JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Jin Liu,Hongyu Chen,Chaosheng Zhu,Songfang Han,Jun Li,Sijia She,Xiaoyong Wu
Advanced oxidation processes (AOPs) based on photo-Fenton reaction has been widely used in refractory organic wastewater treatment . However, the mineralization rate and H 2 O 2 utilization in AOPs is relatively low. Herein, a photothermal-assisted photocatalytic-Fenton-like process with CuO x /γ-Al 2 O 3 catalyst was designed to solve the above issues. The utilization rate of H 2 O 2 and mineralization rate of tetracycline hydrochloride (TC) in the 3%-CuO x /γ-Al 2 O 3 /H 2 O 2 /full spectrum light system were significantly increased to 72.0% and 74.3%, respectively, which were ascribed to the synergy of photothermal effect and photocatalytic-Fenton-like reaction. During the simultaneous removal of TC and Cr(VI), the reaction efficiency of 3%-CuO x /γ-Al 2 O 3 /H 2 O 2 /light system was much higher than that of 3%-CuO x /γ-Al 2 O 3 /H 2 O 2 system. In addition, the 3%-CuO x /γ-Al 2 O 3 /H 2 O 2 /light system was not only active in wider pH range (3–9), but also effective in various organic pollutants and Cr(VI) coexisted solutions as well as different water conditions. More importantly, a possible photothermal-assisted photocatalytic-Fenton-like reaction mechanism for the simultaneous removal of TC and Cr(VI) in the CuO x /γ-Al 2 O 3 /H 2 O 2 /light system was proposed. This work may pave a new way for efficient simultaneous removal of refractory organic pollutants and heavy metals in wastewater.
研究领域:
环境科学
·
废水处理
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Linlin Su,Wei Hu,Xiaolun He,Chao Chen,Min Xu,Xiaoyu Yu,Yan Liu,Gang Yang,Lulu Long
Nanoconfinement is one of the effective strategies to improve the decontamination performance of nanomaterials in Fenton-like reactions. However, conventional nanoconfinement relying on nanotubular architectures suffers from segregated confinement of oxidants or pollutants, failing to establish directional interaction pathways between reactive species and target contaminants. To address this, we designed a hierarchical nanoconfinement strategy using Fe₃O 4 /H₂O₂ system, enabling the simultaneous confinement of both oxidants and pollutants. First, a SiO₂ layer was coated onto Fe₃O₄ and converted into a MnSiO₃ shell, which selectively adsorbed tetracycline (TC), ensuring pollutant confinement. Next, the cavity size was precisely tuned by controlling the SiO₂ interface thickness, spatially restricting H₂O₂ and enhancing bound ·OH generation. This synergistic nanoconfinement mechanism improved the effective contact between active species and contaminants while eliminating active site competition. Compared to the Fe₃O₄/H₂O₂ system, the Fe₃O₄@MnSiO₃/H₂O₂ catalyst exhibited a 1.7-fold increase in TC degradation rate and a 60 % enhancement in TOC removal efficiency. Moreover, it demonstrated robust performance in real aquaculture wastewater, sustained catalytic stability, and effective elimination of TC’s antibacterial activity. This work not only advances nanoconfinement strategies but also offers a new paradigm for optimizing nanoconfined materials to enhance catalytic microenvironments.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Yujia Yang,Lejin Xu,Wuyang Li,Weijie Fan,Shuang Song,Jun Yang
Fe-based heterogeneous Fenton-like catalysts has shown tremendous potential for wastewater treatment, but the investigation of adsorption, reduction and oxidation mechanism remains challenging. In this study, nanoscale zero-valent iron encapsulated in three-dimensional graphene network (3D-GN@nZVI) was synthesized and characterized as a heterogeneous Fenton-like catalyst via the activation of dissolved oxygen (DO) for adsorption and degradation of sulfadiazine (SDZ). 3D-GN@nZVI had the synergistic effect of catalytic reactivity for sulfadiazine removal, which was evaluated in view of the effects of operational factors. The role of adsorption, reduction and oxidation was determined; in 3D-GN@nZVI/DO system, sulfadiazine was removed mainly by the attack of hydroxyl radicals ( OH). The possible degradation pathway of sulfadiazine was inferred by identifying reactive oxidizing species and degradation intermediates. According to the X-ray photoelectron spectroscopy (XPS) analysis, Fourier Transform infrared spectroscopy (FTIR) analysis and density functional theory (DFT) calculations, the distribution and transfer of electrons on the surface of 3D-GN@nZVI were illustrated, and the adsorption and oxidation mechanisms of sulfadiazine through DO-driven and micro-electrolysis-enhanced heterogeneous Fenton-like reaction were proposed. The comprehensive mechanism was elucidated to provide new insights to advance the DO-driven Fenton-like process and to inspire the development of nZVI and relevant composites.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2018
