JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Xiaofeng Yi,Shenhua Huang,Lu Chang,Zhaoshou Wang,Yuanpeng Wang
The redistribution process of arsenate (As(V)) and the variation in As(V) content in different locations must be clarified to ensure low mobility of As(V) during microbial ferrihydrite reduction. In this study, we investigated As(V) immobilization and redistribution processes when ferrihydrite was incubated with Geobacter sulfurreducens in the presence of titanium dioxide (TiO 2 ) nanoparticles . Our study results showed that, As(V) in the aqueous phase and ferrihydrite were redistributed on light minerals (goethite), heavy minerals (ferrihydrite and magnetite), and extracellular polymeric substances (EPS) induced by G. sulfurreducens during ferrihydrite reduction. Interestingly, we found that As(V) in the form of arsenate ion (AsO 4 3- ) was adsorbed by the functional groups of the EPS, while the formed Fe II 3 (As V O 4 ) 2 was wrapped in the network structure of EPS. Moreover, the addition of TiO 2 nanoparticles did not promote but delayed the entire ferrihydrite reduction, As(V) immobilization and redistribution processes. Furthermore, changes in the aqueous arsenic and iron concentrations are closely related to the formation time of secondary minerals. Our study findings provide new insights into the As(V) immobilization process mediated by G. sulfurreducens under anaerobic conditions .
研究领域:
环境科学
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微生物学
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DOI
PubMed
高影响因子
Journal of Geophysical Research-Biogeosciences
·
2025
·Vol. 130
·期 3
·e2024JG008675
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IF 3.5
Zhengqi Su,Huaming Guo,Zhipeng Gao,Tiantian Ke,Xiaojun Feng,Lingzhi Zhang
Although the reduction of pentavalent arsenic (As(V)) bound to Fe(III) (hydr)oxides (As(V)-containing FeOOH) coupled with organic matter (OM) degradation has received extensive attention, little is known about in situ reduction of FeOOH mineral-bound As(V) (As(V) (s) ) via electron shuttling in the presence of As(V)-reducing bacteria (AsRB). Here, anthraquinone-2,6-disulfonate (AQDS), Suwannee River humic acid (SRHA), and fulvic acid (SRFA) were used to establish an agar electron shuttle system with ferrihydrite-As(V)/goethite-As(V) and AsRB, which was isolated from high-As groundwater as the candidate strain (RA-1). We found that AQDS was more efficient in shuttling electrons to reduce As(V) (s) and Fe(III) than SRHA and SRFA. High contents of quinone moieties in AQDS indicated that quinone moieties were conducive to As(V) (s) and Fe(III) reduction. The reduction kinetic rates ( K red ) of As(V) (s) were higher than those of Fe(III), indicating the occurrence of in situ As(V) (s) reduction via electron shuttling. Furthermore, K red of As(V) (s) for ferrihydrite-As(V) systems was greater than that of goethite-As(V) systems, demonstrating that As(V) bound to ferrihydrite via monodentate was more easily reduced than that bound to goethite via bidentate. The relative expression levels of As metabolic genes ( ars C, arr A, and ars B) initially increased and then decreased in the late stage of experiments. High As concentrations in suspension inhibited the transcriptional activity of As metabolic genes in the late stage, reducing the electron production efficiency of RA-1 and subsequently slowing in situ reduction of As(V) (s) . This study highlights the importance of OM electron shuttling in the reduction of As(V) (s) , offering new perspectives in As enrichment in groundwater. Plain Language Summary OM can promote microbial As(V) reduction in high As groundwater systems. As a result, we explored how FeOOH mineral-bound As(V) could be in situ reduced via electron shuttling between AsRB and different OM. Our findings showed that AQDS was more effective than other two natural organic matter (NOM, i.e., SRHA and SRFA) in reducing both As(V) (s) and Fe(III), due to its high content of quinone moieties. The results of kinetic analysis demonstrated in situ reduction of As(V) (s) , and As(V) bound to ferrihydrite was more readily reduced than As(V) bound to goethite. In addition, the transcriptional activities of three As metabolic genes initially increased but later declined due to high As concentrations, which further slowed the As(V) (s) reduction process. Overall, these findings provide new insights into organic-mediated As cycling in contaminated groundwater. Key Points High quinone contents in AQDS led to a higher reduction extent of As(V) (s) than in SRHA and SRFA The values of K red, As were greater than those of K red, Fe , demonstrating in situ reduction of As(V) (s) Changes in As metabolic genes affected the electron production efficiency of RA-1 and As(V) (s) reduction
研究领域:
环境科学
