Bottom-up evolution of perovskite clusters into high-activity rhodium nanoparticles toward alkaline hydrogen evolution

Gaoxin Lin, Zhuang Zhang, Qiangjian Ju, Tong Wu, Carlo U. Segre, Wei Chen, Hongru Peng, Hui Zhang, Qiunan Liu, Zhi Liu, Yifan Zhang, Shuyi Kong, Yuanlv Mao, Wei Zhao, Kazu Suenaga, Fuqiang Huang () and Jiacheng Wang ()
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Gaoxin Lin: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Zhuang Zhang: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Qiangjian Ju: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Tong Wu: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Carlo U. Segre: Illinois Institute of Technology
Wei Chen: Materials and Aerospace Engineering, Illinois Institute of Technology
Hongru Peng: ShanghaiTech University
Hui Zhang: Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences
Qiunan Liu: Osaka University
Zhi Liu: ShanghaiTech University
Yifan Zhang: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Shuyi Kong: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Yuanlv Mao: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Wei Zhao: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Kazu Suenaga: Osaka University
Fuqiang Huang: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Jiacheng Wang: Shanghai Institute of Ceramics, Chinese Academy of Sciences

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Self-reconstruction has been considered an efficient means to prepare efficient electrocatalysts in various energy transformation process for bond activation and breaking. However, developing nano-sized electrocatalysts through complete in-situ reconstruction with improved activity remains challenging. Herein, we report a bottom-up evolution route of electrochemically reducing Cs3Rh2I9 halide-perovskite clusters on N-doped carbon to prepare ultrafine Rh nanoparticles (~2.2 nm) with large lattice spacings and grain boundaries. Various in-situ and ex-situ characterizations including electrochemical quartz crystal microbalance experiments elucidate the Cs and I extraction and Rh reduction during the electrochemical reduction. These Rh nanoparticles from Cs3Rh2I9 clusters show significantly enhanced mass and area activity toward hydrogen evolution reaction in both alkaline and chlor-alkali electrolyte, superior to liquid-reduced Rh nanoparticles as well as bulk Cs3Rh2I9-derived Rh via top-down electro-reduction transformation. Theoretical calculations demonstrate water activation could be boosted on Cs3Rh2I9 clusters-derived Rh nanoparticles enriched with multiply sites, thus smoothing alkaline hydrogen evolution.

Date: 2023
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DOI: 10.1038/s41467-023-35783-y

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