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IF 6.434
Lingshuai Kong,Guodong Fang,Ya Kong,Meng Xie,Vinothkumar Natarajan,Dongmei Zhou,Jinhua Zhan
Wastewater systems contain a large number of compounds, such as anthropogenic aromatic pollutants and natural organic matter (NOM), and usually have pH higher than 4. Fenton-like reaction is the most widespread method for removal of organic pollutants, but their reactivity with H 2 O 2 may be inhibited by NOM due to the competition of hydroxyl radicals and chelating agents. In this work, Cu 2 O@β-cyclodextrin was developed to achieve the collaboration between molecular recognition and Fenton-like catalysis to destruct aromatic pollutants at neutral pH. In Cu 2 O@β-CD, covalent Cu O C bond was topotaxially converted from CuCl assisted by β-CD at room temperature. Covalently linked β-CD could keep humic acid from interfering catalytic performance of Cu 2 O surfaces and inhibit the leaching of copper. A higher catalytic ability was observed for Cu 2 O@β-CD with rate constant 0.0331 min −1 than Cu 2 O (0.0064 min −1 ) at neutral pH. A mechanism of synergistic catalysis was proposed on the basis of Cu + , β-CD and phenoxo-Cu 2+ complexes in the Cu 2 O@β-CD/BPA/H 2 O 2 system. The strategy of coupling molecular recognition into Fenton-like reaction provides an efficient and promising approach to the destruction of aromatic pollutants at neutral pH.
研究领域:
环境科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
Advanced Science
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2021
·Vol. 8
·期 22
·2101824
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IF 16.806
Jun Wang,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Wenchao Peng
Fenton-like reactions with persulfates as the oxidants have attracted increasing attentions for the remediation of emerging antibiotic pollutions. However, developing effective activators with outstanding activities and long-term stabilities remains a great challenge in these reactions. Herein, a novel activator is successfully synthesized with single iron atoms anchored on porous N-doped carbon (Fe-N-PC) by a facile chemical vapor deposition (CVD) method. The single Fe atoms are coordinated with four N atoms according to the XANES, and the Fe-N 4 -PC shows enhanced activity for the activation of peroxymonosulfate (PMS) to degrade sulfamethoxazole (SMX). The experiments and density functional theory (DFT) calculations reveal that the introduction of single Fe atoms will regulate the main active sites from graphite N into Fe-N 4 , thus could enhance the stability and tune the PMS activation pathway from non-radical into radical dominated process. In addition, the N atoms connected with single Fe atoms in the Fe-N 4 -C structure can be used to enhance the adsorption of organic molecules on these materials. Therefore, the Fe-N 4 -C here has dual roles for antibiotics adsorption and PMS activation. The CVD synthesized Fe-N 4 -C shows enhanced performance in persulfates based Fenton-like reactions, thus has great potential in the environmental remediation field.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Yi Ren,Jinyan Yu,Jingyue Zhang,Lu Lv,Weiming Zhang
Iron-copper bimetals for Fenton-like catalysis were developed, due to efficient enhancement of catalytic activity by iron-copper synergy. However, deviation exists in mechanism analysis of multi-effect catalysis. In this study, a new in-situ strategy of shielding Fe(II) and Cu(I) from further reaction by trapping agents was developed, for analysis of iron catalysis alone, copper catalysis alone and synergistic effect in bimetallic catalyst systems. Inhibition efficiency and influence of trapping agents on Fe(II)/Cu(I) catalysis were quantitatively evaluated for reliability confirmation and method correction. The possible application scope was identified as pH of 4–6, and this strategy was available for analysis of five different groups of catalysts. The potential superiority and difference of the proposed strategy compared with current ex-situ strategy were also analyzed. The overestimation (12.1%–35.4%) of copper catalysis and biased analysis (0.1%–12.6%) of iron catalysis by ex-situ strategy can be alleviated, thereby improving accuracy for synergistic effect. In summary, this study proposed a new strategy to improve the understanding of iron-copper bimetallic catalysis, which can provide reference for other polymetallic catalysis analysis development.
