SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Shilin Xu,Ying-Jie Zhang,Rui Tang,Xinyu Zhang,Zhen-Hu Hu,Han-Qing Yu
Introducing reductive species into heterogeneous catalysts can improve their catalytic efficiency in Fenton-like processes. Iodide ions (I − ), a typical reductive species with good reducibility, might enhance the catalytic performance of H 2 O 2 activation when doped in heterogeneous catalysts. In this study, the iodine-doped Bi 2 WO 6 (I X -Bi 2 WO 6 ) nanosheets were synthesized with a facile hydrothermal method and used to activate H 2 O 2 to degrade bisphenol A (BPA). Compared with Bi 2 WO 6 , which was almost inactive, the I X -Bi 2 WO 6 exhibited great improvement for BPA degradation. Among the fabricated catalysts, the I 0.50 -Bi 2 WO 6 with an iodine content of 0.50 mmol was found to be most effective and could work efficiently in a wide pH range from 4.0 to 10.0. Moreover, with a low consumption of H 2 O 2 (H 2 O 2 : pollutant molar ratio = 10:1), 78% BPA was degraded within 10 min at initial pH 7.0. Unlike the conventional H 2 O 2 activation mechanism, the direct electron transfer was verified to be the main mechanism for the BPA degradation based on the results of electron paramagnetic resonance (EPR) analysis, radical quenching, and electrochemical experiments in this work. Furthermore, the activation of H 2 O 2 by iodine-doped BiVO 4 and Bi 2 MoO 6 was also conducted to validate the applicability of such an iodine doping approach. These results indicate that the introduction of reductive species I − is a promising and effective method to develop highly efficient Bi-based catalysts for H 2 O 2 activation.
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhipeng Guo,Wei Wei,Yihang Li,Xianghong Niu,Fengming Hou,Jin Li,Xiaoke Zhang,Xiuyun Zhang,Ang Wei
Single-atom photo-Fenton (PF) reaction is widely employed for the degradation of antibiotics and water disinfection. However, the key fundamental issues of the valence state cycling of single-atom metals and the activation of hydrogen peroxide (H 2 O 2 ) in the PF process remain indistinct. Herein, we developed a catalyst donated as Cu single atoms anchored hydrangea-like carbon nitride (Cu-SA/CNH) with Cu−N 4 coordination for PF reaction. Compared to pristine CNH, the Cu-SA/CNH exhibited a 2.42-fold increase in PF kinetics. The Cu-SA/CNH/PF system achieved 98.1% degradation efficiency of tetracycline and effectively inactivated Escherichia coli within 30 min. Density functional theory calculations demonstrated that the formation of Cu−N 4 effectively improved the energy of the Cu d orbitals, leading to the generation of intermediate states that facilitated the Cu 2+ /Cu + cycle. The adsorption capacity of Cu d xz orbitals on H 2 O 2 increased nearly 10 times. This work provides valuable insights for enhancing single-atom PF activity to address environmental pollution.
研究领域:
环境科学
·
材料科学
·
理论化学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2023
·
IF 2.8
Yajing Wang,Quanxi Zhu,Taiping Xie,Yuan Peng,Jiankang Wang,Zhongping Yao
Developing a highly efficient Fenton-like catalyst working in a wide pH range is imperative to accomplish its practical wastewater treatment. Herein, FeS2/FeSxOy catalyst was synthesized by hydrothermal-solvothermal vulcanization with thioacetamide as a sulfur source. Characterization results confirmed FeS2/FeSxOy consisted of pyrite, kornelite, and szomolnokite. FeS2/FeSxOy exhibited superior catalytic activity toward H2O2 activation with more than 96% phenol removal within 5 min in pH 3.0 ∼ 8.0 at 30°C. Radical scavenging experiment and EPR analysis revealed both hydroxyl radicals (·OH) and superoxide anion radicals (O2·-) anticipated in phenol elimination, but ·OH played a dominant role. The detailed degradation experiments and density functional theory (DFT) calculation confirmed the vital role of FeS2 in enhancing phenol abatement. This study not only developed a highly active catalyst for H2O2 activation but also theoretically analyzed the FeS2 function in depth, which provided a guide for designing a highly efficient Fenton-like catalyst.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Shengjia Ma,Bingtao Dong,Yuxin Zheng,Shuai Tang,Tao Zhang,Yaping Zhao
This work elucidated the dual-substrate activation mechanism of a Fenton-like system, enabled by the upcycling of plastics into a highly efficient catalyst. A synergistic pyrolysis strategy was employed to upcycle polyethylene microplastics into nitrogen-doped carbon while simultaneously constructing Fe clusters and WS 2 co-catalyst (WS 2 /Fe-N-C). In the H 2 O 2 activation system, WS 2 /Fe-N-C achieved a remarkable rate constant of 0.949 min −1 toward bisphenol A, which was 52 times higher than that of Fe-N-C, outperforming previously reported representative co-catalyst systems and Fe-based carbon catalysts. Correlation analysis, electrochemical tests and theoretical calculations demonstrated that Fe sites primarily activated H 2 O 2 to generate •OH, while WS 2 adsorbed bisphenol A and facilitated a non-radical electron transfer pathway, enabling dual-substrate synergistic catalysis for highly efficient pollutant removal. This work provides a feasible strategy for plastic upcycling and offers innovative insights into the synergy between metal centers and cocatalysts, paving the way for the rational design of high-performance catalysts.
