CO Dissociation on Face-Centered Cubic and Hexagonal Close-Packed Nickel Catalysts: A First-Principles Study

doi:10.1021/acs.jpcc.6b08742

	CO Dissociation on Face-Centered Cubic and Hexagonal Close-Packed Nickel Catalysts: A First-Principles Study
	Zhang, Bing-Yan 2; Liu, Jin-Xun 1,2; Chen, Pei-Pei 2; Su, Hai-Yan 2; Li, Wei-Xue 1,2
刊名	JOURNAL OF PHYSICAL CHEMISTRY C
	2016-11-03
卷号	120 期号:43 页码:24895-24903
ISSN号	1932-7447
DOI	10.1021/acs.jpcc.6b08742
文献子类	Article
英文摘要	Exploring the dependence of the structure activity relationship of catalysts is important for improving the activity and selectivity in heterogeneous catalysis. Among other factors, the influence of the crystal phases, face-centered cubic (FCC) and hexagonal close packed (HCP), of Ni catalysts on CO dissociation is studied by density functional theory (DFT). Surface energies of numerous FCC and HCP facets are calculated to construct the corresponding morphologies, and the exposed facets (six facets for FCC Ni and five facets for HCP Ni) are used to investigate the CO dissociation. For FCC Ni, (311) is the most active facet with the least barrier of 1.58 eV, followed by (100) and (211) with barriers of 1.63 and 1.75 eV, respectively. For HCP Ni, (10 (1) over bar2) is the most active facet with the least barrier of 1.73 eV, followed by (10 (1) over bar1) with a barrier of 1.86 eV. On both FCC and HCP Ni, CO dissociation shows a dramatic structural sensitivity irrespective of direct or H-assisted pathway. Compared to;the direct dissociation, the H-assisted dissociation is kinetically favorable on both FCC and HCP Ni. With increase of dissociation barrier, the preferred dissociation pathway changes from COH intermediate to CHO intermediate. FCC Ni can expose abundant facets with low barrier. The result is compared with more active cobalt catalysts showing an opposite dependence on the crystal phases. The revealed insights regarding the crystal phase and the composition of catalysts upon activation of the diatomic molecules provide a new perspective for rational design of catalysts to expose more active sites for a higher specific activity.
WOS关键词	FISCHER-TROPSCH SYNTHESIS ; COBALT PARTICLE-SIZE ; DENSITY-FUNCTIONAL THEORY ; MINIMUM ENERGY PATHS ; ELASTIC BAND METHOD ; STRUCTURE SENSITIVITY ; METHANOL SYNTHESIS ; BOND SCISSION ; CRYSTAL PHASE ; SADDLE-POINTS
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000387198400043
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/169838]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Li, Wei-Xue
作者单位	1.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, CAS Ctr Excellence Nanosci,Coll Chem & Mat Sci, iChEM Collaborat Innovat Ctr Chem Energy Mat, Hefei, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, State Key Lab Catalysis, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	Zhang, Bing-Yan,Liu, Jin-Xun,Chen, Pei-Pei,et al. CO Dissociation on Face-Centered Cubic and Hexagonal Close-Packed Nickel Catalysts: A First-Principles Study[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2016,120(43):24895-24903.
APA	Zhang, Bing-Yan,Liu, Jin-Xun,Chen, Pei-Pei,Su, Hai-Yan,&Li, Wei-Xue.(2016).CO Dissociation on Face-Centered Cubic and Hexagonal Close-Packed Nickel Catalysts: A First-Principles Study.JOURNAL OF PHYSICAL CHEMISTRY C,120(43),24895-24903.
MLA	Zhang, Bing-Yan,et al."CO Dissociation on Face-Centered Cubic and Hexagonal Close-Packed Nickel Catalysts: A First-Principles Study".JOURNAL OF PHYSICAL CHEMISTRY C 120.43(2016):24895-24903.