研究领域:
环境科学
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化学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Zhongmou Liu,Pan Zhang,Xiangyu Zhao
Reduced graphene oxide supported with ferric ion (Fe(III)-rGO) was successfully prepared, and performed as an excellent catalyst to activate hydrogen peroxide (H 2 O 2 ) and peroxymonosulfate (PMS) for isoprothiolane (IPT) degradation. IPT removal efficiency was proven to be better in the Fe(III)-rGO/H 2 O 2 /PMS system (96.2%) than in the Fenton-like reaction (72.6%) and PMS-AOP (80.0%) individually. X-ray photoelectron spectroscopy showed that Fe(III) was reduced in Fenton-like reaction, and the reduced Fe(II) played a crucial role in the subsequent PMS-AOP. The combination of the Fenton-like reaction and PMS-AOP involved the valence state conversion of Fe, which consequently improved Fe(III)-rGO utilization rate and IPT removal efficiency. Fe(III)-rGO remarkably boosted the Fe(III)/Fe(II) cycle and generated superoxide radical (O 2 − •) and singlet oxygen ( 1 O 2 ) in the Fe(III)-rGO/H 2 O 2 /PMS system. Fe(III)-rGO acts as the electron transfer mediator; thus, promoting electron transfer from IPT to H 2 O 2 and PMS and accelerating the generation of active species. Fe(IV) with high oxidation performance was formed in PMS-AOP and efficiently removed some of the IPT. IPT removal efficiency was more than 90% at a pH range of 3–11; this efficiency could be maintained above 50% even after five consecutive degradation experiments, exhibiting excellent stability and reusability of Fe(III)-rGO. Additionally, iron sludge formation was greatly reduced because of the stable chemical bonding of iron ions to the rGO surface. Therefore, this study provides a new multisystem and synergistic approach for the efficient removal of organic micro-pollutants from water.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
Fundamental Research
·
2023
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IF 6.2
Qian Hu,Taoyu Yang,Shanli Wang,Licong Xu,Minghua Wu,Deyou Yu,Kaixing Fu,Jinming Luo
Peracetic acid (PAA) has recently been considered a promising oxidant candidate for heterogeneous Fenton-like reactions; however, the main generation and contribution of organic radicals (R-O•) with unsatisfactory oxidation potential compromises wastewater decontamination efficiency. In this study, we demonstrate the rational design and synthesis of ultrafine FeO x nanocluster-anchored carbonaceous nanosheets (UFe-CN) for altering the PAA activation pathway from R-O• to •OH dominant process via in situ framework collapse carbonization of MIL-53(Fe). The constructed UFe-CN/PAA system effectively accelerated refractory micropollutant ( e.g. , p-nitrophenol (4-NP)) decomposition by the enhanced •OH formation (up to 65.24 μmol L − 1 ) under a wide pH range (3.0–9.0), outperforming the benchmark iron-based catalyst counterparts by 4.2–10.8 times. This outstanding Fenton-like catalytic activity of UFe-CN is primarily attributed to the significant improvement in electron mitigation, ca. 49 times higher than that of its MIL-53(Fe) counterpart, for interface catalysis reactions triggered by iron species cycling. Furthermore, to facilitate adaptive engineering, the organic pollutant removal efficiency could be easily tuned by varying several key treatment factors, including the initial pH, PAA concentration, and UFe-CN dosage. More importantly, the excellent practicality of UFe-CN/PAA was demonstrated by systematically evaluating the impact of the water matrix, catalyst regeneration capability, and wastewater treatment efficiency. Overall, this study provides a significant understanding of •OH-dominated PAA activation and an effective catalyst development paradigm to facilitate the practical application of PAA-based Fenton-like oxidation.
