Selective pore regulation of activated carbon using trace carbonate-assisted catalytic activation: Revealing the effect of cation catalysis on pore topology

Activated carbon is an important adsorbent for the adsorption removal of water or gas pollutants due to its low cost, high efficiency, and large-scale production potential; however, currently commercial activated carbon prepared through physical or chemical activation commonly shows a single microporous characteristic, making it difficult to match different kinds of pollutants. Here, we propose a convenient and cost-effective pore regulation strategy by introducing a trace carbonate catalysis process into the activation reaction, in which we find that the types of cations (Na, K, Ca) in carbonate have a significant impact on the pore topology of coal-based activated carbon, further revealing the role of cation induced catalytic gasification in pore regulation. Therein, K and Ca enhance the formation of micropores and meso-/macropores respectively, while Na promotes the pore development across the entire size range resulting in a hierarchically porous structure with high specific surface area. Kinetic analysis, density functional theory calculations, and three-dimensional pore fractal network characterization reveal that the pore development is collectively determined by the gasification reaction rate and depth. Evaluated as adsorbents, the obtained NaAC sample by Na catalysis demonstrates excellent adsorption capacities for both small-molecule toluene (467 mg g-1) and large-molecule tetracycline (374 mg g-1). This work for the first time elucidates the cation-induced gasification effect and provides a simple and cost-effective method for regulating the pore topology of activated carbon with only trace catalyst dosage.