离解(化学)
催化作用
钌
电解质
化学
分解水
铂金
无机化学
光化学
材料科学
物理化学
有机化学
电极
光催化
作者
Chengdong Yang,Zihe Wu,Zhenyang Zhao,Yun Gao,Tian Ma,Chao He,Changzhu Wu,Xikui Liu,Xingguang Luο,Shuang Li,Chong Cheng,Changsheng Zhao
出处
期刊:Small
[Wiley]
日期:2023-01-04
卷期号:19 (14)
被引量:17
标识
DOI:10.1002/smll.202206949
摘要
Ruthenium (Ru)-based catalysts have displayed compelling hydrogen evolution activities, which hold the promising potential to substitute platinum in alkaline H2 -evolution. In the challenging alkaline electrolytes, the water-dissociation process involves multistep reactions, while the profound origin and intrinsic factors of diverse Ru species on water-dissociation pathways and reaction principles remain ambiguous. Here the fundamental origin of water-dissociation pathways of Ru-based catalysts in alkaline media to be from their unique electronic structures in complex coordination environments are disclosed. These theoretical results validate that the modulated electronic structures with delocalization-localization coexistence at their boundaries between the Ru nanocluster and single-atom site have a profound influence on water-dissociation pathways, which push H2 O* migration and binding orientation during the splitting process, thus enhancing the dissociation kinetics. By creating Ru catalysts with well-defined nanocluster, single-atom site, and also complex site, the electrocatalytic data shows that both the nanocluster and single-atom play essential roles in water-dissociation, while the complex site possesses synergistically enhanced roles in alkaline electrolytes. This study discloses a new electronic structure-dependent water-dissociation pathway and reaction principle in Ru-based catalysts, thus offering new inspiration to design efficient and durable catalysts for the practical production of H2 in alkaline electrolytes.
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