Spin-Polarized Photocatalytic CO2Reduction of Mn-Doped Perovskite Nanoplates

Cheng Chieh Lin, Ting Ran Liu, Sin Rong Lin, Karunakara Moorthy Boopathi, Chun Hao Chiang, Wen Yen Tzeng, Wan Hsiu Chang Chien, Hua Shu Hsu, Chih Wei Luo, Hui Ying Tsai, Hsin An Chen, Pai Chia Kuo, Jessie Shiue, Jau Wern Chiou, Way Faung Pong, Chia Chun Chen, Chun Wei Chen*

*此作品的通信作者

研究成果: 雜誌貢獻期刊論文同行評審

8 引文 斯高帕斯(Scopus)

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.

原文英語
頁(從 - 到)15718-15726
頁數9
期刊Journal of the American Chemical Society
144
發行號34
DOIs
出版狀態已發佈 - 2022 8月 31

ASJC Scopus subject areas

  • 催化
  • 化學 (全部)
  • 生物化學
  • 膠體和表面化學

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