JOURNAL OF HAZARDOUS MATERIALS
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2023
·
IF 13.6
Xin Zhang,Qingling Fu,Hongqing Hu,Jun Zhu,Yonghong Liu
The co-oxidation of Fe(II) and As(III) occurs under aerobic conditions , and Fe(II) may largely determine the fate of As(III), but the effect of Fe(II) on the As(III) oxidation is barely explored. In this research, the limiting and driving roles of Fe(II) in As(III) oxidation were systematically studied through batch kinetic studies in combination with X-ray photoelectron spectroscopy (XPS) depth profiling, scanning electron microscopy and energy dispersive X-ray spectrometry (SEM-EDS), and quenching experiments. The results showed that As(III) oxidation efficiency increased with the increase of Fe/As molar ratio (from 63.1% to 98.3%), but decreased with the increase of pH (from 96.0% to 44.2%) and the increase of air flow rate (from 88.1% to 75.1%). The Fe(II) oxidation rate increased with the increase of pH and air flow rate. When Fe(II) was oxidized rapidly, As(III) was more likely to be immobilized in the “inner sphere” of formed Fe (hydr)oxides, limiting As(III) oxidation. On the other hand, Fe(II) was oxidized to produce Fe (hydr)oxides to adsorb or fix As(III); meanwhile, the ROS generated by Fenton-like reaction of Fe(II) promoted As(III) oxidation, especially, •O 2 − and H 2 O 2 were important ROS that drove the As(III) oxidation. These findings might provide a new insight for Fe(II) and As(III) geochemistry cycling in naturally occurring environment.
研究领域:
环境科学
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地球化学
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DOI
PubMed
高影响因子
Nanomaterials
·
2020
·Vol. 10
·期 3
·551
·
IF 4.324
Teng Chen,Haitao Wang,Zhouping Wang,Mingqian Tan
As(III) is a toxic heavy metal which causes serious health problems. Therefore, the development of highly sensitive sensors for As(III) detection is of great significance. Herein, a turn-on luminescence resonance energy transfer (LRET) method based on luminous nanorods was designed for As(III) detection. Biotin-labelled As(III) aptamers were tagged to avidin functionalized luminous nanorods as energy donors, while graphene oxide (GO) acted as the energy acceptor. The adsorption of single-stranded DNA on graphene oxide resulted in the efficient quenching of the luminescence of the nanorods through the LRET process. In the presence of As(III), aptamers bonded to As(III) preferentially and resulted in the formation of aptamer-As(III) complexes. The aptamer-As(III) complexes were rubbed off from the GO surface due to their conformational change, which led to the recovery of the luminescence of the nanorods. A good linear relationship between the luminescence intensity and concentration of As(III) was obtained in the range from 1 to 50 ng·mL−1, with a detection limit of 0.5 ng·mL−1. Furthermore, the developed sensors showed good specificity towards As(III) and proved capable of detecting As(III) in the environment and food samples. The proposed time-resolved sensors provide a promising sensing strategy for the rapid and sensitive detection of As(III).Keywords:As(III);time-resolved luminescence;aptamer;nanorods
研究领域:
环境科学
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分析化学
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材料科学
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DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2021
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IF 4.126
Dai Sun,Yu-Le Wang,Peng-Yue Zhu,Hai-Tao Ren,Yong Liu,Song-Hai Wu,Shao-Yi Jia,Xu Han
Mechanisms involved in the photocatalytic oxidation of As(III) are complicated in that various oxidizing species (such as h+, •OH, and O2•–) have been suggested to play important roles in different photocatalytic systems. In this study, Bi2.15WO6 shows high reactivity in the photocatalytic oxidation of As(III) under visible light. Quenching experiments indicate that apart from h+, the surface superoxo (≡Bi–OO•) and peroxo species (≡Bi–OOH) formed on Bi2.15WO6 also contribute to As(III) oxidation. The increased production of H2O2 with increasingly consumed As(III) or with the addition of H-donors such as glucose and various phenolics further reveals that H-abstraction from As(III) or H-donors to ≡Bi–OO• and then to ≡Bi–OOH is an important pathway involved in H2O2 production and As(III) oxidation. In addition, various characterizations confirm that the As(III)–O–Bi(III) surface complexes formed on Bi2.15WO6 enhance the photocatalytic reactivity of Bi2.15WO6 via the ligand-to-metal charge transfer pathway. We therefore suggest that dissolved oxygen is sequentially reduced to ≡Bi–OO• and then to ≡Bi–OOH on Bi2.15WO6, accompanied by H-abstraction from adsorbed or aqueous As(III) to ≡Bi–OO• and ≡Bi–OOH with the formation of H2O2 and the oxidation of As(III). This work enriches our understanding of the mechanisms involved in the photocatalytic oxidation of As(III).
