文献类型：期刊文献

英文题名：Tuning selectivity and stability in propane dehydrogenation by shaping Pt particles: A combined experimental and DFT study

作者：Yang, Ming-Lei[1];Zhu, Jun[2];Zhu, Yi-An[1];Sui, Zhi-Jun[1];Yu, Ying-Da[3];Zhou, Xing-Gui[1];Chen, De[2]

机构：[1]E China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Norwegian Univ Sci & Technol NTNU, Dept Chem Engn, N-7491 Trondheim, Norway;[3]Norwegian Univ Sci & Technol NTNU, Dept Mat Sci & Engn, N-7491 Trondheim, Norway

年份：2014

卷号：395

起止页码：329

外文期刊名：JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL

收录：;EI(收录号：20144100088690);WOS:【SCI-EXPANDED(收录号:WOS:000347498500042)】；

基金：This research was supported by 973 Project of Ministry of Science and Technology of China (No. 2012CB720500), Natural Science Foundation of China (No. 21003046, 21403066, and 21473053), Fundamental Research Funds for Central Universities (No. WA1313006), and China Postdoctoral Science Foundation (No. 2013M531143). The computational time provided by the Notur project (NN4685K) is highly acknowledged.

语种：英文

外文关键词：Shaped metal particle; DFT; Pt; Propane dehydrogenation

摘要：Shaped metal particles are known to possess distinct catalytic properties, which is often attributed to the catalytic activities of different particle facets. In this contribution, propane dehydrogenation on Pt particles of different shapes is investigated by a combination of experiments and DFT calculations. The selectivity toward propylene and catalyst stability in propane dehydrogenation can be enhanced by shaping Pt nanoparticles under industrially relevant conditions. Octahedral particles (12.0 nm) dominated by the Pt(1 1 1) surface have higher selectivity toward propylene production and better stability than cubic particles (11.5 nm) that are dominated by the Pt(1 0 0) surface. Combined experiments and DFT calculations suggest that the weakened binding strength of propylene and increased energy barrier for the C-H bond cleavage in propylene dehydrogenation on Pt(1 1 1) compared to Pt(1 0 0) and Pt(2 1 1) contribute to the higher selectivity toward propylene by lowering the formation possibility of the deeply dehydrogenated intermediates. When coke is formed on the Pt surface, the d-band of surrounding Pt atoms is shifted farther below the Fermi level, leading to the deactivation of Pt catalyst. Our DFT calculations provide a rational interpretation of the experimental observations regarding the shape effects on propane dehydrogenation. (C) 2014 Elsevier B.V. All rights reserved.