CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yuxin Li,Zhimin Wang,Yuanfeng Wei,Ting Wang,Maosong Zhao,Jie Luo,Jun Zhou,Zhaoshuang Li,Kai Yin,Chengbin Liu
Water decontamination from arsenic-contaminated groundwater is critical to the health of millions of households worldwide. However, efficiently removing the low-adsorbing As(III) remains challenging. Herein, a multifunctional biocomposite bead UiO-66-NH 2 -Cl@PCB integrating defects, oxidation and adsorption properties was prepared to effectively remove As(III). The N -chlorosulfonamide bound within the embedded UiO-66-NH 2 -Cl oxidizes the lower-adsorbing As(III) to As(V), which could be effectively adsorbed by the defect-rich MOF, while the porous chitosan bead (PCB) host ensures the utilisation of the reactive sites of UiO-66-NH 2 -Cl. Using 1 g/L of UiO-66-NH 2 -Cl@PCB, 1 mg/L of As(III) can be reduced to under 10 μg/L in 300 min. Furthermore, similar As(III) removal efficiencies were achieved across a wide pH spectrum (3–9) or in the presence of interfering substances (anions, cations, organic matter). High concentrations of phosphate will inhibit its performance. As(III) removal followed the Freundlich isotherm modal, and its maximum removal capacity reached 58.09 mg/g at pH 7. Furthermore, at equilibrium concentrations of 10 μg/L, its As(III) removal capacity exceeded 10 mg/g. UiO-66-NH 2 -Cl@PCB can purify the As(III)-spiked groundwater to meet the drinking standard level. Using NaOH solution for regeneration, the removal efficiency maintained above 70 % in the fifth cycle. Additional chlorination treatment can significantly improve reusability. 2.4 g of UiO-66-NH 2 -Cl@PCB packed fixed-bed column was capable of purifying 3820 BV of groundwater containing 100 μg/L of As(III). The proposed UiO-66-NH 2 -Cl@PCB has the potential to be an easy-to-use and reliable material for efficient As(III) removal.
研究领域:
环境科学
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材料科学
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水处理技术
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化学工程
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吸附与催化
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高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Wei Shi,Xueye Wang,Fei Gao,Zhiwei Wang
The effective removal of trace levels of the highly toxic arsenite (As(Ⅲ)) from groundwater is crucial to address the threat to drinking water supply. Herein, we developed an electrochemical separation system utilizing redox-active ferrocene-based metal-organic frameworks (termed Fe-DFc) for selective removal of As(III). This system leveraged 1,1′-ferrocenedicarboxylic acid as a ligand coordinated with iron, enabling the highly selective capture and conversion of As(III) from groundwater. The Fe-DFc electrode-based electrochemical system not only effectively removed As(III) even in the presence of a 1250-fold excess of competing electrolytes, but also converted about 96 % of the adsorbed As(III) into the less toxic As(V), surpassing the results of those documented in the current literature. X-ray absorption fine structure analysis and density functional theory calculations demonstrated that the high selectivity of Fe-O 6 moiety and the exceptional redox activity of Fc synergistically contributed to the efficient removal of As(III). Moreover, the electrochemical separation system enabled the remediation of arsenic-contaminated groundwater at a low energy cost of 0.033 kWh m −3 during long-term operation, highlighting the application potential of the electrochemical technology for arsenic removal from contaminated water.
研究领域:
环境科学
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化学
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材料科学
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电化学
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水处理
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ENVIRONMENTAL POLLUTION
·
2018
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IF 4.358
Jian Zhang,Wei Li,Ying Li,Lixiang Zhou,Yeqing Lan
Schwertmannite (SCH) has strong adsorption ability to As(III). However, there are few reports on the stability of SCH load with As(III) (SCH-As(III)). In this study, the effects of tartaric acid (TA), pH and coexisting ions including K + , Ca 2+ , Al 3+ and CO 3 2− on the photoreductive dissolution of SCH- As(III) and the release of the adsorbed As (III) were investigated. The results showed that under UV irradiation TA could greatly enhance the release of total Fe and total As from SCH-As(III). Nevertheless, the total Fe and total As in the solution decreased when TA was consumed up. Compared to SCH, the reductive dissolution of SCH-As(III) was obviously suppressed. In the dark, TA could slowly enhance the dissolution of SCH-As(III), but its effect on the release of adsorbed As(III) was weak. Low pH was conducive to the release of iron and arsenic. Ca 2+ , K + , and CO 3 2− promoted the decrease of the dissolved total Fe in the later reaction. However, Al 3+ inhibited the decrease of the dissolved total Fe and total As. The analyses of FTIR and XRD demonstrated that the mineralogical phase of SCH-As(III) after reaction changed. With light, the dissolved total Fe and total As existed mainly as Fe(II) and As(V), respectively. This is because Fe(II) was generated via ligand to metal charge transfer and As(III) was oxidized to As(V) by ·OH produced during the reaction. Thus, this study provides us with a comprehensive understanding of the stability of SCH-As(III) and the release of adsorbed As(III) in natural environments.