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
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Wenlan Ji,Xinyu Miao,Tian C. Zhang,Yuan Wang,Shaojun Yuan
The elimination of arsenic pollution has attracted increasing concerns due to its toxicity and severe carcinogenicity. Herein, we proposed an in-situ crystal growth strategy without surfactant to fabricate MIL-88B uniformly anchored on the surface of MnO 2 /GAC (MIL-88B/MnO 2 /GAC). Such innovative MIL-88B/MnO 2 /GAC nanostructured composites not only exhibited the synergetic functions of simultaneously oxidizing As(III) and adsorbing the generated As(V), but also effectively reduced the cost of metal–organic frameworks (MOFs) adsorbents. Impressively, the as-prepared sample achieved remarkably boosted As(III) removal capacity of 15.13 mg g −1 compared to 4.1 mg g −1 of MnO 2 /GAC composite and 2.1 mg g −1 of GAC , which was mainly ascribed to the synergistic effect between the excellent adsorption abilitiy of MIL-88B and oxidation property of MnO 2 /GAC. Owing to the unique construction and properties, the constructed MIL-88B/MnO 2 /GAC composites presented a desirable As(III) removal ability under a wide pH scope of 2 to 10. Moreover, the possible mechanism of the synergistic removal over MIL-88B/MnO 2 /GAC was elucidated by X-ray photoelectron spectroscopy (XPS), electron spin resonance (ESR) and radical trapping experiment. This work not only offers a superior bifunctional catalyst for high-efficient removal of arsenic, but also provides a new perspective for rational construction of MOF derivatives for their further applications.
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
WATER RESEARCH
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2018
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IF 7.051
Wei Ding,Jing Xu,Tao Chen,Chengshuai Liu,Jinjun Li,Feng Wu
Previous studies have shown that the oxidation of Fe(II) by molecular oxygen can lead to the co-oxidation of As(III) at neutral pH. However, the mechanism of As(III) oxidation in the presence of Fe(II) with respect to the interaction between As(III) and Fe(II) is still unclear. In this work, we examined the oxidation of As(III) in the presence of Fe(II) in air-saturated water, which is affected by pH, co-existing phosphate, and scavengers ( tert -butanol, superoxide dismutase, catalase and dimethylsulfoxide). Results confirm that the formation of the Fe(II)–As(III) complex (formation constant, K Fe(II)–As(III) = 10 3.86 M –1 ) plays an extremely important role in the initial stage of As(III) oxidation at pH 7.25. The oxidation of Fe(II)–As(III) promotes the production of H 2 O 2 and colloidal ferric hydroxide. H 2 O 2 reacts with the Fe(II)–As(III) complex through oxidizing Fe(II) to Fe(IV), which then causes the partial oxidation (ca. 50%) of As(III). The other part of As(III) oxidation by H 2 O 2 occurs, in the form of Fe(III)–As(III) complex, through direct electron transfer from As(III) to H 2 O 2 but not through Fe(IV). This work provides new mechanistic insight into arsenic and iron redox chemistry in the environment and furthers our understanding of Fenton reactions at neutral pH.
研究领域:
环境化学
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氧化还原化学
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水处理
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Ming Xiao,Ruixue Li,Xinyu Hu,Wenke Zhu,Zhuo Yu,Hongbo Xiao,Wenlei Wang,Ting Yang
This paper is focused on the functional photocatalyst of in-situ carbon-doped TiO 2 decorated Fe 3 O 4 heterojunctions (C/TiO 2 @Fe 3 O 4 ) for the efficient photocatalytic oxidation of As(III). Series of characterizations show that the photocatalytic activity of TiO 2 changes from a single UV wavelength to visible light excitation when carbon atoms are successfully doped in the TiO 2 lattice, expanding the utilization rate of light energy. DFT calculation further confirmed that the C–O–Ti bonds can diminish the theoretical band-gap of TiO 2 . Furthermore, the successful construction of C–O–Ti and Ti–O–Fe interface bonds provide pathways for fast electron transfermation, which can effectively prompt the separation of photo-generated carriers and enhance the photocatalytic oxidation efficiency of As(III). The application results showed that the synthesized C/TiO 2 @Fe 3 O 4 photocatalyst by introducing Fe 3 O 4 with a mass fraction of 1% can complete the transformation of As(III) (10,000 μg/L, 40 mL) to As(Ⅴ) within 12 min under visible light irradiation. In addition, C/TiO 2 @Fe 3 O 4 exhibits excellent reusability, which remains 100% photooxidation efficiency of As(III) without changing crystal structure after 6 cycles and can also be recovered completely with magnet. The remarkable photocatalytic oxidation performances of C/TiO 2 @Fe 3 O 4 can be ascribed to the synergistic effects of OH, O 2 − and h + in the photocatalytic oxidation process and the constructed C–O–Ti and Ti–O–Fe interface bonds.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
