Modulation of active center distance of hybrid perovskite for boosting photocatalytic reduction of carbon dioxide to ethylene
Linjuan Li, Dawei Xu, Xiankui Xu, Z. Ryan Tian, Xuedong Zhou, Shenbo Yang, Zhonghai Zhang
Abstract
Solar-driven photocatalytic CO 2 reduction is an energy-efficient and sustainable strategy to mitigate CO 2 levels in the atmosphere. However, efficient and selective conversion of CO 2 into multi-carbon products, like C 2 H 4 , remains a great challenge due to slow multi-electron-proton transfer and sluggish C–C coupling. Herein, a two-dimensional thin-layered hybrid perovskite is fabricated through filling of oxygen into iodine vacancy in pristine DMASnI 3 (DMA = dimethylammonium). The rational-designed DMASnI 3 (O) induces shrinkage of active sites distance and facilitates dimerization of C–C coupling of intermediates. Upon simulated solar irradiation, the DMASnI 3 (O) photocatalyst achieves a high selectivity of 74.5%, corresponding to an impressive electron selectivity of 94.6%, for CO 2 to C 2 H 4 conversion and an effective C 2 H 4 yield of 11.2 μmol g −1 h −1 . In addition, the DMASnI 3 (O) inherits excellent water stability and implements long-term photocatalytic CO 2 reduction to C 2 H 4 in a water medium. This work establishes a unique paradigm to convert CO 2 to C 2+ hydrocarbons in a perovskite-based photocatalytic system.