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

Nat Commun. 2023 Mar 28;14(1):1720. doi: 10.1038/s41467-023-37451-7.

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.