Aluminum Cation Doping in Ruddlesden-Popper Sr2TiO4 Enables High-Performance Photocatalytic Hydrogen Evolution

Hydrogen (H2) is regarded as a promising and renewable energy carrier to achieve a sustainable future. Among the various H2 production routes, photocatalytic water splitting has received particular interest; it strongly relies on the optical and structural properties of photocatalysts such as their sunlight absorption capabilities, carrier transport properties, and amount of oxygen vacancy. Perovskite oxides have been widely investigated as photocatalysts for photocatalytic water splitting to produce H2 because of their distinct optical properties, tunable band gaps and excellent compositional/structural flexibility. Herein, an aluminum cation (Al3+) doping strategy is developed to enhance the photocatalytic performance of Ruddlesden-Popper (RP) Sr2TiO4 perovskite oxides for photocatalytic H2 production. After optimizing the Al3+ substitution concentration, Sr2Ti0.9Al0.1O4 exhibits a superior H2 evolution rate of 331 μmol h−1 g−1, which is ~3 times better than that of Sr2TiO4 under full-range light illumination, due to its enhanced light harvesting capabilities, facilitated charge transfer, and tailored band structure. This work presents a simple and useful Al3+ cation doping strategy to boost the photocatalytic performance of RP-phase perovskites for solar water splitting.