In situ constructing atomic interface in ruthenium-based amorphous hybrid-structure towards solar hydrogen evolution.
In situ constructing atomic interface in ruthenium-based amorphous hybrid-structure towards solar hydrogen evolution.
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DOI：
10.1038/s41467-023-37451-7
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发表时间：
2023-03-28
影响因子：
16.6
通讯作者：
Yao, Tao
中科院分区：
文献类型：
--
作者：
Liu, Dong;Ding, Tao;Wang, Lifeng;Zhang, Huijuan;Xu, Li;Pang, Beibei;Liu, Xiaokang;Wang, Huijuan;Wang, Junhui;Wu, Kaifeng;Yao, Tao
The rational steering and construction of efficient and stable atomic interfaces is highly desirable but rather challenging in solar energy conversion. Here, we report an in-situ oxygen impregnation strategy to build abundant atomic interfaces composed of homogeneous Ru and RuOx amorphous hybrid-mixture with ultrafast charge transfer, for solar hydrogen evolution with sacrificial agent free. Via in-situ synchrotron X-ray absorption and photoelectron spectroscopies, we can precisely track and identify the gradual formation of atomic interfaces towards homogeneous Ru-RuOx hybrid-structure at the atomic level. Benefiting from the abundant interfaces, the amorphous RuOx sites can intrinsically trap the photoexcited hole within an ultrafast process (<100 fs), and the amorphous Ru sites enable subsequent electron transfer (~1.73 ps). Hence, this hybrid-structure triggers long-lived charge-separated states, and results in a high hydrogen evolution rate of 60.8 μmol·h−1. This design integrating the two sites fulfilled each half-reaction in a single hybrid-structure suggests potential guidelines towards efficient artificial photosynthesis. Solar-driven hydrogen evolution coupled with organic synthesis is important but challenging. Here, the authors report an in-situ oxygen impregnation strategy to build a ruthenium-based amorphous hybrid-mixture with abundant atomic interfaces and show efficient hydrogen evolution with small molecule oxidation.
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