Critical Role of Interfacial Sites between Nickel and CeO2 Support in Dry Reforming of Methane: Revisit of Reaction Mechanism and Origin of Stability

doi:10.1021/acs.jpcc.9b09856

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	Critical Role of Interfacial Sites between Nickel and CeO2 Support in Dry Reforming of Methane: Revisit of Reaction Mechanism and Origin of Stability
	Lian, Zan 1,2; Olanrele, Samson O.1,2; Si, Chaowei 1,2; Yang, Min 1,2; Li, Bo 2
刊名	JOURNAL OF PHYSICAL CHEMISTRY C
	2020-03-05
卷号	124 期号:9 页码:5118-5124
ISSN号	1932-7447
DOI	10.1021/acs.jpcc.9b09856
通讯作者	Li, Bo(boli@imr.ac.cn)
英文摘要	Dry reforming of methane (DRM) is one of the effective catalytic routes to utilize methane and carbon dioxide molecules. The supported Ni catalysts on lanthanide oxides show remarkable reactivities and stabilities in DRM. However, it remains inconclusive regarding the mechanism and origin of stability of supported Ni catalysts. In this work, first-principles density functional theory (DFT) calculations are performed to investigate the catalytic properties of CeO2-supported Ni-based catalyst. The reactivities of several sites including metal, support, interface, and vacancy on support and interface are evaluated on the same footing for the activation of reactants, CH4 and CO2. The distinct features revealed from comparisons provide the decisive proof to identify the active sites in DRM. Moreover, the different routes leading to the formation of products of H-2 and CO are described. Besides CO2 dissociation, CO is also possibly formed from the successive oxidation of CH*. The stability of catalysts is attributed to the facile elimination of cokes, which are mostly consumed by the interfacial oxygen. The calculations also indicate the inadequate description provided by the current accepted mechanism of supported Ni. Instead, an updated reaction mechanism is proposed, which is consistent with the experimental observations and underscores the importance of interface. The current work not only deepens the understanding of catalytic properties of supported Ni catalysts in DRM but also signifies the effectiveness of interface engineering for the improvement of catalytic performance.
资助项目	NSFC[21573255] ; Natural Science Foundation of Liao Ning Province[20180510014] ; Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science ; State Key Laboratory of Catalytic Materials and Reaction Engineering (RIPP, SINOPEC) ; Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund (the second phase)[U1501501]
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:000518703000020
资助机构	NSFC ; Natural Science Foundation of Liao Ning Province ; Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science ; State Key Laboratory of Catalytic Materials and Reaction Engineering (RIPP, SINOPEC) ; Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund (the second phase)
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/137722]
专题	金属研究所_中国科学院金属研究所
通讯作者	Li, Bo
作者单位	1.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Liaoning, Peoples R China 2.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Liaoning, Peoples R China
推荐引用方式 GB/T 7714	Lian, Zan,Olanrele, Samson O.,Si, Chaowei,et al. Critical Role of Interfacial Sites between Nickel and CeO2 Support in Dry Reforming of Methane: Revisit of Reaction Mechanism and Origin of Stability[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2020,124(9):5118-5124.
APA	Lian, Zan,Olanrele, Samson O.,Si, Chaowei,Yang, Min,&Li, Bo.(2020).Critical Role of Interfacial Sites between Nickel and CeO2 Support in Dry Reforming of Methane: Revisit of Reaction Mechanism and Origin of Stability.JOURNAL OF PHYSICAL CHEMISTRY C,124(9),5118-5124.
MLA	Lian, Zan,et al."Critical Role of Interfacial Sites between Nickel and CeO2 Support in Dry Reforming of Methane: Revisit of Reaction Mechanism and Origin of Stability".JOURNAL OF PHYSICAL CHEMISTRY C 124.9(2020):5118-5124.