CHEMOSPHERE
·
2022
·
IF 8.943
Hanlin Wang,Haibo Liu,Xuehua Zou,Fuwei Sun,Luyao Wang,Jingchao Hu,Dong Chen,Meng Liu,Jianfei Shen,Tianhu Chen
In this work, the effect of Co substitution in the Fe 1-x S (CSP) on the activation of H 2 O 2 to degrade tetracycline (TC) is investigated. A series of CSP samples with different Co content are synthesized via a high-temperature sulfidation method and characterized by XRD , XPS , SEM, and electrochemical analysis . The result showed that low Co content (≤1%) promotes the catalytic activity of Fe 1-x S, while excessive Co (1%﹤x ≤ 3%) inhibits its catalytic activity. The investigation of Behnajady-Modirshahla-Ghanbery kinetic model (BMG) showed that the maximum initial degradation rate of TC over 1.0% CSP/H 2 O 2 was 1.6 times than that of in CSP/H 2 O 2 system. The Box-Behnken with Response Surface Methodology was employed to verify optimum condition for TC degradation. The quenching experiments and ESR determined that ·OH, ·O 2 − and 1 O 2 were involved in TC degradation with the treatment of 1.0% CSP/H 2 O 2 system. Electrochemical analysis, ·OH quantification, and metal ion concentrations measure reveal that Co substitution accelerates electron transfer efficiency and Fe 2+ regeneration. Furthermore, nine intermediates are identified and the possible degradation pathway of TC is proposed. The unique effect of Co provides novel insight and efficient strategies for improving the reactivity of iron sulfide.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
Frontiers of Environmental Science & Engineering
·
2018
·Vol. 12
·期 6
·1-10
·
IF 1.961
Mao Jie,Quan Xie,Wang Jing,Gao Cong,Chen Shuo,Yu Hongtao,Zhang Yaobin
Heterogeneous Fenton-like reaction has been extensively investigated to eliminate refractory organic contaminants in wastewater, but it usually shows low catalytic performance due to difficulty in reduction from Fe(III) to Fe(II). In this study, enhanced catalytic efficiency was obtained by employing Cu-doped BiFeO 3 as heterogeneous Fenton-like catalysts, which exhibited higher catalytic performance toward the activation of H 2 O 2 for phenol degradation than un-doped BiFeO 3 . BiFe 0.8 Cu 0.2 O 3 displayed the best performance, which yielded 91% removal of phenol (10 mg L –1 ) in 120 min. The pseudo first-order kinetic rate constant of phenol degradation in BiFe 0.8 Cu 0.2 O 3 catalyzed heterogeneous Fenton-like reaction was 5 times higher than those of traditional heterogeneous Fenton-like catalysts, such as Fe 3 O 4 and goethite. The phenol degradation efficiency could still reach 83% after 4 cycles, which implied the good stability of BiFe 0.8 Cu 0.2 O 3 . The high catalytic activity of BiFe 0.8 Cu 0.2 O 3 was attributed to the fact that the doping Cu into BiFeO 3 could promote the generation of Fe(II) in the catalyst and then facilitate the activation of H 2 O 2 to degrade the organic pollutants.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2023
·
IF 11.1
Yang Yang,Wenqing Zhen,Tingting Zhao,Maoquan Wu,Shouchun Ma,Liyan Zhao,Jie Wu,Li Liu,Jiaxu Zhang,Tongjie Yao
Fenton/photo-Fenton reaction was limited by slow Fe 3+ /Fe 2+ cycle, low H 2 O 2 activation efficiency, and narrow applicable pH range. Here, Fe atoms doped MoS 2 (Fe–MoS 2 ) with abundant of low-valence Mo δ+ (0 < δ < 4) was prepared. Benefiting from the powerful reduction capacity of Mo δ+ , the rate-limiting step of Fe 3+ reduction was significantly accelerated. Nearly 100% of H 2 O 2 utilization efficiency was realized. Importantly, 90% of H 2 O 2 was effectively activated to be • OH. As a result, tetracycline degradation rate in photo-Fenton reaction catalyzed by Fe–MoS 2 was 5.8 and 4.2 times higher than those of MoS 2 and Fe–MoS 2 -Hyd (prepared by hydrothermal reaction). In comparison with MoS 2 and Fe–MoS 2 -Hyd whose efficient work range were limited in acidic condition, Fe–MoS 2 was a pH-universal catalyst (pH = 2.6–14.0) by taking advantage of the exposed Mo δ+ and photoinduced electrons, largely improving the environmental tolerance. This work simultaneously addressed three bottlenecks in Fenton/photo-Fenton reaction, and provided a new strategy for the preparation of catalysts with powerful catalytic performance and high environmental adaptability.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Yue Yin,Ruolin Lv,Xiaoyang Li,Lu Lv,Weiming Zhang
