科研之友
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摘要
Understanding the site interaction nature of single‐atom catalysts (SACs), especially densely populated SACs, is vital for their application to various catalytic reactions. Herein, we report a site distance effect, which emphasizes how well the distance of the adjacent copper atoms (denoted as dCu1?Cu1) matches with the reactant peroxydisulfate (PDS) molecular size to determine the Fenton‐like reaction reactivity on the carbon‐supported SACs. The optimized dCu1?Cu1 in the range of 5–6??, which matches the molecular size of PDS, endows the catalyst with a nearly two times higher turnover frequency than that of dCu1?Cu1 beyond this range, accordingly achieving record‐breaking kinetics for the oxidation of emerging organic contaminants. Further studies suggest that this site distance effect originates from the alteration of PDS adsorption to a dual‐site structure on Cu1?Cu1 sites when dCu1?Cu1 falls within 5–6??, significantly enhancing the interfacial charge transfer and consequently resulting in the most efficient catalyst for PDS activation so far.(#br)Site distance effects are important in a Cu1/N‐doped graphene (Cu1/GN) single‐atom catalyst with record‐breaking kinetics in the oxidation of emerging organic pollutants. A strategy is reported to achieve the desired catalyst behavior by matching the active site with the properties of the reaction molecule peroxydisulfate (PDS).
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