Yan Zixin, Liu Zirui, Zhou Guosheng, Jin Tianchen, Zhang Huanhuan, Gu Lin, Gao Tong, Shen Shijie, Zhong Wenwu
Zhejiang Key Laboratory for Island Green Energy and New Materials, Taizhou University, Jiaojiang, Zhejiang, 318000, China.
The Key Laboratory of Bionic Engineering, Ministry of Education, Jilin University, Changchun, 130022, China.
Angew Chem Int Ed Engl. 2025 May;64(19):e202501964. doi: 10.1002/anie.202501964. Epub 2025 Mar 11.
Hydrogen spillover in supported metal electrocatalysts has garnered significant research attention for its potential to enhance the hydrogen evolution reaction (HER) efficiency. However, challenges remain in facilitating hydrogen spillover and reducing the associated energy barriers. Herein, PtPd alloy clusters are anchored to the CeO surface, enabling short-path hydrogen spillover and lowering the reaction energy barrier in acidic environments. During HER, hydrogen is initially adsorbed on the noble metal surface and subsequently migrates to the interface, rather than precipitating directly on the CeO surface. This interface exhibits a near-zero Gibbs free energy of hydrogen adsorption (0.023 eV). Consequently, the catalyst demonstrates an exceptionally low overpotential of only 5.7 mV at 10 mA cm in acidic media, along with remarkable long-term stability. These findings provide valuable insights into designing highly efficient HER electrocatalysts for acidic environments based on hydrogen spillover mechanisms.
负载型金属电催化剂中的氢溢流因其提高析氢反应（HER）效率的潜力而备受研究关注。然而，在促进氢溢流和降低相关能垒方面仍存在挑战。在此，PtPd合金簇锚定在CeO表面，在酸性环境中实现了短程氢溢流并降低了反应能垒。在HER过程中，氢最初吸附在贵金属表面，随后迁移到界面，而不是直接沉淀在CeO表面。该界面表现出接近零的氢吸附吉布斯自由能（0.023 eV）。因此，该催化剂在酸性介质中，在10 mA cm时仅表现出5.7 mV的极低过电位，同时具有出色的长期稳定性。这些发现为基于氢溢流机制设计用于酸性环境的高效HER电催化剂提供了有价值的见解。