Bimetallic Fenton catalyst has attracted widespread attention in refractory organics removal. Herein, we firstly investigated the influence of ZrO 2 structure features on H 2 O 2 activation in Zr-Fe bimetallic catalyst. The results show that the heterojunction structure will be formed after high temperature calcination , which makes the ability of Zr-Fe bimetallic catalyst to activate H 2 O 2 for bisphenol A degradation is 3.1 times higher than that of α-Fe 2 O 3 without Zr doping. Through characterization and density functional theory, it was identified that compared to (1 1 0) interface, the adsorption energy of H 2 O 2 on iron sites at (1 1 0)-(1 0 0) interface reduced by 1.27 kJ mol −1 , while the Fe–O bond length in the stable configuration of Fe-OOH increased by 0.16 Å, which was beneficial to the association and dissociation of H 2 O 2 on iron sites. Besides, the surface -OH of amorphous ZrO 2 in Zr-Fe bimetallic catalyst synthesized under low temperature conditions could promote HO 2 • /O 2 •- formation through the surface electron transfer, accelerating the Fe(III) reduction. In conclusion, this study reveals the influence of environment-friendly ZrO 2 structure features on H 2 O 2 activation, proposes a new insight into strengthening the synergistic effect between bimetals, and provides a reference for the structural optimization of bimetallic catalysts.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2014
·Vol. 5
·期 13
·9374-9380
·
IF 3.708
Nan Li,Wangyang Lu,Kemei Pei,Wenxing Chen
The rapid diffusional mass transfer process (DMTP) always results in a highly efficient reaction. Herein, cobalt phthalocyanine (CoPc) was covalently anchored on to multiwall carbon nanotubes (MWCNTs) by an easy and moderate one-step deamination method to obtain the catalyst MWCNT-immobilized CoPc (CoPc-MWCNT). The interfacial peroxidase-like catalytic activity of CoPc-MWCNTs is described for controllable H2O2 activation. According to the experimental results and density functional theory calculations, we can be confident that high-valent cobalt-oxo intermediates are formed during the H2O2 activation. Such active species are anchored and exposed on the surface of MWCNTs, shortening the DMTP and enhancing the resistance of CoPc-MWCNTs to oxidative decay. The introduction of linear alkylbenzene sulphonates (LAS) facilitates the catalytic H2O2 activation by CoPc-MWCNTs, and at the same time, CoPc-MWCNTs could maintain a high and sustained catalytic activity because of the specific hydrophobic interactions between the long-chain alkyl group of LAS and the π-conjugated surface of the MWCNTs.
研究领域:
材料科学
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催化化学
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2022
·
IF 0
Shuqian Dong,Xu Chen,Linfeng Su,Yingjie Wen,Yuechu Wang,Qihao Yang,Li Yi,Wenwen Xu,Qiu Yang,Peilei He,Yunqing Zhu,Zhiyi Lu
Photo-Fenton degradation as a promising strategy for antibiotic wastewater treatment attracted extensive attention, while the unsatisfactory catalytic performance vitally limits its industrial application. Herein, we demonstrate that confining atomically dispersed Cu into C3N4 (Cu–C3N4) enables fast H2O2 activation and efficient separation of photogenerated electron–hole pairs, resulting in a dramatic improvement of the degradation efficiency of the Photo-Fenton reaction. Photo-Fenton degradation of ciprofloxacin (CIP) was close to 99% within 30 min over optimized Cu–C3N4, corresponding to a pseudo-first-order rate constant of ∼0.0978 min–1, almost 4.5 times higher than pure C3N4 counterpart. The electron paramagnetic resonance, quenching experiments, and X-ray absorption fine structure results reveal that the superior Photo-Fenton catalytic performance is attributed to a nonradical reaction pathway, where the H2O2 is activated by the formation of the O═Cu–N4═O intermediate. The advanced catalyst as well as the refreshing H2O2 activation mechanism are of profound significance for the materials design in the wastewater treatment field.
