Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 267, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2020.118720
Keywords
Single-atom catalysts; Large mesopores; Bifunctional electrocatalysis; Oxygen reduction reaction; Carbon dioxide reduction
Funding
- One Thousand Young Talents Program under the Recruitment Program of Global Experts
- National Natural Science Foundation of China (NSFC) [21901246, 21905278, 21771179]
- Natural Science Foundation of Fujian Province [2019J05158, 2019J01133]
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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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