研究领域:
环境科学
·
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2025
·
IF 2
Yali Zhao,Ziru Wang,Jinxiu Zhai,Xingjian Cao,Peilei He
Graphical The lacunary polyoxometalate ([PW 11 O 39 ] 7− , PW 11 ) can self-assemble with TBAB to form tetrakaidecahedron-like nanodices (NDs). These NDs exhibit significantly higher catalytic activity for the epoxidation of cyclooctene compared to PW 11 alone and nanospheres (NSs) formed from the non-lacunary polyoxometalate ([PW 12 O 40 ] 3− , PW 12 ). DFT studies confirm the critical role of hydroperoxo species generated at the lacunary site in facilitating oxygen transfer to cycloalkenes over PW 11 . The activation of hydrogen peroxide (H 2 O 2 ) as a terminal oxidant holds great promise for catalytic oxidation processes. However, developing an efficient catalyst for the epoxidation of bulky organic molecules with H 2 O 2 , including cyclic alkenes, remains challenging. In this research, a lacunary polyoxometalate (POM)-based tetrakaidecahedron nanodices (NDs) are synthesized by [PW 11 O 39 ] 7− (PW 11 ) clusters with tetrabutylammonium bromide (TBAB). The NDs exhibit significantly enhanced catalytic activity in the epoxidation of cyclooctene, with a yield 55.4 times greater than that of the raw PW 11 . Conversely, nanospheres (NSs) assembled from non-lacunary POM clusters of [PW 12 O 40 ] 3− (PW 12 ) under the same conditions achieve only a 2.9 % yield, highlighting the essential role of the lacunary PW 11 structure in NDs. Raman spectroscopy and density functional theory (DFT) calculations confirm that the active hydroperoxo species from H 2 O 2 activation serves as the effective epoxidizing agent. The reduced energy barrier for H 2 O 2 activation on PW 11 , relative to PW 12 , corroborates the superior activity of the NDs. Furthermore, the intermediate generated post-H 2 O 2 activation shows stronger adsorption of cyclooctene, increasing oxygen transfer to cyclooctene during the epoxidation process. This study demonstrates the exceptional performance of an assembly structure utilizing lacunary POMs for the activation of H 2 O 2 and subsequent oxidation reactions.
