Micropores-confined peroxymonosulfate activation for enhanced catalytic performance and durability

A carbon-activated peroxymonosulfate (PMS) process suffers from decay of catalytic activity due to pore-filling of intermediates. Controllable regulation of pore structure might be a feasible way to achieve continuous exposure of active sites and retard deactivation of the nanocatalysts. 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 a catalyst with higher micropore abundance exhibited efficient kinetic performance (2.38 min⁻¹). Density functional theory calculations demonstrated that the spatial micropore-confined effect strongly elevated the interaction between PMS and the catalyst, which accelerated acetaminophen degradation through enhanced van der Waals attraction toward PMS. Furthermore, the negligible attenuation of catalytic activity in multiple rounds of cycles could be attributed to the micropore-rich structure, which tends to avoid the pore plugging and ensure the continuous exposure of active sites during catalytic process. Reactive oxygen species were evidenced by quenching experiments and EPR analysis. The work proposed a new insight into enhancing the reusability of carbon-based catalysts through pore-structure tuning for PMS activation.