Dry reforming of methane over the cobalt catalyst: Theoretical insights into the reaction kinetics and mechanism for catalyst deactivation

doi:10.1016/j.apcatb.2020.118859

	Dry reforming of methane over the cobalt catalyst: Theoretical insights into the reaction kinetics and mechanism for catalyst deactivation
	Chen, Shuyue1,2,3 ; Zaffran, Jeremie1 ; Yang, Bo1
	2020-08-05
发表期刊	APPLIED CATALYSIS B-ENVIRONMENTAL
ISSN	0926-3373
EISSN	1873-3883
卷号	270
发表状态	已发表
DOI	10.1016/j.apcatb.2020.118859
摘要	Cobalt shows high catalytic activity for the important dry reforming of methane (DRM) reaction. However, it is prone to deactivation and the corresponding mechanism remains controversial. In this work, we combined density functional theory calculations and microkinetic modeling to study the active site and reaction mechanism of Co catalyzed DRM reaction, employing face centered cubic Co(111) and Co(211) as models. It was found that the step site over Co(211) is the active site for the reaction, and on Co(111), the C+O and CH+O paths are the preferred reaction pathways, while the C+O path is dominant on Co(211). The dissociation of CH4 is the rate-controlling step of DRM over both Co(111) and Co(211). We found that Co(111) is mainly deactivated due to carbon deposition whilst Co(211) undergoes surface oxidization. In addition, Co(111) tends to follow the surface carbon coupling mechanism, and surface carbon clusters formed will lead to catalyst deactivation.
关键词	Dry reforming of methane Cobalt catalyst Catalyst deactivation Reaction kinetics DFT
收录类别	SCI ; SCIE ; EI
资助项目	National Natural Science Foundation of China[91745102] ; National Natural Science Foundation of China[21950410522]
WOS研究方向	Chemistry ; Engineering
WOS类目	Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical
WOS记录号	WOS:000526110500017
出版者	ELSEVIER
EI入藏号	20201108284791
EI主题词	Association reactions ; Catalyst activity ; Catalytic reforming ; Cobalt ; Density functional theory ; Methane ; Reaction kinetics
EI分类号	Nonferrous Metals and Alloys excluding Alkali and Alkaline Earth Metals:549.3 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Probability Theory:922.1
WOS关键词	DENSITY-FUNCTIONAL THEORY ; TOTAL-ENERGY CALCULATIONS ; NI-BASED CATALYSTS ; CO-BASED CATALYSTS ; CARBON-DIOXIDE ; REDUCTION TEMPERATURE ; SYNTHESIS GAS ; SUPPORTED NI ; COMBINED DFT ; HYDROGENATION
原始文献类型	Article
引用统计
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/119312
专题	物质科学与技术学院_PI研究组_杨波组物质科学与技术学院_博士生
通讯作者	Yang, Bo
作者单位	1.Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China 2.Chinese Acad Sci, Shanghai Adv Res Inst, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai 201210, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
第一作者单位	物质科学与技术学院
通讯作者单位	物质科学与技术学院
第一作者的第一单位	物质科学与技术学院
推荐引用方式 GB/T 7714	Chen, Shuyue,Zaffran, Jeremie,Yang, Bo. Dry reforming of methane over the cobalt catalyst: Theoretical insights into the reaction kinetics and mechanism for catalyst deactivation[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2020,270.
APA	Chen, Shuyue,Zaffran, Jeremie,&Yang, Bo.(2020).Dry reforming of methane over the cobalt catalyst: Theoretical insights into the reaction kinetics and mechanism for catalyst deactivation.APPLIED CATALYSIS B-ENVIRONMENTAL,270.
MLA	Chen, Shuyue,et al."Dry reforming of methane over the cobalt catalyst: Theoretical insights into the reaction kinetics and mechanism for catalyst deactivation".APPLIED CATALYSIS B-ENVIRONMENTAL 270(2020).