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Simultaneous removal of Cd(Ⅱ)and As(Ⅴ)by ferrihydrite-biochar composite:Enhanced effects of As(Ⅴ)on Cd(Ⅱ)adsorption

Journal of Environmental Sciences 2024年第5期139卷 267-280页

作者： Wenjun Zeng Yang Lu Jingyan Zhou Jie Zhang Yuanxiao Duan Changxun Dong Wencheng Wu College of Sciences Nanjing Agricultural UniversityNanjing 210095China South China Institute of Environmental Sciences Ministry of Ecology and EnvironmentGuangzhou 510655China Guangdong Engineering&Technology Research Center for System Control of Livestock and Poultry breeding Pollution Guangzhou 510655China

The coexistence of cadmium(Cd(Ⅱ))and arsenate(As(Ⅴ))pollution has long been an environmental problem.Biochar,a porous carbonaceous material with tunable functionality,has been used for the remediation of contaminated soils.However,it is still challenging for the dynamic quantification and mechanistic understanding of the simultaneous sequestration of multi-metals in biochar-engineered environment,especially in the presence of anions.In this study,ferrihydrite was coprecipitated with biochar to investigate how ferrihydritebiochar composite affects the fate of heavy metals,especially in the coexistence of Cd(Ⅱ)and As(Ⅴ).In the solution system containing both Cd(Ⅱ)and As(Ⅴ),the maximum adsorption capacities of ferrihydrite-biochar composite for Cd(Ⅱ)and As(Ⅴ)reached 82.03μmol/g and 531.53μmol/g,respectively,much higher than those of the pure biochar(26.90μmol/g for Cd(Ⅱ),and 40.24μmol/g for As(Ⅴ))and ferrihydrite(42.26μmol/g for Cd(Ⅱ),and 248.25μmol/g for As(Ⅴ)).Cd(Ⅱ)adsorption increased in the presence of As(Ⅴ),possibly due to the changes in composite surface charge in the presence of As(Ⅴ),and the increased dispersion of ferrihydrite by biochar.Further microscopic and mechanistic results showed that Cd(Ⅱ)complexed with both biochar and ferrihydrite,while As(Ⅴ)was mainly complexed by ferrihydrite in the Cd(Ⅱ)and As(Ⅴ)coexistence system.Ferrihydrite posed vital importance for the co-adsorption of Cd(Ⅱ)and As(Ⅴ).The different distribution patterns revealed by this study help to a deeper understanding of the behaviors of cations and anions in the natural environment.

关键词： Ferrihydrite Biochar Cadmium arsenate Simultaneous sequestration Binding mechanisms

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Insights into the conversion of dissolved organic phosphorus favors algal bloom, arsenate biotransformation and microcystins release of Microcystis aeruginosa

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Journal of Environmental Sciences 2023年第3期125卷 205-214页

作者： Xiaoyan Zhang Zhenhong Wang Zhuanxi Luo Yan Chen Xuguang Huang College of Chemistry Chemical Engineering and EnvironmentMinnan Normal UniversityKey Laboratory of Modern Separation and Analysis Science and TechnologyKey Laboratory of Pollution Monitoring and ControlZhangzhou 363000China College of Chemical Engineering Huaqiao UniversityXiamen 361021China

Little information is available on influences of the conversion of dissolved organic phosphorus(DOP) to inorganic phosphorus(IP) on algal growth and subsequent behaviors of arsenate(As(V)) in Microcystis aeruginosa(M. aeruginosa). In this study, the influences factors on the conversion of three typical DOP types including adenosine-5-triphosphate disodium salt(ATP), β-glycerophosphate sodium(βP) and D-glucose-6-phosphate disodium salt(GP)were investigated under different extracellular polymeric secretions(EPS) ratios from M.aeruginosa, and As(V) levels. Thus, algal growth, As(V) biotransformation and microcystins(MCs) release of M. aeruginosa were explored in the different converted DOP conditions compared with IP. Results showed that the three DOP to IP without EPS addition became in favor of algal growth during their conversion. Compared with IP, M. aeruginosa growth was thus facilitated in the three converted DOP conditions, subsequently resulting in potential algal bloom particularly at arsenic(As) contaminated water environment. Additionally, DOP after conversion could inhibit As accumulation in M. aeruginosa, thus intracellular As accumulation was lower in the converted DOP conditions than that in IP condition. As(V) biotransformation and MCs release in M. aeruginosa was impacted by different converted DOP with their different types. Specifically, DMA concentrations in media and As(III) ratios in algal cells were promoted in converted βP condition, indicating that the observed dissolved organic compositions from βP conversion could enhance As(V) reduction in M. aeruginosa and then accelerate DMA release. The obtained findings can provide better understanding of cyanobacteria blooms and As biotransformation in different DOP as the main phosphorus source.

