APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Runliang Zhu,Yanping Zhu,Haiyang Xian,Lixia Yan,Haoyang Fu,Gangqiang Zhu,Yunfei Xi,Jianxi Zhu,Hongping He
The generation of Fe(II) from Fe(III) is the rate-limiting step in the heterogeneous Fenton reaction, and accelerating this step is critical for enhancing the reaction efficiency and also the subject of extensive studies. In this work, the oxidized multi-walled carbon nanotubes (CNTs) were coupled with ferrihydrite (Fh) to synthesize novel and highly efficient heterogeneous Fenton catalysts (CNTs/Fh). Interestingly, the calculated apparent rate constants by 3%CNTs/Fh could reach ∼7.1 times as high as that by Fh, well in agreement with the accelerated decomposition rate of H 2 O 2 , as well as the enhanced generation rate of Fe(II) and hydroxyl radicals in the CNTs/Fh system. The density functional theory calculations and the cyclic voltammograms curves both well indicated that the Fe(III)/Fe(II) redox cycling on CNTs/Fh could be significantly enhanced during the Fenton reaction, from both dynamic (accelerating the electron transfer from H 2 O 2 to Fh) and thermodynamic (lowering Fe(III)/Fe(II) redox potential) aspects.
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Jiandong Guo,Husheng Jia,Aiqin Zhang,Zhen Pei,Man Luo,Jinbo Xue,Qianqian Shen,Xuguang Liu,Bingshe Xu
Iron-based MOFs have been considered as the candidate for Fenton-like reagents owing to their open pore size and uniformly dispersed Fe active centers. However, the strong coordination of metal ions with organic ligands greatly reduces the exposed active sites of most iron-based MOFs, thus reducing Lewis acid sites and limiting the activation efficiency of H 2 O 2 . At the same time, low Fe 3+ /Fe 2+ cycle efficiency also restricts H 2 O 2 activation efficiency. Hence, in this work, a series of MIL-100 (Fe) containing mixed valence coordinatively unsaturated metal site (CUS) with different Fe 2+ /Fe 3+ ratios was synthesized by heat treatment and used for tetracycline hydrochloride (TC-HCL) degradation with the assistance of visible light. Interestingly, accelerated Fe 3+ /Fe 2+ cycle was observed with the aid of visible light. Among the prepared samples, CUS-MIL-250 prepared under vacuum at 250℃ has superior degradation performance, primarily owing to its large specific surface area and pore volume, improved visible light absorption, and the introduction of more Fe 2+ CUS. Meanwhile, compared with Fenton-like system and photocatalytic system, the CUS-MIL-250/H 2 O 2 /Vis system, with effective separation of photogenerated electrons and holes, demonstrates a synergistic effect to generate more reactive oxidation species, thereby improving the degradation efficiency. In addition, the catalyst shows good stability and recyclability.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Zhongmin Feng,Jingwen Yang,Liangyuan Zhu,Ting Sun
Fe–based metal–organic frameworks (Fe–MOFs) have been widely used in heterogeneous Fenton-like processes. However, the catalytic performance of Fe-MOFs is limited by the relatively slow Fe (III)/Fe (II) redox cycle. For Fe-MOFs, increasing the interfacial electron transfer and reducing the electron density of Fe-MOFs are expected to accelerate the reduction of Fe (III) and improve the catalytic performance. Here, by mixing Fe/Cu metal species and introducing bromine groups, we successfully prepared bromine-functionalized bimetallic MOFs–FeCu(BDC-Br), and we used it to effectively degrade phenol in a Fenton-like process. Compared with most other catalysts, FeCu(BDC-Br) achieved a higher phenol degradation kinetic rate of 0.106 min –1 at a low dose. Effects of pH, humic acid (HA) and coexisting ions on the degradation of phenol were examined. The FeCu(BDC-Br) /H 2 O 2 system can remove phenol in the near neutral pH range of 4–6 and 0–50 mg/L HA range. Chloride ion , sulfate, or phosphate with a concentration of 100 mg/L showed an inhibitory effect on the catalytical performance of phenol degradation. This work provides insights for the preparation of Fe-MOFs Fenton-like catalyst in water/wastewater treatment.
