Rational Regulation of Co-N-C Coordination for High-Efficiency Generation of 1 O 2 toward Nearly 100% Selective Degradation of Organic Pollutants.

Single oxygen-based advanced oxidation processes ( 1 O 2 -AOPs) exhibit great prospects in selective degradation of organic pollutants. However, efficient production of 1 O 2 via tailored design of catalysts to achieve selective oxidation of contaminants remains challenging. Herein, we develop a simple strategy to regulate the components and coordination of Co-N-C catalysts at the atomic level by adjusting the Zn/Co ratio of bimetallic zeolitic imidazolate frameworks (Zn x Co 1 -ZIFs). Zn 4 Co 1 -C demonstrates 98% selective removal of phenol in the mixed phenol/benzoic acid (phenol/BA) solutions. Density functional theory calculations and experiments reveal that more active CoN 4 sites are generated in Zn 4 Co 1 -C, which are beneficial to peroxymonosulfate activation to generate 1 O 2 . Furthermore, the correlation between the origin of selectivity and well-defined catalysts is systematically investigated by the electron paramagnetic resonance test and quenching experiments. This work may provide novel insights into selective removal of target pollutants in a complicated water matrix.