Highly Efficient Electroreduction of CO2 on Nickel Single-Atom Catalysts: Atom Trapping and Nitrogen Anchoring

doi:10.1002/smll.201903668

	Highly Efficient Electroreduction of CO2 on Nickel Single-Atom Catalysts: Atom Trapping and Nitrogen Anchoring
	Mou, Kaiwen 3,9,10; Chen, Zhipeng 3,9,10; Zhang, Xinxin 3,9,10; Jiao, Mingyang 9,10; Zhang, Xiangping 4,5,6; Ge, Xin 1,7,8; Zhang, Wei 1,2,7,8; Liu, Licheng 9,10
刊名	SMALL
	2019-10-24
页码	8
关键词	carbon dioxide electrocatalysis Faradaic efficiency single atom sites
ISSN号	1613-6810
DOI	10.1002/smll.201903668
英文摘要	Construction of single atom catalysts (SACs) with high activity toward electroreduction of CO2 still remains a great challenge. A very simple and truly cost-effective synthetic strategy is proposed to prepare SACs via a impregnation-pyrolysis method, through one-step pyrolysis of graphene oxide aerogel. Compared with other traditional methods, this process is fast and free of repeated acid etching, and thus it has great potential for facile operation and large-scale manufacturing. Both X-ray absorption fine structure and high-angle annular dark-field scanning transmission electron microscopy images confirm the presence of isolated nickel atoms, with a high Ni loading of approximate to 2.6 wt%. The obtained 3D porous Ni- and N-codoped graphene aerogel exhibits excellent activity toward electroreduction of CO2 to CO, in particular exhibiting a remarkable CO Faradaic efficiency of 90.2%. Density functional theory calculations reveal that free energies for the formation of intermediate *COOH on coordinatively unsaturated Ni-N sites are significantly lower than that on Ni-N-4 site, suggesting the outstanding activities of CO2 electroreduction originate from coordinatively unsaturated Ni-N sites in catalysts.
资助项目	National Natural Science Foundation of China[21676288] ; National Natural Science Foundation of China[51872115] ; Dalian National Laboratory for Clean Energy (DNL) Cooperation Fund, CAS[DNL 180406] ; Dalian National Laboratory for Clean Energy (DNL) Cooperation Fund, QIBEBT[QIBEBT ZZBS 201805] ; Open Project Program of Wuhan National Laboratory for Optoelectronics[2018WNLOKF022]
WOS关键词	SELECTIVE ELECTROCHEMICAL REDUCTION ; CARBON-DIOXIDE ; GRAPHENE ; FORMATE ; SITES ; CONVERSION
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
语种	英语
出版者	WILEY-V C H VERLAG GMBH
WOS记录号	WOS:000492086800001
资助机构	National Natural Science Foundation of China ; Dalian National Laboratory for Clean Energy (DNL) Cooperation Fund, CAS ; Dalian National Laboratory for Clean Energy (DNL) Cooperation Fund, QIBEBT ; Open Project Program of Wuhan National Laboratory for Optoelectronics
内容类型	期刊论文
源URL	[http://ir.ipe.ac.cn/handle/122111/39136]
专题	中国科学院过程工程研究所
通讯作者	Zhang, Wei; Liu, Licheng
作者单位	1.Jilin Univ, Dept Mat Sci, Changchun 130012, Jilin, Peoples R China 2.Huazhong Univ Sci & Technol, Wuhan Natl Lab Optoelect, Wuhan 430074, Hubei, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 4.Chinese Acad Sci, CAS Key Lab Green Proc & Engn, Beijing 100190, Peoples R China 5.Chinese Acad Sci, Inst Proc Engn, Beijing 100190, Peoples R China 6.Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 7.Jilin Univ, Electron Microscopy Ctr, Changchun 130012, Jilin, Peoples R China 8.Jilin Univ, Key Lab Mobile Mat MOE, Changchun 130012, Jilin, Peoples R China 9.Chinese Acad Sci, CAS Key Lab Biobased Mat, Qingdao 266101, Shandong, Peoples R China 10.Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Qingdao 266101, Shandong, Peoples R China
推荐引用方式 GB/T 7714	Mou, Kaiwen,Chen, Zhipeng,Zhang, Xinxin,et al. Highly Efficient Electroreduction of CO2 on Nickel Single-Atom Catalysts: Atom Trapping and Nitrogen Anchoring[J]. SMALL,2019:8.
APA	Mou, Kaiwen.,Chen, Zhipeng.,Zhang, Xinxin.,Jiao, Mingyang.,Zhang, Xiangping.,...&Liu, Licheng.(2019).Highly Efficient Electroreduction of CO2 on Nickel Single-Atom Catalysts: Atom Trapping and Nitrogen Anchoring.SMALL,8.
MLA	Mou, Kaiwen,et al."Highly Efficient Electroreduction of CO2 on Nickel Single-Atom Catalysts: Atom Trapping and Nitrogen Anchoring".SMALL (2019):8.