关键词： Organic phosphorus arsenate Phosphate Methylation Extracellular polymeric secretions

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Synthesis of mesoporous Cu/Mg/Fe layered double hydroxide and its adsorption performance for arsenate in aqueous solutions

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Journal of Environmental Sciences 2013年第5期25卷 944-953页

作者： Yanwei Guo Zhiliang Zhu Yanling Qiu Jianfu Zhao State Key Laboratory of Pollution Control and Resource Reuse Tongji University Key Laboratory of Yangtze River Water Environment Ministry of EducationTongji University

The mesoporous Cu/Mg/Fe layered double hydroxide（Cu/Mg/Fe-LDH） with carbonate intercalation was synthesized and used for the removal of arsenate from aqueous solutions.The Cu/Mg/Fe-LDH was characterized by Fourier transform infrared spectrometry,X-ray diffraction crystallography,scanning electron microscopy,X-ray photoelectron spectroscopy and Brunauer-Emmett-Teller.Effects of various physico-chemical parameters such as pH,adsorbent dosage,contact time and initial arsenate concentration on the adsorption of arsenate onto Cu/Mg/Fe-LDH were investigated.Results showed that it was efficient for the removal of arsenate,and the removal efficiency of arsenate increased with the increment of the adsorbent dosage,while the arsenate adsorption capacity decreased with increase of initial pH from 3 to 11.The adsorption isotherms can be well described by the Langmuir model with R 2 〉 0.99.Its adsorption kinetics followed the pseudo second-order kinetic model.Coexisting ions such as HPO42-,CO32-,SO42and NO3could compete with arsenate for adsorption sites on the Cu/Mg/Fe-LDH.The adsorption of arsenate on the adsorbent can be mainly attributed to the ion exchange process.It was found that the synthesized Cu/Mg/Fe-LDH can reduce the arsenate concentration down to a final level of 〈 10 μg/L under the experimental conditions,and makes it a potential material for the decontamination of arsenate polluted water.

关键词： arsenate adsorption mesoporous layered double hydroxide anion exchange

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Nanoencapsulation of arsenate with nanoscale zero-valent iron(nZVI):A 3D perspective

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Science Bulletin 2018年第24期63卷 1641-1648页

作者： Airong Liu Wei Wang Jing Liu Rongbing Fu Wei-xian Zhang State Key Laboratory for Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongii UniversityShanghai 200092China School of Chemical Sdence and Engineering Tongji UniversztyShanghai 200092China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

The principal forces driving the efficient enrichment and encapsulation of arsenic(As) into nanoscale zero-valent iron(nZVI) are the disordered arrangement of the atoms and the gradient chemical potentials within the core-shell interface. The chemical compositions and the fine structure of nZVI are characterized with a combination of spherical aberration corrected scanning transmission electron microscopy(Cs-STEM), X-ray energy-dispersive spectroscopy(XEDS), electron energy loss spectroscopy(EELS), and high-resolution X-ray photoelectron spectroscopy(HR-XPS). Atomically resolved EELS at the oxygen K-edge unfolds that the Fe species in nZVI are well stratified from Fe(Ⅲ) oxides in the outermost periphery to a mixed Fe(Ⅲ)/Fe(Ⅱ) interlayer, then Fe(Ⅱ) oxide and the pure Fe(0) phase. Reactions between As(Ⅴ)and nZVI suggest that a well-structured local redox gradient exists within the shell layer, which serves as a thermodynamically favorable conduit for electron transfer from the iron core to the surface-bound As(Ⅴ). HR-XPS with ion sputtering shows that arsenic species shift from As(Ⅴ), As(Ⅲ)/As(Ⅴ) to As(Ⅴ)/As(Ⅲ)/As(0) from the iron oxide shell–water interface to the Fe(0) core. Results reinforce previous work on the efficacy of nZVI for removing and remediating arsenic while the analytical TEM methods are also applicable to the study of environmental interfaces and surface chemistry.