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微生物学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Weiwei Li,Wenlan Ji,Murat Yılmaz,Tian C. Zhang,Shaojun Yuan
Arsenic is a toxic carcinogen, and arsenic pollution in groundwater is one of the most serious environmental problems in the world. Thus, it is an urgent problem to efficient removal of arsenic from groundwater. In this work, a novel MWCNTs/MIL-53(Fe) nanocomposite was successfully synthesized to improve the water stability of MIL-53(Fe) by incorporation of carboxylated multi-walled carbon nanotubes (MWCNTs) using a one-pot hydrothermal method, and was then used to efficiently adsorb As(V) ions from groundwater. Adsorption experimental results demonstrated an ultrafast adsorption rate of As(V) on the MWCNTs/MIL-53(Fe) nanocomposites in solution pH values of 3 to 10, and the adsorption equilibrium could be reached in circa 20 min with an adsorption capacity of 27.24 mg·g −1 in a low As(V) concentration of 10 mg·L −1 . The adsorption kinetics of As(V) on the MWCNTs/MIL-53(Fe) was found in line with the pseudo-second-order (PSO) kinetic model, and was simultaneously controlled by both internal diffusion and liquid film diffusion. The adsorption isotherm data conformed to the Redlich-Peterson isotherm model, indicating both physical and chemical adsorption occurred at heterogeneous interfaces. Moreover, the postulated adsorption mechanism of As(V) on MWCNTs/MIL-53(Fe) nanocomposites was ascribed to hydrogen-bond interaction, electrostatic attraction and chemical complexation. Therefore, the as-prepared MWCNTs/MIL-53(Fe) nanocomposites not only exhibit superior water stability and outstanding adsorption performance in removing arsenic-contaminated groundwater, but also offer a novel insight for rational preparation of water-stable MOF-based composites.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chen Wang,Zewei Hu,Wei Lou,Mingjie Huang,Wei Xiang,Tao Zhou,Juan Mao,Xiaohui Wu
This study has demonstrated that the Fenton fluidized bed (FFB) technology could successfully immobilize As ions on the iron-crystallized (IC) carriers, with simultaneous crystallization of ferric and mineralization of organic pollutants. It was found that rapid fluidized immobilization of aqueous As(V) on the IC carriers was through surface favorable bidentate complexion, while the adsorptive removal of As(III) was rather slow. Adding Fe 3+ caused competitive complexion and inhibited the As(V) immobilization. However, effective oxidative crystallization of Fe(II) and As(III) in FFB would take place. With the simultaneous generation of As(V) and Fe(III) by rapid •OH oxidation, two different crystalline precursors would be formed on the IC carriers, leading to efficient co-crystallization of As(V)/Fe(III). Recursive Fe(III) crystallization in the FFB continuously provided essential surface hydroxyl groups for capturing As(V), inducing layer-by-layer co-crystallized immobilization As(V)/Fe(III). The long-term continuous-flow treatment of a practical As(III)-containing industrial organic wastewater exhibited effective/stable co-crystallizations of As(V)/Fe(III), as well as COD removal. The FFB technology is expected to be a good option in treating complex industrial wastewater containing heavy metal and recalcitrant organic pollutants.
研究领域:
环境科学
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化学工程
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废水处理
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DOI
高影响因子
EUROPEAN POLYMER JOURNAL
·
2021
·
IF 4.598
Zhanfeng He,Qiang Chen,Yuanyuan Luo,Yuan He,Yinshan Zhang,Tong Liu,Wenyuan Xu,Jiali Zhang,Yongxin Liu,Leyan Xiong,Shaohui Wang,Zanru Guo
Adsorbent with high and recyclable adsorption for pollutants without secondary pollution is one of great potential in water treatment. Here, degradable CO 2 -responsive microgels with big size and wrinkled porous structure were prepared. The microgels underwent reversible volume phase changes upon alternative stimulus of CO 2 and N 2 , and thereby exhibited a switchable, selective, and recyclable adsorption for anionic dyes and metalloids (Cr(VI) and As(V)). The adsorption performance was improved due to the wrinkled porous structure, and the maximum adsorption capacity was up to 1537 mg g −1 for metanil yellow (MY). The competitive adsorption in binary and ternary system revealed that the affinity was in the order of MY > ponceau S (PS) > Cr(VI). Besides, the adsorbates could be desorbed by heating or treating with solution of pH 12. Microgels regenerated with CO 2 trigger exhibited high adsorption ability after ten consecutive recycling trials, and could be applied to fixed-bed adsorption/desorption system. Moreover, microgels could be degraded. Thus, this kind of degradable microgels have potential applications in the treatment of complex industrial wastewaters and avoid the additional pollution caused by the accumulation of waste adsorbents.
