Climbing the Apex of the ORR Volcano Plot via Binuclear Site Construction: Electronic and Geometric Engineering.

08:00 EDT 11th October 2019 | BioPortfolio

Summary of "Climbing the Apex of the ORR Volcano Plot via Binuclear Site Construction: Electronic and Geometric Engineering."

Great enthusiasms in single-atom catalysts (SACs) for the oxygen reduction reaction (ORR) are aroused by the discovery of M-Nx as a promising ORR catalysis center. However, the performance of SACs lags far behind that of state-of-the-art Pt due to the unsatisfactory adsorption-desorption behaviors of the reported catalytic centers. To address this issue, ra-tional manipulation of the active site configuration towards a well-managed energy level and geometric structure is ur-gently desired, yet still remains a challenge. Herein, we report a novel strategy to accomplish this task through the con-struction of an Fe-Co dual-atom centered site. A spontaneously absorbed electron-withdrawing OH ligand was proposed to act proactively as an energy level modifier to empower easy intermediate desorption, while the triangular Fe-Co-OH coordination facilitates O-O bond scission. Benefiting from these attributes, the as-constructed FeCoN5-OH site enables an ORR onset potential and half-wave potential of up to 1.02 and 0.86 V (vs. RHE) respectively, with an intrinsic activity over 20 times higher than the single-atom FeN4 site. Our finding not only opens up a novel strategy to tailor the electronic structure of an atomic site towards boosted activity, but also provides new insights into the fundamental understanding of diatomic sites for ORR electrocatalysis.


Journal Details

This article was published in the following journal.

Name: Journal of the American Chemical Society
ISSN: 1520-5126


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