文献类型：期刊文献

英文题名：Ammonia decomposition on Fe(110), Co(111) and Ni(111) surfaces: A density functional theory study

作者：Duan, Xuezhi[1];Ji, Jian[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 Engn, Shanghai 200237, Peoples R China;[2]Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway

年份：2012

卷号：357

起止页码：81

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

收录：;EI(收录号：20121214886331);WOS:【SCI-EXPANDED(收录号:WOS:000302664000011)】；

基金：This work is financially supported by the Fundamental Research Funds for the Central Universities (WA1114006), the National Basic Research Program of China (2011CB201201), and the 111 Project of Ministry of Education of China (B08021).

语种：英文

外文关键词：Density functional theory; Ammonia decomposition; Fe catalysts; Co catalysts; Ni catalysts

摘要：Ammonia decomposition on transition metal surfaces is of great importance in energy and environmental industries. With the aim to obtain a systematic knowledge about the reaction mechanism of NH3 decomposition on the close-packed surfaces of the 3d-late transition metals, we perform first-principles calculations to determine the preferred adsorption sites and the adsorption energies of NHx (x = 0-3) and H, and identify the transition states of the NH3 stepwise dehydrogenation reactions and the N recombination reactions on the close-packed Fe(1 1 0), Co(1 1 1) and Ni(1 1 1) surfaces. The results show that the calculated adsorption energies and activated energies mainly depend on the d-band center of metal surfaces. Barrier decomposition analysis reveals that the interaction among binding species in transition states will increase the energy barrier while the bonding to the surface of the species in the initial states and the transition states will decrease the energy barrier. Moreover, a linear relationship, known as the Bronsted-Evans-Polanyi relation, also exists between the activation energy of the N recombination reaction and the adsorption energy of N on the close-packed surfaces of the 3d-late transition metals. (C) 2012 Elsevier B.V. All rights reserved.