Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 6, Pages 3212-3221Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202012798
Keywords
cobalt; density-functional calculations; heterogeneous catalysis; metal– organic frameworks; oxygen reduction
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Funding
- National Key R&D Program of China [2018YFA0702003]
- National Natural Science Foundation of China [21890383, 21671117, 21871159, 21802076, 51871001]
- Science and Technology Key Project of Guangdong Province of China [2020B010188002]
- Beijing Municipal Science & Technology Commission [Z191100007219003]
- National Postdoctoral Program for Innovative Talents [BX20180160]
- China Postdoctoral Science Foundation [2018M640113]
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This study demonstrates the correlation between atomic configuration induced electronic density of single-atom Co active sites and oxygen reduction reaction (ORR) performance. The designed and synthesized Co-1-N3PS/HC catalyst shows outstanding ORR activity in alkaline and acidic media, surpassing Pt/C and most non-precious ORR electrocatalysts. Insights from this work promote rational design of efficient catalysts.
Demonstrated here is the correlation between atomic configuration induced electronic density of single-atom Co active sites and oxygen reduction reaction (ORR) performance by combining density-functional theory (DFT) calculations and electrochemical analysis. Guided by DFT calculations, a MOF-derived Co single-atom catalyst with the optimal Co-1-N3PS active moiety incorporated in a hollow carbon polyhedron (Co-1-N3PS/HC) was designed and synthesized. Co-1-N3PS/HC exhibits outstanding alkaline ORR activity with a half-wave potential of 0.920 V and superior ORR kinetics with record-level kinetic current density and an ultralow Tafel slope of 31 mV dec(-1), exceeding that of Pt/C and almost all non-precious ORR electrocatalysts. In acidic media the ORR kinetics of Co-1-N3PS/HC still surpasses that of Pt/C. This work offers atomic-level insight into the relationship between electronic density of the active site and catalytic properties, promoting rational design of efficient catalysts.
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