Abstract
Two intermediates are observed in the time-resolved IR spectra of the photoinitiated alkane (RH) activation reaction of Tp*Rh(CO)2 (Tp* = HB−(3,5-dimethylpyrazolyl). Density functional calculations suggest that the first observed intermediate is (η3-Tp*)Rh(CO)···(RH) (RH weakly bound), which subsequently rearranges to (η2-Tp*)Rh(CO)(RH) (RH strongly bound) before undergoing oxidative addition to the product (η3-Tp*)Rh(CO)(R)(H).
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