Electron-Level Kinetics of Spin Catalysis on Curved Carbon Nanosheets

Understanding how electron-spin dynamics govern catalytic reactions remains challenging in designing metal-free spin catalysts. Herein, we report curved carbon nanosheets (CCNs) with a high density of pentagonal topological defects that induce strong spin polarization and mixed σ/π spin states, leading to high performance for aerobic oxidation reactions. An exponential relationship between electron spin-lattice relaxation time (T₁) of CCNs and O₂ percentage is observed through in situ gas blowing electron paramagnetic resonance (EPR). Various catalytic aerobic oxidation reactions have been conducted at different O₂ percentage and a kinetic formula Conversion (%) = a_n + b_n * lnT₁ is summarized, which indicates a T₁ controlled spin catalytic mechanism in the aerobic oxidation reaction. The study provides valuable insights into the spin dynamics of catalysts and their interactions with triplet O₂, deepening the understanding of catalysis to an electron level, which also paves the way for investigating catalytic processes in other spin involving reactions.