Modulation of active center distance of hybrid perovskite for boosting photocatalytic reduction of carbon dioxide to ethylene

• 成果类型: Article
• 署名作者: Li, Linjuan; Xu, Dawei; Xu, Xiankui; Tian, Zheng; Zhou, Xue; Yang, Shenbo; Zhang, Zhonghai
• 署名单位: East China Normal University; East China Normal University
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-11408
• DOI: 10.1073/pnas.2318970121
• 发表日期: 2024-02-13
• 关键词: catalytic-reduction; co2 photoreduction; driven; c2h4; ftir

摘要

Solar- driven photocatalytic CO2 reduction is an energy- efficient and sustainable strategy to mitigate CO2 levels in the atmosphere. However, efficient and selective conversion of CO2 into multi- carbon products, like C2H4, 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 DMASnI3 (DMA = dimethylammonium). The rational- designed DMASnI3(O) induces shrinkage of active sites distance and facilitates dimerization of C-C coupling of intermediates. Upon simulated solar irradiation, the DMASnI3(O) photocatalyst achieves a high selectivity of 74.5%, corresponding to an impressive electron selectivity of 94.6%, for CO2 to C2H4 conversion and an effective C2H4 yield of 11.2 mu mol g-1 h-1. In addition, the DMASnI3(O) inherits excellent water stability and implements long - term photocatalytic CO2 reduction to C2H4 in a water medium. This work establishes a unique paradigm to convert CO2 to C2+ hydrocarbons in a perovskite-based photocatalytic system. Significance The attempt to perform photocatalytic CO2reduction into multi- carbon ethylene in water on perovskite- based photocatalysts is challengeable. The two- dimensional thin- layered hybrid perovskite of DMASnI3(O) was synthesized and presented long - term water stability for photocatalytic CO2reduction and production of ethylene. The heterogeneous atom filling vacancy strategy, that is, the filling of oxygen into iodine vacancy, induces shrinkage of active sites distance, which shortened active center distance and facilitates dimerization of C-C coupling of intermediates for facilitating C-C coupling. The DMASnI3(O) boosted a high selectivity of 94.6% for C2H4production in pure aqueous solution.