PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2020
·Vol. 22
·期 22
·12456-12464
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IF 3.43
Xiang-Ming Wang,Song-Hai Wu,Hai-Tao Ren,Peng-Yue Zhu,Cong Wang,Yong Liu,Shi-Wei Sun,Xiao-Cong Zhang,Yi-Ying Lin,Zi-He Meng,Shao-Yi Jia,Xu Han
Bi2+xWO6 is a cost-effective and environmentally friendly photocatalyst that shows high reactivity in the oxidation of various contaminants under visible light. However, under alkaline conditions, the reactive oxidative species in the Bi2+xWO6 system are still not clear yet. In this study, it is observed that the oxidation rates of As(III) increase with increasing pH values in the Bi2.15WO6 system. Photoluminescence and the Mott–Schottky analyses confirm that OH− promotes the separation and transfer of photogenerated electron–hole pairs over Bi2.15WO6, thus facilitating the oxidation of As(III). Electron spin resonance spectra analysis and quenching experiments rule out contributions of •OH, O2˙−, 1O2 and superoxo species to As(III) oxidation and indicate that surface –OOH and/or H2O2 are indeed the predominant species under alkaline conditions. The improved production of H2O2 by H-donors such as glucose and phenol, as well as the UV-vis diffuse reflectance and Raman analyses, further confirms the formation of surface –OOH on Bi2.15WO6 under alkaline conditions. In the dark, the significant higher oxidation rate of As(III) by H2O2–Bi2.15WO6 than that by H2O2 alone reveals that surface −OOH, instead of H2O2, plays an important role in As(III) oxidation. This study enriches our understanding of the diversity of reactive oxygen species (ROS) in the Bi2.15WO6 system and gives new insight into the mechanism involved in the oxidation of As(III) under alkaline conditions.
研究领域:
环境科学
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光催化
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材料科学
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PubMed
高影响因子
TALANTA
·
2026
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IF 6.7
Du Yuan,Linhua Jiang,Yong Liu,Hongfei Liu,Xiangmin Huang,Zongqing He,Haodian Peng,Shaoshuai Sheng,Song Ma,Ning Duan
Effective arsenic pollution control necessitates real-time arsenic compositional monitoring, a demand that conventional analytical techniques struggle to meet due to limitations in timeliness and economy. Herein, an innovative deep ultraviolet (DUV) spectroscopy method is proposed, enabling the direct speciation and quantification of high concentration arsenic in copper smelting wastewater. High fidelity DUV spectra were acquired via a specialized measurement system that eliminated oxygen and stray light interferences, wherein the specific arsenic-related features revealed the capability for inorganic As(III)/As(V) quantification. TD-DFT simulations elucidated the differentiated spectral signatures of As species via distinct electronic transition mechanisms. In addition, matrix interference mechanisms on arsenic quantification were studied, with sulfuric acid modulating arsenic protonation states, and Fe(III) alongside Cu(II) inducing linear DUV spectral superposition. Incorporating these mechanistic insights, an optimized partial least squares (PLS) model was developed for the proposed analytical method, ensuring effective quantitative analysis of the arsenic species. Compared with conventional analytical techniques, the developed method achieved competitive accuracy across simulated and authentic wastewater samples with arsenic concentrations exceeding 0.1 M, while demonstrating significantly better green analytical chemistry scores. This approach realizes direct arsenic speciation and quantification without complex pretreatments, providing a rapid, economical, and sustainable analytical tool for arsenic pollution control. Furthermore, it offers a novel DUV analytical paradigm for monitoring highly concentrated and complex aqueous solutions across a broad range of process industries.
