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

• Published in: Nature communications 2023-01, Vol.14 (1), p.280-280, Article 280
• Main 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
• Format: Article
• Language: English
• Subjects: 140/133; 140/58; 639/301/299/886; 639/638/161; 639/638/675; 639/638/77/886; Chemical reduction; Clusters; Electrocatalysts; Electrochemistry; Energy conversion; Evolution; Grain boundaries; Humanities and Social Sciences; Hydrogen; Hydrogen evolution reactions; multidisciplinary; Nanoparticles; Perovskites; Quartz crystal microbalance; Quartz crystals; Reconstruction; Rhodium; Science; Science & Technology - Other Topics; Science (multidisciplinary); Ultrafines
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-023-35783-y

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 Cs 3 Rh 2 I 9 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 Cs 3 Rh 2 I 9 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 Cs 3 Rh 2 I 9 -derived Rh via top-down electro-reduction transformation. Theoretical calculations demonstrate water activation could be boosted on Cs 3 Rh 2 I 9 clusters-derived Rh nanoparticles enriched with multiply sites, thus smoothing alkaline hydrogen evolution. Self-reconstruction is an efficient method to synthesize active electrocatalysts. Here, the authors demonstrate a bottom-up evolution route of electrochemically reducing Cs 3 Rh 2 I 9 halide-perovskite clusters to prepare ultrafine Rh nanoparticles with multiply sites for alkaline hydrogen evolution.