Insight into the performance-boosting mechanism of Mn3O4 prepared by reduction method for oxidation of toluene

IF 4.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2025-03-15 Epub Date: 2025-02-15 DOI:10.1016/j.mcat.2025.114917
Xiufeng Shi, Yudong Han, Chen Wang, Haohong Zhang, Lifei Liu, Bin Xing, Xu Wu
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Abstract

Toluene, a typical volatile organic compound (VOCs), is harmful to environment . There are significant challenges for preparing high-perform catalyst and understanding the reaction mechanism of toluene oxidation over trimanganese tetroxide (Mn3O4). Herein, a spiny spherical Mn3O4-H was prepared by reduction method. Mn3O4-H exhibits higher catalytic activity and maintains a stable operation of >90 % conversion of toluene at 230 °C for 100 h. The stronger adsorption ability to oxygen and toluene, abundant surface adsorbed oxygen, the higher lattice oxygen activity, and the stronger redox ability are essential to the performance of Mn3O4-H. The in-situ DRIFTS confirm the branched methyl group on toluene is preferentially oxidized at low temperature, and intermediates including unidentate benzoate and benzene ring metal complexes adsorbed on Mn3O4-H were identified. These findings not only clarify the reaction pathway of toluene oxidation over Mn3O4, but provide a novel design strategy for toluene removal catalysts.

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探讨还原法制备的Mn3O4对甲苯氧化性能的提升机理
甲苯是一种典型的挥发性有机化合物(VOCs),对环境有害。制备高性能催化剂和了解甲苯在四氧化三锰(Mn3O4)上氧化的反应机理是目前面临的重大挑战。本文采用还原法制备了一种针状球形Mn3O4-H。Mn3O4-H表现出较高的催化活性,在230℃下保持100 h甲苯转化率90%的稳定运行。Mn3O4-H对氧和甲苯较强的吸附能力、丰富的表面吸附氧、较高的晶格氧活性和较强的氧化还原能力是Mn3O4-H性能的关键。原位漂移证实了甲苯上的支链甲基在低温下优先氧化,并鉴定了未识别苯甲酸酯和苯环金属配合物等中间体吸附在Mn3O4-H上。这些发现不仅阐明了甲苯在Mn3O4上氧化的反应途径,而且为脱甲苯催化剂的设计提供了一种新的思路。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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