| Abstract
| - The complex [(η6-p-cymene)OsCl(CHPh)(IPr)]OTf(1) releases the arene in acetonitrile at 40 °C. The resulting12-valence-electron metallic fragment is trapped by the solventto afford the tris(solvento) compound [OsCl(CHPh)(NCCH3)3(IPr)]OTf (2), which reacts with AgOTf in acetonitrile at roomtemperature to give the tetrakis(solvento) derivative [Os(CHPh)(NCCH3)4(IPr)](OTf)2 (3). In dichloromethane at 40 °C,the treatment of 1 with triisopropylphosphine and triphenylphosphine yields the unsaturated five-coordinate mixedphosphine−NHC hydride−alkylidyne−osmium species [OsHCl(⋮CPh)(IPr)(PR3)]OTf (R = iPr (4), Ph (5)).
- An alkylidene ligand favors the dissociation of the arene from the octahedral half-sandwich osmium derivative [(η6-p-cymene)OsCl(CHPh)(IPr)]OTf, which is trapped by acetonitrile to afford tris- and tetrakis(solvento) alkylidene−osmium complexes. Reactions with phosphines yield the unsaturated five-coordinate mixed phosphine−NHC hydride−alkylidyne−osmium species [OsHCl(⋮CPh)(IPr)(PR3)]OTf (R = iPr, Ph).
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