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

文献类型：期刊论文

作者Zhao, Shiyong4,5; Wang, Tianshuai6; Zhou, Guanmin7; Zhang, Liji8,11; Lin, Chao6; Veder, Jean-Pierre9; Johannessen, Bernt10; Saunders, Martin1,2; Yin, Lichang12; Liu, Chang12
刊名CHEMNANOMAT
出版日期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
DOI10.1002/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
WOS记录号WOS:000529198500001
出版者WILEY-V C H VERLAG GMBH
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
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.Univ Western Australia, CMCA, Perth, WA 6009, Australia
2.Univ Western Australia, Sch Mol Sci, Perth, WA 6009, Australia
3.Univ Queensland, Sch Chem & Mol Biosci, Brisbane, Qld 4072, Australia
4.Curtin Univ, Fuels & Energy Technol Inst, Perth, WA 6102, Australia
5.Curtin Univ, WA Sch Mines Minerals Energy & Chem Engn, Perth, WA 6102, Australia
6.Beihang Univ, Sch Mat Sci & Engn, Beijing 100191, Peoples R China
7.Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA
8.Zhengzhou Univ, Sch Mat Sci & Engn, Zhengzhou 450001, Henan, Peoples R China
9.Curtin Univ, John de Laeter Ctr, Perth, WA 6102, Australia
10.Australian Synchrotron, Clayton, Vic 3168, Australia
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.

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来源：金属研究所

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