关键词： arsenate Nanoscale zero-valent iron Spherical aberration corrected scanning transmission electron microscopy X-ray energy-dispersive spectroscopy Electron energy-loss spectroscopy X-ray photoelectron spectroscopy

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Enhanced adsorption of arsenate by spinel zinc ferrite nano particles: Effect of zinc content and site occupation

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Journal of Environmental Sciences 2019年第5期31卷 248-255页

作者： Can Wu Yunyun Xu Si Xu Jingwei Tu Chen Tian Zhang Lin School of Environment and Energy The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters (Ministry of Education) South China University of Technology Guangdong Engineering and Technology Research Center for Environmental Nanomaterials South China University of Technology

In this work, zinc ferrite spinel with different zinc contents(ZnxFe_3-xO_4) was synthesized by a hydrothermal method and used for removing As(V) in aqueous solution. X-ray diffraction(XRD) results indicated that in the crystal structure of ZnxFe_3-xO_4, the zinc atoms tended to occupy the octahedral sites for x 0.6. The size of ZnxFe_3-xO_4 crystallites increased with the increasing zinc content. Batch adsorption experiments showed that the adsorption isotherms could be well described by the Langmuir model, while the adsorption kinetics followed the pseudo-second-order kinetic model. Zinc ferrite exhibited the highest adsorption capacity towards As(V) when x = 0.6. Study of the mechanism indicated that doping with zinc increased the number of surface hydroxyl groups on ferrite spinel, and thus enhanced the adsorption capacity when x = 0.6. This work revealed the effects of doping site and content of metal atoms on the adsorption ability of ferrite spinel towards As(V).

关键词： Zinc ferrite arsenate Adsorption Atom occupancy Hydroxyl groups

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Effects of pore size and dissolved organic matters on diffusion of arsenate in aqueous solution

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Journal of Environmental Sciences 2017年第2期29卷 190-196页

作者： Yulong Wang Shaofeng Wang Xin Wang Yongfeng Jia Key Laboratory of Pollution Ecology and Environmental Engineering Institute of Applied EcologyChinese Academy of SciencesShenyang 110016China University of Chinese Academy of Sciences Beijing 100049China

Presented here is the influence of membrane pore size and dissolved organic matters on the diffusion coefficient（D） of aqueous arsenate, investigated by the diffusion cell method for the first time. The p H-dependent diffusion coefficient of arsenate was determined and compared with values from previous studies; the coefficient was found to decrease with increasing p H, showing the validity of our novel diffusion cell method. The D value increased dramatically as a function of membrane pore size at small pore sizes, and then increased slowly at pore sizes larger than 2.0 μm. Using the Exp Assoc model, the maximum D value was determined to be 11.2565 × 10^-6cm^2/sec. The presence of dissolved organic matters led to a dramatic increase of the D of arsenate, which could be attributed to electrostatic effects and ionic effects of salts. These results improve the understanding of the diffusion behavior of arsenate, especially the important role of various environmental parameters in the study and prediction of the migration of arsenate in aquatic water systems.

关键词： arsenate Diffusion Pore p H Dissolved organic matters Migration

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Characterization of arsenate transformation and identification of arsenate reductase in a green alga Chlamydomonas reinhardtii

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Journal of Environmental Sciences 2011年第7期23卷 1186-1193页

作者： Xixiang Yin Lihong Wang Guilan Duan Guoxin Sun Key Laboratory of Urban Environment and Health Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China State Key Laboratory of Urban and Regional Ecology Research Center for Eco-environmental Sciences Chinese Academy of Sciences Beijing 100085 China Shandong Analysis and Test Center Shandong Academy of Sciences Shandong 250014 China

Arsenic （As） is a pervasive and ubiquitous environmental toxin that has created catastrophic human health problems world-wide. Chlamydomonas reinhardtii is a unicellular green alga, which exists ubiquitously in freshwater aquatic systems. Arsenic metabolism processes of this alga through arsenate reduction and sequent store and efflux were investigated. When supplied with 10 μmol/L arsenate, arsenic speciation analysis showed that arsenite concentration increased from 5.7 to 15.7 mg/kg dry weight during a 7-day period, accounting for 18%–24% of the total As in alga. When treated with different levels of arsenate （10, 20, 30, 40, 50 μmol/L） for 7 days, the arsenite concentration increased with increasing external arsenate concentrations, the proportion of arsenite was up to 23%–28% of the total As in alga. In efflux experiments, both arsenate and arsenite could be found in the efflux solutions. Additionally, the efflux of arsenate was more than that of arsenite. Furthermore, two arsenate reductase genes of C. reinhardtii （CrACR2s） were cloned and expressed in Escherichia coli strain WC3110 （？arsC） for the first time. The abilities of both CrACR2s genes to complement the arsenate- sensitive strain were examined. CrACR2.1 restored arsenate resistance at 0.8 mmol/L. However, CrACR2.2 showed much less ability to complement. The gene products were demonstrated to reduce arsenate to arsenite in vivo. In agreement with the complementation results, CrACR2.1 showed higher reduction ability than CrACR2.2, when treated with 0.4 mmol/L arsenate for 16 hr incubation.

