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Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading
Zhao, Shiyong; Wang, Tianshuai; Zhou, Guanmin; Zhang, Liji; Lin, Chao; Veder, Jean-Pierre; Johannessen, Bernt; Saunders, Martin; Yin, Lichang; Liu, Chang; De Marco, Roland; Yang, Shi-Ze; Zhang, Qianfan; Jiang, San Ping
2020-07-01
Source PublicationCHEMNANOMAT
Volume6Issue:7Pages:1063-1074
AbstractSingle-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.
DOI10.1002/cnma.202000223
WOS IDWOS:000529198500001
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Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/82927
Collection中国科学院金属研究所
Recommended Citation
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,2020,6(7):1063-1074.
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,6(7),1063-1074.
MLA Zhao, Shiyong,et al."Controlled One-pot Synthesis of Nickel Single Atoms Embedded in Carbon Nanotube and Graphene Supports with High Loading".CHEMNANOMAT 6.7(2020):1063-1074.
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