期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 142, 期 36, 页码 15527-15535出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c07300
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资金
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences Energy Frontier Research Centers program [DE-SC-0019466]
- NSF [CHE-1112299, CHE-1566258]
A low-coordinate, high spin (S = 3/2) organometallic iron(I) complex is a catalyst for the isomerization of alkenes. A combination of experimental and computational mechanistic studies supports a mechanism in which alkene isomerization occurs by the allyl mechanism. Importantly, while substrate binding occurs on the S = 3/2 surface, oxidative addition to an eta(1)-allyl intermediate only occurs on the S = 1/2 surface. Since this spin state change is only possible when the alkene substrate is bound, the catalyst has high immunity to typical sigma-base poisons due to the antibonding interactions of the high spin state.
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