Wu Wubin, Yin Baipeng, Peng Wei, Zhao Yukun, Zhou Zeyang, Sheng Hua, Ma Wanhong, Zhang Chuang
Key Laboratory of Photochemistry, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
University of Chinese Academy of Sciences, Beijing 100049, China.
iScience. 2021 Apr 21;24(5):102458. doi: 10.1016/j.isci.2021.102458. eCollection 2021 May 21.
The chemical reactions involving excited-state radical pairs (RPs) of parallel/anti-parallel spin configurations are sensitive to magnetic field, leading to the possibilities of magnetically controlled synthesis of chemical compounds. Here we show that the reaction of anthraquinone (AQ) in sodium dodecyl sulfate (SDS) micellar solution under UV excitation is significantly influenced by applying external field. The steady state and time-resolved spectroscopies reveal that the reaction intermediate (pairs of AQH-SDS radicals) can undergo two distinct pathways depending on whether it is spin singlet or triplet, and the field is beneficial to the conversion between spin configurations of RPs. The applied field not only affects the reaction rate constant but also changes the final products. Besides, the aggregation of AQ molecules would change the population of singlets and triplets and thus enhance magnetic field effect. This work represents a promising way of controlling chemical reaction and improving reaction selectivity magnetic field methods.
涉及平行/反平行自旋构型的激发态自由基对(RPs)的化学反应对磁场敏感,这使得通过磁场控制化合物的合成成为可能。在此我们表明,在紫外光激发下,蒽醌(AQ)在十二烷基硫酸钠(SDS)胶束溶液中的反应受到外部磁场的显著影响。稳态光谱和时间分辨光谱表明,反应中间体(AQH-SDS自由基对)根据其是自旋单重态还是三重态可经历两种不同的途径,并且磁场有利于自由基对自旋构型之间的转换。施加的磁场不仅影响反应速率常数,还会改变最终产物。此外,AQ分子的聚集会改变单重态和三重态的数量,从而增强磁场效应。这项工作代表了一种通过磁场方法控制化学反应并提高反应选择性的有前景的方式。