Abstract
The synthesis of RuCp(PPh2NHR)2Cl (1a,b; R = Ph, n-Pr) and RuTp(PPh2NHR)2Cl (2a,b) is reported. Chloride abstraction from 1a with AgCF3SO3 affords RuCp(PPh2NHPh)2(η1-OSO2CF3) (3), whereas when AgSbF6 is used instead [RuCp(κ2(P,P)-PPh2NHC6H4PPh2)(NH2Ph)]+ (4) is formed. In the course of this reaction the P−N bond of one PPh2NHPh ligand is cleaved while a new P−C bond is formed, with concomitant formation of an aniline ligand. In the presence of Ag+ (CF3SO3- or SbF6-) complexes 1 and 2 react with terminal alkynes HC⋮CR‘ (R‘ = Ph, p-C6H4Me, n-Bu) and propargylic alcohols to give novel azaphosphacarbene complexes of the types [RuCp(κ2(C,P)C(CH2R‘)N(R)PPh2)(κ1(P)-PPh2NHR)]+ (5a−c, 6a−c), [RuTp(κ2(C,P)C(CH2R‘)N(R)PPh2)(κ1(P)-PPh2NHR)]+ (14a,b, 15a−c), [RuCp(κ2(C,P)C(CHCPh2)N(Prn)PPh2)(κ1(P)-PPh2NHPrn)]+ (12), and [RuTp(κ2(C,P)C(CHCPh2)N(Prn)PPh2)(κ1(P)-PPh2NHPrn)]+ (17). These reactions proceed via vinylidene and allenylidene intermediates, respectively, which could be isolated in some cases: viz. [CpRu(PPh2NH...
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