文献类型：期刊文献

英文题名：Effects of Oxygen Vacancy and Pt Doping on the Catalytic Performance of CeO2 in Propane Dehydrogenation: A First-Principles Study

作者：Zeeshan, Muhammad[1];Chang, Qing-Yu[1];Zhang, Jun[1];Hu, Ping[1];Sui, Zhi-Jun[1];Zhou, Xing-Gui[1];Chen, De[2];Zhu, Yi-An[1]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, UNILAB, Shanghai 200237, Peoples R China;[2]Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway

年份：2021

卷号：39

期号：9

起止页码：2391

外文期刊名：CHINESE JOURNAL OF CHEMISTRY

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000668883200001)】；

基金：This work is supported by the Natural Science Foundation of China (Nos. 91645122 and 22073027), the Natural Science Foundation of Shanghai (No. 20ZR1415800), the National Key Research and Development Program of China (No. 2018YFB0604700), and the Fundamental Research Funds for the Central Universities (No. 222201718003). The computational time provided by the Notur project is highly acknowledged.

语种：英文

外文关键词：Dehydrogenation; Adsorption; Doping; Heterogeneous catalysis; Ab initio calculations

摘要：Main observation and conclusion The catalytic properties of the CeO2 catalyst for propane dehydrogenation (PDH) are examined by employing the density functional theory calculations. Surface modifications and their effects on the surface reactivity are explored by creating the oxygen vacancy and single Pt atom doping. A comparative study between the binding energies of the different PDH reaction species reveals a considerable Lewis acid-base interaction over the pristine and defective surfaces, which dominantly strengthens the bond formation between the adsorbates and the catalyst surface, resulting in the enhancement of surface reactivity. The creation of oxygen vacancy and doping the CeO2(111) surface with single Pt atoms changes the charge distribution over the surface on account of excess 4f electrons. This electronic change increases the bond formation abilities of the inactive Ce atom and hence increases the adsorption strength. Oxygen vacancy in the defective CeO2(111) surface migrates over the surface with the addition of an appropriate adsorbate. Moreover, it is revealed that the propylene is more strongly adsorbed on the single-Pt-atom-doped CeO2(111) surface than the pristine and defective surfaces, which decreases the deep dehydrogenation energy barrier and ultimately results in the lowering of the selectivity.