期刊
ACS NANO
卷 13, 期 3, 页码 3177-3187出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.8b08692
关键词
bottom-up fabrication; single molecular building blocks; ORR; Cu-N-4 active sites; orbital symmetry
类别
资金
- National Natural Science Foundation of China [21363012, 51374117, 11764026, 51764030]
Bottom-up construction of efficient active sites in transition metal-nitrogen-carbon (M-N-C) catalysts for oxygen reduction reaction (ORR) from single molecular building blocks remains one of the most difficult challenges. Herein, we report a bottom-up approach to produce a highly active Cu-N-4-C catalyst with well-defined Cu-N-4 coordination sites derived from a small molecular copper complex containing Cu-N-4 moieties. The Cu-N-4 moieties were found to be covalently integrated into graphene sheets to create the Cu-N-4 active sites for ORR. Furthermore, the activity was boosted by tuning the structure of active sites. We find that the high ORR activity of the Cu-N-4-C catalyst is related to the Cu-N-4 center linked to edges of the graphene sheets, where the electronic structure of the Cu center has the right symmetry for the degenerate pi* orbital of the O-2 molecule. These findings point out the direction for the synthesis of the M-N-C catalysts at the molecular level.
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