Wet peroxide oxidation of catechol over copper-based catalysts: inorganic ions effect and degradation pathway of organics

IF 1.7 4区 化学 Q4 CHEMISTRY, PHYSICAL Reaction Kinetics, Mechanisms and Catalysis Pub Date : 2025-01-03 DOI:10.1007/s11144-024-02786-9
Wumin Zhang, Qing Li, Yu Guo, Yanjun Ren, Yao Zhang, Yanyan Xi, Xufeng Lin
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Abstract

In this study, Cu/Al2O3 catalysts were prepared by equal volume wet impregnation for catalytic wet peroxide oxidation (CWPO) of catechol. The crystal structure and elemental composition of the catalysts were investigated by characterization tools like XRD and XPS. The CWPO performance of the catalyst was evaluated through catalytic degradation of catechol in aqueous solution. It was found that 5%Cu/Al2O3 (in wt%) catalyst showed an excellent catalytic performance for catechol degradation. The total organic carbon (TOC) removal rates reached 91% under optimized reaction conditions. Moreover, anions and cations both had an inhibition effect on TOC removal rates. Combined with hydroxyl radical quenching experiments and density functional theory (DFT) study, the catalytic degradation mechanism was proposed to illustrate the degradation pathway of catechol. The catalytic test results as well as the proposed mechanism can provide an insight into studying the degradation pathway of organics in CWPO.

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铜基催化剂上儿茶酚的湿式过氧化氧化:无机离子效应和有机物的降解途径
本研究采用等体积湿浸渍法制备了Cu/Al2O3催化剂,用于催化邻苯二酚湿过氧化物氧化反应。采用XRD、XPS等表征手段对催化剂的晶体结构和元素组成进行了研究。通过对水溶液中儿茶酚的催化降解,评价了催化剂的CWPO性能。结果表明,5%Cu/Al2O3 (wt%)的催化剂对邻苯二酚具有良好的催化性能。在优化的反应条件下,总有机碳(TOC)去除率达到91%。阴离子和阳离子对TOC去除率均有抑制作用。结合羟基自由基猝灭实验和密度泛函理论(DFT)研究,提出了催化降解机理,阐明了邻苯二酚的降解途径。催化实验结果和提出的机理为研究有机污染物在CWPO中的降解途径提供了新的思路。
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来源期刊
CiteScore
3.30
自引率
5.60%
发文量
201
审稿时长
2.8 months
期刊介绍: Reaction Kinetics, Mechanisms and Catalysis is a medium for original contributions in the following fields: -kinetics of homogeneous reactions in gas, liquid and solid phase; -Homogeneous catalysis; -Heterogeneous catalysis; -Adsorption in heterogeneous catalysis; -Transport processes related to reaction kinetics and catalysis; -Preparation and study of catalysts; -Reactors and apparatus. Reaction Kinetics, Mechanisms and Catalysis was formerly published under the title Reaction Kinetics and Catalysis Letters.
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