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

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 Co-1-P-4 site confined on g-C3N4 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-C3N4, and boost water molecular adsorption and activation for oxygen evolution. This single-site photocatalyst exhibits steady and high water splitting activity with H-2 evolution rate up to 410.3 mu mol h(-1) g(-1), and quantum efficiency as high as 2.2% at 500 nm.