Perovskite-Nanoparticle-Incorporated NH₂-MIL-125(Ti) Nanoreactors with an Optimal Conduction Band Offset for Visible-Light-Driven CO₂ Reduction

Abstract

To alleviate the intense global warming crisis, developing high-performance photocatalysts for CO2 reduction reaction (CO2RR) to green fuels is of great importance. CsPbBr3 (CPB) has been proved as a promising photocatalyst for CO2RR due to the excellent visible-light response and energetic reduction potential, but its practical performance is still deficient, suffering from severe carrier recombination and poor CO2 adsorption capability. Herein, we demonstrate novel CPB-nanocrystal-incorporated NH2-MIL-125(Ti) (NH2-MIL-125(Ti)/CPB) nanoreactors for solar-driven CO2RR. Attributed to the optimal conduction band offset (CBO) in the NH2-MIL-125(Ti)/CPB heterojunction, excellent carrier transfer is obtained with retained energetic photoreduction potential. Moreover, strong interfacial interaction is demonstrated, enabling the synergistic effect of promoted CO2 adsorption on NH2-MIL-125(Ti) and facilitating interfacial carrier injection. Therefore, greatly enhanced photocatalytic CO2RR performance is achieved by as-designed nanoreactors. This work offers a deep understanding into the synthesis of functionalized perovskite-based materials with rationally designed carrier transfer behaviors for not only photocatalytic reactions but also photovoltaic fields.