Single oxygen-based advanced oxidation processes (1O2-AOPs) exhibit great prospects in selective degradation of organic pollutants. However, efficient production of 1O2 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 Co1-ZIFs). Zn4Co1–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 CoN4 sites are generated in Zn4Co1–C, which are beneficial to peroxymonosulfate activation to generate 1O2. 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.

Carbon aerogels (CAs) with 3D interconnected networks hold promise for application in areas such as pollutant treatment, energy storage,a nd electrocatalysis.I n spite of this,i tr emains challenging to synthesizeh ighperformance CAsonalarge scale in asimple and sustainable manner.W er eport an eco-friendly method for the scalable synthesis of ultralight and superporous CAs by using cheap and widely available agarose (AG) biomass as the carbon precursor.Zeolitic imidazolate framework-8 (ZIF-8) with high porosity is introduced into the AG aerogels to increase the specific surface area and enable heteroatom doping. After pyrolysis under inert atmosphere,the ZIF-8/AG-derived nitrogen-doped CAsshow ahighly interconnected porous mazelike structure with al ow density of 24 mg cm À3 ,ahigh specific surface area of 516 m 2 g À1 ,a nd al arge pore volume of 0.58 cm À3 g À1 .T he resulting CAs exhibit significant potential for application in the adsorption of organic pollutants.