Ball-milled prepared Fe3O4-FeSAs-NPs@NC catalyst synergistically facilitate the generation of reactive oxygen species for oxidative trifluoromethylation of alkenes

Heterogeneous catalysts have recently regarded as a promising chose for the thermally-driven generation of the reactive oxygen species (ROS) through catalytic reactions with molecular oxygen , which can facilitate this process by specific geometric and electronic structure. However, the oxidative trifluoromethylation of alkenes to α-trifluoromethylated ketones by CF 3 SO 2 Na is rarely reported in this system. In this work, we report a one-pot polymerization ball milling strategy to construct precursor, and then pyrolyze it to obtain specific carbon nanotubes matrix with Fe/Fe 3 O 4 nanoparticles and single atoms Fe. Remarkably, the optimized catalyst (Fe 3 O 4 -Fe SAs - NPs @NC-1) displays excellent catalytic performance, broad substrates and recyclability for this fluorination reaction via radical pathway. Based on characterizations and mechanistic studies , we discover that the coexistence of Fe/Fe 3 O 4 and Fe-N x not only synergistically facilitates the catalytic efficiency in altering the electronic structure of Fe sites, but also benefits the absorption of O 2 and the ability of the thermally-driven generating ROS which can activate CF 3 SO 2 Na to CF 3 radical. This work offers a method of designing Fe-based catalysts and also opens up a new thermal-heterogeneous catalysis way for the oxidative trifluoromethylation of alkenes .