Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading

doi:10.1002/cnma.202000223

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	Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading
	Zhao, Shiyong 1,2; Wang, Tianshuai 3; Zhou, Guanmin 4; Zhang, Liji 5,10; Lin, Chao 3; Veder, Jean-Pierre 6; Johannessen, Bernt 7; Saunders, Martin 8,9; Yin, Lichang 11; Liu, Chang 11
刊名	CHEMNANOMAT
	2020-04-29
页码	13
关键词	Ni single-atom catalysts controlled synthesis carbon nanotube graphene carbon dioxide reduction (CO2RR)
ISSN号	2199-692X
DOI	10.1002/cnma.202000223
通讯作者	Liu, Chang(cliu@imr.ac.cn) ; Zhang, Qianfan(qianfan@buaa.edu.cn) ; Jiang, San Ping(s.jiang@curtin.edu.au)
英文摘要	Single-atom catalysts (SACs) have attracted much attentions due to the advantages of high catalysis efficiency and selectivity. However, the controllable and efficient synthesis of SACs remains a significant challenge. Herein, we report a controlled one-pot synthesis of nickel single atoms embedded on nitrogen-doped carbon nanotubes (NiSA-N-CNT) and nitrogen-doped graphene (NiSA-N-G). The formation of NiSA-N-CNT is due to the solid-to-solid rolling up mechanism during the high temperature pyrolysis at 800 degrees C from the stacked and layered Ni-doped g-C3N4, g-C3N4-Ni structure to a tubular CNT structure. Addition of citric acid introduces an amorphous carbon source on the layered g-C3N4-Ni and after annealing at the same temperature of 800 degrees C, instead of formation of NiSA-N-CNT, Ni single atoms embedded in planar graphene type supports, NiSA-N-G were obtained. The density functional theory (DFT) calculation indicates the introduction of amorphous carbon source substantially reduces the structure fluctuation or curvature of layered g-C3N4-Ni intermediate products, thus interrupting the solid-to-solid rolling process and leading to the formation of planar graphene type supports for Ni single atoms. The as-synthesized NiSA-N-G with Ni atomic loading of similar to 6 wt% catalysts shows a better activity and stability for the CO2 reduction reaction (CO2RR) than NiSA-N-CNT with Ni atomic loading of similar to 15 wt% due to the open and exposed Ni single atom active sites in NiSA-N-G. This study demonstrates for the first time the feasibility in the control of the microstructure of carbon supports in the synthesis of SACs.
资助项目	Australian Research Council[DP180100568] ; Australian Research Council[DP180100731] ; Office of Science of the U.S. Department of Energy[DE-AC02-05CH11231] ; National Science Foundation[ACI-1053575] ; National Natural Science Foundation of China[51521091] ; Australian Research Council LIEF grant[LE120100026]
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science
语种	英语
出版者	WILEY-V C H VERLAG GMBH
WOS记录号	WOS:000529198500001
资助机构	Australian Research Council ; Office of Science of the U.S. Department of Energy ; National Science Foundation ; National Natural Science Foundation of China ; Australian Research Council LIEF grant
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/138628]
专题	金属研究所_中国科学院金属研究所
通讯作者	Liu, Chang; Zhang, Qianfan; Jiang, San Ping
作者单位	1.Curtin Univ, Fuels & Energy Technol Inst, Perth, WA 6102, Australia 2.Curtin Univ, WA Sch Mines Minerals Energy & Chem Engn, Perth, WA 6102, Australia 3.Beihang Univ, Sch Mat Sci & Engn, Beijing 100191, Peoples R China 4.Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA 5.Zhengzhou Univ, Sch Mat Sci & Engn, Zhengzhou 450001, Henan, Peoples R China 6.Curtin Univ, John de Laeter Ctr, Perth, WA 6102, Australia 7.Australian Synchrotron, Clayton, Vic 3168, Australia 8.Univ Western Australia, CMCA, Perth, WA 6009, Australia 9.Univ Western Australia, Sch Mol Sci, Perth, WA 6009, Australia 10.Inst Met Sci & Technol, Shenyang Natl Lab Mat Sci, Engn Alloys Div, Shenyang 110016, Liaoning, Peoples R China
推荐引用方式 GB/T 7714	Zhao, Shiyong,Wang, Tianshuai,Zhou, Guanmin,et al. Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading[J]. CHEMNANOMAT,2020:13.
APA	Zhao, Shiyong.,Wang, Tianshuai.,Zhou, Guanmin.,Zhang, Liji.,Lin, Chao.,...&Jiang, San Ping.(2020).Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading.CHEMNANOMAT,13.
MLA	Zhao, Shiyong,et al."Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading".CHEMNANOMAT (2020):13.