In situ constructing atomic interface in ruthenium-based amorphous hybrid-structure towards solar hydrogen evolution.

Liu, Dong; Ding, Tao; Wang, Lifeng; Zhang, Huijuan; Xu, Li; Pang, Beibei; Liu, Xiaokang; Wang, Huijuan et al. · Nat Commun · 2023

basic_science · Level V

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Abstract

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.