Enhancing photoredox catalysis by suppressing back electron transfer with the aid of a spin catalyst

作者：Zhiqiang Dong, Chenli Chen, Lingfang Chen, Mingli Sun, Jun-Zheng Zhan, Shen Zhou, Lijia Cao, Jianyu Liu, Shuming Bai, Jialong Jie, Hongmei Su, Song Gao, Linan Zhou · 发表于：Chemical Science · 年份：2025 · DOI：10.1039/d5sc03124a · 被引用次数：2 · 研究领域：Advanced Photocatalysis Techniques、Electrocatalysts for Energy Conversion、CO2 Reduction Techniques and Catalysts

640 min without spin catalyst). The generality of SCE was demonstrated across diverse substrates spanning varied functional groups and halides (Cl/Br/I). Through integrated time-resolved spectroscopic measurements and density functional theory calculations, we established a quantitative kinetic model revealing that the Gd(iii) center promotes spin conversion of RIPs from singlet to triplet states, thereby effectively suppressing BET to enhance forward reaction flux. This work pioneers the integration of spin catalysis strategy into photoredox systems, offering both a mechanistic framework for spin-state manipulation in reaction engineering and a transformative kinetic approach to boost catalytic efficiency beyond current thermodynamic consideration solely based on redox properties.