研究领域:
环境科学
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催化材料
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产品关联
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2025
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IF 8.4
Maolin Wang,Mi Deng,Gang Zhao,Yanchun Fan,Tianwen Liu,Ying Huang,Lan Peng,Haoyang Fu,Shengqiong Fang
The remediation of organic-contaminated water is a critical environmental challenge, and iron-based persulfate (PS) activation processes have emerged as a promising solution. However, the introduction of reductive sulfur species, while accelerating the Fe(III)/Fe(II) redox cycle, may also quench reactive species, potentially compromising the efficiency of Fenton-like systems. Here we systematically investigate the trade-off between accelerated Fe(III)/Fe(II) cycling and quenching effects in the zerovalent iron/PS (ZVI/PS) system using thiosulfate (TSF) as an activator. Our results show that low-level TSF (0.03–1.00 mmol/L) effectively facilitated the removal of naphthalene (Nap) and atrazine (ATZ), respectively. This enhancement is attributed to accelerated ZVI dissolution and FeS x formation, which promote the Fe(III)/Fe(II) cycle, with Fe(IV) was identified as the primary active species. However, high-level TSF (>1.0 mmol/L) drastically reduced Nap removal due to PS consumption and active species elimination. The optimal TSF dosage of 0.20 mmol/L (TSF/PS molar ratio of 1:10) demonstrated robust organic pollutant degradation, achieving a 22-fold increase in the rate constant ( k obs ) for Nap removal and 0.47–7.5-fold increases for ATZ removal. These findings highlight the potential of the TSF-ZVI/PS system as a versatile and efficient solution for degrading a wide range of organic pollutants, including PAHs and herbicides, in water treatment applications.
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
PubMed
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Hui Wang,Xuefeng Zhang,Xiangfeng Wu,Yewei Kang,Yirui Huang,Zhaoye Zhao,Ziyan Li,Tingting Zhou,Junchuan Wang,Wei Zhu,Chengsi Pan
Bimetallic iron-based metal organic frameworks (MFe-MOFs) exhibit promising photocatalytic properties but face challenges typical of pristine MOFs, including low photoresponsive activity, inadequate band gap regulation, and weak photoconductivity. Here, we designed porphyrin-based COFs (TpPAM-COFs) to serve as a shell grown on NH2-Fe-MIL-101 nanoparticles (NPs) using an in situ solvothermal approach. Subsequently, a ligand-anchoring full-range metallization process was applied to introduce hetero metal ions throughout the core–shell composites, establishing a type-II scheme heterojunction (Fe/Cu-M@PC-Cu) via covalent bonding between NH2-Fe/Cu-MIL-101 and Cu-TpPAM-COFs. The Cu-TpPAM-COF shell, with broad light absorption range, enhanced the generation of photogenerated electrons, facilitating the reduction of Cu2+ and Fe3+ within the Fe/Cu-M@PC-Cu heterojunction and promoting the regeneration of Cu+ and Fe2+ Fenton active sites. Moreover, rapid electron transfer between Fe3+ and Cu+ centers amplified the Fe3+/Fe2+ redox cycle, accelerating the catalytic decomposition of H2O2 and increasing ·OH radical production. Additionally, the optimized bandgap structure of Cu-TpPAM-COFs enhanced the oxidation capacity, as evidenced by the Fe/Cu-M@PC-Cu composite achieving exceptional photo-Fenton catalytic efficiency with 92.7% tetracycline hydrochloride (TCH) degradation in 35 minutes, surpassing that of most reported similar catalysts. Furthermore, the composite showed excellent stability, with only an 11.9% loss in photo-Fenton degradation efficiency after 8 cycles, highlighting its great potential for addressing challenging environmental pollutants.