研究领域:
催化化学
·
材料科学
·
理论计算化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2022
·Vol. 12
·期 27
·17237-17248
·
IF 4.036
Dongqing Feng,Jianxin Shou,Sen Guo,Mengna Ya,Jianfa Li,Huaping Dong,Yimin Li
Activation of hydrogen peroxide (H2O2) with biochar is a sustainable and low-cost approach for advanced oxidation of organic pollutants, but faces the challenge of a low yield of hydroxyl radical (˙OH). Herein, we hypothesize that the activation efficiency of H2O2 can be enhanced through co-catalysis of trace dissolved iron (Fe) with biochar. Two biochar samples derived from different feedstock, namely LB from liquor-making residue and WB from wood sawdust, were tested in the co-catalytic systems using trace Fe(III) (0.3 mg L−1). The cumulative ˙OH production in [Fe(III) + LB]/H2O2 was measured to be 3.28 times that in LB/H2O2, while the cumulative ˙OH production in [Fe(III) + WB]/H2O2 was 11.9 times that in WB/H2O2. No extra consumption of H2O2 was observed in LB/H2O2 or WB/H2O2 after addition of trace Fe(III). Consequently, the reaction rate constants (kobs) for oxidation of pollutants (2,4-dichlorophenoxyacetic acid and sulfamethazine) were enhanced by 3.13–9.16 times. Other iron species including dissolved Fe(II) and iron minerals showed a similar effect on catalyzing 2,4-D oxidation by biochar/H2O2. The interactions involved in adsorption and reduction of Fe(III) by biochar in which the defects acted as electron donors and oxygen-containing functional groups bridged the electron transfer. The fast regeneration of Fe(II) in the co-catalytic system resulted in the sustainable ˙OH production, thus the efficient oxidation of pollutants comparable to other advanced oxidation processes was achieved by using dissolved iron at a concentration as low as the concentration that can be found in natural water.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Peipei Huang,Qing Chang,Guodong Jiang,Keru Xiao,Xu Wang
Metal organic frameworks are important Fenton-like materials in environment remediation. Nevertheless, the slow Fe(III)/Fe(II) cycling and low H 2 O 2 utilization limit their application. In this study, we develop the ferrous bimetallic MIL-101(Fe II 3 , Mn), which significantly enhanced catalytic performance (5.8 and 31.4-fold higher phenol removal rate and apparent rate constant, respectively) compared with the original MIL-101(Fe). The mechanisms are fully investigated by XPS, EPR and DFT. The Fe 2+ substitution affords the mixed-valences of Fe(III)/Fe(II) in the frameworks, which serve as stronger sites for H 2 O 2 activation. Mn in MIL-101(Fe II 3 , Mn) can also function as another reaction center to activate H 2 O 2 . Catalysts could coordinate with the π–electrons of pollutants, resulting in the electron transfer from pollutants to MIL-101(Fe II 3 , Mn). Moreover, electrons around Mn atoms tends to transfer to the region of Fe atoms owing to the electronegativity difference, inducing to strengthen the electron-rich Fe micro-region. Therefore, H 2 O 2 was primarily adsorbed onto electron-rich regions where it would be efficiently reduced to •OH, contributing to a higher H 2 O 2 utilization (81.2 %). This study opens new insight into design of Fe-based MOFs as highly efficient Fenton-like catalysts in wastewater treatment.
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yuhe Bai,Qiangqiang Tao,Li Wang,Shuai Lu,Aixin Zhang,Kang Li,Ning Hu
A novel Cu 0 nanoparticle-anchored, magnetically separable spinel high-entropy catalyst ( Cu 0 NPs @ HEOs ) was synthesized via co-precipitation, freeze-drying, and high-temperature calcination for rapid catalytic degradation of sulfadiazine (SDZ) through H 2 O 2 activation. During the high-temperature calcination process, a fraction of Cu 0 nanoparticles precipitated and anchored on the catalyst surface, enhancing electron transfer at the interface while suppressing metal leaching. Cu 0 NPs @ HEOs system achieves a 99.34 % degradation rate for SDZ within 20 min—surpassing the 75.6 % degradation obtained using conventional medium- and low-entropy catalysts. Toxicity prediction software confirmed the low biotoxicity of degradation intermediates, ensuring environmental safety. The catalyst’s magnetic properties allowed for easy recovery using an external magnetic field, enabling reuse without performance degradation. Experimental characterization combined with density functional theory (DFT) calculations revealed that surface Cu sites acted as the primary active centers, effectively promoting H 2 O 2 adsorption and activation through electron transfer, accelerating ·OH generation. The main reactive species involved were ·OH, with minor contributions from O 2 – ·. Other metal sites provided electrons to sustain the high-entropy catalytic reaction. This study offers a new perspective on high-entropy material synthesis and highlights its potential in environmental remediation, especially for treating refractory 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
ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Binrong Li,Chen Wang,Na Li,Chunyang Chen,Zhi Zhu,Xu Tang,Yanhua Cui,Tingting Liu,Collins Kwashie Attatsi,Xuedong Wang
