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
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2021
·
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
·
材料科学
✓ 已验证
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
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2018
·
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
·
氧化还原化学
·
水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2024
·
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
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
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
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Yuanjie Xiong,Xiang Liu,Tian Cheng Zhang,Shaojun Yuan
The conversion of As(III) to As(V) in groundwater is an urgent issue, owing to the higher mobility, stronger toxicity, and weaker binding ability of As(III). In this work, the electrocatalytic oxidation of As(III) was efficiently achieved with a facile and environmentally benign method by using hierarchical MnO2-deposited TiO2 nanotube arrays (MnO2/TNAs) as the anode. The electrocatalytic oxidation performance of the as-fabricated MnO2/TNA-coated anode was systematically investigated. The results exhibited that such as-fabricated MnO2/TNAs had a high oxidation efficiency of 90% at a low concentration of As(III) (1 mg L–1). Furthermore, the reaction mechanism was systematically studied by electron spin resonance and free radical capture experiments. The oxidation of As(III) was accomplished via both direct oxidation on the anode surface and indirect oxidation of the reactive oxygen species. The highly efficient TNA-based anode offers a potentially promising advanced material for electrochemical oxidation of trace As(III) in the practical field.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Like Ouyang,Yan Zhang,Yuan Wang,Xinlong Wang,Shaojun Yuan
The coupled adsorption–photocatalytic oxidation process provides a great potential scenario to enhance the removal efficiency of arsenite contaminants by converting As(III) to As(V) and simultaneous adsorption. In this study, the boron-doped black TiO2/g-C3N4 nanocomposite is synthesized by combination of sol–gel and in situ decomposition-thermal polymerization methods as a photocatalyst for the photocatalytic oxidation and adsorption of As(III). Under dark conditions, the boron-doped samples (B-TiO2 and B-TiO2/g-C3N4) display an increase in the As(III) adsorption capacity by one order of magnitude up to circa 3.2 mg g–1 with an initial As(III) concentration of 2 mg L–1 at 298.15 K and pH 5. The adsorption kinetics of As(III) on B-TiO2/g-C3N4 conform to the pseudo-second-order kinetic model, revealing the chemical adsorption mechanism. Under visible light irradiation, the total arsenic removal capacity is substantially improved by 20% with a removal capacity of 3.9 mg g–1. The enhancement of arsenic adsorption is attributed to the chemical complexation and hydrogen bond, in which B–OH bonds play a dominant role. The photocatalytic oxidation mechanism of the as-synthesized B-TiO2/g-C3N4 is attributed to the synergism of superoxide radicals, hydroxyl radicals, and photogenerated holes.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Jihong Chen,Xiaoyu Dong,Dali Zhuo,Jiayuan Tang,Xiaoli Xiong,Hong Luo,Zhirong Zou
Metal-organic frameworks (MOFs) are porous materials that constructed by various metal nodes and organic ligands, taking the advantages of high porosity, large specific surface areas and more reactive sites etc. However, the applications of MOFs in hydride generation (HG)/chemical vapor generation (CVG)-colorimetric systems are rare. Herein, a series of silver-based MOFs (Ag-MOFs) were synthesized and served as substrates for As(III) and S 2- colorimetric analysis. As(III) and S 2- were converted into its volatile species (AsH 3 and H 2 S) via HG and CVG process, respectively, providing merits of low matrix interferences (selectivity) and high vapor generation efficiency (sensitivity). Ag-MOF-3 exhibits the best performances for As(III) and S 2- analysis, its reaction mechanisms were further explored. Ag nanoparticles (redox reaction) and Ag 2 S nanoparticles (combination reaction) were formed after Ag-MOF-3 reacted with AsH 3 and H 2 S, respectively, leading to color change from light yellow to black. The variation was recognized by naked eye and smartphone. Standard cards/curves of visual method and smartphone RGB method were thus established for As(III) and S 2- . It is a potential analytical method for on-site and rapid analysis of As(III) and S 2- with merits of low-cost, easy-to-use and portability.