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高影响因子
GEOCHIMICA ET COSMOCHIMICA ACTA
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2012
·
IF 4.259
Hui Yin,Wenfeng Tan,Lirong Zheng,Haojie Cui,Guohong Qiu,Fan Liu,Xionghan Feng
Hexagonal birnessite is the most ubiquitous manganese oxide in geological environments. It is often highly enriched in trace metal ions such as Ni and plays an important role in metal(loids) geochemistry . Nanostructured birnessites containing different amounts of Ni were synthesized by addition of Ni 2+ to initial reactants. Powder X-ray diffraction (XRD), element analysis, field emission scanning electron microscopy (FE-SEM), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), X-ray absorption spectroscopy (XAS) and isothermal adsorption and oxidation of metal(loids) were carried out to investigate the effects of Ni doping on the substructure and physicochemical properties of birnessite, and Ni crystal chemistry in birnessite. These Ni-rich birnessites have Ni contents as high as 2.99% (Ni5) and 6.08% (Ni10) in weight. EXAFS results show that Ni5 has 23.7% of the total Ni (0.71 wt.%) and Ni10 has 34.5% of the total Ni (2.10 wt.%) in Mn octahedral layer with the remaining Ni located at vacancies and edge sites. The Ni-rich birnessites have weaker crystallinity and thermal stability, fewer layers stacked along the c axis, ∼1.5–2.7 times larger surfaces areas, and a higher Mn average oxidation numbers (AONs) compared to the birnessite without Ni. Additionally, the doping of Ni during birnessite crystallization enhances the formation of vacancies in the layer; however, adsorption capacities for Pb 2+ and Zn 2+ by these Ni-rich birnessites are reduced, mainly because of vacancies and edge sites occupation by a large amount of Ni. The Ni-rich birnessites exhibit much higher oxidation capability and can completely oxidize As(III) in solution at rapid initial reaction rates under the experimental condition. The results indicate that incorporation of Ni into the natural birnessite in ferromanganese nodules may be achieved both by direct coprecipitation with Mn to build the layers and migration over time from adsorbed Ni on the surface into the layer structure. It is also implied that Ni doping in birnessite has great impact on the geochemical behaviors of heavy metals, either in adsorption or oxidation reactions.
研究领域:
地球化学
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环境科学
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高影响因子
Environmental Science-Nano
·
2018
·Vol. 5
·期 12
·2978-2992
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IF 6.087
Dongfang Wang,Zhangyu Dai,Xian Shu,Po Bian,Lifang Wu,Dongqing Cai,Zhengyan Wu
In this work, amido-functionalized Fe3O4 microspheres (AFFMs) were loaded in network-structured MnO2 to form a nanocomposite named as OAM. OAM could remove chlortetracycline hydrochloride (CTC) and trivalent arsenic (As(III)) simultaneously from swine urine aqueous solution and soil. Therein, OAM has a high adsorption capability for CTC through hydrogen bonds. Additionally, OAM could effectively adsorb As(III) through electrostatic attraction and then oxidize it to pentavalent arsenic (As(V)). Afterward, the resulting OAM/CTC/As could be conveniently removed with a magnet. When OAM was deposited on the surface of a piece of cotton fabric (CF), the obtained OAM/CF could efficiently control the migration of CTC and As(III) in a sand–soil mixture. Importantly, OAM could effectively reduce the uptake of CTC and As by zebrafish, water spinach, and pakchoi, and promote the growth of water spinach. Finally, OAM possessed good biosafety for embryos of Caenorhabditis elegans. Thus, this work provides a new method to remove CTC and As(III) simultaneously in swine urine aqueous solution and soil, which may have a high application value.