关键词： arsenate accumulation reduction efflux arsenate reductase Chlamydomonas reinhardtii

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Competitive and cooperative adsorption of arsenate and citrate on goethite

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Journal of Environmental Sciences 2009年第1期21卷 106-112页

作者： SHI Rong,JIA Yongfeng,WANG Chengzhi Institute of Applied Ecology,Chinese Academy of Sciences,Shenyang 110016,China Institute of Applied Ecology Chinese Academy of Sciences Shenyang 110016 China

The fate of arsenic in natural environments is influenced by adsorption onto metal （hydr）oxides. The extent of arsenic adsorption is strongly affected by coexisting dissolved natural organic acids. Recently, some studies reported that there existed competitive adsorption between arsenate and citrate on goethite. Humic acid is known to interact strongly with arsenate by forming complexes in aqueous solution, hence it is necessary to undertake a comprehensive study of the adsorption of arsenate/citrate onto goethite in the presence of one another. The results showed that at the arsenate concentrations used in this study （0.006-0.27 mmol/L）, citrate decreased arsenate adsorption at acidic pH but no effect was observed at alkaline pH. In comparison, citrate adsorption was inhibited at acidic pH, but enhanced at alkaline pH by arsenate. This was probably due to the formation of complex between arsenate and citrate like the case of arsenate with humic acid. These results implied that the mechanism of the adsorption of arsenate and citrate onto goethite in the presence of one another involved not only competition for binding sites, but the cooperation between the two species at the watergoethite interface as well.

关键词： adsorption arsenate citrate goethite

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Comparative Proteomic Analysis of Rice Shoots Exposed to High arsenate

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Journal of Integrative Plant Biology 2013年第10期55卷 965-978页

作者： Yanli Liu Ming Li Chao Han Fengxia Wu Bingkun Tu Pingfang Yang College of Horticulture and Forestry Sciences Huazhong Agricultural University Key Laboratory of Plant Germplasm Enhancement and Specialty Agriculture Wuhan Botanical Garden the Chinese Academy of Sciences

Consumption of arsenic contaminated water and cereals is a serious threat to humans all over the world. Rice （Oryza sativa ＂Nipponbare＂）, as a main cereal crop, can accumulate arsenic more than 10-fold that of in other cereals. To gain a comprehensive understanding of the response of rice subjected to 100 μM arsenate stress, a comparative proteomic analysis of rice shoots in combination with morphological and biochemical investigations have been performed in this study. The results demonstrated that arsenate suppressed the growth of rice seedlings, destroyed the cellular ultra-structure and changed the homeostasis of reactive oxygen species. Moreover, a total of 38 differentially displayed proteins, which were mainly involved in metabolism, redox and protein-metabolism, were identified. The data suggest the arsenic can inhibit rice growth through negatively affecting chloroplast structure and photosynthesis. In addition, upregulation of the proteins involved in redox and protein metabolism might help the rice to be resistant or tolerant to arsenic toxicity. In general, this study improves our understanding about the rice arsenic responsive mechanism.

关键词： arsenate metabolism proteomics rice ultra-structure.

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Combined Effect of Fluoride and arsenate on Gene Expression of Osteoclast Differentiation Factor and Osteoprotegerin

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Biomedical and Environmental Sciences 2006年第5期19卷 375-379页

作者： LIN JIA TAI-YIJIN Department of Toxicology School of Public Health Fudan University Shanghai 200032 China

Objective To study the combined effect of fluoride and arsenate on the expression of SD rat osteoblastic osteoclast differentiation factor （ODF） mRNA and osteoprotegerin （OPG） mRNA. Methods Osteoblasts were obtained by enzymatic isolation from newborn SD rats. A factorial experiment was performed. Osteoblasts were exposed to NaF （0.5 mmolF/L, 4 molF/L） and Na3AsH2 （12.5 μmolAs/L and 200 μmolAs/L） separately or F plus As and cultured for 48 h. The gene expression of osteoblastic ODF and OPG was observed by RT-PCR. Results The expression ofODF mRNA increased in F0.5, F4 groups compared with control group and two groups of F0.As200, F,As200 compared with As200 group, and decreased significantly in groups of F4As12.5, F0.5As200, and F4As200. The expression of OPG rnRNA decreased in groups of F4, As200, F4As12.5, F0.5As200, and F4As200. Conclusion The joint effect of fluoride and arsenate on the gene expression of ODF is antagonistic, while the combined effect on the gene expression of OPG is synergistic. F4, F4As12.5, and F0.5As200 promote bone resorption of rat osteoclasts, whereas F0.5As12.5 inhibits osteolytic effect of rat osteoclasts.

关键词： Fluoride arsenate ODF OPG Combined effect

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