In situ tuning of platinum 5d valence states for four-electron oxygen reduction

Wanlin Zhou, Baojie Li, Xinyu Liu, Jingjing Jiang, Shuowen Bo, Chenyu Yang, Qizheng An, Yuhao Zhang, Mikhail A. Soldatov, Huijuan Wang, Shiqiang Wei and Qinghua Liu ()
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Wanlin Zhou: University of Science and Technology of China
Baojie Li: University of Science and Technology of China
Xinyu Liu: University of Science and Technology of China
Jingjing Jiang: University of Science and Technology of China
Shuowen Bo: University of Science and Technology of China
Chenyu Yang: University of Science and Technology of China
Qizheng An: University of Science and Technology of China
Yuhao Zhang: University of Science and Technology of China
Mikhail A. Soldatov: Southern Federal University
Huijuan Wang: University of Science and Technology of China
Shiqiang Wei: University of Science and Technology of China
Qinghua Liu: University of Science and Technology of China

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract The oxygen reduction reaction (ORR) catalyzed by efficient and economical catalysts is critical for sustainable energy devices. Although the newly-emerging atomically dispersed platinum catalysts are highly attractive for maximizing atomic utilization, their catalytic selectivity and durability are severely limited by the inflexible valence transformation between Pt and supports. Here, we present a structure by anchoring Pt atoms onto valence-adjustable CuOx/Cu hybrid nanoparticle supports (Pt1-CuOx/Cu), in which the high-valence Cu (+2) in CuOx combined with zero-valent Cu (0) serves as a wide-range valence electron reservoir (0‒2e) to dynamically adjust the Pt 5d valence states during the ORR. In situ spectroscopic characterizations demonstrate that the dynamic evolution of the Pt 5d valence electron configurations could optimize the adsorption strength of *OOH intermediate and further accelerate the dissociation of O = O bonds for the four-electron ORR. As a result, the Pt1-CuOx/Cu catalysts deliver superior ORR performance with a significantly enhanced four-electron selectivity of over 97% and long-term durability.

Date: 2024
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DOI: 10.1038/s41467-024-51157-4

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