Zr dopant acting shallow donor and active site in CdS lattice for co-catalyst free photocatalytic H2 evolution

Abstract

Hydrogen evolution by photocatalysis shows great potential in solar energy conversion process and thus has become an active field of research. Separation efficiency of photogenerated carriers, light absorption and surface reaction are the dominant aspects that affect the photocatalytic hydrogen evolution. Creating traps to prolong the lifetime of photogenerated charge carriers has been widely used but may be considered detrimental if they lead to recombination process of the photogenerated charge carriers. Herein, we design a kind of efficient atomic substitution strategy to create shallow donor for highly efficient hydrogen evolution reaction. The photocatalytic hydrogen evolution reaction rate reaches 3766.9 μmol h−1 g−1, which is about 2.98 times higher of pure CdS. The injected foreign atoms (Zr) not only reduce bandgap to extend light absorption but also generate shallow trap level to reduce recombination of photogenerated carriers. Moreover, the introduced atoms could downshift Fermi level to supply more carriers and act the role as active center to reduce Gibbs free energy, leading to the enhanced hydrogen generation rate and superior stability. This report offers new enlightenment into designing noble-metal free photocatalysts with extraordinary catalytic performance and excellent stability.