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磁场控制下镍掺杂钙钛矿纳米晶光催化CO2还原性能的增强

Enhanced photocatalytic CO2 reduction performance in Ni-doped perovskite nanocrystals controlled by magnetic fields

  • 摘要: 近年来,磁场已被广泛应用于催化领域,作为一种重要的非接触方式来增强电催化、光催化和热催化的性能。本研究通过在CsPbCl3卤化钙钛矿纳米晶体中掺杂镍离子(Ni2+)并施加外加磁场,显著提高了光催化二氧化碳还原反应(CO2RR)的性能。镍掺杂的CsPbCl3在500 mT磁场下的CO2RR效率提高了6倍。通过光生电流密度测量和X射线磁圆二色性实验,深入了解了这种增强效应的机制。结果表明,磁场对催化性能的显著增强是由于磁元素掺杂与外磁场的协同作用,导致电子-空穴复合减少,载流子寿命延长。本研究提供了一种利用非接触外磁场操纵光催化半导体中的自旋极化电子来提高光催化CO2RR效率的有效策略。

     

    Abstract: In recent years, magnetic fields have been widely applied in catalysis to increase the performance of electrocatalysis, photocatalysis, and thermocatalysis through an important noncontact way. This work demonstrated that doping CsPbCl3 halide perovskite nanocrystals with nickel ions (Ni2+) and applying an external magnetic field can significantly enhance the performance of the photocatalytic carbon dioxide reduction reaction (CO2RR). Compared with its counterpart, Ni-doped CsPbCl3 exhibits a sixfold increase in CO2RR efficiency under a 500 mT magnetic field. Insights into the mechanism of this enhancement effect were obtained through photogenerated current density measurements and X-ray magnetic circular dichroism. The results illustrate that the significant enhancement in catalytic performance by the magnetic field is attributed to the synergistic effects of magnetic element doping and the external magnetic field, leading to reduced electron‒hole recombination and extended carrier lifetimes. This study provides an effective strategy for enhancing the efficiency of the photocatalytic CO2RR by manipulating spin-polarized electrons in photocatalytic semiconductors via a noncontact external magnetic field.

     

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