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
Frontiers in Chemistry
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2025
·
IF 4.2
Xianbing Zhang,Yuheng Liu,Jiajia Yuan
Metal-organic frameworks (MOFs) are recognized as important Fenton-like materials for environmental remediation. However, their applications are often hindered by slow cycling between Fe (III) and Fe (II). This study aimed to address the slow Fe (III)/Fe (II) cycling limitation of Fe-MOFs through dual modification strategy: bimetallic modification and amino functionalization. A series of NH2-MOF(Fe, Co) catalysts with varying Fe/Co ratios were synthesized via a hydrothermal method and evaluated for sulfamethoxazole (SMX) degradation. The optimized NH2-MOF(Fe, Co) catalyst (Fe/Co ratio = 7:3) exhibited substantially enhanced catalytic performance, with SMX removal rate and rate constant in the H2O2 system being 3.2 and 43.5 times higher than those of the Fe-MOF/H2O2 system, respectively. The catalyst demonstrated robust performance across a wide pH range (3.05–7.00), addressing a common limitation of Fenton-like systems. Physicochemical characterization revealed that the enhanced performance was attributed to two key factors: the synergistic effect between Co and Fe in the bimetallic active center, and improved electron transfer to the central metal due to -NH2 functionalization. These modifications effectively addressed the Fe (III)/Fe (II) redox cycling limitation. The proposed reaction mechanism provides insights into SMX degradation pathways in the NH2-MOF(Fe, Co)/H2O2 system. This study presents an efficient and stable MOF-based Fenton-like catalyst with potential applications in wastewater treatment and environmental remediation.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yiming Sun,Peng Zhou,Peng Zhang,Shuang Meng,Chenying Zhou,Yang Liu,Heng Zhang,Zhaokun Xiong,Xiaoguang Duan,Bo Lai
Fenton reaction is most important in advanced oxidation processes, however, the sluggish kinetics of H 2 O 2 induced Fe(II) regeneration relatively limits the hydroxyl radicals generation. This study finds that carbon catalysis is a green and sustainable strategy to boost the Fenton chemistry and provides a new insight to carbon mediated Fe(III)/Fe(II) cycles. Multilayer graphene (MG), as a typical carbon material, can significantly enhance the Fe(III)/H 2 O 2 system to produce hydroxyl radicals. Unlike the classical electron sacrifices, MG can enhance the Fe-O bond of FeOH 2+ and Fe(III) oxidation potential, thus MG can further mediate and accelerate Fe(III) induced H 2 O 2 oxidation to produce Fe(II) and initiate Fenton chain reactions. Kinetics model results reveal that the reaction rate constant between Fe(III) and H 2 O 2 on MG surface is at least 100 times higher than that in aqueous solution. Therefore, carbon catalysis can overcome the speed-limiting process of Fenton system by elevating Fe(III) reactivity at acidic conditions.
研究领域:
环境化学
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催化
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水处理
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产品关联
DOI
高影响因子
Small
·
2024
·Vol. 20
·期 27
·2309541
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IF 13
Tingting Liu,Kaiyue Hu,Yansheng Li,Yanhong Wang,Dongmei Han,Zhihua Wang,Fubo Gu
The Z-scheme MIL-88B/BiOBr (referred to as M x B y , whereas x and y are the mass of MIL-88B(Fe) and BiOBr) heterojunction photocatalysts are successfully prepared by a facile ball milling method. By adding low concentration H 2 O 2 under visible light irradiation, the Z-scheme heterojunction and photocatalytic-Fenton-like reaction synergistically enhance the degradation and mineralization of ciprofloxacin (CIP). Among them, M50B150 showed efficient photodegradation efficiency and excellent cycling stability, with 94.6% removal of CIP (10 mg L −1 ) by M50B150 (0.2 g L −1 ) under 90 min of visible light. In the M x B y heterojunctions, the rapid transfer of photo-generated electrons not only directly decomposed H 2 O 2 to generate · OH, but also improved the cycle of Fe 3+ /Fe 2+ pairs, which facilitated the reaction with H 2 O 2 to generate · OH and · O 2 − radicals. In addition, the effects of photocatalyst dosages, pH of CIP solution, and coexisting substances on CIP removal are systematically investigated. It is found that the photocatalytic- Fenton-like reaction can be carried out at a pH close to neutral conditions. Finally, the charge transfer mechanism of the Z-scheme is verified by electron spin resonance (ESR) signals. The ecotoxicity of CIP degradation products is estimated by the T.E.S.T tool, indicating that the constructed photocatalysis-Fenton-like system is a green wastewater treatment technology.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CHEMOSPHERE
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2024
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IF 8.1
Jie Zhang,Xufei Wang,Yiwei Liu,Tao Jin,Liang Liu,Xiaodong Ma,Gengbo Ren
The efficiency and stability of the electrical activation of persulfate (PS) by transition metal-based cathode are controlled by the cycling of Fe(III)/Fe(II) and the mass transfer of PS. In this study, the mixed-valence MOFs catalyst (Fe II -MIL-53(Fe)) modified flow-through cathode was prepared for the first time. Fe II -MIL-53(Fe) was prepared by replacing part of the iron-oxygen network structure in MIL-53(Fe) with Fe(II), resulting in the formation of coordinated unsaturated iron centers (CUICs). The increase of the Fe(III) CUICs facilitated the conversion of Fe(III) to Fe(II). Furthermore, the cycling of Fe(III)/Fe(II) was further promoted by the electric field. Meanwhile, the hydrodynamic behavior of flow-through cathode was indicated by the computational fluid dynamics (CFD) simulation. The quenching experiments and electron paramagnetic resonance (EPR) results showed that several reactive specie (SO 4 ·- , ·OH, O 2 ·- and 1 O 2 ) were produce. In summary, this work provided an effective strategy for the efficient and stable electrical activation of PDS.
