Issue 9, 2024

Breaking Sabatier's vertex via switching the oxygen adsorption configuration and reaction pathway on dual active sites for acidic oxygen reduction

Abstract

Single-atom catalysts are promising alternatives to platinum-based catalysts for the oxygen reduction reaction (ORR). However, the ORR process with multiple-step proton-coupled electron transfer occurring on a single-active site follows the linear scaling relation, making it difficult to break through Sabatier's limitation. Herein, we switch the ORR process from a sluggish associative pathway to a favorable dissociative one by constructing diatomic active sites with a Pt-like adsorption configuration, enabling the thermodynamic limit potential to break through Sabatier's vertex. Theoretical calculations and in situ characterization fully corroborate the Pt-like adsorption configuration of O2 on Ru–Fe dual sites, which renders the direct cleavage of O–O bonds and avoids the formation of *OOH intermediates, thus boosting the ORR kinetics. Consequently, the well-designed Ru and Fe co-doped catalysts with dual active sites (Ru, Fe-NC DAS) deliver extraordinary ORR catalytic performance, as manifested by the high half-wave potential of 0.843 V in an acid medium and a record-breaking peak power density of 1.152 W cm−2 in H2/O2 fuel cells, ranking at the top level of non-Pt catalysts reported so far. This work provides a new approach for designing highly efficient atomically dispersed catalysts and steering the corresponding catalytic reaction mechanisms.

Graphical abstract: Breaking Sabatier's vertex via switching the oxygen adsorption configuration and reaction pathway on dual active sites for acidic oxygen reduction

Supplementary files

Article information

Article type
Paper
Submitted
22 Feb 2024
Accepted
25 Mar 2024
First published
25 Mar 2024

Energy Environ. Sci., 2024,17, 3077-3087

Breaking Sabatier's vertex via switching the oxygen adsorption configuration and reaction pathway on dual active sites for acidic oxygen reduction

P. Guo, B. Liu, F. Tu, Y. Dai, Z. Zhang, Y. Xia, M. Ma, Y. Zhang, L. Zhao and Z. Wang, Energy Environ. Sci., 2024, 17, 3077 DOI: 10.1039/D4EE00823E

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