文献类型：期刊文献

英文题名：First-principles calculations of ammonia decomposition on Ni(110) surface

作者：Duan, Xuezhi[1];Qian, Gang[1];Fan, Chen[1];Zhu, Yian[1];Zhou, Xinggui[1];Chen, De[2];Yuan, Weikang[1]

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

年份：2012

卷号：606

期号：3-4

起止页码：549

外文期刊名：SURFACE SCIENCE

收录：;EI(收录号：20120214671455);WOS:【SCI-EXPANDED(收录号:WOS:000300458600069)】；

基金：This work is financially supported by the National Basic Research Program of China (No. 2011CB201201) and the 111 Project of Ministry of Education of China (B08021).

语种：英文

外文关键词：Density functional theory; Ni catalysts; Ammonia decomposition; Structure sensitivity; Kinetic analysis

摘要：First-principles calculations based on density functional theory (DFT) have been performed to study the adsorption and decomposition of NH3 on Ni(110). The adsorption sites, the adsorption energies, the transition states and the activation energies of the stepwise dehydrogenation of NH3 and the associative desorption of N are determined, and the zero point energy correction is included, which makes it possible to compute the rate constants of the elementary steps in NH3 decomposition. Combined DFT calculations and kinetic analysis at 350 K indicate that the associative desorption of N has a reaction rate lower than NHx dehydrogenation and is therefore the rate determining step. The distinctly different rate constants over Ni(110), Ni(111) and Ni(211) imply that ammonia decomposition over Ni-based catalyst is a structure-sensitive reaction. (C) 2011 Elsevier B.V. All rights reserved.