Theoretical Investigation of CO2 Adsorption and Dissociation on Low Index Surfaces of Transition Metals

doi:10.1016/acs.jpcc.7b12660

	Theoretical Investigation of CO2 Adsorption and Dissociation on Low Index Surfaces of Transition Metals
	Liu, Xuejing; Deng, Wei-Qiao; Sun, Lei
刊名	JOURNAL OF PHYSICAL CHEMISTRY C
	2018-04-19
卷号	122 期号:15 页码:8306-8314
ISSN号	1932-7447
DOI	10.1016/acs.jpcc.7b12660
文献子类	Article
英文摘要	Adsorption and dissociation processes of gas molecules on bulk materials and nanomaterials are essential for catalytic conversion of carbon dioxide (CO2). In this work, we systematically investigated the CO2 adsorption and dissociation on low index surfaces of different transition metals by Density Functional Theory (DFT) calculations. A comparison study demonstrates that the open surfaces (Fe(100), Ni(100), Ni(110), Rh(100), and Ir(100)) have stronger interactions with CO2 molecules than the close-packed surfaces. The order of energy barriers for CO2 dissociation is Fe(110), Ir(100) < Ru(0001), Rh(100), Co(0001), Ni(100) < Os(0001), Ni(111) < Ir(111), Rh(111), Ni(110) < Fe(100), Pt(111) < Cu(100), Pd(111) < Cu(111). The interaction order between the dissociative CO, O species and the surfaces is Fe(100) > Fe(110) > Ru(0001) > Os(0001) > Ir(100), Rh(100) > Ni(110) > Co(0001) > Rh(111), Ir(111) > Ni(100), Ni(111) > Cu(100) > Pt(111) > Cu(111), Pd(111). In addition, we found that the change trend of adsorption energy is consistent with that of charge transfer amounts from the low index surfaces to CO2. The Bronsted-Evans-Polanyi relation showed that the electronic effects of Ni(111) and Ni(110), Cu(111) and Cu(100) and the geometric effects of Fe(110) and Fe(100), Ir(111) and Ir(100) have great influence on the CO2 dissociation, which is closely related to cleavage of C-O in transition states. Our results may provide an insight into the design of highly efficient nanocatalysts for CO2-involved reactions.
WOS关键词	GENERALIZED GRADIENT APPROXIMATION ; SHAPE-CONTROLLED SYNTHESIS ; DENSITY-FUNCTIONAL THEORY ; TOTAL-ENERGY CALCULATIONS ; AUGMENTED-WAVE METHOD ; CARBON-DIOXIDE ; FCC METALS ; BASIS-SET ; ACTIVATION ; CATALYSIS
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:000430896500030
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/167194]
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	Deng, Wei-Qiao
作者单位	Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	Liu, Xuejing,Deng, Wei-Qiao,Sun, Lei. Theoretical Investigation of CO2 Adsorption and Dissociation on Low Index Surfaces of Transition Metals[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2018,122(15):8306-8314.
APA	Liu, Xuejing,Deng, Wei-Qiao,&Sun, Lei.(2018).Theoretical Investigation of CO2 Adsorption and Dissociation on Low Index Surfaces of Transition Metals.JOURNAL OF PHYSICAL CHEMISTRY C,122(15),8306-8314.
MLA	Liu, Xuejing,et al."Theoretical Investigation of CO2 Adsorption and Dissociation on Low Index Surfaces of Transition Metals".JOURNAL OF PHYSICAL CHEMISTRY C 122.15(2018):8306-8314.