Copper Isolated Sites on N-Doped Carbon Nanoframes for Efficient Oxygen Reduction

被引:33
作者
Huang, Cong [1 ,2 ,3 ]
Zheng, Lirong [4 ]
Feng, Wenshuai [2 ]
Guo, Aimin [2 ]
Gao, Xiaohui [2 ]
Long, Zhen [1 ]
Qiu, Xiaoqing [3 ]
机构
[1] Tianjin Univ Technol, Inst Funct Crystals, Tianjin 300384, Peoples R China
[2] Cent South Univ, Sch Phys & Elect, Changsha 410083, Peoples R China
[3] Cent South Univ, Coll Chem & Chem Engn, Changsha 410083, Peoples R China
[4] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
copper isolated sites; oxygen reduction reaction; ZIF-8; N-doped carbon support; electrochemical catalysis; SINGLE IRON ATOMS; POROUS CARBON; CATALYST; ELECTROCATALYST;
D O I
10.1021/acssuschemeng.0c04094
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
In recent years, metal isolated site catalysts with the high exposure and maximized availability of metal species provide a new route to boost the oxygen reduction performance. However, in the absence of clusters and nanoparticles, the synthesis of this catalyst with metal high-loading, especially for copper, is still a big challenge. In this work, a metal isolated site catalyst with high copper content (1.12 wt %), copper isolated sites anchored on N-doped carbon materials (donated as Cu ISs/NC-1000), was prepared by the pyrolysis of copper acetylacetone within the metal-organic framework (ZIF-8) at 1000 degrees C. The successful preparation of products can be demonstrated by high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption spectra. With the merits of the atomically dispersed surface metal atoms and abundant ORR-favored copper active sites, the present Cu ISs/NC-1000 exhibits an excellent ORR electrochemical activity with a half-wave potential of 0.855 V (vs RHE) and a limiting current density of 5.2 mA cm(-2) in the electrochemical tests, superior to the results from commercial Pt/C and previously reported Cu-based materials. For the durability, the negligible activity decay after 10,000 continuous potential cycles and good resistance to methanol crossover can be noted. The outstanding catalytic activity from the present Cu ISs/NC-1000 demonstrates the superiority of metal isolated sites as electrocatalytic centers.
引用
收藏
页码:14030 / 14038
页数:9
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