研究领域:
环境科学
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化学工程
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材料科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Chenying Zhou,Zixuan Zhang,Shuang Meng,Jian Zhang,Chuanshu He,Yang Liu,Yanbiao Shi,Gang Yao,Peng Zhou,Bo Lai
Phthalates are a class of widely used endocrine-disrupting chemicals, presenting substantial health hazards upon their release into aquatic environments. Herein, the catalytic potential of two-dimensional transition metal borides (MBenes, including Fe 2 B 2 , MnB, MoB, and Mo 1.33 B) as co-catalysts for activating diverse peroxides in Fenton/Fenton-like oxidation processes, with particular emphasis on optimizing the Fe(III)/Fe(II) cycling efficiency. Under optimized conditions, the Fe 2 B 2 /hydrogen peroxide (H 2 O 2 ) system demonstrated superior catalytic performance, achieving complete degradation of dimethyl phthalate (DMP) within 15 min. This system exhibited pseudo-first-order rate constants that were 5.7–154.3 times higher than those of other MBenes/Fe(III)/H 2 O 2 systems, highlighting its exceptional catalytic efficiency. Notably, Fe 2 B 2 exhibited exceptional stability through five consecutive cycles, maintaining DMP degradation rates (∼100 %) with minimal boron leaching (∼1.05 mg/L). Mechanistic studies revealed a dual activation pathway. Surface-bound Fe(II) species decompose H 2 O 2 directly to produce hydroxyl radicals. Meanwhile, B–Fe–B bridges facilitate Fe(II) regeneration by transferring electrons from iron atoms or B B bonds in Fe 2 B 2 to dissolved FeOH 2+ species. This synergistic interaction establishes a self-sustaining catalytic cycle that significantly enhances the Fenton reaction kinetics. These findings establish Fe 2 B 2 MBene as dual-functional material that serves as both a sustainable dual-function catalyst and an efficient iron source, providing new perspectives for designing MBene-based catalysts for environmental remediation applications.
研究领域:
环境科学
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催化
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纳米技术
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
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IF 3.99
Qingwen Long,Feng Liu,Yanjie Yuan,Yuting Dai,Chunli Wang,Xuheng Li,Jing Zhang
In this study, heterogeneous Fenton-like catalyst, nano-Fe° encapsulated in hydrothermal carbon (Fe°/HTCC), was prepared via a green chemistry route, aiming at increasing the degradation efficiency of p-chlorophenol (4-CP) by controlling the stability of the catalyst and Fe(III)/Fe(II) cycling in the advanced oxidation process. The degradation of 4-CP by heterogeneous Fenton reactions was conducted with the assistance of visible light, which was monitored with the aid of the HPLC and total organic carbon analysis. The results revealed that Fe°/HTCC composite markedly enhanced both the degradation (100 %) and the mineralization efficiency (∼73.9 %) for 100 mg/L 4-CP within 60 min at pH 4.0. More importantly, the catalyst presented a high stability to resist the side oxidation, where the removal efficiency was maintained even after 5 successive cycling experiments. Electron spin resonance confirmed that in the presence of both HTCC and visible light irradiation greatly enhanced the production of •OH for the degradation and mineralization of 4-CP, which can be attributed to the enhancement of Fe(III)/Fe(II) cycling. This study paves a new way toward the rational design of Fe°–carbon composites as heterogeneous Fenton-like catalysts for potential applications into wastewater treatment.
研究领域:
环境科学
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Saudi Chemical Society
·
2023
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IF 5.6
Sen Guo,Cong Shen,Yao Gui,Huiming Li,Jinhong Lü,Jianfa Li
Biochar (BC) and ferrihydrite (Fh) were used together in activation of H 2 O 2 for removal of sulfamethazine (SMZ), a refractory antibiotic pollutant. The results show a complementary effect between biochar and ferrihydrite on activation of H 2 O 2 , namely biochar accelerated Fe(Ⅲ)/Fe(Ⅱ) cycle through electron donation/transfer, while ferrihydrite enhanced the yield of • OH through a sustainable release of dissolved Fe. Thus several times more • OH was produced in the co-activated system (BC + Fh/H 2 O 2 ) than either in the ferrihydrite-catalyzed Fenton-like system (Fh/H 2 O 2 ) or in the biochar-activated system (BC/H 2 O 2 ). Consequently, a more efficient oxidation of SMZ was observed in BC + Fh/H 2 O 2 , in which the reaction rate constant ( k obs ) is 30.7 times in Fh/H 2 O 2 and 6.08 times in BC/H 2 O 2 , respectively. This research provides a simple and sustainable strategy for enhancing the efficiency of Fenton-like oxidation of pollutants.
研究领域:
环境科学
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化学工程
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水处理
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污染控制
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）