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The Mechanism of a C-H Bond Activation Reaction in Room-Temperature Alkane Solution

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Science  10 Oct 1997:
Vol. 278, Issue 5336, pp. 260-263
DOI: 10.1126/science.278.5336.260

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Abstract

Chemical reactions that break alkane carbon-hydrogen (C–H) bonds are normally carried out under conditions of high temperature and pressure because these bonds are extremely strong (∼100 kilocalories per mole), but certain metal complexes can activate C–H bonds in alkane solution under the mild conditions of room temperature and pressure. Time-resolved infrared experiments probing the initial femtosecond dynamics through the nano- and microsecond kinetics to the final stable products have been used to generate a detailed picture of the C–H activation reaction. Structures of all of the intermediates involved in the reaction of Tp*Rh(CO)2 (Tp* = HB–Pz3*, Pz* = 3,5-dimethylpyrazolyl) in alkane solution have been identified and assigned, and energy barriers for each reaction step from solvation to formation of the final alkyl hydride product have been estimated from transient lifetimes.

  • * Present address: Department of Chemistry, Emory University, Atlanta, GA 30322, USA.

  • Present address: Pacific Northwest National Laboratory, Post Office Box 999, Richland, WA 99352, USA.

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