CATALYSIS LETTERS
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2025
·Vol. 155
·期 4
·1-19
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IF 2.4
Gan Yuxin,Liu Dan,Wang Zhipu,Huang Ge,Ze Rumei,Wang Xiaohong,Zhou Jiabin
Iron-based spinel oxides, with excellent catalytic activity and stability, hold promising potential in the photo-Fenton degradation of organic pollutants. In this study, (Fe 0.2 Co 0.2 Ni 0.2 Cu 0.2 Mn 0.2 )Fe 2 O 4 was prepared via the solution combustion method. Multiple characterization techniques confirmed the good stability and morphology of (Fe 0.2 Co 0.2 Ni 0.2 Cu 0.2 Mn 0.2 )Fe 2 O 4 . It exhibited high-entropy oxide properties, making it suitable as a photo-Fenton catalyst for the efficient degradation of oxytetracycline hydrochloride (OTC-HCl). Under visible light (Vis) with 10 mM H 2 O 2 , 0.06 g/L OTC-HCl, and pH 4.0, the catalyst achieved a degradation efficiency of 92.9%. In the photo-Fenton system, the utilization rate of H 2 O 2 (calculated as the ratio of the degradation amount of OTC-HCl to the consumption amount of H 2 O 2 ) was 34.5, which is 8.3 times higher than that of pure H 2 O 2 (4.2). The catalyst showed good acid–base adaptability, achieving OTC-HCl removal rates exceeding 92.0% across a pH range of 3–11, with a reaction rate constant of 0.08 min −1 at pH 11. Free-radical capture experiments showed that (Fe 0.2 Co 0.2 Ni 0.2 Cu 0.2 Mn 0.2 )Fe 2 O 4 catalyzed H 2 O 2 to generate · OH, · O 2 − , and e − , which are the main free radicals involved in the degradation of OTC-HCl. In summary, (Fe 0.2 Co 0.2 Ni 0.2 Cu 0.2 Mn 0.2 )Fe 2 O 4 not only addresses the issue of low H 2 O 2 utilization in traditional photo-Fenton systems but also catalyzes the generation of H 2 O 2 under light conditions. Thus, it can serve as an excellent photo-Fenton catalyst for OTC-HCl degradation. Graphical
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
ACS Catalysis
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2017
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IF 10.614
Meng Liu,Song Shi,Li Zhao,Min Wang,Guozhi Zhu,Xi Zheng,Jin Gao,Jie Xu
A core–shell catalyst (Co–SiO2@Ti–Si) with cobalt-based SiO2 nanocomposite (Co–SiO2) as the core and Ti-doped mesoporous silica as the shell was designed to catalyze a one-pot reaction of sulfide oxidation with in situ generated hydroperoxide. The catalyst was characterized by SEM, TEM, UV–vis spectroscopy, and XPS, among other methods. Compared to Co–SiO2 and the physical mixture of the two components (Co–SiO2 + Ti–Si), the core–shell catalyst significantly enhanced the reaction rate of the sulfide oxidation. The utilization efficiency of the hydroperoxide was an important factor responsible for the differences in the reaction rates. A further mechanism study showed that the improvement of the efficiency was due to the existence of a coordination pathway. The core–shell structure of a bifunctional catalyst represents a strategy for improving the utilization efficiency of hydroperoxide.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Zhiqun Xie,Jiali Zhou,Jinnan Wang,Corvini Philippe François-Xavier,Thomas Wintgens
Novel Fenton-like catalyst γ-Cu-Al 2 O 3 -Bi 12 O 15 Cl 6 with electron-poor Cu centre and electron-rich Bi centre was synthesized for selective degradation of phenolic compounds. Different from electron-rich Cu centre catalysts, the electron-poor Cu centre, which was induced by high electronegativity of Bi, could facilitate the formation of σ-Cu-ligand with phenolic compounds. On one hand, H 2 O 2 could directly oxidize σ-Cu-ligand to HO-adduct radicals with the generation of OH. Meanwhile, Cu(II) in the σ-Cu(II) complexes could be reduced to Cu(I) by oxidization of the HO-adduct radicals to hydroxylation products. Such reaction not only prevented Cu(II) from oxidizing H 2 O 2 to HO 2 /O 2 − but also enhanced the redox cycle of Cu(II)/Cu(I), which improved the catalytic activity and H 2 O 2 utilization. On the other hand, although the σ-Cu-ligand was gradually decreased with the decrease of phenolic compounds, dual-reaction centre played the dominant role in catalytic reaction . In addition, large amounts of oxygen vacancies (OVs) are formed in Bi 12 O 15 Cl 6 during the calcining process (BiOCl→Bi 12 O 15 Cl 6 ) , which can also increase the generation of OH. Thus, both electron-rich Bi center and OVs could still reduce H 2 O 2 to · OH for organics degradation even without the formation of σ-Cu-ligand. Being attributed to the synergistic effect of σ-Cu-ligand, dual-reaction centre and OVs mentioned above, γ-Cu-Al 2 O 3 -Bi 12 O 15 Cl 6 achieved high catalytic activity for phenolic compounds degradation and utilization efficiency of H 2 O 2 (η). In addition, various analytic methods (XPS, TPR, FT-IR, Raman, EPR and solid-state EPR) were used to prove the synergistic effect of the electron-poor/rich centre, σ-Cu-ligand and OVs of catalyst.
