Spontaneous Fe^III/Fe^II redox cycling in single-atom catalysts: Conjugation effect and electron delocalization.

ABSTRACT: The mechanism of spontaneous Fe^III/Fe^II redox cycling in iron-centered single-atom catalysts (I-SACs) is often overlooked. Consequently, pathways for continuous SO₄ ^·-/HO⋅ generation during peroxymonosulfate (PMS) activation by I-SACs remain unclear. Herein, the evolution of the iron center and ligand in I-SACs was comprehensively investigated. I-SACs could be considered as a coordination complex created by iron and a heteroatom N-doped carbonaceous ligand. The ligand-field theory could well explain the electronic behavior of the complex, whereby electrons delocalized by the conjugation effect of the ligand were confirmed to be responsible for the Fe^III/Fe^II redox cycle. The possible pyridinic ligand in I-SACs was demonstrab

SUBMITTER: Qian Z 

PROVIDER: S-EPMC9860487 | biostudies-literature | 2023 Jan

REPOSITORIES: biostudies-literature