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Environ. Sci. Technol.合作论文:乙酸乙酯氧化铈上催化燃烧—水解氧化途径、有机酸盐表面聚集

已有 1605 次阅读 2023-2-23 08:10 |个人分类:科研点滴启发|系统分类:论文交流

https://pubs.acs.org/doi/10.1021/acs.est.2c07991

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Mechanistic Insight into Catalytic Combustion of Ethyl Acetate on Modified CeO2 Nanobelts: Hydrolysis–Oxidation Process and Shielding Effect of Acetates/Alcoholates | Environmental Science & Technology (acs.org)

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Abstract

In this study, based on the comparison of two counterparts [Mn- and Cr-modified CeO2 nanobelts (NBs)] with the opposite effects, some novel mechanistic insights into the ethyl acetate (EA) catalytic combustion over CeO2-based catalysts were proposed. The results demonstrated that EA catalytic combustion consisted of three primary processes: EA hydrolysis (C–O bond breakage), the oxidation of intermediate products, and the removal of surface acetates/alcoholates. Rapid EA hydrolysis typically occurs on surface acid/base sites or hydroxyl groups, and the removal of surface acetates/alcoholates resulting from EA hydrolysis is considered the rate-determining step. The deposited acetates/alcoholates like a shield covered the active sites (such as surface oxygen vacancies), and the enhanced mobility of the surface lattice oxygen as an oxidizing agent played a vital role in breaking through the shield and promoting the further hydrolysis–oxidation process. The Cr modification impeded the release of surface-activated lattice oxygen from the CeO2 NBs and induced the accumulation of acetates/alcoholates at a higher temperature due to the increased surface acidity/basicity. Conversely, the Mn-substituted CeO2 NBs with the higher lattice oxygen mobility effectively accelerated the in situ decomposition of acetates/alcoholates and facilitated the re-exposure of surface active sites. This study may contribute to a further mechanistic understanding into the catalytic oxidation of esters or other oxygenated volatile organic compounds over CeO2-based catalysts.




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