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
·
2024
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IF 7.7
Guangchao Si,Li Zhang,Jingfeng Gao,Jiachun Yang,Akira Miyazawa,Yongzhen Peng
Covalent organic framework (COF) catalytic photocatalysts mediating Fenton-like reactions have been applied to the treatment of organic dyes in printing and dyeing wastewater. However, the photocatalytic performance of original COF is often unsatisfactory. This study investigated the impact of porosity modification strategies on the performance of COF photocatalysts in mediating the removal of organic dyes via Fenton-like reaction. Porosity modification was achieved by increasing the concentration of acetic acid (HAc) catalyst during COF preparation. The modified TAPB-DMTA COF (12M COF) exhibited excellent adsorption and photocatalytic properties. The Fenton-like reaction mediated by 12M COF photocatalysis removed nearly 96% of malachite green (MG) within 20 min, with a rate constant of 0.091 min −1 , which was 2.9 and 6.5 times higher than that of g-C 3 N 4 and original COF under the same reaction conditions, respectively. Additionally, the modulation mechanism of porosity modification on COF photocatalysis was explored. The conduction band (CB) of COF was reduced from −0.14 eV to −0.38 eV after porosity modification, facilitating the generation of longer-lived O 2 •- in the reaction system, which was conducive to efficient MG removal. Anti-interference experiments showed that the photocatalytic Fenton-like reaction system based on 12 M COF was less affected by common anions, cations and dissolved organics, while maintaining a high MG removal rate in tap water, mid-water, secondary clarifier effluent and river water. In summary, porosity modification was an effective strategy to improve the catalytic performance of original COFs. This study presented an efficient metal-free photocatalyst modification strategy for the Fenton-like reaction while avoiding the production of toxic by-products during dye degradation.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
Catalysts
·
2019
·Vol. 9
·期 1
·85
·
IF 3.444
Pan Gao,Mengjie Hao,Yue He,Yuan Song,Shaoxia Yang
Fe2O3–ZrO2catalysts with different morphologies (nanoplates (HZNPs), nanorods (HZNRs), nanocubes (HZNCs), and nanotubes (HZNTs)) were prepared by a hydrothermal method to investigate the effect of the morphology on the catalytic performance in the Fenton-like reaction for sulfamethazine (SMT) degradation. The Fe2O3–ZrO2catalysts were characterized by scanning electron microscope (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Brunauer–Emmett–Teller (BET) analysis. The H2O2adsorption and the Fe2+density sites on the Fe2O3–ZrO2catalysts had a close relationship with the morphologies and exhibited an important effect on the ·OH formation in the Fenton-like reaction. Free ·OH radicals were the main oxidative species in the reaction, and the normalized ·OH concentration per surface area of the catalysts was 4.52, 2.24, 2.20, and 0.37 μmol/m2for HZNPs, HZNRs, HZNCs, and HZNTs, respectively. The Fe2O3–ZrO2catalysts with different morphologies showed good catalytic performance, and the order of SMT degradation was HZNPs > HZNRs > HZNCs > HZNTs. Total SMT removal was achieved in the Fenton-like reaction over HZNPs at pH 3.0 and 45 °C after 240 min.Keywords:Fenton-like reaction;hematite;structure-dependent reactivity;ZrO2;sulfamethazine
研究领域:
环境科学
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催化化学
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DOI
高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 6
·期 3
·1275-1283
·
IF 8.867
Rui Zhou,Ningfei Shen,Jian Zhao,Yu Su,Hejun Ren
Magnetic glutathione (GSH)-functionalized nanocomposites (Fe3O4@GSH) were synthesized via an oxidative polymerization method and characterized as a heterogeneous Fenton-like catalyst for 2,4-dichlorophenol (2,4-DCP) degradation at neutral pH (pH = 6.5). The performance of the composite was extensively investigated in terms of catalytic activity and factors (H2O2 dosage, catalyst loading, initial solution pH, and 2,4-DCP concentration) influencing 2,4-DCP degradation. Iron leaching, primary reactive oxidizing species, and catalyst reusability were also investigated. The results showed that the removal efficiency can reach up to 99% within 240 min in the presence of Fe3O4@GSH, whereas pure Fe3O4 cannot operate under the same circumstances. Hydroxyl radicals (˙OH) were found as the main reactive oxidizing species responsible for pollutant degradation, and the final removal efficiency still reached 94% after recycling three times. The role of GSH can be ascribed to the acceleration of iron leaching from the surface of Fe3O4 and collective action for H2O2. The Fe3O4@GSH catalyst may provide new insights into the Fenton-like process for enhancing contaminant degradation.
研究领域:
环境科学
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纳米材料科学
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催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2010
·
IF 4.144
Lejin Xu,Jianlong Wang
The removal of biocide 4-chloro-3-methyl phenol (CMP) was investigated by heterogeneous Fenton-like system using nanoparticulate zero-valent iron (nZVI) as catalyst. The properties of nZVI before and after reaction were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM). The effects of pH value, initial concentration of CMP, nZVI dose and hydrogen peroxide (H 2 O 2 ) concentration were determined. The experimental results showed that lower pH value and CMP concentration brought faster degradation rate. With the initial pH value of 6.1 and initial CMP concentration of 0.7 mM, the optimal dosage of reagents were 0.5 g nZVI/L and 3.0 mM H 2 O 2 . At pH 6.1, the degradation of CMP followed two-stage first-order kinetic that composed of an induction period (first-stage) and a followed rapid degradation stage (second-stage). According to the effects of scavengers n -butanol and KI, hydroxyl radicals ( OH), especially the surface-bounded •OH, had a dominant role in the oxidation of CMP. The degradation intermediates, carboxylic acids and chloride ion produced during the reaction process were monitored by high performance liquid chromatography (HPLC), liquid chromatography/mass spectrometry (LC/MS) and ion chromatography (IC). On the basis of these findings, the possible mechanistic steps of CMP degradation were proposed.
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
高影响因子
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