JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Zhengyuan Zhou,Jingyao Huang,Guilu Zeng,Rumin Yang,Zhiqiang Xu,Mudassir Habib,Qian Sui,Shuguang Lyu
The application of S(IV) for the regeneration of Fe(II) has been widely investigated. As the common S(IV) sources, sodium sulfite (Na 2 SO 3 ) and sodium bisulfite (NaHSO 3 ) are soluble in the solution, resulting in excessive SO 3 2− concentration and redundant radical scavenging problems. In this research, calcium sulfite (CaSO 3 ) was applied as the substitution for the enhancement of different oxidant/Fe(II) systems. The advantages of CaSO 3 could be summarized as follows: (1) it could sustainedly supplement SO 3 2− for Fe(II) regeneration, preventing radical scavenging and unnecessary reagent waste; (2) the cost and toxicity of CaSO 3 were extremely lower than that of other S(IV) sources; (3) the concentration of reactive species increased in the presence of CaSO 3 ; and (4) after the reaction, SO 4 2− would form CaSO 4 precipitate, which would not increase the burden of SO 4 2− in the solution. In the participation of CaSO 3 , the removal of trichloroethylene (TCE) and other organic contaminants were significantly promoted and different enhanced systems had high tolerance on complex solution conditions. The major reactive species in different systems were determined through qualitative and quantitative analyses. Eventually, the dechlorination and mineralization of TCE were measured and the differentiated degradation pathways in different CaSO 3 -enhanced oxidants/Fe(II) systems were elucidated.
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CHEMOSPHERE
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2023
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IF 8.8
Chunsheng Ding,Xinze Song,Zhongyi Zheng,Hainan Wang,Yuqiang Pan,Hangtian Zhang,Xueyan Li,Jing Deng
Fe(II)-catalyzed PMS process was widely used in the degradation of refractory pollutants in wastewater, while its performance was restricted by the slow regeneration efficiency of Fe(II). Herein, caffeic acid (CFA), a representative of hydroxycinnamic acids, was introduced into Fe(III)/PMS system to accelerate the transformation of Fe(III) to Fe(II) and promote the removal of bisphenol A (BPA). Under optimum condition of 0.1 mM CFA, 0.05 mM Fe(III), and 0.5 mM PMS, almost complete removal of BPA can be achieved within 20 min, which was roughly 6.2 times higher than that in Fe(III)/PMS system. As the addition of CFA into Fe(III)/PMS system, pH application range was widened from acidic to alkaline conditions. The reduction and chelation of CFA expedited the Fe(III)/Fe(II) cycle by forming CFA-Fe chelate, thereby facilitating the PMS activation . Based on LC-MS analysis and DFT calculation, the intermediate products of CFA were found to play a decisive role in boosting the regeneration of Fe(II), and the toxicity of these intermediates towards organisms was evaluated by ECOSAR . The alcohol-scavenging and chemical probe tests certified that hydroxyl radical (•OH), sulfate radical (SO 4 •- ), and Fe(IV) coexisted in Fe(III)/CFA/PMS system, and the second-order reaction rate constants of •OH and SO 4 •- reacted with CFA were calculated to be 3.16✕10 9 and 2.30✕10 10 M −1 s −1 , respectively. Two major degradation pathways of BPA, •OH addition and SO 4 •- induced hydroxylation reaction, were proposed. This work presented a novel green phenolic compound that expedited the Fe(II)-catalyzed PMS activation process for the treatment of organic contaminants .
