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Article Abstract
The advancement of atomically precise dinuclear heterogeneous catalysts holds great potential in achieving efficient catalytic ozonation performance and contributes to the understanding of synergy mechanisms during reaction conditions. Herein, we demonstrate a "ship-in-a-bottle and pyrolysis" strategy that utilizes Fe(CO) dinuclear-cluster to precisely construct Fe site, consisting of two Fe-N units connected by Fe-Fe bonds and firmly bonded to N-doped carbon. Systematic characterizations and theoretical modeling reveal that the Fe-Fe coordination motif markedly reduced the devotion of the antibonding state in the Fe-O bond because of the strong orbital coupling interaction of dual Fe - orbitals. This facilitates O-O covalent bond cleavage of O and enhances binding strength with reaction intermediates (atomic oxygen species; *O and *OO), thus boosting catalytic ozonation performance. As a result, Fe dinuclear site catalyst exhibits 100% ozonation efficiency for CHSH elimination, outperforming commercial MnO catalysts by 1,200-fold. This research provides insights into the atomic-level structure-activity relationship of ozonation catalysts and extends the use of dinuclear catalysts in catalytic ozonation and beyond.
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| http://www.ncbi.nlm.nih.gov/pmc/articles/PMC11032441 | PMC |
| http://dx.doi.org/10.1073/pnas.2319119121 | DOI Listing |
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