High-Performance H2 Photosynthesis from Pure Water over Ru-S Charge Transfer Channels.

Abstract

As a versatile energy carrier, H2 is considered as one of the most promising sources of clean energy to tackle the current energy crisis and environmental concerns, which can be produced from photocatalytic water splitting. However, solar-driven photocatalytic H2 production from pure water in the absence of sacrificial reagents remains a great challenge. Herein, we demonstrate that the incorporation of Ru single atoms (SAs) into ZnIn2S4 (Ru-ZIS) can enhance the light absorption, reduce the energy barriers for water dissociation, and construct a channel (Ru-S) for separating photogenerated electron-hole pairs, as a result of a significantly enhanced photocatalytic water splitting process. Impressively, the productivity of H2 reaches 735.2 μmol g-1 h-1 under visible light irradiation in the absence of sacrificial agents. The apparent quantum efficiency (AQE) for H2 evolution reaches 7.5% at 420 nm, with a solar-to-hydrogen (STH) efficiency of 0.58%, which is much higher than the value of natural synthetic plants (∼0.10%). Moreover, Ru-ZIS exhibits steady productivity of H2 even after exposure to ambient conditions for 330 days. This work provides a unique strategy for constructing charge transfer channels to promote the separation of photogenerated electron-hole pairs, which may motivate the fundamental researches on catalyst design for photocatalysis and beyond.