Iron Single Atoms and Clusters Anchored on Natural N-Doped Nanocarbon with Dual Reaction Sites as Superior Fenton-Like Catalysts

Abstract

Ultra-small metal clusters have emerged as one of the most promising alternatives to heterogeneous Fenton-like catalysts. Despite the high atom utilization and structural stability of catalysts with ultra-small clusters and single-atom sites, there is still challenging for the synthesis of these catalysts due to their facile aggregation. Herein, we successfully fabricated a catalyst (Fe-NC-900) with single-atom sites and ultra-small clusters by a ball milling method, which showed high efficiency and superior stability in catalytic oxidation of refractory organic compounds by activation of peroxymonosulfate (PMS). Combined with chemical quenching experiments and electron spin resonance (ESR), which showed that the 1O2 oxidation and electron transfer mechanism were the main non-radical pathway rather than the high-valent iron oxidation for the degradation of RhB in the Fe-NC-900/PMS system. This work provides useful insights into the design and synthesis of catalysts with single atoms and ultra-small clusters for practical applications in catalytic Fenton-like processes.

Keywords: Natural N-codoped nanocarbon, Fenton-like processes, single atoms and clusters, dual reaction sites catalyst, ball milling