研究领域:
环境科学
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材料科学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Li Liu,Qianqian Wei,Yeqing Lan,Cheng Chen
Efficient purification of the wastewater containing organoarsenic by activated peroxymonosulfate (PMS) usually faces with a great challenge because the degradation of organoarsenic is coupled with the release of its byproduct As(V). Heterogeneous catalysts with catalytic and adsorption functions show great potential in activating PMS for the degradation of organoarsenic and the removal of secondary inorganic arsenic. In this study, Co-CeMnO was designed and fabricated to realize simultaneous elimination of p -arsanilic ( p -ASA) and As(V) in Co-CeMnO (0.2 g/L)/PMS (0.25 mM) system, in which 50 µM p -ASA was almost completely degraded within 5 min and approximately 100% of the produced As(V) was removed within 30 min. The rate constant of the pseudo-first-order kinetics for the p -ASA degradation by PMS mediated with Co-CeMnO was high up to 0.65 min −1 , approximately 6.5 times higher than that in the system of CeMnO/PMS. It was revealed that SO 4 •− , • OH and 1 O 2 acted as the main oxidant species responsible for the oxidation of organics and As(III), and the surface −OH of Co-CeMnO led to the adsorption of As(V) via ion exchange. The excellent reusability and stability of Co-CeMnO was verified by five cycles with high removal efficiencies of p -ASA (>92% within 10 min) and arsenic (>98% within 90 min) and low leached metal ion concentrations (Co ions < 0.27 mg/L; Mn ions < 0.15 mg/L; Ce ions ≈ 0). Under the condition of initial pH 5, p -ASA was degraded completely and over 98% of total arsenic was adsorbed in different water matrices, indicating the practical application potential of Co-CeMnO/PMS system. Thus, the present study provided a reliable PMS activation strategy by constructing bifunctional catalysts to achieve satisfactory treatment of the wastewater containing p -ASA.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
GREEN CHEMISTRY
·
2019
·Vol. 21
·期 9
·2286-2294
·
IF 9.405
Yuqing Qin,Fei Peng,Yonggang Hu
The oxidation of As(III) to As(V) is a critical process in the treatment of contaminated water. We found that 95% As(III) (10 mg L−1) could be rapidly oxidized to As(V) by a laccase–2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) system in 1 h. Based on this finding, we used Bacillus subtilis spores instead of laccase for As(III) oxidation with the same effect because the former had plenty of CotA–laccase on their surface. The catalytic ability of CotA protein and spores was confirmed by expressing the CotA protein and knocking out the cotA gene from wild-type spores. Both laccase– and spore–TEMPO systems displayed similar oxidation rate constants, Michaelis–Menten constants, and maximal velocities owing to the formation of the oxoammonium cation of TEMPO in the presence of dissolved oxygen. Several other laccase mediators such as 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic-acid) (ABTS), acetosyringone (AS), 1-hydroxybenzotriazole (HBT), 2-hydroxybutyl acrylate (HBA), violuric acid (VLA), 4-oxo-TEMPO, 4-amino-TEMPO, 4-methoxy-TEMPO, 4-hydroxy-TEMPO benzoate, and 4-hydroxy-TEMPO coupled with spores for As(III) oxidation were also investigated in detail. The spore–TEMPO system exhibited the highest oxidation efficiency and tolerated the addition of 10 mg L−1 Al3+, Ti4+, Cu2+, K+, Fe3+, Zn2+, Ni2+, Mg2+, Co2+, and Mn2+. Both laccase and spores recovered via ultrafiltration and centrifugation, respectively, could be reused for at least five cycles. The developed spore-based system has several advantages including eco-friendliness, ease of operation and storage, low cost, recyclability, sustainability, and without the need for enzyme purification. These findings may have promising implications for developing a new eco-friendly and cost-effective technology for the treatment of arsenic-containing water.
