Mesocrystalline Ta₃N₅ superstructures with long-lived charges for improved visible light photocatalytic hydrogen...

Highly ordered mesocrystalline semiconductors often indicate tremendous prospects in the clean energy production and environmental photocatalysis mainly because of their unique superstructure for efficient charge transport pathways and long-lived charges. Here, superstructure Ta₃N₅ mesocrystals with the high-energy surface {2 0 0} planes exposed were the first time to be successfully fabricated by topological transformation of Ta₂O₅ mesocrystals. The prepared Ta₃N₅ mesocrystals showed enhanced visible-light photocatalytic hydrogen production activity of 98.67 μmol g^-1 for 180 min irradiation, which was approximately 5.28 times that of comm-Ta₃N₅ prepared with commercial Ta₂O₅ as the starting material, mainly due to the formation of long-distance electron conduction pathways and long-lived charges. The detailed electronic band structures of the prepared Ta₃N₅ mesocrystals were also investigated by electrochemical method. Finally, possible visible-light photocatalytic mechanisms of Ta₃N₅ mesocrystals for enhanced hydrogen production was also proposed in detail. Current work also indicates that tantalum-based mesocrystals show great potential to enhance the charge separation for efficient photocatalytic water splitting.