Synthesis and characterisation of bulky guanidines and phosphaguanidines: precursors for low oxidation state metallacycles

Journal Publication ResearchOnline@JCU
Jin, Guoxia;Jones, Cameron;Junk, Peter C.;Lippert, Kai-Alexander;Rose, Richard P.;Stasch, Andreas
Abstract

Reactions of alkali metal amides or phosphides with the bulky carbodiimide, ArN[double bond, length as m-dash]C[double bond, length as m-dash]NAr (Ar = C6H3Pri2-2,6), followed by aqueous work-ups, have yielded several guanidines, ArNC(NR2)N(H)Ar (R = cyclohexyl (GisoH) or Pri (PrisoH); NR2 = cis-NC5H8Me2-2,6 (PipisoH)), a bifunctional guanidine, {ArNCN(H)Ar}2{µ-N(C2H4)2N} (Pip(GisoH)2), and two phosphaguanidines, ArNC(PR2)N(H)Ar (R = cyclohexyl (CyP-GisoH) or Ph (PhP-GisoH)). A very bulky guanidine, ArNC{N(Ar)SiMe3}N(H)Ar (ArSi-Giso), and an aryl coupled bifunctional guanidine, {ArN(H)C(NPri2)NC6H2Pri2-2,6-}2 (PrisoH)2, have been prepared by other routes. All compounds have been crystallographically characterised and shown to exist in a number of isomeric forms in the solid state. These appear to be largely retained in solution. The deprotonation of GisoH with BunLi in either hexane or THF led to crystallographically characterised dimeric and monomeric complexes respectively, viz. [Li{Li(κ2-N,N'-Giso)2}] and [Li(THF)(η1-N,η3-Ar-Giso)]. Deprotonation of PrisoH and Pip(GisoH)2 with K[N(SiMe3)2] gave the unsolvated polymer, [{K(η1-N,η6-Ar-Priso)}∞], and the solvated complex, [{K(THF)2}{Pip(Giso)2}{K(THF)3}], respectively.

Journal

New Journal of Chemistry

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Volume

33

ISBN/ISSN

1369-9261

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Issue

1

Pages Count

12

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Publisher

Royal Society of Chemistry

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DOI

10.1039/b809120j