研究领域:
环境科学
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生物技术
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水处理
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微生物学
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DOI
高影响因子
LANGMUIR
·
2025
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IF 3.9
Qintao Yang,Zechao Zheng,Chenhua Shu,Qinglin Xie,Xiangpeng Gao
In this study, a novel As(V) ion-imprinted and 4-picolinic acid (4-PA)-grafted porous diatomite (DE)-based adsorbent (As(V)-IID) was prepared by using the surface ion imprinting technique. The results of the selective adsorption experiment show that the adsorption capacity of As(V) on As(V)-IID reaches 62.78 mg/g in a solution with an initial As(V) concentration of 25 mg/L and a pH value that is near pH 4.0 of the imprinting. The selectivity coefficients (K) of As(V) with respect to Cr(VI) and Mo(VI) were up to 12.14 and 27.79, respectively. The binding process was described well by the pseudo-second-order kinetics and Weber–Morris and Langmuir models. Fourier transform infrared spectra (FTIR), scanning electron microscopy energy dispersive X-ray spectroscopy (SEM-EDS), and X-ray photoelectron spectroscopy (XPS) analyses suggested that the nitrogen of secondary amide and pyridine was the main imprinting site and played a crucial role in the selectivity of binding of As(V) to As(V)-IID. To further validate the sorption mechanisms, density functional theory (DFT) was employed to study the properties of binding of As(V), Cr(VI), and Mo(VI) with As(V)-IID. The computational results showed that the As(V) was selectively recognized by complexing with N-containing functional groups of the As(V)-IID surface into a tridentate mononuclear configuration with a minimal binding energy (Eb) of −18.16 eV, which was completely consistent with characterization analyses. This work revealed the selective adsorption mechanisms of As(V)-IID for As(V) and provided new insight into the selective recognition of oxyanions from water by ion-imprinted adsorbents.
研究领域:
环境科学
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材料科学
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化学工程
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分析化学
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物理化学
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DOI
PubMed
高影响因子
Environmental Science-Nano
·
2019
·Vol. 6
·期 5
·1406-1417
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IF 7.704
Yili Xie,Chen Tian,Weiyi Chen,Can Wu,Zhangbin Liu,Ping Ning,Hong Deng,Zhang Lin
Manganese ferrite (MnxFe3−xO4) microspheres with a spinel structure are very effective adsorbents for arsenic (As) removal. In this study, highly ordered mesoporous MnxFe3−xO4 has been synthesized by a facile and convenient solvothermal method. By comparing the different doping amounts of manganese (Mn), the results show that Mn1.8Fe1.2O4 has a relatively higher efficiency for arsenate (As(V)) removal due to the modified surface complexes caused by the optimum Mn substitution. Rietveld XRD refinement reveals that Mn1.8Fe1.2O4 microspheres possess the highest distribution ratio of Mn/Fe situated between the octahedral (Oh) and the tetrahedral (Td) sites of the unit cell. The as-prepared Mn1.8Fe1.2O4 microspheres with MnO6Oh sites in Fdm symmetry exhibit a promising ability for toxic As(V) adsorption, which is mainly attributed to the increase of coordinated complexes. Extended X-ray absorption fine structure (EXAFS) analysis indicates that the coordination structures of As(V) on Mn1.8Fe1.2O4 are present as bidentate binuclear complexes with a regular distance of As–Fe = 3.41 Å. Apart from this, As(V) can also bind with Mn-doped sites through the monodentate coordination mode at a distance of As–Mn = 3.51 Å with a preferred coordination number (CN) of 4.4. This work discloses the correlation between the superior As(V) adsorption ability and MnO6Oh sites in Mn1.8Fe1.2O4 and provides an emerging and promising method to enhance the adsorption capacity of As via modifying Mn doping sites based on the pollutant structure to achieve synergistic adsorption effects.
