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

Dongping Xue, Yifang Yuan, Yue Yu, Siran Xu, Yifan Wei, Jiaqi Zhang, Haizhong Guo, Minhua Shao and Jia-Nan Zhang ()
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Dongping Xue: Zhengzhou University
Yifang Yuan: Zhengzhou University
Yue Yu: Zhengzhou University
Siran Xu: Zhengzhou University
Yifan Wei: Zhengzhou University
Jiaqi Zhang: Zhengzhou University
Haizhong Guo: Zhengzhou University
Minhua Shao: The Hong Kong University of Science and Technology
Jia-Nan Zhang: Zhengzhou University

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract Disentangling the limitations of O-O bond activation and OH* site-blocking effects on Pt sites is key to improving the intrinsic activity and stability of low-Pt catalysts for the oxygen reduction reaction (ORR). Herein, we integrate of PtFe alloy nanocrystals on a single-atom Fe-N-C substrate (PtFe@FeSAs-N-C) and further construct a ferromagnetic platform to investigate the regulation behavior of the spin occupancy state of the Pt d-orbital in the ORR. PtFe@FeSAs-N-C delivers a mass activity of 0.75 A mgPt−1 at 0.9 V and a peak power density of 1240 mW cm−2 in the fuel-cell, outperforming the commercial Pt/C catalyst, and a mass activity retention of 97%, with no noticeable current drop at 0.6 V for more than 220 h, is attained. Operando spectroelectrochemistry decodes the orbital interaction mechanism between the active center and reaction intermediates. The Pt dz2 orbital occupation state is regulated to t2g6eg3 by spin-charge injection, suppressing the OH* site-blocking effect and effectively inhibiting H2O2 production. This work provides valuable insights into designing high-performance and low-Pt catalysts via spintronics-level engineering.

Date: 2024
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DOI: 10.1038/s41467-024-50332-x

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