Metal-organic framework-derived mesoporous carbon nanoframes embedded with atomically dispersed Fe-Nx active sites for efficient bifunctional oxygen and carbon dioxide electroreduction

被引:221
作者
Chen, Xi [1 ,2 ]
Ma, Dong-Dong [1 ]
Chen, Bo [3 ]
Zhang, Kexin [4 ]
Zou, Roqiang [4 ]
Wu, Xin-Tao [1 ]
Zhu, Qi-Long [1 ]
机构
[1] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore
[4] Peking Univ, Coll Engn, Dept Mat Sci & Engn, Beijing Key Lab Theory & Technol Adv Battery Mat, Beijing 100871, Peoples R China
基金
中国国家自然科学基金;
关键词
Single-atom catalysts; Large mesopores; Bifunctional electrocatalysis; Oxygen reduction reaction; Carbon dioxide reduction; HIGH-SURFACE-AREA; POROUS CARBON; REDUCTION; CATALYSTS; CO2; IRON; NITROGEN; DESIGN; ELECTROCATALYST; EXPOSURE;
D O I
10.1016/j.apcatb.2020.118720
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Metal-organic frameworks (MOFs) can be utilized as superior precursors to pyrolytically achieve the single-atom catalysts. However, most of the atomic active sites are buried inside the microporous carbon matrix, which severely impedes the accessibility of active sites and limits mass transport. Herein, the mesoporous carbon nanoframes with hierarchical pore size distribution and atomically dispersed Fe-N-x active sites were synthesized from Fe-doped MOF precursors. The dense Fe atoms within the nanostructures are dispersed in single-atom level with metalloporphyrin-like Fe-N-4 configuration. The introduction of plentiful large mesopores into the nanoframes would not only enhance the accessibility of abundant single-atom active sites, but also boost mass and charge transports. Such distinctive nanostructure led to exceptional bifunctional electrocatalytic performances for oxygen reduction reaction, with more positive onset potential (1.01 V vs. 0.97 V) and half-wave potential (0.89 V vs. 0.82 V) compared with the commercial Pt/C, and electrochemical carbon dioxide reduction.
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页数:10
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