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C-C activation of organic small ring compounds by rearrangement of cycloalkylhydridorhodium complexes to rhodacycloalkanes. Synthesis of metallacyclobutanes, including one with a tertiary M-C bond, by nucleophilic addition to. pi. -allyl complexes

Journal Article · · J. Am. Chem. Soc.; (United States)
DOI:https://doi.org/10.1021/ja00283a033· OSTI ID:6996813

In the initial work on C-H activation by the unsaturated fragment ((eta/sup 5/-C/sub 5/Me/sub 5/)Rh(PMe/sub 3/)) the authors observed, as in the case of the iridium analogue, that generation of this fragment in cyclopropane at -60/sup 0/C resulted only in C-H insertion to give a cyclopropyl hydride 1. Subsequently however, they communicated the observation that 1 rearranges by an intramolecular pathway to the rhodacyclobutane 4 in high yield. This observation presented a unique opportunity to study the direct rearrangement of the initial product of C-H activation, an alkyl hydride, to the C-C insertion product. The following describes, a mechanistic study of the rearrangement of 1 to 4 and the limited success in extending the chemistry to cyclobutane. Additionally some related chemistry on the independent synthesis of rhodacyclobutanes is reported.

Research Organization:
Lawrence Berkeley Lab., CA
DOE Contract Number:
AC03-76SF00098
OSTI ID:
6996813
Journal Information:
J. Am. Chem. Soc.; (United States), Journal Name: J. Am. Chem. Soc.; (United States) Vol. 108:23; ISSN JACSA
Country of Publication:
United States
Language:
English