Phase-Regulatable Synthesis of Single-Atom Alloy Nanocages for Efficient Alkaline Hydrogen Evolution

Crystal phase engineering of metal nanocatalysts presents a promising strategy to modulate the catalyst-adsorbate interaction for enhanced catalysis. However, conventional synthetic methods have faced substantial challenges in achieving regulatable crystal phases and lack precise control over catalyst composition at the atomic level, which is detrimental, especially for reactions involving multiple intermediates. Here, we report a facile strategy for simultaneously regulating the crystal phase and composition (Pt single-atom alloying) of ultrathin Ru nanocages (<2 nm in thickness), enabling efficient hydrogen evolution reaction (HER) in alkaline electrolytes. <i>In situ</i> characterizations and theoretical calculations reveal that both the metastable face-centered cubic (fcc) Ru phase and isolated Pt atoms contribute to stabilizing metallic Ru, facilitating Pt-Ru synergy for optimized adsorption of H* and *OH intermediates and accelerated HER kinetics. Consequently, the Pt-Ru<sub>fcc</sub> single-atom alloy nanocages exhibit impressive alkaline HER performance, with an overpotential as low as 8.5 mV at 10 mA cm<sup>-2</sup>, an 18.0-fold enhancement in mass activity relative to commercial Pt/C and commendable stability over 400 h of operation at ampere-level current densities. This work provides insights into the atomic-level design and preparation of metal nanocrystals with unconventional phases for advanced catalysts.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2025-09-21
DOI
https://doi.org/10.1021/jacs.5c06662
Citations
11
Primary Topic
Electrocatalysts for Energy Conversion
Type
article
Field-Weighted Citation Impact
4.00
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article

Phase-Regulatable Synthesis of Single-Atom Alloy Nanocages for Efficient Alkaline Hydrogen Evolution

Siew Lang Teo, Hong li Liu, Enyi Ye, Ming Zhao et al.
11 citations
Journal of the American Chemical Society
Electrocatalysts for Energy Conversion
4.00
article

Phase-Regulatable Synthesis of Single-Atom Alloy Nanocages for Efficient Alkaline Hydrogen Evolution

Siew Lang Teo, Hong li Liu, Enyi Ye, Ming Zhao, Zhaolin Liu, Wen‐Ya Wu, Jerry Zhi Xiong Heng, Song Lin Zhang, Chui Yu Chan, Xian Jun Loh, Ming Lin, Jing Yang, Jingcong Hu, Ning Ding, Delong Duan, Yujie Xiong, Ziyu Wang, Yong‐Wei Zhang, Mingsheng Zhang, Qingdian Yan, Shengnan Hu, Weiwei Yang, Wenbin Jiang, Jia-Kai Li, Xinyang Liu
article en
11 citations

Abstract

Crystal phase engineering of metal nanocatalysts presents a promising strategy to modulate the catalyst-adsorbate interaction for enhanced catalysis. However, conventional synthetic methods have faced substantial challenges in achieving regulatable crystal phases and lack precise control over catalyst composition at the atomic level, which is detrimental, especially for reactions involving multiple intermediates. Here, we report a facile strategy for simultaneously regulating the crystal phase and composition (Pt single-atom alloying) of ultrathin Ru nanocages (<2 nm in thickness), enabling efficient hydrogen evolution reaction (HER) in alkaline electrolytes. <i>In situ</i> characterizations and theoretical calculations reveal that both the metastable face-centered cubic (fcc) Ru phase and isolated Pt atoms contribute to stabilizing metallic Ru, facilitating Pt-Ru synergy for optimized adsorption of H* and *OH intermediates and accelerated HER kinetics. Consequently, the Pt-Ru<sub>fcc</sub> single-atom alloy nanocages exhibit impressive alkaline HER performance, with an overpotential as low as 8.5 mV at 10 mA cm<sup>-2</sup>, an 18.0-fold enhancement in mass activity relative to commercial Pt/C and commendable stability over 400 h of operation at ampere-level current densities. This work provides insights into the atomic-level design and preparation of metal nanocrystals with unconventional phases for advanced catalysts.

Journal of the American Chemical SocietyVol. 147(39)
Agency for Science, Technology and Research (SG), University of Science and Technology of China (CN), University of Shanghai for Science and Technology (CN), National University of Singapore (SG), Norsk Hydro (Germany) (DE), Institute of High Performance Computing (SG), Hefei National Center for Physical Sciences at Nanoscale (CN), Fusion Innovations (United Kingdom) (GB), Institute of Materials Research and Engineering (SG), Microscale (United States) (US)
Openalex Percentile: Top 6%
Electrocatalysts for Energy Conversion
4.00
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