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JOURNAL OF HAZARDOUS MATERIALS
·
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.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yuanfeng Wei,Weijian Yang,Zhimin Wang,Kai Yin,Tao Chen,Chengbin Liu
Iron oxide-modified biochars are increasingly recognized as a promising arsenic adsorbent. However, most of them face serious challenges in the rapid and efficient removal of As(III). Herein, we integrated the iron oxide nanoneedles vertically covered biochar fibers (Fe-BFs) with H 2 O 2 and Hydroxylamine (HA) to construct a heterogeneous catalytic system for the rapid oxidation and deep removal of As(III) from water. The system oxidized the As(III) to As(V) with high efficiency, and then the generated As(V) could be rapidly removed by adsorption onto Fe-BFs. The removal efficiency of As(III) by Fe-BFs/H 2 O 2 /HA at 120 min reached up to 98.93%, which is much higher than that of by Fe-BFs (69.20%) and Fe-BFs/H 2 O 2 (92.32%). The system could work reliably in a wide pH range (4–10). Moreover, fixed-bed column experiments demonstrated that the addition of H 2 O 2 and HA could increase the effective treatment volume from ~350 bed volume (BV) to ~700 BV to meet the drinking water standard (<10 μg/L). The introduction of HA induced the reduction of surface Fe(III) of Fe-BFs to surface Fe(II), which reacted with H 2 O 2 to produce OH. The OH played a very important role in promoting the removal of As(III). This study offers a new strategy to enhance the applicability of Fe modified biochar for As(III) removal.
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ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Xiaoqing Meng,Xiaomeng Wang,Chunmei Zhang,Su Yan,Guanyu Zheng,Lixiang Zhou
Co-contamination of arsenic and polycyclic aromatic hydrocarbons (PAHs) in groundwater is frequently reported, and it is thus necessary to develop efficient techniques to tackle this problem. Here, we evaluated the feasibility of utilizing schwertmannite to co-adsorb As(III) and phenanthrene from water solution and regenerating spent schwertmannite via a heterogeneous Fenton-like reaction to degrade adsorbed phenanthrene and meanwhile oxidize adsorbed As(III). The results suggested that schwertmannite with a hedgehog-like morphology was superior to that with a smooth surface for the adsorption removal of As(III) or phenanthrene because of the much higher BET surface area and hydroxyl proportion of the former one, and schwertmannite formed at 72 h incubation effectively co-adsorbed As(III) and phenanthrene from water solution. The adsorption of As(III) and phenanthrene on schwertmannite did not interfere with each other, while the acidic initial solution pH delayed the adsorption of As(III) on schwertmannite but enhanced the adsorption capacity for phenanthrene. The adsorption of As(III) on schwertmannite mainly involved its exchange with SO 4 2− (outer-sphere or inner-sphere) and its complexation with iron hydroxyl surface groups, and phenanthrene adsorption mainly occurred through cation-π bonding and OH-π interaction. During the adsorption-regeneration processes, schwertmannite adsorbed As(III) and phenanthrene firstly, and then it can be successfully regenerated via Fenton-like reaction catalyzed by itself to effectively degrade the adsorbed phenanthrene and meanwhile oxidize the adsorbed As(III) to As(V). Therefore, schwertmanite is an outstanding environmental adsorbent to decontaminate As(III) and phenanthrene co-existing in groundwater.
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Nanomaterials
·
2023
·Vol. 13
·期 16
·2288
·
IF 5.3
Haibing Hu,Yunhu Hu,Baozhu Xie,Jianxiong Zhu
Currently, heavy metal ion pollution in water is becoming more and more common, especially As (III), which is a serious threat to human health. In this experiment, a glassy carbon electrode modified with Fe3O4/MoS2nanocomposites was used to select the square wave voltammetry (SWV) electrochemical detection method for the detection of trace As (III) in water. Scanning electron microscopy (SEM) and X-ray diffraction (XRD) showed that Fe3O4nanoparticles were uniformly attached to the surface of MoS2and were not easily agglomerated. Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) showed that Fe3O4/MoS2has higher sensitivity and conductivity. After optimizing the experimental conditions, the Fe3O4/MoS2-modified glassy carbon electrode exhibited high sensitivity (3.67 μA/ppb) and a low detection limit (0.70 ppb), as well as excellent interference resistance and stability for As (III).
