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Environ Sci Technol


Title:Mechanistic Insight into Catalytic Combustion of Ethyl Acetate on Modified CeO(2) Nanobelts: Hydrolysis-Oxidation Process and Shielding Effect of Acetates/Alcoholates
Author(s):Shen Z; Gao E; Meng X; Xu J; Sun Y; Zhu J; Li J; Wu Z; Wang W; Yao S; Dai Q;
Address:"School of Environmental Science and Engineering, Changzhou University, Changzhou 213164, Jiangsu, P. R. China. Key Laboratory for Advanced Materials, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, P. R. China"
Journal Title:Environ Sci Technol
Year:2023
Volume:20230222
Issue:9
Page Number:3864 - 3874
DOI: 10.1021/acs.est.2c07991
ISSN/ISBN:1520-5851 (Electronic) 0013-936X (Linking)
Abstract:"In this study, based on the comparison of two counterparts [Mn- and Cr-modified CeO(2) nanobelts (NBs)] with the opposite effects, some novel mechanistic insights into the ethyl acetate (EA) catalytic combustion over CeO(2)-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 CeO(2) NBs and induced the accumulation of acetates/alcoholates at a higher temperature due to the increased surface acidity/basicity. Conversely, the Mn-substituted CeO(2) 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 CeO(2)-based catalysts"
Keywords:Hydrolysis Oxidation-Reduction *Acetates/chemistry *Oxygen CeO2 nanobelts acetates catalytic combustion ethyl acetate;
Notes:"MedlineShen, Zude Gao, Erhao Meng, Xinyu Xu, Jiacheng Sun, Yan Zhu, Jiali Li, Jing Wu, Zuliang Wang, Wei Yao, Shuiliang Dai, Qiguang eng Research Support, Non-U.S. Gov't 2023/02/23 Environ Sci Technol. 2023 Mar 7; 57(9):3864-3874. doi: 10.1021/acs.est.2c07991. Epub 2023 Feb 22"

 
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