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Ethylene Adsorption on Ag(111), Rh(111) and Ir(111) by (meta)-GGA based Density Functional Theory Calculations
Pei-pei Chen,Bing-yan Zhang,Xiang-kui Gu,Wei-xue Li*
Author NameAffiliationE-mail
Pei-pei Chen State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, China  
Bing-yan Zhang State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, China  
Xiang-kui Gu Department of Chemical Engineering and Materials Science, Wayne State University, Detroit, MI 48202, USA  
Wei-xue Li* Department of Chemical Physics, College of Chemistry and Materials Science, University of Science and Technology of China, Hefei National Laboratory for Physical Sciences at the Microscale, Hefei 230026, China wxli70@ustc.edu.cn 
Abstract:
Accurate description of the adsorption process of reactants on metal surfaces from theory is crucial for mechanistic understanding of activity and selectivity of metal catalysts, but it remains challengeable for the nowadays first-principles theory due to the lack of proper exchange-correlation functional describing the distinct interactions involved. We studied here the potential energy surfaces of ethylene adsorption on Ag(111), Rh(111) and Ir(111) using density functional theory calculations and (meta)-GGA functional including PBE, BEEF-vdW, SCAN, and SCAN+rVV10. For ethylene adsorption on noble metal Ag(111), it is found that BEEF-vdW, SCAN and SCAN+rVV10 predict the presence of the physisorption states only. For Rh(111), both SCAN and SCAN+rVV10 find that there is a precursor physisorption state before the chemisorption state. In contrast, there is no precursor state found based on potential energy surfaces from BEEF-vdW and PBE. Whereas for Ir(111), BEEF-vdW predicts the existence of a rather shallow precursor physisorption state, in addition to the chemisorption state. Irrespective to the transition metals considered, we find that SCAN+rVV10 gives the strongest binding strength, followed by SCAN, and PBE/BEEF-vdW, accordingly. The present work highlights great dependence of potential energy surface of ethylene adsorption on transition metal surfaces and exchange-correlation functionals.
Key words:  Ethylene adsorption, Potential energy curve, Transition metal surface, Exchange-correlation functionals, First-principles theory
FundProject:
采用(meta)-GGA泛函对Ag(111)、Rh(111)和Ir(111)上乙烯吸附的理论研究
陈培培,张冰燕,顾向奎,李微雪*
摘要:
本文针对在多种催化反应的重要中间体乙烯,使用(meta)-GGA等级的包含PBE,BEEF-vdW,SCAN以及SCAN+rVV10在内的多种交换关联泛函,系统研究了在过渡金属表面(Ag,Rh和Ir)上乙烯吸附势能面对泛函的依赖关系. 研究发现,对于乙烯在贵金属Ag(111)上的吸附,除了PBE外,BEEF-vdW,SCAN以及SCAN+rVV10均能预测出物理吸附态的存在. 对于乙烯在Rh(111)面的吸附,SCAN和SCAN+rVV10预测在化学吸附位之前存在有物理吸附前驱态,而基于PBE和BEEF-vdW的势能面并没有发现前驱态的存在. 而对于乙烯在Ir(111)上的吸附,BEEF-vdW也能微弱地预测出化学吸附前驱态的存在. 研究结果表明,无论在哪一种金属表面上,四种泛函中SCAN+rVV10给出的吸附能最强,其次是SCAN,最后是PBE或者BEEF-vdW.
关键词:  乙烯吸附,势能面,过渡金属表面,交换关联泛函,第一性原理
DOI:10.1063/1674-0068/cjcp1902035
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