高影响因子
Biochar
·
2020
·Vol. 2
·期 1
·81-92
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IF 0
Zhu Sihang,Qu Ting,Irshad Muhammad Kashif,Shang Jianying
A novel α-FeOOH modified wheat straw biochar (α-FeOOH@BC) was developed and the findings of the current study showed that α-FeOOH@BC is an efficient material for the simultaneous removal of cations (Cd(II)) and anions (As(III)) from aqueous solutions. The SEM, FTIR, and XRD analysis proved that α-FeOOH@BC was covered by α-FeOOH. In the single adsorption system, the maximum adsorption capacities of α-FeOOH@BC for Cd(II) and As(III) were 62.9 and 78.3 mg/g, respectively. In the dual adsorption system, the maximum adsorption capacities of α-FeOOH@BC for Cd(II) and As(III) dropped to 39.3 and 67.2 mg/g, respectively. The adsorption capacities of Cd(II) and As(III) by α-FeOOH@BC were much higher by BC and α-FeOOH both in single and dual adsorbate system. The adsorption results were well fitted by the Langmuir and pseudo-second-order kinetics models. The Cd(II) and As(III) co-adsorption on α-FeOOH@BC had a competitive effect, and the dominant adsorption mechanisms were co-precipitation and ion exchange. Our study showed that α-FeOOH@BC could be an effective remediation material for Cd(II) and As(III) co-adsorption from aqueous environment.
研究领域:
环境科学
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材料科学
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产品关联
DOI
WATER ENVIRONMENT RESEARCH
·
2022
·Vol. 94
·期 4
·e10714
·
IF 3.306
Yao Shi,Yifei Xing,Zhilian Song,Xueming Dang,Huimin Zhao
Fe–Mn binary oxide (FMBO) is a promising adsorbent for As(III) removal through combined adsorption and oxidation. The calcined oyster shell-supported Fe–Mn binary oxide (FMBO/OS) adsorbent was synthesized by the co-precipitation method. Results indicated that the calcined oyster shell, as a carrier, improved the stability of FMBO and its adsorption capacity for As(III). The maximum adsorption capacity of FMBO/OS on As(III) reached 140.5 mg·g −1 . Under pH 5.0 and 25°C, the removal efficiency of FMBO/OS to As(III) solution (C 0 = 10 mg·L −1 ) reached 87% within 12 h. Moreover, based on the characterization analyses, the removal mechanisms of As(III) were deduced to include the combined adsorption and oxidation process of FMBO and the synergistic effect of oyster shells. This work provides new insights into synthesizing efficient and green adsorbents to remove aqueous As(III). Meanwhile, it provides technical support for reusing waste biomass materials such as the oyster shell. Practitioner Points FMBO/OS was prepared by a simple hydrothermal co-precipitation method. The carrier alleviates the agglomeration of Fe–Mn oxides. The adsorbent shows a strong adsorption capacity of As(III) and good selectivity. The good results benefit from the synergistic effect of calcium arsenate generation. The prepared adsorbent can adsorb arsenic in real samples.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2024
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IF 4.3
Guangbin Zhu,Ning Duan,Linhua Jiang,Fuyuan Xu,Hongping He,Wen Cheng,Rong Zhang,Yong Liu,Yanli Xu,Shaige Xia,Xiaolu Sun,Fawei Lin
The current methods for determining high-concentration As(III) in the high-acid matrix from the copper smelting industry are complex, time-consuming, and costly. This limits effective modulation of sulfurizing agent dosage for As(III) removal via sulfurization, aggravating hazardous waste generation. Herein, a simple, rapid, and nondestructive UV high-reference differential absorption spectroscopy was developed to directly determine high-concentration As(III) in simulated high-acid wastewater. Time-dependent density functional theory calculations indicated that the spectral curve redshift with As(III) concentration increasing was related to the decrease of electron transition energies and energy gaps. When using high-reference solutions, the least redshift in the maximum absorption wavelength and the highest upper limit of linear fitting concentration could be obtained. Therefore, the piecewise quantitative linear model of differential absorbance and concentration was established under high-reference. The quantitative range of the model within 0.06–20.00 g/L As(III) with a mean relative error of < 5.0 % and standard recovery rates within 98.0 %-104.0 % indicated high accuracy. Additionally, the relative standard deviations of < 1.5 % (n = 5) revealed good precision. All results indicated the high feasibility of the developed method in alleviating linear deviation caused by redshift and absorption saturation. Furthermore, it has potential significance in saving sulfurizing agent dosage and reducing hazardous waste generation from the source, thereby facilitating a cleaner process for removing As(III) via sulfurization.
