Single-Site Active Cobalt-Based Photocatalyst with a Long Carrier Lifetime for Spontaneous Overall Water Splitting

Abstract

An active and stable photocatalyst to directly split water is desirable for solar-energy conversion. However, it is difficult to accomplish overall water splitting without sacrificial electron donors. Herein, we demonstrate a strategy via constructing a single site to simultaneously promote charge separation and catalytic activity for robust overall water splitting. A single Co₁ -P₄ site confined on g-C₃ N₄ nanosheets was prepared by a facile phosphidation method, and identified by electron microscopy and X-ray absorption spectroscopy. This coordinatively unsaturated Co site can effectively suppress charge recombination and prolong carrier lifetime by about 20 times relative to pristine g-C₃ N₄ , and boost water molecular adsorption and activation for oxygen evolution. This single-site photocatalyst exhibits steady and high water splitting activity with H₂ evolution rate up to 410.3 μmol h^-1 g^-1 , and quantum efficiency as high as 2.2 % at 500 nm.

Keywords: cobalt; graphitic carbon nitride; photocatalysis; single site catalysts; water splitting.