文献类型：期刊文献

英文题名：Total Oxidation of Light Alkane over Phosphate-Modified Pt/CeO2 Catalysts

作者：Huang, Zhenpeng[1,2];Cao, Shiying[1,2];Yu, Jihang[1,2];Tang, Xuan[1,2,3];Guo, Yanglong[1,2];Guo, Yun[1,2];Wang, Li[1,2];Dai, Sheng[3,4];Zhan, Wangcheng[1,2,4]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat & Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Key Lab Adv Mat & Feringa Nobel Prize Scientist J, Sch Chem & Mol Engn, Inst Fine Chem, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Frontiers Sci Ctr Materiobiol & Dynam Chem, Shanghai 200237, Peoples R China

年份：2022

卷号：56

期号：13

起止页码：9661

外文期刊名：ENVIRONMENTAL SCIENCE & TECHNOLOGY

收录：;EI(收录号：20222812345500);WOS:【SCI-EXPANDED(收录号:WOS:000821706600001)】；

语种：英文

外文关键词：phosphorus modification; surface acidity; redox property; propane oxidation; C-H bond

摘要：Developing efficient catalysts for the total oxidation of light alkane at low temperatures is challenging. In this study, superior catalytic performance in the total oxidation of light alkane was achieved by modulating the acidity and redox property of a Pt/CeO2 catalyst through phosphorus modification. Surface modification with phosphorus resulted in electron withdrawal from Pt, leading to platinum species with high valency and the generation of Bronsted acid sites, leading to increased acidity of the Pt/CeO2 catalyst. Consequently, the ability of the Pt/CeO2 catalyst to activate the C-H bond increased with increasing P content in the catalyst owing to the synergistic effect of Pt delta+-(CeO2-POx)(delta-) dipolar catalytic sites. In contrast, the redox property of the Pt/CeO2 catalyst weakened at first; subsequently, it was partially restored owing to the recovery of a part of the bare ceria surface with increasing P content. The turnover frequency in propane oxidation over the phosphate-modified Pt/CeO2 catalyst with a P/Ce atomic ratio of 0.06 was 10-fold higher than that over the unmodified Pt/CeO2 catalyst at 220 degrees C. This comprehensive study not only sheds light on the mechanism underlying the surface modification process but also offers a strategy for realizing higher catalytic activity in the total oxidation of light alkanes.