Single-Atom Iron Catalysts with Core-Shell Structure for Peroxymonosulfate Oxidation

The chemical tolerance of ketoenamine covalent organic frameworks (COFs) is excellent; however, the tight crystal structure and low surface area limit their applications in the field of catalysis. In this work, a porous single-atom iron catalyst (FeSAC) with a core-shell structure and high surface area was synthesized by using Schiff base COF nanospheres as the core and ketoenamine COF nanosheets growth on the surfaces. Surface defects were created using sodium cyanoborohydride etching treatment to increase specific surface area. The dye degradation experiments by peroxymonosulfate (PMS) catalyzed by the FeSAC proved that methylene blue can be degraded with a degradation rate constant of 0.125 min^-1 under the conditions of 0.1 g L^-1 catalyst dosage and 0.05 g L^-1 peroxymonosulfate. The FeSAC/PMS system effectively degrades various pollutants in the pH range of 4-10 with over 80% efficiency for four cycles and can be recovered by soaking in iron salt solution. Free radical quenching experiments confirmed that singlet oxygen and superoxide radicals are the main active species for catalysis.