研究领域:
环境科学
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分析化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ying Fang,Qianwen Liu,Yang Song,Feiyue Jia,Ying Yang,Haipu Li
Dissolved organic matter (DOM) extensively exists in high-arsenic groundwater with relatively high concentration, which could not only compete with arsenic for adsorption sites, but also depress As(III) oxidation in persulfate-based advanced processes (PS-AOPs) through scavenging free radicals (SO 4 • − and •OH). In order to effectively avoid the negative effect of DOM , an Fe/Co bimetallic metal–organic framework (Fe/Co MOF)-coupled peroxymonosulfate (Fe/Co MOF-PMS) system was rationally constructed for non-radical-dominated As(III) oxidation and chemisorption-driven As(V) adsorption. Results showed that the Fe/Co MOF-PMS system did realize anti-interference As(III) immobilization in DOM-rich high-arsenic groundwater, which was evidenced by no difference in As(III) immobilization efficiencies in the absence and presence of 20 mg/L humic acid (HA). During the oxidation process, 1 O 2 dominated As(III) oxidation while O 2 • − dominated HA oxidation, and the presence of HA significantly promoted the generation of 1 O 2 besides SO 4 • − and •OH. During the adsorption process, chemical adsorption mainly drove As(V) adsorption such as forming M-O-As (M = Fe, Co) bond, while physical adsorption forces played a major role in HA adsorption, such as π-π interaction, hydrogen bonding, and electrostatic attraction. The synergism of oxidation and adsorption processes made the anti-interference As(III) immobilization in DOM-rich high-arsenic groundwater in Fe/Co MOF-PMS system come true. This work is believed to shed light on the highly efficient purification of DOM-rich high-arsenic groundwater.
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高影响因子
JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
·
2026
·
IF 2.2
Rimsha Toor,Abdul Sattar,Uzair Ahmad,Shams ur Rahman,Shahzad Hussain,Fozia Bibi,Muhammad Waseem
Arsenic ranks first among the carcinogenic 1 group of heavy metals. Various techniques have been employed to remove the contaminants from aqueous media, with adsorption being the most suitable. For this purpose, the emerging material, MXene and its functionalized forms with calcium ferrites and magnesium ferrites have been used. The hydrothermal method was adopted for the synthetic purposes. For structure, morphology, magnetic behavior, surface area and functional group determination, X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, vibrating sample magnetometer, Barrett–Joyner–Halenda, and Fourier transform infrared spectroscopy were employed. For adsorption studies, batch tests were conducted with the effects of pH, contact time, temperature, and concentration. The pseudo-second-order kinetics (R2 ≈ 0.98), along with Langmuir and Freundlich isotherms (R2 ≈ 0.98) were found well fitted to the experimental data. Among the synthesized adsorbents, MXene, MXene functionalized with calcium ferrite, and MXene functionalized with magnesium ferrite demonstrated monolayer adsorption capacities of 1829, 4399, and 4631 µg/g, respectively. Ultimately, the reusability of materials was investigated through desorption analyses.
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CHEMOSPHERE
·
2023
·
IF 8.8
Qianting Xu,Fengping Zhou,Qingxin Yu,Ye Xiao,Xinyi Jiang,Weihua Zhang,Rongliang Qiu
In the Pearl River Delta of China, many sites are likely contaminated with aniline in the soil and arsenic (As) in the groundwater because of a high As background level and the prevailing printing and dyeing industry. This study is to explore the remediation performance of thermally activated persulfate oxidation for the sites with these two contaminants, aniline and As. The As influence on the aniline degradation and vice versa are also systematically investigated. When the molar ratio of aniline to persulfate is 1: 4.65, over 85% of aniline can be degraded at 40 °C in 24 h, and 100 μg L −1 As(III) in solution can be completely adsorbed by the soil. A higher pH favored the aniline degradation but disfavored the As(III) oxidation. Due to the strong buffer capacity of the soil, aniline in the soil could be more quickly degraded than those in the solution. The As(III), however, seem more easily oxidized in the absence of soil. The coexisting Fe 2+ can substantially improve As(III) oxidation and immobilization, although the dilute Fe 2+ solution may suppress the aniline degradation. The presence of aniline severely inhibited the As(III) oxidation and adsorption, likely due to the competition for the generated free radicals and the adsorption sites on the soils. In contrast, the existing As(III) has a slight effect on aniline degradation. These findings are believed to provide the theoretical basis for the remediation of aniline-arsenic contaminated sites.
