文献类型：期刊文献

英文题名：Origin of synergistic effect over Ni-based bimetallic surfaces: A density functional theory study

作者：Fan, Chen[1];Zhu, Yi-An[1];Xu, Yue[1];Zhou, Yan[1];Zhou, Xing-Gui[1];Chen, De[2]

机构：[1]E China Univ Sci & Technol ECUST, 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：2012

卷号：137

期号：1

外文期刊名：JOURNAL OF CHEMICAL PHYSICS

收录：;EI(收录号：20122915253582);WOS:【SCI-EXPANDED(收录号:WOS:000306142600048)】；

基金：This work is supported by the Natural Science Foundation of China (No. 21003046), 973 project of Ministry of Science and Technology of China (No. 2012CB720500), and Fundamental Research Funds for Central Universities (No. WA1014027). The computational time provided by the Notur project is highly acknowledged.

语种：英文

外文关键词：Atoms - Binding energy - Catalyst activity - Palladium alloys - Density functional theory - Methane - Nickel alloys - Electronic structure - Transition metals - Binary alloys

摘要：Density functional theory calculations have been conducted to explore the physical origin of the synergistic effect over Ni-based surface alloys using methane dissociation as a probe reaction. Some late transition metal atoms (M=Cu, Ru, Rh, Pd, Ag, Pt, and Au) are substituted for surface Ni atoms to examine the variation in electronic structure and adsorption property of Ni(111). Two types of threefold hollow sites, namely, the Ni2M and Ni-3 sites, are taken into account. The calculated results indicate that the variation in the CHx adsorption energy at the Ni2M and Ni-3 sites is dominated by the ensemble and ligand effect, respectively, and the other factors such as surface and adsorbate distortion and electrostatic interaction affect the catalytic properties of the bimetallic surfaces to a smaller extent. Both the Bronsted-Evans-Polanyi relationship and the scaling correlation hold true on the Ni-based bimetallic surfaces. With the combination of these two linear energy relations, the corrected binding energy of atomic C is found to be a good descriptor for representing the catalytic activity of the alloyed surfaces. Considering the compromise between the catalytic activity and catalyst stability, we suggest that the Rh/Ni catalyst is a good candidate for methane dissociation. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4731811]