Spin-Polarized Photocatalytic CO 2 Reduction of Mn-Doped Perovskite Nanoplates.

Autor: Lin CC; International Graduate Program of Molecular Science and Technology, National Taiwan University (NTU-MST), Taipei 10617, Taiwan.; Molecular Science and Technology Program, Taiwan International Graduate Program (TIGP), Academia Sinica, Taipei 11529, Taiwan., Liu TR; Department of Materials Science and Engineering, National Taiwan University, Taipei 10617, Taiwan., Lin SR; Department of Chemistry, National Taiwan Normal University, Taipei 11677, Taiwan., Boopathi KM; Department of Materials Science and Engineering, National Taiwan University, Taipei 10617, Taiwan., Chiang CH; Department of Materials Science and Engineering, National Taiwan University, Taipei 10617, Taiwan., Tzeng WY; Department of Electrophysics, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan., Chien WC; Department of Applied Physics, National Pingtung University, Pingtung 90044, Taiwan., Hsu HS; Department of Applied Physics, National Pingtung University, Pingtung 90044, Taiwan., Luo CW; Department of Electrophysics, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan.; Institute of Physics and Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan.; National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan.; Taiwan Consortium of Emergent Crystalline Materials (TCECM), Ministry of Science and Technology, Taipei 10622, Taiwan., Tsai HY; Department of Chemistry, National Taiwan Normal University, Taipei 11677, Taiwan., Chen HA; Institute of Materials Science and Engineering, National Taipei University of Technology, Taipei 10608, Taiwan., Kuo PC; Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 10617, Taiwan., Shiue J; Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 10617, Taiwan.; Institute of Physics, Academia Sinica, Taipei 11520, Taiwan., Chiou JW; Department of Applied Physics, National University of Kaohsiung, Kaohsiung 81148, Taiwan., Pong WF; Department of Physics, Tamkang University, New Taipei City 25137, Taiwan., Chen CC; Department of Chemistry, National Taiwan Normal University, Taipei 11677, Taiwan.; Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 10617, Taiwan., Chen CW; International Graduate Program of Molecular Science and Technology, National Taiwan University (NTU-MST), Taipei 10617, Taiwan.; Department of Materials Science and Engineering, National Taiwan University, Taipei 10617, Taiwan.; Center of Atomic Initiative for New Materials (AI-MAT), National Taiwan University (NTU), Taipei 10617, Taiwan.; Center for Condensed Matter Sciences, National Taiwan University, Taipei 10617, Taiwan.
Jazyk: angličtina
Zdroj: Journal of the American Chemical Society [J Am Chem Soc] 2022 Aug 31; Vol. 144 (34), pp. 15718-15726. Date of Electronic Publication: 2022 Aug 17.
DOI: 10.1021/jacs.2c06060
Abstrakt: "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 CsPbBr 3 halide perovskite nanoplates (NPLs) to boost the photocatalytic CO 2 reduction reaction (CO 2 RR) efficiencies by doping manganese cations (Mn 2+ ) and applying an external magnetic field. Mn-doped CsPbBr 3 (Mn-CsPbBr 3 ) NPLs exhibit an outstanding photocatalytic CO 2 RR compared to pristine CsPbBr 3 NPLs due to creating spin-polarized electrons after Mn doping. Notably, the photocatalytic CO 2 RR of Mn-CsPbBr 3 NPLs is significantly enhanced by applying an external magnetic field. Mn-CsPbBr 3 NPLs exhibit 5.7 times improved performance of photocatalytic CO 2 RR under a magnetic field of 300 mT with a permanent magnet compared to pristine CsPbBr 3 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 CO 2 RR efficiencies of Mn-CsPbBr 3 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 CO 2 RR efficiencies.
Databáze: MEDLINE