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

    Year: 2023

    Authors: Lin, Gaoxin; Zhang, Zhuang; Ju, Qiangjian; Wu, Tong; Segre, Carlo U.; Chen, Wei; Peng, Hongru; Zhang, Hui; Liu, Qiunan; Liu, Zhi; Zhang, Yifan; Kong, Shuyi; Mao, Yuanlv; Zhao, Wei; Suenaga, Kazu; Huang, Fuqiang; Wang, Jiacheng

    Keywords: Electrocatalysis; Electrochemistry; Energy

    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.
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