High-spin surface Fe^IV = O synthesis with molecular oxygen and pyrite for selective methane oxidation.

ABSTRACT: Nature-inspired high-spin Fe^IV = O generation enables efficient ambient methane oxidation. By engineering sulfur-bridged dual ≡Fe^II…Fe^II≡ sites on pyrite (FeS₂) mimicking soluble methane monooxygenase, we achieve O₂-driven formation of high-spin (S = 2) surface Fe^IV = O species at room temperature and pressure. Strategic removal of bridging S atoms creates active sites that facilitate O₂ activation via transient ≡Fe-O-O-Fe≡ intermediates, promoting homolytic O - O bond cleavage. The resulting Fe^IV = O exhibits an asymmetrically distorted coordination environment that reduces the crystal field splitting and favors the occupation of higher energy d-orbitals with unpaired electrons. Impressively, this conf

SUBMITTER: Ling C 

PROVIDER: S-EPMC12357931 | biostudies-literature | 2025 Aug

REPOSITORIES: biostudies-literature