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 ( T 1 ) of CCNs and O 2 percentage is observed through in situ gas blowing electron paramagnetic resonance (EPR). Various catalytic aerobic oxidation reactions have been conducted at different O 2 percentage and a kinetic formula Conversion (%) = a n + b n * lnT 1 is summarized, which indicates a T 1 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 O 2 , deepening the understanding of catalysis to an electron level, which also paves the way for investigating catalytic processes in other spin involving reactions.