Mechanistic Insight into Catalytic Combustion of Ethyl Acetate on Modified CeO2 Nanobelts: Hydrolysis-Oxidation Process and Shielding Effect of Acetates/Alcoholates

Zude Shen; Erhao Gao; Xinyu Meng

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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

机译：Mechanistic Insight into Catalytic Combustion of Ethyl Acetate on Modified CeO2 Nanobelts: Hydrolysis-Oxidation Process and Shielding Effect of Acetates/Alcoholates

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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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《Environmental Science & Technology: ES&T》 |2023年第9期|3864-3874|共11页
作者
Zude Shen; Erhao Gao; Xinyu Meng;
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作者单位

School of Environmental Science and Engineering, Changzhou University, Changzhou 213164 Jiangsu, P. R. China;

School of Environmental Science and Engineering Changzhou University, Changzhou 213164 Jiangsu, P. R. China;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
原文格式 PDF
正文语种英语
中图分类环境科学、安全科学;
关键词
ethyl acetate; catalytic combustion; hydrolysis; CeO2 nanobelts; acetates;

Mechanistic Insight into Catalytic Combustion of Ethyl Acetate on Modified CeO2 Nanobelts: Hydrolysis-Oxidation Process and Shielding Effect of Acetates/Alcoholates

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