Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Zulqarnain Haider Khan,Zhongyang Li,Minling Gao,Md. Shafiqul Islam,Ling Xiao,Weiwen Qiu,Zhengguo Song
As(III) and Cd(II) co-existence results in co-contamination in soil and water. It is still a great challenge for As(III) and Cd(II) simultaneous removal in the aqueous medium due to their contrasting chemical behaviour. Herein, we prepared a novel magnesium-manganese modified biochar composite (Mg/Mn@BC) for simultaneous Cd(II) and As(III) elimination from contaminated water . The synergistic effect of Mg/Mn@BC composite on synchronous Cd( II ) and As(I II ) removal was confirmed. In the mixed sorption system, the Langmuir sorption capacity of Mg/Mn@BC for As(III) and Cd( II ) was 164 and 316 mg g −1 , respectively, which was more than that in the single adsorption system (75 and 295 mg g −1 ). In the single sorption system, the Mg/Mn@BC sorption efficiency was > 61% and 100% for As( III ) and Cd( II ), respectively, while > 87% and 100% in the mixed adsorption system. The characterization results revealed that synergistic adsorption was mainly attributed to anion-bridging (Mn/MgO–As–Cd) and cation-bridging (Mn/MgO–Cd–As). The ion exchange, precipitation, Cd–π binding and inner-sphere surface complexation with functional groups were predominant in the sorption process, while hydrogen bonding force and ternary complexation were the primary pathways in mixed adsorption system to eliminate Cd(II) and As(III). The results suggested that Mg/Mn@BC composite can be a potential material for wastewater treatment .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Hao Wang,Yongrong Zou,Tao Luo,Mehdi Benouahmane,Danna Zhou,Feng Wu
In recent years, a new strategy of using sulfite (S(IV)) to replace persulfates (peroxydisulfate (PS) and peroxybisulfate (PMS)) for sulfate radical based advanced oxidation process (SR-AOP) has emerged as one of the potential alternatives in the field of AOPs. Although the thermal activation of PS and PMS has been investigated extensively, that of S(IV) has not yet been explored. In this work, As(III) oxidation in a heat–S(IV) system was investigated first to demonstrate the feasibility of thermal activation of S(IV). Results showed that S(IV) can be activated to oxidize As(III) by heating the reactant solution from room temperature to above 50℃. Almost complete oxidation of 5 μM As(III) in water at pH 7 with addition of 1 mM S(IV) was achieved at 70 °C within 30 min. As(III) oxidation in the heat–S(IV) system was strongly dependent on the dissolved oxygen in water. Radical-scavenging experiments and electron spin resonance analysis demonstrated that the main active species responsible for As(III) oxidation was SO 4 •− . On the basis of thermal activation, a new system of SR-AOPs, namely, heat–electro-S(IV) system, the coupling thermal and electrochemical activations was established with ruthenium-plated iridium electrodes at a voltage of 3 V. It achieved complete oxidation of 50 μM As(III) in water at pH 7 at 50 °C with the addition of 2 mM S(IV) after reaction for 30 min. This work provides a new activation method for SR-AOPs with S(IV) as the precursor of reactive species and helps in understanding the reaction of S(IV) autooxidation.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Junhui Yang,Wenlei Wang,Jinglin Yin,Yanmei Li,Ziyang Xiang,Yi Peng,Ying Yan,Jing Wang,Hongbo Xiao
In this study, a matrix composite material of CdZnS and α-FeOOH on carbon cloth (CZS@FeOOH@CC) was prepared by a hydrothermal method , and was used for the degradation of As(III). The composite material has good photocatalytic activity of removing As(III) in the presence of oxalate. CZS@FeOOH@CC can completely degrade 10 mg/L As(III) within 10 min under visible light irradiation. The influence factors of CZS@FeOOH@CC composite material on catalytic oxidation of As(III) were also studied in the oxalate system. The photocatalytic oxidation efficiency of As(III) is affected by the oxalate concentration in the reaction system, and the atmosphere plays a major role in the degradation of As(III). Under visible light, oxalate first combines with Fe(III) on the surface of iron oxide to form Fe(III)-oxalate complex, and then the Fe(III)-oxalate composite is activated to produce·C 2 O 4 − . In the presence of oxygen, Fe(II) readily reacts with O 2 and oxidizes to Fe(III). The introduction of CdZnS promoted the separation of interfacial electron holes, and accelerated the REDOX cycle of Fe(II)/Fe(III). This study provides a feasible and simple method for accelerating the catalytic removal of heavy metals from wastewater by iron-based materials.