https://scholars.lib.ntu.edu.tw/handle/123456789/632813
標題: | Spin-Polarized Photocatalytic CO2Reduction of Mn-Doped Perovskite Nanoplates | 作者: | Lin, Cheng Chieh Liu, Ting Ran Lin, Sin Rong Boopathi, Karunakara Moorthy Chiang, Chun Hao Tzeng, Wen Yen Chien, Wan Hsiu Chang Hsu, Hua Shu Luo, Chih Wei Tsai, Hui Ying Chen, Hsin An Kuo, Pai Chia Shiue, Jessie Chiou, Jau Wern Pong, Way Faung Chen, Chia Chun CHUN-WEI CHEN |
關鍵字: | NANOCRYSTALS; CONVERSION; EFFICIENT; HYBRIDS | 公開日期: | 31-八月-2022 | 出版社: | AMER CHEMICAL SOC | 卷: | 144 | 期: | 34 | 起(迄)頁: | 15718 | 來源出版物: | Journal of the American Chemical Society | 摘要: | "Spin"has been recently reported as an important degree of electronic freedom to improve the performance of electrocatalysts and photocatalysts. This work demonstrates the manipulations of spin-polarized electrons in CsPbBr3 halide perovskite nanoplates (NPLs) to boost the photocatalytic CO2 reduction reaction (CO2RR) efficiencies by doping manganese cations (Mn2+) and applying an external magnetic field. Mn-doped CsPbBr3 (Mn-CsPbBr3) NPLs exhibit an outstanding photocatalytic CO2RR compared to pristine CsPbBr3 NPLs due to creating spin-polarized electrons after Mn doping. Notably, the photocatalytic CO2RR of Mn-CsPbBr3 NPLs is significantly enhanced by applying an external magnetic field. Mn-CsPbBr3 NPLs exhibit 5.7 times improved performance of photocatalytic CO2RR under a magnetic field of 300 mT with a permanent magnet compared to pristine CsPbBr3 NPLs. The corresponding mechanism is systematically investigated by magnetic circular dichroism spectroscopy, ultrafast transient absorption spectroscopy, and density functional theory simulation. The origin of enhanced photocatalytic CO2RR efficiencies of Mn-CsPbBr3 NPLs is due to the increased number of spin-polarized photoexcited carriers by synergistic doping of the magnetic elements and applying a magnetic field, resulting in prolonged carrier lifetime and suppressed charge recombination. Our result shows that manipulating spin-polarized electrons in photocatalytic semiconductors provides an effective strategy to boost photocatalytic CO2RR efficiencies. |
URI: | https://scholars.lib.ntu.edu.tw/handle/123456789/632813 | ISSN: | 00027863 | DOI: | 10.1021/jacs.2c06060 |
顯示於: | 材料科學與工程學系 |
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