Boosting Photocatalytic Activity and Stability of Lead-Free Cs₃Bi₂Br₉ Perovskite Nanocrystals via In Situ Growth on Monolayer 2D Ti₃C₂T<i>_x</i> MXene for C–H Bond Oxidation

Abstract

Light-driven selective oxidation of saturated C-H bonds with molecular oxygen, as an alternative to conventional thermochemical catalysis, allows a sustainable and eco-friendly manner to convert solar energy into highly value-added oxygenates. However, the photocatalytic oxidation of hydrocarbons still remains a great challenge owing to the low efficiency in the separation and transfer of photogenerated charge of the currently available photocatalytic materials. Herein, we report a novel perovskite-based heterostructure photocatalyst, in which ligand- and lead-free all-inorganic perovskite Cs₃Bi₂Br₉ nanocrystals (NCs) with uniform crystal size and high crystallinity were homogeneously distributed on the surface of ultrathin two-dimensional (2D) monolayer Ti₃C₂T<i>_x</i> MXene nanosheets in an in situ growth manner. The resultant heterostructure featured with intimate interface between Cs₃Bi₂Br₉ NCs and Ti₃C₂T<i>_x</i> MXene and strong visible-light adsorption not only exhibits significant enhancement in the performance of photocatalytic oxidation of challenging aromatic and aliphatic alkanes under visible-light irradiation but also greatly improves the stability of Cs₃Bi₂Br₉ NCs under a reaction environment. Comprehensive characterizations reveal that the formation of an intimate interface between Cs₃Bi₂Br₉ NCs and highly conductive ultrathin 2D Ti₃C₂T<i>_x</i> MXene nanosheets via strong interaction markedly accelerates the separation and transfer efficiency of photogenerated electron-hole pairs and simultaneously suppresses their recombination, resulting in improved utilization of the excited charges, which account for the highly enhanced photocatalytic performance.