Enhancing Oxygen Reduction Activity via Tailoring Microstrain in PdMo Nanoalloy through Repetitive Hydrogen Absorption-Release

Ying Chen, Mingzi Sun, Menghao Wu, Cheng Zhu, Haijing Li, Zih Yi Lin, Hangxuan Li, Haozhe Xu, Dong Li, Xiaoting Chen, Sung Fu Hung, Juncai Dong, Bin Liu*, Olga Demidenko, Bolong Huang*, Yujing Li*

*此作品的通讯作者

科研成果: 期刊稿件文章同行评审

摘要

The catalytic activities of noble-metal electrocatalysts are heavily correlated to their defective surface structures. However, controllably constructing surface defects on noble-metal nanocrystals remains a great challenge. In this work, an electrochemical method is developed to tailor the surface structure of the PdMo nanoalloy electrocatalyst, involving H absorption followed by its subsequent release near the surface of Pd. The optimized PdMo nanoalloy electrocatalyst exhibits an oxygen reduction reaction (ORR) half-wave potential (E1/2) of 0.929 V (vs reversible hydrogen electrode, RHE) with a specific activity (SA) as high as 5.09 mA/cm2 at 0.9 V (vs RHE) in an alkaline electrolyte, ∼10.6 times that of the state-of-the-art Pt/C electrocatalyst. Density functional theory calculations together with ex situ and in situ electrochemical and structural characterizations unravel that the microstrain generated at the PdMo nanoalloy surface by electrochemically induced H absorption-release can downshift the d-band center of Pd (the ORR active site) in PdMo to decrease oxygen binding and promote *OOH to *O transformation as well as *OH desorption for fast ORR. This work provides a surface defect engineering strategy to develop high-performance noble-metal electrocatalysts for energy applications.

源语言英语
页(从-至)9354-9363
页数10
期刊ACS Catalysis
14
12
DOI
出版状态已出版 - 21 6月 2024

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Chen, Y., Sun, M., Wu, M., Zhu, C., Li, H., Lin, Z. Y., Li, H., Xu, H., Li, D., Chen, X., Hung, S. F., Dong, J., Liu, B., Demidenko, O., Huang, B., & Li, Y. (2024). Enhancing Oxygen Reduction Activity via Tailoring Microstrain in PdMo Nanoalloy through Repetitive Hydrogen Absorption-Release. ACS Catalysis, 14(12), 9354-9363. https://doi.org/10.1021/acscatal.4c00403