In iron-catalyzed oxidation reaction, structure regulation of active centers is pivotal in designing their catalytic functions.Here, we developed a potassium (K+)-intercalated iron oxychloride (K-FeOCl) material by reductive intercalation into the FeOCl scaffold. Upon intercalation, the K-FeOCl is subject to not only an interlayer expansion but also the formation of a new phase with layer sliding and formed high-spin Fe(II) species. The intercalation can further steer the catalytic H2O2 activation from a traditional Fenton-like pathway on FeOCl to a non-radical ferryl (Fe(IV)) pathway. Consequently, the K-FeOCl catalyst can efficiently remove various organic pollutants with almost two orders of magnitude faster reaction kinetics via oxidative coupling than other Fe-based materials. This special reactivity is further demonstrated to be strongly correlated with the high-spin Fe(II) states and the generation of ferryl species.

Interlayer electronic structure manipulation of iron oxychloride by potassium cation intercalation to steer activation pathway of H2O2

ACS Fall 2021

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