Journal
SCIENCE
Volume 326, Issue 5952, Pages 559-562Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1178919
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Funding
- NIH [5RO1 GM31332]
- National Research Service Award Postdoctoral Fellowship
- NSF [CHE-0639094]
- [CCDC-724011]
- [CCDC-728138]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [0809418] Funding Source: National Science Foundation
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Compared with the enormous arsenal of catalysts used to produce organic compounds, complementary species that are able to mediate sophisticated organometallic transformations are virtually nonexistent. We found that stable N-heterocyclic carbenes (NHCs) can mediate unusual organometallic transformations in solution at room temperature. Depending on the choice of NHC initiator, stoichiometric or catalytic reactions of bis(cyclooctatetraene) iron [Fe(COT)(2)] ensue. The stoichiometric reaction leads to the isolation of a previously unknown mixed-valent species, featuring distinct and directly bonded Fe(0) and Fe(1) centers. In the catalytic process, three iron atoms are fused to afford the tri-iron cluster Fe-3(COT)(3), which is a hydrocarbon analog of Dewar's classic Fe-3(CO)(12) complex. The key step in both of these processes is proposed to involve the NHC's ability to induce metal-metal bond formation. These NHC-mediated reactions provide a foundation on which to develop future organometallic transformations that are catalyzed by organic species.
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