Hydrogenolysis of [PhBP3]Fe[triple bond]N-p-tolyl: probing the reactivity of an iron imide with H2 |
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Authors: | Brown Steven D Peters Jonas C |
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Institution: | Division of Chemistry and Chemical Engineering, Arnold and Mabel Beckman Laboratories of Chemical Synthesis, California Institute of Technology, Pasadena, California 91125, USA. |
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Abstract: | This paper describes the reductive hydrogenolysis of a low-spin (S = 1/2) iron(III) imide. Pseudotetrahedral PhBP3]FeIIIN-p-tolyl is reduced by hydrogen at ambient temperature and pressure in benzene solution. The reduction appears to proceed in a stepwise fashion. An intermediate S = 2 iron(II) anilide, PhBP3]Fe(N(H)-p-tolyl), is observed and has been independently generated and structurally characterized. Prolonged hydrogenolysis in benzene results in the complete hydrogenolysis of the Fe-N linkage to release H2N-p-tolyl. The major iron-containing product formed from this step is the diamagnetic cyclohexadienyl complex, PhBP3]Fe(eta5-cyclohexadienyl), which has also been independently prepared and structurally characterized. Evidence is presented to suggest that the final PhBP3]Fe(eta5-cyclohexadienyl) product is formed via benzene insertion into a reactive PhBP3]FeII-H intermediate. |
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