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Frustrated Lewis Pair Sites Boosting CO<sub>2</sub> Photoreduction on Cs<sub>2</sub>CuBr<sub>4</sub> Perovskite Quantum Dots

Jianping ShengInstitute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, ChinaYe HeInstitute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, ChinaMing HuangSchool of Chemical and Biomedical Engineering, Nanyang Technological University, 70 Nanyang Drive, 637457, SingaporeChaowei YuanInstitute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, ChinaShengyao WangCollege of Science, Key Laboratory of Environment Correlative Dietology of Ministry of Education, Huazhong Agricultural University, Wuhan 430070, ChinaFan DongInstitute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China
2022en
ABI

Abstract

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 μmol 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.

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