研究领域:
环境科学
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材料科学
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生物医学
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
·
IF 12.2
Shun Qiu,Zhanxun Chen,Ling Yu,Chuying Liu,Chenghan Ji,Pengfei Shen,Sikai Cheng,Hui Qiu,Zhuoyao Fang,Xiaolin Zhang
Herein, a highly efficient As(III) purifier Ce-Mn@N201 with excellent reusability was developed by stepwise precipitating hydrated cerium(IV) oxides (HCO) and hydrated manganese(IV) oxides (HMO) inside N201, a widely-used gel-type anion exchange resin . Owing to confinement of unique nanopores in N201, the in-situ generated nanoparticles (NPs) inside Ce-Mn@N201 were highly dispersed with ultra-small sizes of around 2.6 nm. Results demonstrated that HMO NPs effectively oxidized As(III) to As(V) with the conversion of Mn(IV) to Mn(II), while the generated Mn 2+ was mostly re-adsorbed onto the negatively-charged surface of HMO NPs. During the regeneration process by simple alkaline treatment , the re-adsorbed Mn 2+ was firstly precipitated as (hydr)oxides of Mn(II) and then oxidized to HMO NPs by dissolved oxygen to fully refresh its oxidation capacity. Though HCO NPs mainly served as adsorbent for arsenic, they could partially oxidize As(III) to As(V) at the beginning, while the oxidation capacities continuously diminished with the irreversible conversion of Ce(IV) to Ce(III). In 10 consecutive adsorption-regeneration cycle, Ce-Mn@N201 efficiently decontaminated As(III) from 500 μg/L to below 5 μg/L with Mn 2+ leaching less than 0.3% per batch. During 3 cyclic fixed-bed adsorptions, Ce-Mn@N201 steadily produced 8500–9150 bed volume (BV) and 3150–3350 BV drinkable water from the synthesized and real groundwater, respectively, with Mn leaching in effluent constantly < 100 μg/L.
研究领域:
环境科学
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材料科学
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PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 18
·27037-27051
·
IF 0
Sun Hongyu,Bao Qiongli,Chu Yutan,Li Yan,Shi Jiahao,Huang Yizong
Graphene-based material is widely used to remove arsenic from water due to its layered structure with high surface area. Here, we have successfully synthesized Fe-La bimetallic modified graphite sheet materials to more efficiently remove As(III) from aqueous solution. The results showed that Fe-La-graphite sheets (FL-graphite sheets) have a larger specific surface area (194.28 m 2 ·g −1 ) than graphite sheets (2.80 m 2 ·g −1 ). The adsorption capacity of FL-graphite sheets for As(III) was 51.69 mg·g −1 , which was higher than that of graphite sheets (21.91 mg·g −1 ), La-graphite sheets (26.06 mg·g −1 ), and Fe-graphite sheets (40.26 mg·g −1 ). The FL-graphite sheets conformed to the Freundlich and Dubinin–Radushkevich isotherm, and the maximum adsorption capacity was 53.62 mg·g −1 . The removal process obeys intra-particle diffusion and pore diffusion for As(III). The results of batch adsorption experiments and characterization analyses demonstrated that oxidation, ligand exchange, and inner sphere complexation mechanisms involved in the adsorption of FL-graphite sheets to As(III) in comparison with graphite sheets. In addition, electrostatic attraction mechanism was found vital in the adsorption. Ecotoxicity assessment revealed that FL-graphite sheets have little influence on rice germination and growth, but reduced the toxicity of As(III) to rice. Therefore, the FL-graphite sheets have good practical application value in purifying As(III) polluted water with litter ecotoxicity.
研究领域:
环境科学
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材料科学
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PubMed
WATER RESEARCH
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2026
·
IF 12.8
Zhaoli Liu,Jiahui Fu,Wei-Xian Zhang,Airong Liu
Humic acid (HA), ubiquitous in natural groundwater, affects the efficiency and long-term performance of nanoscale zero-valent iron (nZVI) for in-situ contaminated groundwater remediation. This work aims to clarify how HA affects As(III) removal by nZVI under anoxic conditions. Batch and column experiments were conducted to investigate the removal behaviors of As(III). Multiple characterization techniques, including X-ray absorption fine structure, transmission electron microscopy integrated with energy-dispersive X-ray spectroscopy mapping, and X-ray photoelectron spectroscopy, were employed to analyze interfacial reactivity and electron transfer characteristics. The results showed that HA exhibited concentration-dependent inhibition on both As(III) removal rate and surface-mediated oxidation of As(III). The reaction rate constant decreased to approximately 80% and As(V) proportion declined to roughly 60%. HA exerted no obvious impact on Fe° corrosion and nZVI solid phase evolution. The main inhibitory mechanisms were competitive adsorption on active sites and complexation with aqueous iron ions, which restricted As(III) immobilization and hindered As(III) oxidation induced by surface iron oxides and Fe(II). Furthermore, column experiments verified that HA improved the mobility of nZVI in simulated groundwater environments, but did not offset its inhibitory effect on As(III) sequestration. These findings provide scientific insights into the influence of HA on As(III) sequestration and offer a fundamental basis for enhancing the application performance of nZVI.
