文献类型：期刊文献

英文题名：Density functional study of the chemisorption of C₁, C₂ and C₃ intermediates in propane dissociation on Pt(111)

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

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

年份：2010

卷号：321

期号：1-2

起止页码：42

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

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000276696600007)】；

基金：This research was supported by Natural Science Foundation of China (No. 20736011), Doctoral Fund of Ministry of Education of China (No. 200802511007), Natural Science Foundation of Shanghai (No. 08ZR1406300), Shanghai Educational Development Foundation through Chenguang plan (No. 2007CG41), and "111" Project (No. B08021).

语种：英文

外文关键词：Propane; Pt(111); Adsorption; Propylene; DFT

摘要：DFT-GGA calculations have been used to study the chemisorption of CHx (x = 0-3). C2Hy (y = 3-5) and C3Hz (z = 3-8) on Pt(1 1 1) at the coverage of 1/9 ML The adsorption energies, favored binding sites and geometric parameters of adsorption configurations are determined. All the carbonaceous species are found to be adsorbed on Pt(1 1 1) with C atoms sp(3)-hybridized. The geometries of adsorption configurations have been compared with published experimental data to evaluate the reliability of our calculation method. The calculated adsorption energies of C-1 species, ranked in descending order, are as follows, C > CH > CH2 > CH3, and the similar trend has been observed with respect to the chemisorption of C-2 species. As for the C-3 species, propylene prefers binding to the surface in the di-sigma mode and the adsorption energy is calculated to be -0.93 eV. The stepwise dehydrogenation of propane to propynyl (CCCH3) is investigated by calculating the change of reaction heat, which suggests that propylidyne (CCH2CH3) is the most stable species on Pt(1 1 1). Based on the adsorption energies and Bronsted-Evans-Polanyi (BEP) analysis, propyne is predicted to be the most likely starting point for the C-C scission. (C) 2010 Elsevier B.V. All rights reserved.