研究领域:
环境科学
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材料科学
·
化学工程
✓ 已验证
DOI
ACS Nano
·
2024
·
IF 15.8
Guoqiang Zhao,Xiaoyu Tao,Tongsen Guo,Liangjie Fu,Huaming Yang
Solution-phase epitaxy is a versatile method to synthesize functional nanomaterials with customized properties, where supports play a central role as they not only serve as nucleation templates but also greatly affect the local electronic structures. However, developing functional supports remains a great challenge. Herein, inspired by the commonly observed epitaxy of minerals in the natural environment, we report using calcination-modified kaolinite as the support for the epitaxial growth of hexagonal CoO nanoparticles (h-CoO NPs), which enables over 40 times higher mass-specific activity toward H2O2 electrochemical activation than the counterpart without the support. High-resolution electron microscopy, magic-angle spinning nuclear magnetic resonance, and X-ray absorption fine structure results prove that the Al sites in kaolinite play a crucial role in the formation of h-CoO NPs. Moreover, the five-coordinate Al (AlV) sites produced by the dehydration of kaolinite are indispensable for forming the epitaxial interface. Theoretical calculations reveal that the local electron densities around AlV sites are lower than those of general six-coordinate Al sites, which render AlV sites with strong adsorption capability that facilitates the nucleation of h-CoO NPs. Also, the AlV sites induce the electron transfer from h-CoO to the kaolinite support that results in the upshift of the Co 3d band center and hence improve the H2O2 activation kinetics. Our results demonstrate the superiority of nanoclay as functional supports and could offer a more benign strategy to the solution-phase epitaxy production of functional nanomaterials for diverse applications.
研究领域:
材料科学
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电化学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Hongwei Zhu,Xu Yin,Yi Wang,Kajia Wei,Liankai Gu,Yonghao Zhang,Zhenshan Duan,Zhen Huang,Haoming Chen,Weiqing Han
This study developed a self-supported MOF/FeOOH heterojunction cathode without binders for boosted Fe(Ⅲ) reduction in heterogeneous electro-Fenton (EF) processes. The electron transport channels from FeOOH to in-situ grown NH 2 -MIL-88B(Fe) were established through the spontaneous formation of an internal electric field (IEF), which enhanced the electrical conductivity and disrupted the chemical inertness of the Fe(Ⅲ) reduction. The MOF/FeOOH cathode increased sulfamethazine (SMT) removal up to 95.76 %, 2.5 times better than using PTFE as binders. After ten-consecutive degradation experiments, the Fe(Ⅱ) content at cathode surface increased from 39.23 % to 56.73 %. Density functional theory (DFT) calculations and advanced characterization techniques demonstrated the efficient Fe(Ⅲ) reduction and H 2 O 2 activation during the reaction. These results elucidate the promoting effect of modulating the “contact” between the catalyst and current collectors, as to provide a feasible and promising strategy for the development of efficient heterogeneous EF cathodes.
研究领域:
环境科学
·
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2023
·
IF 7
Chuxuan Zhang,Jianhui Zeng,Zhipeng Ouyang,Xiaomin Li,Luqiu Lin,Yang Peng,Xun Gong
Efficient and economical catalysts are crucial for activating H 2 O 2 in Fenton-like reactions. Microalgae harvesting by magnetic separation will inevitably result in unrecovered Fe 3 O 4 nanoparticles (Fe 3 O 4 NPs) entering the downstream oil production stage. This part of Fe 3 O 4 NPs can play a catalytic role in the co-liquefaction process with microalgae to improve the bio-oil quality, and then be separated from the liquid phase along with microalgae hydrochar (MHC). Herein, this N-rich MHC loaded Fe 3 O 4 NPs composite (Fe 3 O 4 @MHC) as a by-product was recycled without reprocessing to remove Rhodamine B (RhB). Detailed characterization data indicates that Fe 3 O 4 NPs can be well anchored and dispersed on MHC surface after liquefaction . The Fe 3 O 4 @MHC exhibits an outstanding catalytic performance in the activation of H 2 O 2 for RhB degradation, with a removal rate of >97 % within 60 min at a lower dosage (0.17 g/L). MHC act as electron donors due to the abundant oxygen- and nitrogen-containing functional groups to accelerate Fe 2+ /Fe 3+ cycle. OH and O 2 − are the dominant active species in catalytic systems. This study not only provides an economical carbon material with high efficiency for environmental remediation, but also proposes a reliable solution for the disposal of solid residues after microalgae bio-oil production.