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高影响因子
Surfaces and Interfaces
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2026
·
IF 6
Yu Feng,Wenjing Xie,Ao Qian,Yunxuan Xiao,Peng Liu
Phosphate inhibits As sequestration while redirecting interfacial redox pathways. • Passive phosphatization forms a phosphate-enriched mixed corrosion shell. • Surface-associated ROS contribute to enhanced oxic As(III) oxidation. • Surface Fe(II) retention is associated with an anoxic As(0) fraction up to 32.7%. Surface corrosion layers govern the reactivity of zero-valent iron (ZVI), yet their dynamic reconstruction by co-occurring phosphate and its consequences for arsenic (As) transformation remain poorly understood. In this work, we demonstrate that in situ passive phosphatization restructures the ZVI interface into a phosphate-enriched mixed corrosion shell. This interfacial reconstruction decreased overall As sequestration through competitive phosphate occupancy but promoted distinct As(III) redox pathways depending on oxygen availability. Under oxic conditions, phosphate promoted aqueous As(V) accumulation and increased the XPS-derived near-surface As(V) fraction from 52.1% to 78.1% on the finer ZVI. Oxygen-exposure, scavenger, and probe experiments indicated that this enhancement involved surface-associated reactive oxygen species. Under anoxic conditions, phosphate incorporation increased the near-surface Fe(II) fraction to 70.6% and the As(0) fraction from 6.7% to 32.7%, indicating enhanced interfacial As reduction associated with Fe(II) retention. Spectroscopic and electrochemical analyses further showed altered ZVI corrosion behavior and charge-transfer resistance. These findings establish co-occurring phosphate as an active regulator of ZVI interfacial reactivity rather than merely a competitive inhibitor, revealing a trade-off between As redox transformation and sequestration and highlighting its potential for ZVI-based pretreatment coupled with downstream As capture. Download: Download high-res image (212KB) Download: Download full-size image
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ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Minling Gao,Huizhen Deng,Youming Dong,Weiwen Qiu,Zhengguo Song
This study investigated the effects of the antidepressant sertraline hydrochloride (Ser-HCI) on rice physiology when combined with arsenic (III) and cadmium. Hydroponic experiments revealed that combined lower concentrations (0.2 and 0.6 mg L -1 ) of Ser-HCl and As (III) or Cd increased rice biomass and reduced pH and low molecular weight organic acids. The fluorescence intensity was enhanced with Ser-HCl and As-only treatments, with a significant difference ( p < 0.05) in the dissolved organic matter index. There was a decrease in endophyte-specific operational taxonomic units, with proteobacteria dominating the rice root endophytes. The addition of Ser-HCl resulted in a 535% increase in the Verrucomicrobiota , which was positively correlated with malic acid and negatively correlated with pH. Functional annotation highlighted alterations in carbohydrate metabolism pathways. This study provides insights into the interactive effects of Ser-HCl on rice when combined with As (III) and Cd, addressing gaps in our understanding of the impact of antidepressants on plant systems.