研究领域:
分析化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENT INTERNATIONAL
·
2019
·
IF 7.943
Chao Shan,Yan Liu,Yuhao Huang,Bingcai Pan
Heterogeneous catalysis is a promising approach to achieve efficient As(III) oxidation by H 2 O 2 at circumneutral pH. However, radical-attack pathways dominated catalytic As(III) oxidation over most metal oxides is undesirably associated with low utilization of H 2 O 2 induced by rapid self-quenching of radicals. In this study, we developed a non-radical catalytic route to improve H 2 O 2 utilization efficiency for catalytic As(III) oxidation based on nanoceria. The performance and mechanism of As(III) oxidation by H 2 O 2 was investigated by employing four types of nanoceria with different crystallite sizes (9.1–80.6 nm). At the H 2 O 2 /As(III) molar ratio of 2.0, nanoceria exhibited crystallite size-dependent catalytic activity for oxidation of As(III) over a wide pH range (5–9). Based on comprehensive study including scavenging, enzymatic, and pretreatment experiments and miscellaneous spectroscopy techniques, the catalytic As(III) oxidation over nanoceria was proved to be mainly mediated by the non-radical Ce-hydroperoxo surface complexes, whilst the surface hydroperoxyl radical served as a minor oxidant. In contrast, the roles of dissolved oxygen, homogeneous H 2 O 2 , and OH radical were all negligible. No obvious interconversion of Ce(III)/Ce(IV) was observed by XPS for the catalytic process. Such non-radical pathway enabled a stoichiometric reaction with high H 2 O 2 utilization efficiency (90.5%–122%). Moreover, nanoceria could be recycled for five consecutive runs without desorption/regeneration treatment. This study sheds new light on the development of nanoceria-based catalytic processes for efficient oxidation of As(III).
研究领域:
环境化学
·
催化
·
水处理
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zhengliang Zhao,Jun Zhou,Zhu Shu
Piezo-catalysis is an emerging approach for green chemistry and water decontamination, which however is absent in aqueous arsenic remediation. Polymeric carbon nitride (PCN), a new piezoelectric material, was recently up-graded into crystalline carbon nitride, potassium poly(heptazine imide) (K-PHI). But the piezo-catalytic property of K-PHI is still blank in literature. This work first realized the oxidation of As(III) by piezo-catalysis and revealed the advanced piezo-catalytic property of K-PHI in comparison with PCN. A much superior (6.7 times faster) piezo-catalytic oxidation of As(III) was achieved on K-PHI, which benefits from its enhanced piezoelectric response deriving from the extended in-plane conjugation of heptazine units. Apart from the crystallinity of carbon nitride, the solution pH, sonication power and catalyst dosage were also found to be positively correlated with the piezo-catalytic As(III) oxidation. Additionally, h + and ·O 2 − rather than OH· were proved to be the active species. These findings not only supply a novel approach for As(III) pollution regulation in water bodies, but also point out the direction to improve the piezo-catalytic performance of carbon nitride.
研究领域:
环境科学
·
材料科学
·
水处理
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Chengcheng Shen,Li Gu,Sihao Chen,Yajuan Jiang,Peng Huang,Heng Li,Huayang Yu,Dong Xia
Effective utilization and resourcelization of sewage sludge into value-added by-products and insights into its environmental impacts during the fabrication process are urgent tasks to be tackled. Here, we adopt FeCl 3 to activate and functionalize sewage sludge to form FeCl 3 -activated biochars, which exhibited high adsorption capabilities for the treatment of toxic As(III) and Cr(VI) containing wastewaters. Kinetic studies suggested that the adsorption of As(III) and Cr(VI) species onto the biochar surface was attributed to physisorption and chemosorption, respectively. Equilibrium was reached after 3 h for the adsorption of Cr(VI), and slightly slower for that of As(III). Additionally, the structural stability of the adsorbent was maintained even in wastewater with high acidity (pH = 1), as corroborated by microscopic observations. Structural characterization of the adsorbents after adsorption showed that the excellent adsorption performance originated from adsorptive functionalities of the surface functional groups and the active Fe 3 O 4 particles forming Fe-O-As(III)/Fe-O-Cr(VI) complexes with the As(III)/Cr(VI) adsorbates. Evaluation via the green degree method demonstrated that transforming sewage sludge into biochar exerts very low impacts on the environment. Hence, this work offers a green alternative to convert the hazardous sewage sludge into value-added biochar materials, which can be further exploited as supporting frameworks for multifunctional catalysts or expanded to be investigated in reducing carbon footprints and energy conversion areas.
研究领域:
环境科学
·
废物管理
·
水处理
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）