催化作用
联轴节(管道)
化学
光化学
组合化学
材料科学
有机化学
冶金
作者
Wenshan Qu,Zhuoyun Tang,Shanjian Tang,Tao Zhong,Huinan Zhao,Shuanghong Tian,Dong Shu,Chun He
标识
DOI:10.1073/pnas.2319119121
摘要
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 2 (CO) 9 dinuclear-cluster to precisely construct Fe 2 site, consisting of two Fe 1 -N 3 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 d - d orbitals. This facilitates O-O covalent bond cleavage of O 3 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 CH 3 SH elimination, outperforming commercial MnO 2 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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