研究领域:
环境科学
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材料科学
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化学
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DOI
高影响因子
Biochar
·
2024
·Vol. 6
·期 1
·1-14
·
IF 13.1
Wang Shengsen,Li Wenjing,Ding Chengyu,Zhang Jian,Zhang Ni,Li Yuncong C.,Gao Bin,Wang Bing,Wang Xiaozhi
Arsenic (As) detoxification in polluted soils by iron-based materials can be mediated by the endogenous soil organic matter (SOM), nevertheless the mechanisms remain unclear. Herein, endogenous SOM in a paddy soil was substantially removed to understand its roles on As immobilization by biochar-supported zero-valent iron (ZVI/BC). The results demonstrated that ZVI/BC application significantly decreased As bioavailability by 64.2% compared with the control soil under the anaerobic condition. XPS and HR-TEM suggested As immobilization by ZVI/BC mainly invoked the formation of ternary complexes (i.e., As-Fe-SOM). However, SOM depletion compromised the efficacy of ZVI/BC for As immobilization by 289.8%. This is likely because SOM depletion increased the fulvic acid and OH − contents in soils. Besides, ZVI/BC increased the proportion of As(III) in available As fraction, but SOM depletion altered the mechanisms associated with As(V) reduction. That is, As(V) reduction resulted from the reductive capacity of ZVI in the pristine soil, but the As(V)-reducing bacteria contributed greater to As(V) reduction in the SOM-depleted soil. Additionally, SOM depletion boosted the abundances of Fe(III)- and As(V)-reducing bacteria such as Bacillus and Ammoniphilus in soils, which enhanced the dissimilatory arsenate reduction. Thus, this work highlighted the importance of SOM in the remediation of As-contaminated soils by ZVI/BC. Graphical Abstract
研究领域:
环境科学
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土壤化学
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微生物学
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高影响因子
RSC Advances
·
2015
·Vol. 5
·期 83
·67951-67961
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IF 3.84
Jin Zhu,Zimo Lou,Yu Liu,Ruiqi Fu,Shams Ali Baig,Xinhua Xu
Iron–manganese binary oxide (FeMnOx) is considered highly effective for arsenic adsorption, however, the agglomeration effect hindered its practical application. In this study, graphene has been used as a supporting matrix to disperse FeMnOx due to its huge specific surface area, and the synthesized novel composite adsorbent (FeMnOx/RGO) was employed for arsenic removal. Results demonstrated that FeMnOx/RGO (mass ratio of FeMnOx to FeMnOx/RGO nanocomposites is 45%) has larger specific surface area (411 m2 g−1) in comparison with bare FeMnOx, and showed 10.16 mg As g−1 FeMnOx and 11.49 mg As g−1 FeMnOx adsorption capacities for As(III) and As(V), respectively, with 1 mg L−1 initial concentration. Increased in the initial concentration to 7 mg L−1, the adsorption capacities of As(III) and As(V) reached to 47.05 mg As g−1 FeMnOx and 49.01 mg As g−1 FeMnOx, respectively. The removal process perfectly obeys pseudo second-order kinetic model for both As(III) and As(V). And PO43− was found to strongly inhibit arsenic adsorption. Furthermore, adsorption tests and characterization analyses confirmed that MnO2 played a key role on the oxidation of As(III), while iron(III) oxide was found crucial to As(V) removal. Electrostatic interaction and surface complexation mechanisms involved in the adsorption. These findings suggested that the adsorbent could be used in real arsenic-contaminated water treatment.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Varney Edwin Johnson,Qi Liao,Bob Wisdom Jallawide,Richmond Anaman,Charles Amanze,Peicheng Huang,Wei Cao,Chunlian Ding,Yan Shi
Efficient removal of arsenic (As) and lead (Pb) from industrial wastewater has long been a critical environmental issue due to their serious risk to human health. Therefore, in this work, a modified banana peel biochar (MBPB) was prepared by mixing calcium nitrate , diammonium hydrogen phosphate , sulfuric acid, ferric nitrate with dehydrated banana peel biochar as adsorbent for As(V) and Pb(II) removal in wastewater, and their absorption mechanism was investigated. SEM-EDS, TEM, FTIR , XRD , XPS , BET, kinetic, and isothermal characteristics of MBPB and pristine banana peel biochar (PBPB) were conducted. The behavior of both metal ions on MBPB and PBPB was well explained by the pseudo-second-order kinetic with Langmuir and Freundlich models. We found that the two biochar’s behaviors were mixture processes of monolayer and multilayer adsorption , achieving maximum capacities as determined by the Langmuir model of 39.5 mg g −1 (MBPB-As), 33.2 mg g −1 (MBPB-Pb), 30.8 mg g −1 (PBPB-Pb), and 23.5 mg g −1 (PBPB-As), with maximum efficiencies of 98.7% (MBPB-As) and 90.3% (MBPB-Pb) under optimum conditions. Thermodynamic tests showed that As(V) and Pb(II) removal on MBPB was a spontaneous and endothermic physisorption process. MBPB showed great reusability in As(V) and Pb(II) removal, with removal rates as high as 71.4% and 66.5% after five cycles, respectively. Selective adsorption of As(V) and Pb(II) was also investigated on MBPB, and the removal rate was still high in the mixture of heavy metals. These findings provide a feasible method for the environmental-benign utilization of banana peel as a low-priced adsorbent in wastewater treatment .
研究领域:
环境科学
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废物管理
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材料科学
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化学工程
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DOI
高影响因子
危险品化学品经营许可证（带存储）