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Zhuo-Rui Jiang,Yuxin Li,Deyun Zhang,Yu-Xiao Zhou,Genbao Xu,Changhua Wang,Yeqing Lan,Jing Guo
Arsenite (As(III)) is more toxic and difficult to remove than arsenate (As(V)). In this study, an S-doped Cu-La bimetallic oxide (S-CuLaO) decorated with metal-organic framework (MOF) composite (S-CuLaO@UIO-66) was synthesized and applied for the adsorption of As(III). The maximum adsorption capacity of As(III) by S-CuLaO@UIO-66 was as high as 171 mg/g, which was much higher compared with other MOF compounds reported to date. The UIO-66 support improved the dispersion and reduced the size of the S-CuLaO particles, which increased the number of exposed adsorption reactive sites. Study of the mechanism revealed that the synchronous oxidation and adsorption significantly increased the removal of As(III). O 2 ∙ - was produced by the receiving electron from the dissolved oxygen from Cu(I) in S-CuLaO, which converted As(III) to As(V). Furthermore, the stability and reusability S-CuLaO@UIO-66 (without regeneration) was investigated at a low As(III) concentration (approximately 1000 µg/L) in deionized water and well water. The residual arsenic concentration ranged from 0.8 to 2.8 μg/L in deionized water and 3–58.2 μg/L in well water within 240 min during three cycles. Generally, this study suggests that combining an optimal oxide with a stable MOF is a promising approach for the fabrication of composite adsorbents.
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Catalysis Science & Technology
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2018
·Vol. 8
·期 7
·1936-1944
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IF 5.365
Zhongmin Liu,Yongchuan Wu,Jitao Chen,Yaru Li,Jingyu Zhao,Kaihua Gao,Ping Na
A bifunctional cake-like TiO2 was successfully synthesized via calcination of MIL-125(Ti) at a suitable temperature by a one-step method and was applied for As(III) removal by simultaneous photocatalytic oxidation and adsorption. The as-synthesized samples were characterized by XRD, TGA/DSC, SEM, TEM, N2 adsorption–desorption isotherms, PL spectra, photocurrent, FTIR and XPS. The effects of calcination temperature on the specific surface areas of the samples, transformation of the TiO2 crystal phase and properties of As(III) removal were investigated. The results showed that higher calcination temperature resulting in a lower specific surface area and more transformations of the TiO2 crystal phase from anatase to rutile. The TiO2 calcined at 380 °C (MIL-125(Ti)-380 °C) exhibited excellent properties for As(III) removal, including photocatalytic oxidation of As(III) and simultaneous adsorption of the generated As(V). In addition, MIL-125(Ti)-380 °C could be reused at least four times without significant reduction in the photocatalytic oxidation and adsorption performances. The excellent photocatalytic oxidation and adsorption abilities of MIL-125(Ti)-380 °C can be attributed to the synergistic effects of strong photogenerated electron–hole separation and high specific surface area. The bifunctional cake-like TiO2 provides a wonderful strategy to remove As(III) completely from contaminated water using a single step.
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CHEMICAL ENGINEERING JOURNAL
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2016
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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.