研究领域:
环境科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yi Peng,Ying Yan,Jing Wang,Ziyang Xiang,Yanmei Li,Junhui Yang,Jinglin Yin,Wenlei Wang,Hongbo Xiao
In this study, CdSe cluster-modified biogenic α − FeOOH based on macroporous biochar was constructed from rhizosphere iron plaque via pyrolysis. An ultrahigh H 2 O 2 production rate of 655.75 μmol/L was achieved by the photocatalysis-self-Fenton system within 30 min under visible light irradiation. α-FeOOH, with abundant iron ions, can directly activate H 2 O 2 to produce abundant ⋅OH radicals. It was found that As(III) (10 mg/L) could be completely degraded within 20 min. Electron spin resonance spectroscopy (ESR) and density functional theory (DFT) revealed that a suitable energy band structure was achieved by the introduction of CdSe clusters; thus, O 2 was mainly reduced to H 2 O 2 through a two-electron reduction route in the reaction system. The photogenerated electrons promoted the conversion of Fe(III)/Fe(II) by reacting with Fe(III) in α-FeOOH. The presence of H 2 O 2 and Fe 2+ in this system accelerates the oxidation of As(III) by a Fenton-like reaction.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Xiao Ge,Juntao Liu,Xiangyang Song,Guozhong Wang,Haimin Zhang,Yunxia Zhang,Huijun Zhao
The hierarchical flower-like iron containing γ-MnO 2 hollow microspheres assembled by ultrathin nanosheets have been successfully fabricated via a facile one-step co-precipitation route in the absence of additional templates or surfactants. Structural characterization show that iron element is uniformly incorporated into γ-MnO 2 framework, and no segregated iron oxide appears. The resulting iron containing MnO 2 hollow microspheres exhibit a noticeable enhanced performance for As(III) removal compared to that of the undoped counterparts, accompanied by 102.84 mg/g of the saturated removal capacity towards As(III). The excellent performance for the arsenic removal may be attributed to the unique structural characteristics of highly accessible surface and fully exposed active sites inherited from the hierarchical iron containing γ-MnO 2 samples. The co-existence of oxidation and adsorption is another key factor for the improvement of As(III) removal efficiency, in which manganese dioxide is mainly responsible for oxidizing As(III) to As(V) and ferrous species may serve to the adsorption of the generated As(V), as evidenced by X-ray photoelectron spectroscopy (XPS) analysis. Importantly, the composites exhibit an excellent regenerative ability over three cycles without a significant decrease in its removal efficiency towards As(III). Furthermore, the relatively large micrometer-scale particles can be easily separated by filtration, accompanied by fewer secondary contaminants risks than nanoparticles. Therefore, the fabricated hierarchical Fe-containing γ-MnO 2 hollow spheres in the present study will be an excellent candidate for the arsenic transformation and removal from the contaminated water based on the synergistic effects of effective oxidizing and adsorptive performance, good regeneration together with the convenient separation.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Xiaoyu Zheng,Qiuju Wu,Chao Huang,Ping Wang,Hao Cheng,Chengyou Sun,Jian Zhu,Haiyin Xu,Ke Ouyang,Jing Guo,Zhiming Liu
Biochar derived from bamboo was used to support sulfide nanoscale zero-valent iron (S-nZVI@BC) for simultaneous removal of Cd(II) and As (III) from aqueous media. Scanning electron microscopy (SEM) and X-ray diffraction spectroscopy (XRD) characterization confirmed the successful synthesis of the S-nZVI@BC. Adsorption kinetics and isotherms indicated that co-adsorption of Cd(II) and As(III) onto S-nZVI@BC was well represented by pseudo-second-order model ( R 2 Cd(II) = 0.990, R 2 As(III) = 0.995) and Langmuir model ( R 2 Cd(II) = 0.954, R 2 As(III) = 0.936). The maximum adsorption was 162.365 and 276.133 mg/g for Cd(II) and As(III), respectively, in a co-adsorption system, which was significantly higher than that in a single adsorption system (103.195 and 223.736 mg/g, respectively). Batch experiments showed that the Cd(II)-to-As(III) concentration ratio significantly affected the co-adsorption with the optimal ratio of 1:2. Ca 2+ and Mg 2+ significantly inhibited Cd(II) removal. In contrast, phosphate and humic acid significantly inhibited As(III) removal. Electrochemical analysis indicated S-nZVI@BC had a lower corrosion potential and resistance than nZVI@BC, making it more conducive to electron transfer and chemical reaction. Electrostatic adsorption, complexation, co-precipitation, and redox were the primary mechanisms for Cd(II) and As(III) removal. Overall, the present study provides new insights into the synergistic removal of Cd(II) and As(III) by S-nZVI@BC, which is a very promising adsorbent for the effective removal of Cd(II) and As(III) from contaminated wastewater.
研究领域:
环境科学
·
污染治理
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）