研究领域:
环境科学
·
植物生理学
·
微生物学
·
药理学
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Zimo Lou,Zhen Cao,Jiang Xu,Xiaoxin Zhou,Jin Zhu,Xue Liu,Shams Ali Baig,Junliang Zhou,Xinhua Xu
In this study, reduced graphene oxide (RGO) and different stabilizers (hexadecyltrimethylammonium bromide, starch, and carboxymethyl cellulose) were applied to simultaneously support and stabilize Fe-Mn binary oxide (FeMnO x ) nanohybrids, and enhanced removal of As(III)/(V) from water was achieved. TEM images shows that the aggregation of FeMnO x on RGO was effectively inhibited after the starch stabilization, meanwhile, the loading of FeMnO x on RGO was also increased. The adsorption capacity of As(III) and As(V) on starch-FeMnO x /RGO via Langmuir isotherm model was 78.74 mg g −1 and 55.56 mg g −1 , respectively, which was 1.99 and 2.39 times higher than bare FeMnO x . The adsorption kinetics was well fitted by the pseudo-second-order model. The effects of initial pH and coexisted anions were investigated. Over 90% of As(III) and As(V) could be removed by starch-FeMnO x /RGO during the five consecutive adsorption-desorption cycles. The results revealed the potential of the RGO supported and starch stabilized FeMnO x as an efficient adsorbent for arsenic removal from water.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Jinglin Yin,Junhui Yang,Yanmei Li,Ziyang Xiang,Ting Yang,Jing Wang,Tao Xu,Qiong Wang,Wenlei Wang
This study investigated the Fenton-like oxidation of As(III) by three types of iron oxides in oxalate systems. The effects of pH, oxalate concentration and atmosphere on the oxidation of As(III) by iron oxide photocatalyst were studied. Firstly, hydrothermal carbon (HTC) was used as the carrier to load three kinds of iron oxides to prepare new composite materials, including α–FeOOH, α Fe 2 O 3 and Fe 3 O 4 , which can solve the dispersion problem of iron oxide by using a large number of rich functional groups on the HTC surface. The experiment results showed that under the conditions of O 2 , pH = 5.0 and oxalate concentration of 0.5 mmol·L 1 , As(III) was completely oxidized by α–FeOOH and α–Fe 2 O 3 at 15 min and 20 min, respectively. Density functional theory (DFT) was used to study the surface adsorption energy of iron oxide and oxalate. The calculated results showed that the order of adsorption energy of three iron oxides for the oxalate is α FeOOH > α Fe 2 O 3 > Fe 3 O 4 . Fe III (C 2 O 4 ) + , a mononuclear bidentate iron oxalate chelate with the strongest photosensitivity , was constructed in the Fe-Oxalate system containing only Fe(III), resulting in the photocatalytic efficiency of α–FeOOH and α Fe 2 O 3 was superior to that of Fe 3 O 4 . These findings contribute to arsenic remediation of water bodies by using iron materials and oxalate in the natural environment.
研究领域:
环境科学
·
化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhi Xu,Zi-He Meng,Song-Hai Wu,Shi-Jie Wang,Peng-Yue Zhu,Yong Liu,Hai-Tao Ren,Shao-Yi Jia,Xu Han
Sulfate radical (SO 4 •− ) is always thought to be an important oxidizing species in the metal-sulfite [S(IV)] systems, however, the oxidizing species correlated with the metal species have rarely been mentioned. In this study, the oxidizing species that oxidize arsenite [As(III)] in the Cu(II)-S(IV) system were investigated under alkaline conditions. Kinetic results indicate that complexation between Cu(II) and S(IV) is the pre-requisite to initiate various oxidizing species, followed by internal electron transfer from S(IV) to Cu(II) with the formation of SO 3 •− and the Cu I (SO 3 ) n −2n+1 complexes. Quenching experiments rule out contributions of SO 5 •− , peroxymonosulfate (HSO 5 − , PMS), hydroxyl radical ( • OH), superoxide radical (O 2 •− ) and singlet oxygen ( 1 O 2 ) to As(III) oxidation in the Cu(II)-S(IV) system and indicate that some kinds of peroxo species contribute. On the other side, apart from the oxidizing species such as SO 5 •− , PMS and SO 4 •− generated via a series of reactions between SO 3 •− and O 2 , the Cu I (SO 3 ) n −2n+1 complexes also react with O 2 to form Cu II -O 2 •− -(SO 3 2− ) n superoxo species and Cu III -O 2 2− -(SO 3 2− ) n peroxo species, as revealed by Raman analysis. UV–vis spectrum further confirms the presence of Cu(III) in the Cu(II)-S(IV) system. We therefore suggest that both SO 4 •− and the Cu(III)-peroxo species play important roles in the oxidation of As(III) in the Cu(II)-S(IV) system. This study enriches our understanding on the diversity of oxidizing species in the metal-S(IV) systems under alkaline conditions.
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