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ELECTROCHIMICA ACTA
·
2017
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IF 4.798
Yudong Xue,Shili Zheng,Yi Zhang,Wei Jin
Environmental conversion of As(III) to less toxic As(V) is a critical step for the arsenic pollution remediation. In the present study, MoS 2 ultrathin nanosheets modified carbon felt electrode is fabricated by a facile hydrothermal method and employed as the two-electron oxygen reduction reaction (ORR) cathode for the As(III) oxidation in alkaline media. Due to the rich Mo O bonds at MoS 2 ultrathin nanosheets, the two-electron ORR catalytic property, electrical conductivity and hydrophilic behavior are significantly enhanced. Besides, As(III) can be efficiently conversed via adsorption-oxidation scheme on the modified layer, and there is good stability on the MoS 2 modified electrode during the electro-oxidation process. This MoS 2 modified carbon felt can be presented as a cost-effective cathode for the electroperoxidation process and provided further understanding for the environmental remediation in alkaline media.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Zizheng Liu,Jiawei Liu,Haike Yang,Jingyi Guo,Yiqun Chen,Qing Shao,Shuxian Gao,Liting Luo
Arsenic is categorized as a class I carcinogen due to its strong biological toxicity. In this study, a novel treatment process with Cu 2 (OH) 2 CO 3 as catalyst is proposed, whereby As(III) in water is oxidized by activating sulfite to generate SO 4 − and SO 5 − radicals. Under conditions of [Cu 2 (OH) 2 CO 3 ] 0 = 0.01 g·L −1 , [sulfite] 0 = 0.3 mmol·L −1 , and initial pH 8.0, 94% of As(III) was converted into As(V) within 20 min, whereby dissolved oxygen had a pivotal impact on the reaction. However, HCO 3 − , humic acid, and fulvic acid all significantly inhibited the oxidation. Heterogeneous electron transfer on the catalyst surface and homogeneous dissolved Cu 2+ jointly activated sulfite in the Cu 2 (OH) 2 CO 3 /sulfite system, with the heterogeneous process predominating. Density functional theory (DFT) calculations disclose a dominate physical adsorption of sulfite on Cu 2 (OH) 2 CO 3 surface with 1.74 electrons transferred. >90% of As(III) was still oxidized after recycling the material five times, indicating excellent reusability. Overall, it shows good potential for application in the removal of As(III) from real water samples.
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CHEMOSPHERE
·
2019
·
IF 5.108
Junqin Liu,Pingxiao Wu,Shuaishuai Li,Meiqing Chen,Wentin Cai,Dinghui Zou,Nengwu Zhu,Zhi Dang
A high removal rate (>99.7%) of combined arsenite (As(III)) and Cd (Cd(II)) in low concentration (1000 μg/L) from contaminated water was achieved by a calcined MgZnFe-CO 3 layered double hydroxide (CMZF) adsorbent. Batch control studies and a series of spectroscopy detection technologies were employed to investigate the removal mechanism and interactions between As(III) and Cd(II) on the interface of water/CMZF. Synergistic adsorption and photooxidation occurred based on the systematical kinetic and isotherm studies. The enhanced removal of As(III) was achieved by the photooxidation, formation of ternary As(III) Cd(II) surface complexes and enhanced hydrogen bond . Meanwhile, oxidative formed negative charged As(V) could reduce the electrostatic repulsion force between Cd(II) cations and play a role as anion bridging, consequently resulted in a stronger attraction between CMZF and Cd(II). Combined with the verdicts of relevant characterizations such as XRD, XPS and EPR, it was assumed that the deep co-removal mechanism could be attributed to the coupling of various processes including intercalation, complexation, photooxidation of As(III) and precipitation of CdCO 3 . Moreover, the successful removal of As(III) and Cd(II) from real water matrix qualified the CMZF a potentially attractive adsorbent for both As(III) and Cd(II) deep treatment in practical engineering.
