Boosting oxygen reduction performances in Pd-based metallenes by co-confining interstitial H and p-block single atoms
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. PdPbH<sub>x</sub> metallenes exhibit a high mass activity of 1.36 A mg<sup>-1</sup> 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 O<sub>2</sub> while single Pb atoms enhance O<sub>2</sub> adsorption strength. The electroactive PdPbH<sub>x</sub> 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.
Authors
- Bolong Huang (ORCID: https://orcid.org/0000-0002-2526-2002)
- Yujiang Song (ORCID: https://orcid.org/0000-0001-6031-9804)
- Dongxu Jiao
- Jiandong Wu (ORCID: https://orcid.org/0000-0002-6672-5114)
- Jinchang Fan (ORCID: https://orcid.org/0000-0001-9560-6790)
- Xiao Dan Zhao (ORCID: https://orcid.org/0000-0002-8183-8205)
- Dewen Wang
- Yu Qiu (ORCID: https://orcid.org/0000-0001-9836-036X)
- Mingzi Sun (ORCID: https://orcid.org/0000-0001-5136-7265)
- Chunxiao Chai
- Xiaoqiang Cui (ORCID: https://orcid.org/0000-0002-5858-6257)
- Wei Zhang (ORCID: https://orcid.org/0000-0002-6414-7015)
- Xin Ge (ORCID: https://orcid.org/0000-0001-9931-3354)
- Hong Huang (ORCID: https://orcid.org/0000-0001-7487-4876)
- Shan Xu
- Weitao Zheng (ORCID: https://orcid.org/0000-0002-9028-278X)
- Shengwei Wang
Institutions
- Hong Kong Polytechnic University (HK)
- City University of Hong Kong (HK)
- Jilin University (CN)
- Dalian University of Technology (CN)
- Dalian University (CN)
- First Bethune Hospital of Jilin University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-06-06
- DOI
- https://doi.org/10.1038/s41467-025-60400-5
- Citations
- 20
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 7.27
Funders
- National Natural Science Foundation of China
- Natural Science Foundation of Guangdong Province
- Hong Kong Polytechnic University