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WATER RESEARCH
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2022
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IF 13.4
Haolin Xu,Rundong Chen,Sheng Liang,Zhenchao Lei,Wenxiao Zheng,Zhang Yan,Jianxin Cao,Chaohai Wei,Chunhua Feng
The formation of chlorinated byproducts represents a significant threat to the quality of the effluent treated using electrochemical advanced oxidation processes (EAOPs), thus spurring investigation into alleviating their production. This study presents a new strategy to minimize the release of chlorinated intermediates during the electrochemical oxidation of Ni-EDTA by establishing a dual mixed metal oxide (MMO)/Fe anode system. The results indicate that the dual-anode system achieved a substantially higher rate (0.141 min − 1 ) of Ni-EDTA destruction and accordingly allowed a more pronounced removal of aqueous Ni (from 39.85 to 0.63 mg L − 1 ) after alkaline precipitation, compared with its single MMO anode (0.017 min − 1 of Ni-EDTA removal, with 14.38 mg L − 1 Ni remaining) and single Fe anode (insignificant Ni-EDTA removal, with 38.37 mg L − 1 Ni remaining) counterparts. Compared to reactive chlorine species (RCS) produced from the single MMO anode system, Fe(IV) was in situ generated from the dual-anode system and was predominantly responsible for the attenuation of chlorinated byproducts and thus the decrease in the acute toxicity of the treated solution (evaluated using luminescent bacteria). The Fe(IV)-dominated dual-anode system also exhibited superior performance in removing multiple pollutants (including organic ligands, Ni, and phosphite) in the real electroless plating effluent. The findings suggest that the strategy for Fe(II) transition to Fe(IV) by active chlorine paves a new avenue for yielding less chlorinated products with lower toxicity when EAOPs are used to treat chloride-containing organic wastewater.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2023
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IF 9.8
Wangjun Lin,Linfeng Peng,Hui Li,Tangfu Xiao,Jianqiao Wang,Nana Wang,Xiangting Zhang,Hanmo Zhang
Fe(II)-induced phase transformations of secondary iron minerals have attracted considerable attention due to their influence on antimony (Sb) mobility. However, Fe(II)-induced natural multicomponent secondary iron mineral (nmSIM) transformations and the corresponding repartitioning of Sb on nmSIM under acidic conditions upon Fe(II) exposure have not been systematically examined. Herein, we investigated the effect of Fe(II) on nmSIM mineralogy and Sb mobility in Sb(V)-bearing nmSIM at pH 3.8 and 5.6 at various Fe(II) concentrations over 15 d. The Sb(V)-bearing nmSIM phase transformation occurred under both strongly and weakly acidic conditions without Fe(II) exposure, while the presence of Fe(II) significantly intensified the transformation, and substantial amounts of intermediary minerals, including jarosite , ferrihydrite , lepidocrocite and fougerite, formed during the initial reaction stage, especially at pH 5.6. X-ray diffraction (XRD) analyses confirmed that goethite and hematite were the primary final-stage transformation products of Sb(V)-bearing nmSIM, regardless of Fe(II) exposure. Throughout the Sb(V)-bearing nmSIM transformation at pH 3.8, Sb release was inversely related to the Fe(II) concentration in the initial stage, and after maximum release was achieved, Sb was gradually repartitioned onto the nmSIM. No Sb repartitioning occurred in the absence of Fe(II) at pH 5.6, but the introduction of Fe(II) suppressed Sb release and improved Sb repartitioning on nmSIM. This transformation was conducive to Sb reimmobilization on Sb(V)-bearing nmSIM due to the structural incorporation of Sb into the highly crystalline goethite and hematite generated by the Sb(V)-bearing nmSIM transformation, and no reduction of Sb(V) occurred. These results imply that Fe(II) can trigger mineralogical changes in Sb(V)-bearing nmSIM and have important impacts on Sb partitioning under acidic conditions. These new insights are essential for assessing the mobility and availability of Sb in acid mine drainage areas.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Yang Zhang,Zhenglei Li,Dongqing Yan,Hongxia Chen,Meng Zhang,Jun Wang,Guang Yang
In this work, Fe(II)/Peroxymonosulfate (PMS) treatment with dual functionality of pre-oxidation and coagulation was applied to enhance the removal of alkali lignin in water. The removal efficiency of alkali lignin (2 g/L) could reach ∼ 99% at an optimal dosage of [Fe(II)] = 2.4 mM and [PMS] = 7.8 mM, which was efficiently superior than that using ferric and polymeric coagulant individually. Pre-oxidation, involving hydroxyl radical (•OH) and sulfate radical (SO 4 •− ), has been demonstrated to play a crucial role in both oxidative degradation (∼30%) and reducing the molecular weight and hydrophilicity of lignin. Meanwhile, the formation of polynuclear Fe-hydroxide complexes was also fostered, which in turn greatly contribute to the removal of lignin through an enhanced coagulation mechanism. The reductive units