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CHEMICAL GEOLOGY
·
2019
·
IF 3.618
Jian Zhang,Yuxin Li,Wei Li,Lixiang Zhou,Yeqing Lan,Jing Guo
This paper focused on understanding the effect of citric acid (CA) on the reductive dissolution of Schwertmannite loaded with arsenite (SCH-As(III)) under UV irradiation and the release of arsenic (As). Results demonstrated that CA could significantly promote the reductive dissolution of SCH and SCH-As(III) with the assistance of ultraviolet light. Initially, the dissolved total iron (Fe) and As exhibited a rapid increase (0 to 240 min), followed by a quick decline due to the depletion of CA. It was found that the dissolved total Fe and As were present mainly as the species of Fe(II) and As(V), respectively. This can be attributed to the electronic transfer from ligand to metal in the complex of Fe(III)-(CA) n occurring under ultraviolet light, leading to the production of Fe(II) and organic radicals. Moreover, As(V) was further generated via the interaction of As(III) with OH from a series of radical reactions. In the dark, CA could also enhance the total Fe and As released from the SCH-As(III). The lower the initial pH level, the greater the amount of total dissolved Fe and As. The presence of Al 3+ clearly suppressed the reductive dissolution of SCH-As(III) triggered by CA and ultraviolet light. SEM spectra indicated that the mineralogical phases of SCH-As(III) before and after the reaction were discrepant. Thus, this study provides an insight into the stability of SCH-As(III) and the migration of As in the natural environment.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yao Deng,Yanmei Li,Jing Wang,Huidi Zhang,Lin Wang,Qiong Wang,Tao Xu,Wenlei Wang
Nitrogen deficient porous nanosheets(NDCN) are a promising nano template that can combine defect engineering with Mn-FeOOH to suppress photo generated carrier complexation and optimize electron distribution . In this study, a unique structure with N/O double vacancies in Mn-FeOOH@NDCN was prepared using a magnesium thermal denitrification co-precipitation method. Furthermore, a series of Mn-FeOOH/NDCN/PMS reaction systems were constructed by adjusting the dosage of peroxymonosulfate(PMS). The experimental results indicate that the synergistic activation of N/O double vacancies on PMS enables the Mn-FeOOH/NDCN/PMS system to oxidize almost 10 mg/L of As(III) within 90 min. At the same time, the oxidized As(V) was completely adsorbed, thereby completely removing the total arsenic in the water. The reasonable construction of carbon networks is a prerequisite for the stability of Mn-FeOOH/NDCN composite catalysts, enabling them to have good cyclic stability. The experimental results confirm that oxygen vacancies directly participate in the activation of PMS, while nitrogen vacancies effectively adsorb As(III), thereby promoting the contact between As(III) and PMS, improving the mass transfer rate, and accelerating the catalytic degradation process. This study will provide a new way to completely remove arsenic pollution from water bodies.
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Journal of Environmental Sciences
·
2021
·
IF 5.565
Wenjun Huang,Haomiao Xu,Xiaoshuang Liu,Longlong Wang,Shutang Li,Leipeng Ji,Zan Qu,Naiqiang Yan
Fe 3 O 4 -based materials are widely used for magnetic separation from wastewater. However, they often suffer from Fe-leaching behavior under acidic conditions, decreasing their activity and limiting sustainable practical applications. In this study, covalent organic frameworks (COFs) were used as the shell to protect the Fe 3 O 4 core, and the Fe 3 O 4 @COF core-shell composites were synthesized for As(III) removal from acid wastewater. The imine-linked COFs can in situ grow on the surface of the Fe 3 O 4 core layer by layer with [COFs/Fe 3 O 4 ] mol ratio of up to 2:1. The Fe-leaching behavior was weakened over a wide pH range of 1-13. Moreover, such composites keep their magnetic characteristic, making them favorable for nanomaterial separation. As(III) batch adsorption experiments results indicated that, when COFs are used as the shell for the Fe 3 O 4 core, a balance between As(III) removal efficiencies and the thickness of the COF shell exists. Higher As(III) removal efficiencies are obtained when the [COFs/Fe 3 O 4 ] mol ratios were < 1.5:1, but thicker COF shells were not beneficial for As(III) removal. Such composites also exhibited better As(III) removal performances in the pH range of 1–7. Over a wide pH range, the zeta potential of Fe 3 O 4 @COF core-shell composites becomes more positive, which benefits the capture of negative arsenic ions. In addition, thinner surface COFs were favorable for mass transfer and facilitating the reaction of Fe and As elements. Our study highlights the promise of using COFs in nanomaterial surface protection and achieving As(III) depth removal under acidic conditions.
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