Spatial Confinement Effect of Mof Derived Carbon Nanoreactor: the Crucial Role of Micropores in Selective Capture of Peroxymonosulfate in Aops-Based Process

Carbon-based catalyst activated peroxymonosulfate process suffers from the decay of catalytic activity due to the pore-filling of intermediates. Controllable regulation of pore structure might be a feasible way to selectively capture PMS and prevent organics from entering pores. Herein, a series of carbocatalysts with tunable micropore abundance were synthesized for boosted PMS activation with negligible attenuation within consecutive runs. The results showed that catalyst with higher micropore abundance exhibited efficient kinetic performance (2.38 min-1). DFT calculation demonstrated that the spatial micropore-confined effect strongly elevated the interaction between PMS and catalyst, which accelerated acetaminophen degradation through enhanced van der Waals attraction toward PMS. The selective capture of PMS was proved to be responsible for the negligible attenuation of catalytic activity. Reactive oxidation species were evidenced by quenching experiment and EPR analysis. The findings proposed a brand new insight in enhancing the reusability of carbon-based catalyst through pore-structure tuning for PMS activation.