present in alkali lignin was demonstrated to initiate a dynamic transition between Fe(III) and Fe(II) by donating electrons. This redox activity is anticipated to continuously promote the formation of electro-neutral and loose flocs, thereby resulting in an enhanced coagulation performance. Furthermore, ultrafiltration (UF) was also demonstrated as a viable liquid/solid separation method following Fe(II)/PMS treatment, effectively promoting membrane flux recovery rate to ∼90%. This highlights the remarkable potential of this method when combined with other treatment processes. This study aims to offer a complementary strategy for remediating alkali lignin wastewater while advancing the fundamental understanding of redox-reaction enhanced in-situ coagulation in water treatment applications.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Junlei Zhang,Wei Zhao,Zhi Li,Gang Lu,Mingshan Zhu
Advanced oxidation processes involving the visible-light-assisted peroxymonosulfate (PMS) are emerging as promising approaches for treating antibiotic pollutants. Here, Fe(II)/V(IV) self-doped FeVO 4 nanobelts were synthesized and employed to build a visible-light-assisted PMS activation system for degrading antibiotic sulfamethoxazole (SMX). Compared with PMS/FeVO 4 , PMS/Visible light (VL), or PMS system, the PMS/FeVO 4 /VL system showed 3.9, 14.0, or 14.1 times improved for the removal of SMX, respectively. The reason behind this is the organic combination of the VL photocatalysis and transformation of Fe(II)/V(IV) to Fe(III)/V(V) over FeVO 4 , namely when photocatalytic behavior over FeVO 4 can produce electrons (e - ) and holes (h + ) to activate PMS or directly degrade SMX, the transformation of Fe(II)/V(IV) to Fe(III)/V(V) will also happen to donate some e - for PMS activation simultaneously. Such a system can also effectively remove SMX from actual water bodies such as medicine wastewater, river water, tap water, and rainwater. This work not only provides an effective system for treating SMX polluted wastewater, but also gives some new insights to understanding the mechanism involving Fe-based binary metal oxide activating peroxymonosulfate.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Cong Gao,Yan Su,Xie Quan,Virender K. Sharma,Shuo Chen,Hongtao Yu,Yaobin Zhang,Junfeng Niu
Heterogeneous Fenton-like reaction was a promising approach for generating •OH. However, the heterogeneous catalysts generally exhibited low activity because of slow reduction of Fe(III) in Fe(III)/Fe(II) redox cycle. Here, decreasing electron density was expected to quicken Fe(III) reduction and consequently enhance the catalytic activity of heterogeneous catalysts. This hypothesis was validated by the enhanced hydroxyl radicals generation and accelerated Fe(III) reduction on MIL-88B(Fe)-X (2-X-terephthalic acid, X = NH 2 , CH 3 , H, Br and NO 2 ) by reducing electron density of Fe(III) with substituent of higher electrophilicity. MIL-88B(Fe)-NO 2 , with the substituent of highest electrophilicity among these catalysts, has the lowest electron density of Fe(III) and highest redox potential ( E Fe(III)/Fe(II) = 0.35 V). As a result, it exhibited the best catalytic performance, which was 1.7–20 times higher than that for other MIL-88B(Fe)-X and was comparable to that of homogeneous Fe 2+ . This study provides scientific basis for rational construction of highly effective heterogeneous Fenton-like catalyst.
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SENSORS AND ACTUATORS B-CHEMICAL
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2019
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IF 6.393
Ning Xia,Dehua Deng,Xiangsheng Mu,Ang Liu,Jiaxun Xie,Dandan Zhou,Ping Yang,Yun Xing,Lin Liu
This work reported a novel redox cycling in which pyrroloquinoline quinone (PQQ) promoted the reduction of Fe(III)-ferrozine by tris(2-carboxyethyl)phosphine (TCEP). Specifically, PQQ was reduced into pyrroloquinoline quinol (PQQH 2 ) by TCEP, and then the produced PQQH 2 reduced colorless Fe(III)-ferrozine into dull red Fe(II)-ferrozine. The redox cycling was employed for development of colorimetric immunosensors through the generation of colorful Fe(II)-ferrozine. Mesoporous silica nanoparticle (MSN) was used as the carrier for both PQQ and recognition antibody through electrostatic interactions. Magnetic bead (MB) was used as the support for the immobilization of capture antibody. After the sandwich-type immunoreactions and magnetic separation, the MSN-PQQ nanolabels on the MB surface triggered the production of Fe(II)-ferrozine. The limit of detection was found to be 1 pg/mL with prostate specific antigen (PSA) as the model target. The result for the analysis of serum sample is in agreement with that achieved by the commercial enzyme-linked immunosorbent assay kits. The proposed immunosensor obviated the use of enzyme molecules for signal amplification and did not require expensive instruments for signal readout. This work should be valuable for the design of novel nanolabels and the proposed sensing strategy by the redox cycling could be applied to develop more sensitive biosensors.
