitous in the environment.In this study, a novel microbial consortium QY1 that performed outstanding PAHs-degrading capacity has been enriched.The degradation characteristics of single and mixed PAHs treated with QY1 were studied, and the effect of biochar on biodegradation of mixed PAHs and the potential of biochar in PAHs-heavy metal combined pollution bioremediation were also investigated.Results showed that, in single substrate system, QY1 degraded 94.5% of 500 mg/L phenanthrene(PHE) and 17.8% of 10 mg/L pyrene(PYR) after 7 days, while in PHE-PYR mixture system, the biodegradation efficiencies of PHE(500 mg/L) and PYR(10 mg/L) reached 94.0%and 96.2%, respectively, since PHE served as co-metabolic substrate to have significantly improved PYR biodegradation.Notably, with the cooperation of biochar, the biodegradations of PHE and PYR were greatly accelerated.Further, biochar could reduce the adverse impact of heavy metals(Cd^(2+), Cu^(2+), Cr_(2)O_(7)^(2-)) on PYR biodegradation remarkably.The sequencing analysis revealed that Methylobacterium, Burkholderia and Stenotrophomonas were the dominant genera of QY1 in almost all treatments, indicating that these genera might play key roles in PAHs biodegradation.Overall, this study provided new insights into the efficient bioremediation of PAHs-contaminated site.

关键词： Polycyclic aromatic hydrocarbons Microbial consortium Co-metabolism Biochar Heavy metals Microbial community

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Degradation of 2,2′,4,4′-tetrabromodiphenyl ether by Pycnoporus sanguineus in the presence of copper ions

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Journal of Environmental Sciences 2019年第9期31卷 133-143页

作者： Meiqian Wang Hua Yin Hui Peng Mi Feng Guining Lu zhi dang Key Laboratory of Ministry of Education on Pollution Control and Ecosystem Restoration in Industry Clusters Guangdong Provincial Engineering and Technology Research Center for Environmental Risk Prevention and Emergency Disposal School of Environment and Energy South China University of Technology Guangzhou 510006 China Department of Chemistry Jinan University Guangzhou 510632 China

The degradation of 2,2′,4,4′-tetrabromodiphenyl ether(BDE-47) by Pycnoporus sanguineus was investigated in order to explore the impact of the heavy metal Cu2+ on BDE-47 decomposition and the subsequent formation of metabolites, as well as to further elucidate the degradation mechanism of BDE-47. An increase in degradation rate from 18.63% to49.76% in the first four days and its stabilization at(51.26 ± 0.08)% in the following days of BDE-47 incubation were observed. The presence of Cu2+ at 1 and 2 mg/L was found to promote the degradation rate to 56.41% and 60.79%, respectively, whereas higher level of Cu2+(≥ 5 mg/L) inhibited the removal of BDE-47. The similar concentration effects of Cu2+ was also found on contents of fungal protein and amounts of metabolites. Both intracellular and extracellular enzymes played certain roles in BDE-47 transportation with the best degradation rate at 27.90% and 27.67% on the fourth and third day, individually. During the degradation of BDE-47, four types of hydroxylated polybrominated diphenyl ethers(OH-PBDEs), i.e., 6′-OH-BDE-47, 5′-OH-BDE-47, 4′-OH-BDE-17, 2′-OH-BDE-28, and two bromophenols, i.e., 2,4-DBP and 4-BP were detected and considered as degradation products. These metabolites were further removed by P. sanguineus at rates of 22.42%,23.01%, 27.04%, 27.96%, 64.21%, and 40.62%, respectively.

关键词： Degradation BDE-47 Copper Pycnoporus sanguineus OH-PBDEs

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