研究领域:
环境科学
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催化
·
废水处理
·
生物技术
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Wei Li,Lei Zhang,Kajia Wei,Xu Yin,Hongwei Zhu,Siyuan Cao,Qi Zhang,Weiqing Han,Xiaoyuan Zhang
Appropriate tuning of the nonradical pathway in the heterogeneous Fenton process is important for enhancing its anti-interference ability in wastewater treatment. However, the difficulty in O–H bond cleavage of H 2 O 2 hinders its oxidation routine for nonradical production. Herein, a charge-regulating linkage M–S–Fe (M = Co, Ni, Zn) with S-bridged asymmetric dual-metal centers was established on multiwall carbon nanotubes, i.e., M-FeS 2 /MWCNT, to effectively tune the H 2 O 2 nonradical pathway. The high-charge-positive M centers in M–S–Fe structure significantly reduced the H 2 O 2 oxidation energy barrier by 72%, thereby enhancing the 1 O 2 generation and model pollutant removal efficiency by 1.72 and ~24 times, respectively, compare to the sole-Fe center catalyst. Moreover, the S-bridged asymmetric dual-metal centers catalysts showed excellent complex pollutant adaptability (> 80% organic decontamination in phenolic, antibiotic and dye mixed matrices), ion-resistance and stability. This work offers a new strategy for constructing a charge-asymmetry dual-metallic-center for tunable nonradical pathways in H 2 O 2 activation.
研究领域:
环境科学
·
催化
·
材料科学
·
化学工程
·
水处理技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry C
·
2025
·
IF 5.1
Yonghao Wang,Liting Ling,Zhenghao Lu,Ming Zhou,Xiaomei Zheng,Yongjing Wang
Spinel-structured materials are considered promising electrocatalysts for environmental remediation, yet their mechanisms in the electrocatalytic reduction of O2 to H2O2 and the activation of H2O2 remain poorly understood. Herein, we synthesized a novel MgFe2O4/carbon nanotube (CNT) composite via a hydrothermal method and systemically investigated its electrocatalytic performance in the degradation of phenol through the in situ electrocatalytic-reduction of O2 to H2O2 and activation to ˙OH. The composite exhibited exceptional catalytic activity, achieving 99% phenol degradation within 30 minutes under optimized conditions (MgFe2O4/CNT mass ratio of 10 : 1, applied voltage of −0.9 V, pH 3, and catalyst loading of 0.44 mg cm−2). Moreover, the total organic carbon (TOC) reached 78.6% in 90 minutes, with the catalyst maintaining 91.4% efficiency after four recycling experiments. Mechanistic studies using XPS and control experiments indicate that introducing CNTs considerably improves electron transfer and enriches active oxygen and defect degrees. Importantly, abundant defects and active oxygen species facilitate the generation of H2O2 and dominate the conversion of H2O2 into ˙OH by heterogeneous activation for MgFe2O4/CNT, while MgFe2O4 mainly depends on homogeneous activation. This work offers a significant case for the degradation of organic contaminants utilizing spinel-structured electrocatalysts.
研究领域:
环境催化
·
电化学
·
材料科学
·
环境修复
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Lu Liu,Jian Wang,Huijuan Yang,Di Gao,Yaya Cui,Hao Chen,Yaxin Qin,Ranfeng Ye,Xing Ding
The widespread use of polychlorophenols poses enormous environmental challenges. Biochar has the potential to accelerate the transformation of polychlorophenols. But the biochar-triggered photochemical decomposition mechanism of polychlorophenols still remains unclear. Herein, the photochemical behavior of pyrochar was comprehensively investigated in 2,4,6-trichlorophenol (TCP) remediation. Researches revealed that persistent free radicals (PFRs) and oxygenated functional groups (OFGs) on the surface of pyrochar cooperatively promoted ROS generation for TCP degradation. PFRs performed a key role of electron-donating and energy transfer in ROS conversion, especially in the activation of H 2 O 2 into •OH. The hydroxyl groups of photosensitive components of pyrochar were photo-excited and provided electrons for enhanced ROS formation as well. With photogenerated ROS involved, more TCP was decomposed through dechlorination under light irradiation than that in the dark, in which 1 O 2 , •OH, and •O 2 − were the dominant active species. During this process, stronger light intensities (3 W/m 2 ) and shorter light wavelengths (400 nm) can provide more energy for the activation of PFRs and OFGs, promoting the decomposition of TCP. This work casts a new light on the environmental roles of pyrochar in the photochemical removal of polychlorophenol pollutants.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）