文献类型：期刊文献

英文题名：Selective Oxidation of Hydrogen in the Presence of Propylene over Pt-Based Core Shell Nanocatalysts

作者：Yang, Ming-Lei[1,2];Fan, Chen[1,2];Zhu, Yi-An[1,3];Sui, Zhi-Jun[1];Zhou, Xing-Gui[1];Chen, De[4]

机构：[1]E China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]E China Univ Sci & Technol, Minist Educ, Key Lab Adv Control & Optimizat Chem Proc, Shanghai 200237, Peoples R China;[3]E China Univ Sci & Technol, Shanghai Key Lab Multiphase Mat Chem Engn, Shanghai 200237, Peoples R China;[4]Norwegian Univ Sci & Technol NTNU, Dept Chem Engn, N-7491 Trondheim, Norway

年份：2015

卷号：119

期号：37

起止页码：21386

外文期刊名：JOURNAL OF PHYSICAL CHEMISTRY C

收录：;EI(收录号：20153801292087);WOS:【SCI-EXPANDED(收录号:WOS:000361868400013)】；

基金：This research was supported by Natural Science Foundation of China (Nos. 21003046, 21303102, 21403066, and 21473053), 973 Project of Ministry of Science and Technology of China (No. 2012CB720500), and Fundamental Research Funds for Central Universities (No. WA1414043, 222201313006). The computational time provided by the Notur project is highly acknowledged.

语种：英文

外文关键词：Dehydrogenation - Dissociation - Propylene - Catalytic oxidation - Catalyst activity - Nanocatalysts - Density functional theory - Shells (structures)

摘要：Coupling of propane dehydrogenation with selective hydrogen oxidation is a practical strategy to achieve high propylene yield and low energy consumption. In this work, the detailed reaction mechanism on Pt(111) is explored using density functional theory calculations and microkinetic modeling to benefit the design of new catalysts. Calculated results indicate that the O-2 dissociation pathway is dominant for hydrogen oxidation, and the dissociation of O-2 is kinetically relevant. With the comparison between the energy barriers for dehydrogenation and oxidation, propyne is found to be the starting point for C3 oxidation. To obtain a high hydrogen oxidation rate and suppress the consumption of propylene, the catalytic performance of 11 M@Pt = Fe, Co, Ni, Cu, Ru, Rh, Os, Ir, Pd, Ag, and Au) core shell surfaces is examined. Among all the core shells, Ag@Pt not only has a high catalytic activity for hydrogen oxidation, but also exhibits a high selectivity toward propylene and is, therefore, the best candidate for selective hydrogen oxidation in the presence of propylene.