研究领域:
环境科学
·
污染修复
·
化学工程
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高影响因子
ANALYTICA CHIMICA ACTA
·
2023
·
IF 6.2
Zhongxin Zhuang,Jiawei Xu,Yan Chen,Zheng Guo,Zhonggang Liu,Xingjiu Huang
The highly toxic arsenite (As(III)) could cause serious cytotoxicity on metabolism, resulting in several diseases. However, it is still a great challenge on the precise sensing of As(III) in complicated conditions, especially in cellular environment. In this work, a nanoporous gold microelectrode (NPG-μE) was fabricated by a simple electrochemical alloying/dealloying method and developed for the electroanalysis of As(III) in the lung cancer cellular (A549 cells) environment. The as-fabricated NPG-μE exhibited the excellent electrochemical performance towards As(III) detection at physiological pH (0.1 M PBS solution , pH 7.4) with a high sensitivity of 5.07 μA ppb −1 cm −2 and a low limit of detection of 0.25 ppb (S/N = 3). The large surface area derived from the nanoporous structure, and the well-dispersed active sites as well as the highly electro-catalytic activity of gold played a critical role on the improved electrochemical behaviors. Furthermore, the effect of the exposure time on electrochemical monitoring As(III) in A549 cellular environment was successfully investigated, revealing the fatal impact of As(III) on cell cycle. This work offered a great trial on investigating of the cytotoxicity of arsenite and their precise detection in complicated cellular environment.
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Materials
·
2022
·Vol. 15
·期 20
·7156
·
IF 3.748
Huimei Shan,Yunquan Liu,Chunya Zeng,Sanxi Peng,Hongbin Zhan
A magnetite graphene oxide chitosan (MGOCS) composite microsphere was specifically prepared to efficiently adsorb As(III) from aqueous solutions. The characterization analysis of BET, XRD, VSM, TG, FTIR, XPS, and SEM-EDS was used to identify the characteristics and adsorption mechanism. Batch experiments were carried out to determine the effects of the operational parameters and to evaluate the adsorption kinetic and equilibrium isotherm. The results show that the MGOCS composite microsphere with a particle size of about 1.5 mm can be prepared by a straightforward method of dropping FeCl2, graphene oxide (GO), and chitosan (CS) mixtures into NaOH solutions and then drying the mixed solutions at 45 °C. The produced MGOCS had a strong thermal stability with a mass loss of <30% below 620 °C. The specific surface area and saturation magnetization of the produced MGOCS was 66.85 m2/g and 24.35 emu/g, respectively. The As(III) adsorption capacity (Qe) and removal efficiency (Re) was only 0.25 mg/g and 5.81% for GOCS, respectively. After 0.08 mol of Fe3O4modification, more than 53% of As(III) was efficiently removed by the formed MGOCS from aqueous solutions over a wide pH range of 5–10, and this was almost unaffected by temperature. The coexisting ion of PO43−decreasedQefrom 3.81 mg/g to 1.32 mg/g, but Mn2+increasedQefrom 3.50 mg/g to 4.19 mg/g. The As(III) adsorption fitted the best to the pseudo-second-order kinetic model, and the maximumQewas 20.72 mg/g as fitted by the Sips model. After four times regeneration, theRevalue of As(III) slightly decreased from 76.2% to 73.8%, and no secondary pollution of Fe happened. Chemisorption is the major mechanism for As(III) adsorption, and As(III) was adsorbed on the surface and interior of the MGOCS, while the adsorbed As(III) was partially oxidized to As(V) accompanied by the reduction of Fe(III) to Fe(II). The produced As(V) was further adsorbed through ligand exchange (by forming Fe–O–As complexes) and electrostatic attraction, enhancing the As(III) removal. As an easily prepared and environmental-friendly composite, MGOCS not only greatly adsorbs As(III) but also effectively removes Cr(VI) and As(V) (Re> 60%) and other metals, showing a great advantage in the treatment of heavy metal-contaminated water.Keywords:chitosan;graphene oxide;magnetite;As(III) removal
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