Efficient photocatalytic hydrogen evolution on single-crystalline metal selenide particles with suitable cocatalysts

Abstract

It is important to improve the apparent quantum yields (AQYs) of narrow bandgap photocatalysts to achieve efficient H₂ production. The present work demonstrates a particulate solid solution of zinc selenide and copper gallium selenide (denoted as ZnSe:CGSe) that evolves H₂ efficiently and is responsive to visible light up to 725 nm. This material was synthesized using a flux-assisted method and was found to comprise single-crystalline tetrahedral particles. The coloading of Ni and Rh, Pt, Pd or Ru as cocatalysts further improved the photocatalytic H₂ evolution rate over this photocatalyst. With the optimal coloading of a Ni–Ru composite cocatalyst, an AQY of 13.7% was obtained at 420 nm during a sacrificial H₂ evolution reaction, representing the highest value yet reported for a photocatalyst with an absorption edge longer than 700 nm. The present study demonstrates that the preparation of single-crystalline particles and the rational assembly of composite cocatalysts are effective strategies that allow the efficient utilization of long wavelengths by metal selenide photocatalysts for solar fuel production.