Frustrated Lewis Pair Sites Boosting CO2 Photoreduction on Cs2CuBr4 Perovskite Quantum Dots

被引:159
作者
Sheng, Jianping [1 ,2 ]
He, Ye [1 ]
Huang, Ming [3 ]
Yuan, Chaowei [1 ]
Wang, Shengyao [4 ]
Dong, Fan [1 ,2 ]
机构
[1] Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 611731, Peoples R China
[2] Univ Elect Sci & Technol China, Yangtze Delta Reg Inst Huzhou, Huzhou 313001, Peoples R China
[3] Nanyang Technol Univ, Sch Chem & Biomed Engn, Singapore 637457, Singapore
[4] Huazhong Agr Univ, Minist Educ, Coll Sci, Key Lab Environm Correlat Dietol, Wuhan 430070, Peoples R China
基金
中国国家自然科学基金;
关键词
photocatalytic CO2 reduction; Cs2CuBr4; perovskite quantum dots; CO2 adsorption and activation; catalytic mechanism; REDUCTION; EFFICIENT; CU; CATALYSTS; FTIR; NANOPARTICLES; NANOCRYSTALS; METHANATION; CHEMISTRY;
D O I
10.1021/acscatal.2c00037
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Lead (Pb) halide perovskite quantum dots (PQDs) are promising candidates for the photochemical reduction of CO2. However, the intrinsically weak adsorption and activation toward inert CO2 molecules have seriously hindered their practical application. This study reports alternative Cs2CuBr4 PQDs for gas-solid phase photocatalytic CO2 reduction under simulated solar irradiation. Cs2CuBr4 PQDs exhibited CO2 photoreduction performance with CH4 and CO yields of 74.81 and 148.98 mu mol g(-1), respectively. In situ diffuse reflectance infrared Fourier transform spectra and density functional theory calculations cooperatively revealed the synergistic strengthening of microelectronic polarization in Cs2CuBr4 PQDs induced by surface-frustrated Lewis pair-like properties and intrinsic Cu d-band properties facilitated robust CO2 adsorption and activation. This study demonstrated the potential of Cs2CuBr4 PQDs as a platform for highly efficient CO2 photoreduction and provided a distinct concept for CO2 adsorption and activation based on the catalytic mechanism of Cu-based PQDs.
引用
收藏
页码:2915 / 2926
页数:12
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