A critical evaluation of the catalytic role of CO2 in propane dehydrogenation catalyzed by chromium oxide from a DFT-based microkinetic simulation

doi:10.1039/d2cp00027j

IMR OpenIR

	A critical evaluation of the catalytic role of CO2 in propane dehydrogenation catalyzed by chromium oxide from a DFT-based microkinetic simulation
	Zhi, ShuaiKe 1,2; Lian, Zan 1,2; Si, ChaoWei 1,2; Jan, Faheem 1,2; Yang, Min 1,2; Li, Bo 1,2
通讯作者	Li, Bo(boli@imr.ac.cn)
	2022-05-11
发表期刊	PHYSICAL CHEMISTRY CHEMICAL PHYSICS
ISSN	1463-9076
卷号	24 期号:18 页码:11030-11038
摘要	Propane dehydrogenation under CO2 is an important catalytic route to obtain propene with a good balance between selectivity and stability. However, a precise description of the catalytic role of CO2 in propane dehydrogenation is still absent. In this work, we focus on the elucidation of the role of CO2 by using DFT-based microkinetic simulation. The influence of CO2 is categorized as direct and indirect effects. It was found that the chemisorbed CO2 can directly abstract hydrogen from propane and propyl with a comparable barrier to the counterpart at the surface oxygen site. On the other hand, the dissociation of CO2 yields active surface species of CO* and O* which are actively involved in the removal of surface hydroxyls. It is found that the TOFs of both propane conversion and propene formation are significantly increased with the presence of CO2, which is explained by the reduced apparent activation energy. The primary hydrogen abstraction is identified to be the most influential step from the DRC analysis. The main effects of CO2 are concluded to be removing hydrogen and restoring oxygen vacancies from reaction pathway analysis.
资助者	National Natural Science Foundation of China ; Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science ; Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund (the second phase) ; Super Computation of Beijing ; State Key Laboratory of Catalytic Materials and Reaction Engineering (RIPP, SINOPEC)
DOI	10.1039/d2cp00027j
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[21573255] ; Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science ; Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund (the second phase)[U1501501] ; Super Computation of Beijing ; State Key Laboratory of Catalytic Materials and Reaction Engineering (RIPP, SINOPEC)
WOS研究方向	Chemistry ; Physics
WOS类目	Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS记录号	WOS:000787354000001
出版者	ROYAL SOC CHEMISTRY
引用统计	被引频次：9[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/172729
专题	中国科学院金属研究所
通讯作者	Li, Bo
作者单位	1.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China 2.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Liaoning, Peoples R China
推荐引用方式 GB/T 7714	Zhi, ShuaiKe,Lian, Zan,Si, ChaoWei,et al. A critical evaluation of the catalytic role of CO2 in propane dehydrogenation catalyzed by chromium oxide from a DFT-based microkinetic simulation[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2022,24(18):11030-11038.
APA	Zhi, ShuaiKe,Lian, Zan,Si, ChaoWei,Jan, Faheem,Yang, Min,&Li, Bo.(2022).A critical evaluation of the catalytic role of CO2 in propane dehydrogenation catalyzed by chromium oxide from a DFT-based microkinetic simulation.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,24(18),11030-11038.
MLA	Zhi, ShuaiKe,et al."A critical evaluation of the catalytic role of CO2 in propane dehydrogenation catalyzed by chromium oxide from a DFT-based microkinetic simulation".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 24.18(2022):11030-11038.