LAUSR

Structural regulation of the active centers is often pivotal in controlling the catalytic functions, especially in iron-based oxidation systems. Here, we discovered a significantly altered catalytic oxidation pathway via a simple cation intercalation into a layered iron oxychloride (FeOCl) scaffold. Upon intercalation of FeOCl with potassium iodide (KI), a new stable phase of K+-intercalated FeOCl (K-FeOCl) was formed with slided layers, distorted coordination, and formed high-spin Fe(II) species compared to the pristine FeOCl precursor. This structural manipulation steers the catalytic H2O2 activation from a traditional Fenton-like pathway on FeOCl to a nonradical ferryl (Fe(IV)═O) pathway. Consequently, the K-FeOCl catalyst can efficiently remove various organic pollutants with almost 2 orders of magnitude faster reaction kinetics than other Fe-based materials via an oxidative coupling or polymerization pathway. A reaction-filtration coupled process based on K-FeOCl was finally demonstrated and could potentially reduce the energy consumption by almost 50%, holding great promise in sustainable pollutant removal technologies.