A Multiple Structure-Design Strategy towards Ultrathin Niobate Perovskite Nanosheets with Thickness-Dependent Photocatalytic Hydrogen-Evolution Performance

Hydrogen production by catalytic water splitting using sunlight holds great promise for clean and sustainable energy source. Despite the efforts made in the past decades, challenges still exist in pursuing solid catalysts with light-harvesting capacity, large surface areas and efficient utilities of the photogenerated carrier, at the same time. Here, a multiple structure design strategy leading to highly enhanced photocatalytic performance on hydrogen production from water splitting in Dion-Jacobson perovskites KCa2Nan-3NbnO3n+1 is described. Specifically, chemical doping (N/Nb4+) of the parent oxides via ammoniation improved the ability of sunlight harvesting efficiently; subsequent liquid exfoliation of the doped perovskites yielded ultrathin [Ca2Nan-3NbnO3n+1](-) nanosheets with greatly increased surface areas. Significantly, the maximum hydrogen evolution appears in the n=4 nanosheets, which suggests the most favorable thickness for charge separation in such perovskite-type catalysts. The optimized black N/Nb4+-[Ca2NaNb4O13](-) nanosheets show greatly enhanced photocatalytic performance, as high as 973 mu molh(-1) with Pt loading, on hydrogen evolution from water splitting. As a proof-of-concept, this work highlights the feasibility of combining various chemical strategies towards better catalysts and precise thickness control of two-dimensional materials.