Synergy of Single-Atom Ni-1 and Ru-1 Sites on CeO2 for Dry Reforming of CH4

doi:10.1021/jacs.8b10910

	Synergy of Single-Atom Ni-1 and Ru-1 Sites on CeO2 for Dry Reforming of CH4
	Tang, Yu 2,4,5; Wei, Yuechang 2; Wang, Ziyun 3; Zhang, Shiran 2; Li, Yuting 2; Nguyen, Luan 2; Li, Yixiao 2; Zhou, Yan 1; Shen, Wenjie 1; Tao, Franklin Feng 2,4,5
刊名	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
	2019-05-08
卷号	141 期号:18 页码:7283-7293
ISSN号	0002-7863
DOI	10.1021/jacs.8b10910
通讯作者	Tao, Franklin Feng(franklin.feng.tao@ku.edu) ; Hu, Peijun(p.hu@qub.ac.uk)
英文摘要	Heterogeneous catalysis performs on specific sites of a catalyst surface even if specific sites of many catalysts during catalysis could not be identified readily. Design of a catalyst by managing catalytic sites on an atomic scale is significant for tuning catalytic performance and offering high activity and selectivity at a relatively low temperature. Here, we report a synergy effect of two sets of single-atom sites (Ni-1 and Ru-1) anchored on the surface of a CeO2 nanorod, Ce0.95Ni0.025Ru0.025O2. The surface of this catalyst, Ce0.95Ni0.025Ru0.025O2, consists of two sets of single-atom sites which are highly active for reforming CH4 using CO2 with a turnover rate of producing 73.6 H-2 molecules on each site per second at 560 degrees C. Selectivity for producing H-2 at this temperature is 98.5%. The single-atom sites Ni-1 and Ru-1 anchored on the CeO2 surface of Ce0.95Ni0.025Ru0.025O2 remain singly dispersed and in a cationic state during catalysis up to 600 degrees C. The two sets of single-atom sites play a synergistic role, evidenced by lower apparent activation barrier and higher turnover rate for production of H-2 and CO on Ce0.95Ni0.025Ru0.025O2 in contrast to Ce0.95Ni0.05O2 with only Ni-1 single-atom sites and Ce0.95Ru0.05O2 with only Ru-1 single-atom sites. Computational studies suggest a molecular mechanism for the observed synergy effects, which originate at (1) the different roles of Ni-1 and Ru-1 sites in terms of activations of CH4 to form CO on a Ni-1 site and dissociation of CO2 to CO on a Ru-1 site, respectively and (2) the sequential role in terms of first forming H atoms through activation of CH4 on a Ni-1 site and then coupling of H atoms to form H-2 on a Ru-1 site. These synergistic effects of the two sets of single-atom sites on the same surface demonstrated a new method for designing a catalyst with high activity and selectivity at a relatively low temperature.
资助项目	NSF Career Award[NSF-CHE-1462121] ; Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy[DE-SC0014561] ; DOE Office of Science[DE-SC0012704] ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences[DE-AC02-76SF00515]
WOS关键词	INITIO MOLECULAR-DYNAMICS ; TOTAL-ENERGY CALCULATIONS ; COKE FORMATION ; METHANE ; CATALYSTS ; METAL ; CONVERSION ; OXIDATION ; NICKEL ; OXIDE
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000467781600012
资助机构	NSF Career Award ; NSF Career Award ; Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy ; Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy ; DOE Office of Science ; DOE Office of Science ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; NSF Career Award ; NSF Career Award ; Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy ; Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy ; DOE Office of Science ; DOE Office of Science ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; NSF Career Award ; NSF Career Award ; Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy ; Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy ; DOE Office of Science ; DOE Office of Science ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; NSF Career Award ; NSF Career Award ; Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy ; Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy ; DOE Office of Science ; DOE Office of Science ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/171853]
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	Tao, Franklin Feng; Hu, Peijun
作者单位	1.Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 2.Univ Kansas, Dept Chem & Petr Engn, Lawrence, KS 66045 USA 3.Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland 4.Fuzhou Univ, State Key Lab Photocatalysis Energy & Environm, Inst Mol Catalysis & In Situ Operando Studies, Fuzhou 350116, Fujian, Peoples R China 5.Fuzhou Univ, Coll Chem, Fuzhou 350116, Fujian, Peoples R China
推荐引用方式 GB/T 7714	Tang, Yu,Wei, Yuechang,Wang, Ziyun,et al. Synergy of Single-Atom Ni-1 and Ru-1 Sites on CeO2 for Dry Reforming of CH4[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2019,141(18):7283-7293.
APA	Tang, Yu.,Wei, Yuechang.,Wang, Ziyun.,Zhang, Shiran.,Li, Yuting.,...&Hu, Peijun.(2019).Synergy of Single-Atom Ni-1 and Ru-1 Sites on CeO2 for Dry Reforming of CH4.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,141(18),7283-7293.
MLA	Tang, Yu,et al."Synergy of Single-Atom Ni-1 and Ru-1 Sites on CeO2 for Dry Reforming of CH4".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 141.18(2019):7283-7293.