The transamination reaction of M[N(SiMe3)2]2 with (2‐pyridylmethyl)(tert‐butyldimethylsilyl)amine yields the corresponding homoleptic metal bis[(2‐pyridylmethyl)(tert‐butyldimethylsilyl)amides] of Mg (1), Mn (2), Fe (3), Co (4) and Zn (5). All these compounds crystallize from hexane isotypic in the space group C2/c. From toluene the zinc derivative precipitates as toluene solvate 5·toluene. The molecular structures of these compounds are very similar with large NMN angles to the amide nitrogen atoms with NMN values of 148° (1) and 150° (5) for the diamagnetic compounds and 156° for the paramagnetic derivatives 2 and 3. The Co derivative 4 displays a rather small NCoN angle of 142°. Different synthetic routes have been explored for compound 3 which is also available via the metallation reaction of bis(2,4,6‐trimethylphenyl)iron with (2‐pyridylmethyl)(tert‐butyldimethylsilyl)amine and via the metathesis reaction of lithium (2‐pyridylmethyl)(tert‐butyldimethylsilyl)amide with [(thf)2FeCl2]. In course of the metathesis reaction, an equimolar amount of lithium (2‐pyridylmethyl)(tert‐butyldimethylsilyl)amide and [(thf)2FeCl2] yields heteroleptic (2‐pyridylmethyl)(tert‐butyldimethylsilyl)amido iron(II) chloride (6) which crystallizes as a centrosymmetric dimeric molecule. The oxidative C‐C coupling reaction of 5 with Sn[N(SiMe3)2]2 leads to the formation of tin(II) 1,2‐bis(2‐pyridyl)‐1,2‐bis(tert‐butyldimethylsilylamido)ethane, tin metal and Zn[N(SiMe3)2]2.

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The green title complex, [Co2(CH3)2(C12H21N2Si)2], was obtained from bis­{[μ-N-tert-butyl­dimethyl­silyl-N-(pyridin-2-ylmeth­yl)amido]­chloridocobalt(II)} and methyl­lithium in diethyl ether at 195 K via a metathesis reaction. The dimeric cobalt(II) complex exhibits a crystallographic center of inversion in the middle of the Co2N2 ring (average Co—N = 2.050 Å). The CoII atom shows a distorted tetra­hedral coordination sphere. The exocyclic Co—N bond length to the pyridyl group shows a similar value of 2.045 (4) Å. The exocyclic methyl group has a rather long Co—C bond length of 2.019 (5) Å.