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
CHEMICAL ENGINEERING SCIENCE
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2024
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IF 4.1
Yang Xu,Dong Lin,Ze Zong,Qiuming He,Zhe Ma,Xuliang Deng,De Chen,Chaohe Yang,Xiang Feng
Demetalation-metalation method has gained prominence for its higher metal loading, efficiency and shortened synthetic period, particularly in the incorporation of metal atoms with large radii into zeolite framework in recent years. An ammonia-regulated approach has been developed for selectively evolved deep-substituted Ti precursors in dealuminized beta zeolites, which enables a controlled promotion of metalation of Ti atoms. Additionally, this ammonia-regulated approach could also enhance 1-hexene kinetic adsorption by constructing mesopores, which is demonstrated by the lower reaction order of 1-hexene. The synthesized ammonia-regulated N-Ti-beta exhibits rich framework Ti species and a high specific surface area, leading to significantly improved 1-hexene epoxidation performance (conversion of 61%, selectivity of 98%, and a high H 2 O 2 utilization efficiency of 93%). This study not only provides a new strategy to dynamically regulate evolution of Ti precursors by ammonia but also holds promise for advancing related industrial processes in demetalation-metalation methods.
研究领域:
催化
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材料科学
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化学工程
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DOI
高影响因子
Nature Communications
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2024
·Vol. 15
·期 1
·1-12
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IF 14.7
Jiang Xiaoyi,Ke Le,Zhao Kai,Yan Xiaoyu,Wang Hongbo,Cao Xiaojuan,Liu Yuchen,Li Lingjiao,Sun Yifei,Wang Zhiping,Dang Dai,Yan Ning
Electrochemical carbon dioxide reduction reaction using sustainable energy is a promising approach of synthesizing chemicals and fuels, yet is highly energy intensive. The oxygen evolution reaction is particularly problematic, which is kinetically sluggish and causes anodic carbon loss. In this context, we couple CO 2 electrolysis with hydrogen oxidation reaction in a single electrochemical cell. A Ni(OH) 2 /NiOOH mediator is used to fully suppress the anodic carbon loss and hydrogen oxidation catalyst poisoning by migrated reaction products. This cell is highly flexible in producing either gaseous (CO) or soluble (formate) products with high selectivity (up to 95.3%) and stability (>100 h) at voltages below 0.9 V (50 mA cm −2 ). Importantly, thanks to the “transferred” oxygen evolution reaction to a water electrolyzer with thermodynamically and kinetically favored reaction conditions, the total polarization loss and energy consumption of our H 2 -integrated CO 2 reduction reaction, including those for hydrogen generation, are reduced up to 22% and 42%, respectively. This work demonstrates the opportunity of combining CO 2 electrolysis with the hydrogen economy, paving the way to the possible integration of various emerging energy conversion and storage approaches for improved energy/cost effectiveness.
研究领域:
电化学
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能源转换与存储
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可持续能源
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DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）