Boosting oxygen reduction performances in Pd-based metallenes by co-confining interstitial H and p-block single atoms

Yu Qiu, Mingzi Sun, Jiandong Wu, Chunxiao Chai, Shengwei Wang, Hong Huang, Xiao Zhao, Dongxu Jiao, Shan Xu, Dewen Wang, Xin Ge, Wei Zhang, Weitao Zheng, Yujiang Song, Jinchang Fan (), Bolong Huang () and Xiaoqiang Cui ()
Additional contact information
Yu Qiu: Jilin University
Mingzi Sun: City University of Hong Kong, Kowloon
Jiandong Wu: Jilin University
Chunxiao Chai: Dalian University of Technology
Shengwei Wang: Jilin University
Hong Huang: Jilin University
Xiao Zhao: Jilin University
Dongxu Jiao: Jilin University
Shan Xu: Jilin University
Dewen Wang: Jilin University
Xin Ge: Jilin University
Wei Zhang: Jilin University
Weitao Zheng: Jilin University
Yujiang Song: Dalian University of Technology
Jinchang Fan: Jilin University
Bolong Huang: City University of Hong Kong, Kowloon
Xiaoqiang Cui: Jilin University

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract The efficiency of the oxygen reduction reaction (ORR) is limited by the scaling relationship in the conventional oxygen associative pathway. To break such limitations, we present an approach to effectively activate the oxygen dissociative pathway through co-confining single p-block (In, Sn, Pb) atoms and interstitial H atoms within Pd metallenes, leading to good ORR performance. PdPbHx metallenes exhibit a high mass activity of 1.36 A mg−1 at 0.95 V (vs. RHE), which is 46.9 times higher than that of the benchmark Pt/C. The minimal performance decay after 50,000 potential cycles confirms a good stability. In situ vibrational spectroscopy investigations and theoretical calculations highlight that interstitial H atoms facilitate the direct dissociation of O2 while single Pb atoms enhance O2 adsorption strength. The electroactive PdPbHx metallenes is attributed to the up-shifted Pd-4d orbitals induced by H and Pb atoms. This research supplies critical inspiration for developing highly efficient ORR electrocatalysts.

Date: 2025
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DOI: 10.1038/s41467-025-60400-5

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