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Yunfei Xue,Qian Sui,Mark L. Brusseau,Xiang Zhang,Zhaofu Qiu,Shuguang Lyu
Calcium peroxide (CaO 2 ) is a stable hydrogen peroxide (H 2 O 2 ) carrier, and the CaO 2 /Fe(II) system has been applied for treatment of various pollutants. It is commonly reported in the literature that hydroxyl radical (HO ) and superoxide radical anions (O 2 − ) are the two main reactive oxygen species (ROSs) generated in the CaO 2 /Fe(II) system. However, many of the reported results were deduced from degradation performance rather than specific testing of radical generation. Thus, the specific generation of ROSs and the influence of system conditions on ROSs yield are still unclear. To our knowledge, this is the first study specifically focusing on the generation of HO and O 2 − in the CaO 2 /Fe(II) system. Experimental conditions were optimized to investigate the production of HO and O 2 − . The results showed the influences of CaO 2 , Fe(II), and solution pH on HO and O 2 − generation, and the HO generation efficiency was reported for the first time. In addition, the ROSs generation pathways in the CaO 2 /Fe(II) system were elucidated. A strategy for enhancing HO yield is developed, based on the continuously dosing Fe(II). This proposed strategy has implications for the effective application of in situ chemical oxidation employing CaO 2 /Fe(II) for groundwater remediation.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Lingjie Liu,Shaoqing Mo,Shaopo Wang,Jing Chang,Jianhui Zhao,Jingjie Yu
Low temperatures were a critical factor that inhibited anaerobic ammonium oxidizing bacteria (AnAOB) activity. This study demonstrated the effect of exogenous zero-valent iron (ZVI) on Anammox-hydroxyapatite (HAP) system at 17°C. The results showed that long-term addition of ZVI increased the system nitrogen removal efficiency by 8.59% and alleviated the inhibition of AnAOB by low temperature. After addition of ZVI, the activity of AnAOB and the heme c content increased by 58.20% and 4.83%, respectively. Moreover, the functional enzyme activities of NIR, HZS, and HZO increased by 94.12%, 36.36%, and 16.67%, respectively. The concentrations of quorum sensing molecules, i.e., C 6 -HSL and C 8 -HSL, increased by 191.17% and 41.54%, respectively, after ZVI addition. Metagenomic analysis revealed that the addition of 5 g/L ZVI stimulated the relative abundance relative abundance of Fe(II) metabolism-related genes in AnAOB at 17 °C, thereby contributing to the uptake, transport, utilization, and storage of Fe(II). The addition of ZVI could improve the nitrogen removal performance of the anammox-HAP system at the low temperature.
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ENVIRONMENTAL RESEARCH
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2025
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IF 7.7
Dawei Gao,Haixiang Wang,Qiaoli Lu,Chao Ye,Jingsheng Cai,Lili Wang
Antibiotics, widely used to treat bacterial infections and as agricultural feed additives, pose significant environmental threats due to their persistence, particularly sulfamethoxazole (SMX), which is frequently detected in various ecosystems. Traditional wastewater treatment methods are often ineffective in their removal. This study presents a cost-effective three-dimensional CCF@MoS 2 @GA-Fe (CMGF) catalyst, with cotton fabric as a support to enhance peroxymonosulfate (PMS) activation in advanced oxidation processes (AOPs). Findings indicates that Mo(IV) active sites in CMGF significantly enhanced electron transfer and redox cycling of Fe(II)/Fe(III), ensuring sustained PMS activation and achieving approximately 3.8 times higher degradation efficiency compared to non-catalytic processes. After five cycles, CMGF retains its high catalytic activity. Key active species during PMS activation include singlet oxygen ( 1 O 2 ), hydroxyl radicals (•OH), and sulfate radicals (SO 4 − •). This research elucidates the catalytic mechanisms and degradation pathways of the CMGF/PMS system, highlighting its potential for removing organic pollutants from water.
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Journal of Materials Chemistry C
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2024
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IF 5.7
Xiaomeng Sun,Xinfeng Cheng,Xiya Chen,Hongwei Wang,Qian Zhao,Chunxia Yang,Xianchao Du,Xiaojing Xing,Dongfang Qiu
A novel three-arm terpyridine ligand L with flexible methylenoxyl (–CH2–O–) groups was synthesized by a one-step chemical reaction, and the uniform two-dimensional supramolecular films with various sizes and thicknesses were simply prepared on the surface of indium tin oxide (ITO) conductive glass by an Fe2+-induced self-assembly method at the dichloromethane–water interface. The morphology, structure and composition were confirmed by ultraviolet-visible (UV-vis) absorption spectroscopy, scanning electron microscope/energy dispersive spectrometer (SEM/EDS), Fourier transform infrared (FT-IR) spectroscopy, and X-ray photoelectron spectroscopy (XPS), respectively. The sandwiched solid-state devices (1.3 × 1.4 cm2), fabricated by employing L-Fe film coated ITO as the electrochromic layer and LiClO4/poly(methyl methacrylate) (PMMA)/propylene carbonate (PC)/CH3CN based gel as the supporting electrolyte, showed a reversible color change from purple to light yellow with the optical contrast (ΔT%) of 56.6%, the coloring and bleaching times of 3.9 s and 3.7 s, and the coloring and bleaching efficiencies of 875.2 cm2 C−1 and 182.3 cm2 C−1 under the applied double-step voltages of −2.0 V and +3.0 V. The device had good stability, maintaining 70% of its initial optical contrast after 500 cycles. Meanwhile, a large-sized solid-state device with an active area of 7 × 7 cm2 showed its application potential in smart windows or displays.
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