Immobilizing Fe-based nanoparticles on electron-rich biochar has becoming an attractive heterogeneous Fenton-like catalysts (Fe/BC) for wastewater decontamination. However, the insufficient graphitization of biochar causing low electron transfer and by slow H 2 O 2 activation limited its application. Herein, we firstly constructed FeS/biochar composite through all-solid molten salt method (Fe/MSBCs), which can provide strong polarization force and liquid reaction environment to improve carbonization. As expected, the obtained Fe/MSBCs exhibits high surface area and fast interfacial electron transfer between FeS and biochar. More importantly, the partially oxidized FeS (001) facet facilitate H 2 O 2 adsorption and thermodynamically easily decomposition into •OH. Such a synergistic effect endowed them excellent photo-Fenton degradation performance for methyl orange (MO) with large kinetic rate constants (0.079 min −1 ) and high H 2 O 2 utilization efficiency (95.9%). This study first demonstrated the critical regulatory role of molten salt method in iron-based biochar composites, which provide an alternative for H 2 O 2 activator in water pollutant control.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Jiangli Sun,Huizhong Wu,Chunhong Fu,Chaohui Zhang,Zhongzheng Hu,Minghua Zhou
A novel photoelectrocatalytic (PEC) system consisting of S-scheme MgO/g-C 3 N 4 photoanode and modified carbon felt (MCF) cathode was designed for efficient degradation of tetracycline , in which photoanode had both efficient photocatalytic performance and activation of H 2 O 2 produced by the MCF cathode. After 30 min of LED irradiation, the PEC system could completely remove tetracycline at cathodic bias of −0.5 V (vs. Ag/AgCl), and the degradation rate constants were 5.3 and 1.5 times that of electrocatalysis and photocatalysis . The charge transfer mechanism of S-scheme MgO/g-C 3 N 4 was verified by experimental studies and DFT calculations. Mg-N coordination was the key to activate H 2 O 2 to produce singlet oxygen ( 1 O 2 ) and hydroxyl radicals ( • OH). The PEC system had excellent degradation performance at pH ranges 4–10, which solved the bottleneck that Fenton system is effective at narrow pH range. This study provides new ideas for preparation of bifunctional photoanodes and new insights into the PEC process.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2015
·
IF 7.435
Jiangkun Du,Jianguo Bao,Xiaoyan Fu,Chenghang Lu,Sang Hoon Kim
A mesoporous sulfur-modified iron oxide (MS-Fe) was prepared as a heterogeneous H 2 O 2 catalyst for degradation of BPA. The physico-chemical properties of MS-Fe and bare M-Fe were characterized by BET surface area measurement, SEM, XRD, FTIR and XPS. Both M-Fe and MS-Fe composites appeared as cubic microparticles with abundant pores and cracks as well as large surface area. As depicted by XRD, EDX and XPS, M-Fe is mainly consisted of hematite while MS-Fe is a kind of S-doped iron oxide with about 5–6% of sulfur element in terms of atomic ratio. In contrast to the poor catalytic activity of bare M-Fe, the MS-Fe composites showed greatly improved efficiencies for H 2 O 2 activation for BPA degradation. The high catalytic activity of this new Fenton-like catalyst can be obtained at different initial pH in range of 3.0–9.0. The time evolution of degradation of BPA followed pseudo-first-order kinetics, and the first-order rate constants showed a linear relationship with parameters of initial pH, catalyst dosage and concentration of BPA. However, the H 2 O 2 dosage showed a dual effect on BPA degradation because excessive H 2 O 2 addition lead to scavenging of hydroxyl radicals ( OH). The investigation of working mechanisms of MS-Fe suggested a synergistic effect of homogeneous and heterogeneous degradation reaction, wherein a strong acidic environment, abundant surface-bonded hydroxyl group and electron-mediating effect of sulfur all contributed to fast activation of H 2 O 2 . Overall, this new material overcomes the limitation of narrow working pH range and shows a fast oxidation of BPA with a low H 2 O 2 and catalyst dosage, would have a good potential for environmental application.
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 HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Weilu Yang,Mingshan Zhu,Wanbin Li,Guoqiang Liu,Eddy Y. Zeng
Activation of H 2 O 2 with metal-free catalysts is an efficient and environmentally benign alternative to electron-Fenton (EF) for organics degradation . In the present study, flexible nanocatalysts were synthesized with self-regulated metal oxide nanoparticles (FeOx NPs) for efficient removal of plasticizers from secondary wastewater effluent (SWE). Compared with NGr/EF and FeOx@Gr/EF systems, FeOx@NGr/EF could enhance the decay kinetics of plasticizers by 3.9–4.4 times and reduce 48–59% of the disposal cost. Reactive oxygen species tests and trapping experiments proved that the surface-catalyzed EF effectively broadened the range of solution pH. Density functional theory calculations coupled with electrochemical measurements indicated that the electron transfer rates between Fe-O-C atoms were enhanced with N-doping due to strong interactions between N-Fe bond. The synergistic effects of FeOx and N could improve the oxygen reduction activity for H 2 O 2 generation, and accelerate electron transfer between FeOx/NGr and H 2 O 2 for • OH generation, offering an alternative for wastewater treatment .
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）