期刊
CHEMSUSCHEM
卷 14, 期 21, 页码 4680-4689出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202101341
关键词
Bader charge; electrochemistry; oxidative degradation; oxygen reduction reaction; proton exchange membrane fuel cells
资金
- National Science Foundation [1729787, 1806147, ACI-1053575, ACI-1548562]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1806147] Funding Source: National Science Foundation
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1729787] Funding Source: National Science Foundation
By optimizing the interaction between nitrogen-coordinated transition metal clusters embedded in a more stable and corrosion-resistant carbide matrix, a new ORR electrocatalyst with enhanced activity and stability compared to traditional Fe-N-C catalysts was developed. A potential electrostatics-based descriptor of catalytic activity was identified during first-principles calculations, showing promise as a tool for designing active and stable PGM-free electrocatalysts.
Clusters of nitrogen- and carbon-coordinated transition metals dispersed in a carbon matrix (e. g., Fe-N-C) have emerged as an inexpensive class of electrocatalysts for the oxygen reduction reaction (ORR). Here, it was shown that optimizing the interaction between the nitrogen-coordinated transition metal clusters embedded in a more stable and corrosion-resistant carbide matrix yielded an ORR electrocatalyst with enhanced activity and stability compared to Fe-N-C catalysts. Utilizing first-principles calculations, an electrostatics-based descriptor of catalytic activity was identified, and nitrogen-coordinated iron (FeN4) clusters embedded in a TiC matrix were predicted to be an efficient platinum-group metal (PGM)-free ORR electrocatalyst. Guided by theory, selected catalyst formulations were synthesized, and it was demonstrated that the experimentally observed trends in activity fell exactly in line with the descriptor-derived theoretical predictions. The Fe-N-TiC catalyst exhibited enhanced activity (20 %) and durability (3.5-fold improvement) compared to a traditional Fe-N-C catalyst. It was posited that the electrostatics-based descriptor provides a powerful platform for the design of active and stable PGM-free electrocatalysts and heterogenous single-atom catalysts for other electrochemical reactions.
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