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

doi:10.1002/cphc.201700051

QIBEBT-IR > 微藻生物技术研究组

	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
	2017-04-19
发表期刊	CHEMPHYSCHEM
卷号	18 期号:8 页码:906-916
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.
文章类型	Article
关键词	Carbon Monomers Density Functional Theory Ethylene Ir(111) Microkinetic Modeling
WOS标题词	Science & Technology ; Physical Sciences
DOI	10.1002/cphc.201700051
关键词[WOS]	TRANSITION-METAL SURFACES ; TOTAL-ENERGY CALCULATIONS ; FINDING SADDLE-POINTS ; WAVE BASIS-SET ; CATALYTIC-HYDROGENATION ; ETHYLIDYNE FORMATION ; ADSORPTION ; PT(111) ; ETHENE ; PD
收录类别	SCI
语种	英语
WOS研究方向	Chemistry ; Physics
项目资助者	National Natural Science Foundation of China(21573270 ; 21603257 ; U1510104)
WOS类目	Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS记录号	WOS:000402711700007
引用统计
文献类型	期刊论文
条目标识符	http://ir.qibebt.ac.cn/handle/337004/9709
专题	微藻生物技术研究组
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.