Spin occupancy regulation of the Pt d-orbital for a robust low-Pt catalyst towards oxygen reduction

• DOI: 10.1038/s41467-024-50332-x
• Publication Date: 2024-07-16T22:01:21Z
• Authors: Dongping Xue; Yifang Yuan; Yue Yu; Siran Xu; Yifan Wei; Jiaqi Zhang; Haizhong Guo; Minhua Shao; Jia-Nan Zhang
• Keywords: HOMO/LUMO; Spin states

Abstract Disentangling the limitations of O-O bond activation and OH* site-blocking effects on Pt sites is key to improving intrinsic activity stability low-Pt catalysts for oxygen reduction reaction (ORR). Herein, we integrate PtFe alloy nanocrystals a single-atom Fe-N-C substrate (PtFe@Fe SAs -N-C) further construct ferromagnetic platform investigate regulation behavior spin occupancy state d -orbital in ORR. PtFe@Fe -N-C delivers mass 0.75 A mg −1 at 0.9 V peak power density 1240 mW cm −2 fuel-cell, outperforming commercial Pt/C catalyst, retention 97%, with no noticeable current drop 0.6 more than 220 h, attained. Operando spectroelectrochemistry decodes orbital interaction mechanism between active center intermediates. The dz 2 occupation regulated t 2g 6 e g 3 by spin-charge injection, suppressing effect effectively inhibiting H O production. This work provides valuable insights into designing high-performance via spintronics-level engineering.