Mechanistic Insights into Ethylene Transformations on Ir(111) by Density Functional Calculations and Microkinetic Modeling

doi:10.1002/cphc.201700051

CORC > 青岛生物能源与过程研究所 > 中国科学院青岛生物能源与过程研究所 > 微藻生物技术团队

	Mechanistic Insights into Ethylene Transformations on Ir(111) by Density Functional Calculations and Microkinetic Modeling
	Shi, Xue-Rong 1,2; Kong, Haijuan 1; Wang, Shengguang 3; Wang, Hui 4; Qin, Zhangfeng 5; Wang, Jianguo 5
刊名	CHEMPHYSCHEM
	2017-04-19
卷号	18 期号:8 页码:906-916
关键词	Carbon Monomers Density Functional Theory Ethylene Ir(111) Microkinetic Modeling
DOI	10.1002/cphc.201700051
文献子类	Article
英文摘要	Ethylidyne, ethane, and carbon monomer formations from ethylene over Ir(111) at different coverages are investigated using density functional theory methods. Two possible reaction mechanisms for ethylidyne formation are investigated. The calculations show that vinyl prefers the dehydrogenation to yield vinylidene (M2) over the hydrogenation to produce ethylidene (M1) kinetically and thermodynamically at 1/9 (1/3) ML. Ethylidyne formation could be a competitive side reaction of ethylene hydrogenation, however, the ethylidyne species does not directly participate in the ethylene hydrogenation mechanism. The mechanism for C monomer formation is also studied. Microkinetic modeling shows that the ethylene hydrogenation reactivity decreases in the sequence Ir(111) > Rh(111) > Pd(111) > Pt(111) under typical hydrogenation conditions. The catalytic activity of ethylene hydrogenation decreases with increased stability of ethylene adsorption and reaction barrier of the rate-limiting step.
WOS关键词	TRANSITION-METAL SURFACES ; TOTAL-ENERGY CALCULATIONS ; FINDING SADDLE-POINTS ; WAVE BASIS-SET ; CATALYTIC-HYDROGENATION ; ETHYLIDYNE FORMATION ; ADSORPTION ; PT(111) ; ETHENE ; PD
WOS研究方向	Chemistry ; Physics
语种	英语
WOS记录号	WOS:000402711700007
资助机构	National Natural Science Foundation of China(21573270 ; 21603257 ; U1510104)
内容类型	期刊论文
源URL	[http://ir.qibebt.ac.cn/handle/337004/9709]
专题	青岛生物能源与过程研究所_微藻生物技术团队
作者单位	1.Shanghai Univ Engn Sci, Coll Mat Engn, Shanghai 201620, Peoples R China 2.Univ Innsbruck, Inst Phys Chem, Innrain 80-82, Innsbruck, Austria 3.Univ Houston, Dept Chem & Biomol Engn, Houston, TX 77204 USA 4.Chinese Acad Sci, Key Lab Biofuels, Qingdao Inst Bioenergy & Bioproc Technol, Qingdao 266101, Peoples R China 5.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China
推荐引用方式 GB/T 7714	Shi, Xue-Rong,Kong, Haijuan,Wang, Shengguang,et al. Mechanistic Insights into Ethylene Transformations on Ir(111) by Density Functional Calculations and Microkinetic Modeling[J]. CHEMPHYSCHEM,2017,18(8):906-916.
APA	Shi, Xue-Rong,Kong, Haijuan,Wang, Shengguang,Wang, Hui,Qin, Zhangfeng,&Wang, Jianguo.(2017).Mechanistic Insights into Ethylene Transformations on Ir(111) by Density Functional Calculations and Microkinetic Modeling.CHEMPHYSCHEM,18(8),906-916.
MLA	Shi, Xue-Rong,et al."Mechanistic Insights into Ethylene Transformations on Ir(111) by Density Functional Calculations and Microkinetic Modeling".CHEMPHYSCHEM 18.8(2017):906-916.