Tris (2-pyridylthio) me than e ([Tptm]H) has been employed to synthesize a series of cadmium carbatrane compounds that feature an [N3C] coordination environment. Specifically, [Tptm]H reacts with Cd[N(SiMe3)(2)](2) to afford [Tptm]CdN(SiMe3)(2), which thereby provides access to other derivatives. For example, [Tptrn]CdN(SiMe3)(2) reacts with (i) CO2 to form {[Tptm]Cd(mu-NCO)}(2) and (ii) Me3SiOH and Ph3SiOH to form {[K-3-Tptm]Cd(mu-OSiMe3)}(2) and [Tptm]-CdOSiPh3, respectively. The siloxide compound {k(3)-Tptm]Cd(mu-OSiMe3)}(2) reacts with Me3SiX (X = Cl, Br, O2CMe) to give [Tptm]CdX, while the reaction with PhSiH3 in the presence of CO2 generates the formate complex, [Tptm]CdO2CH, thereby providing evidence for the generation of a proposed cadmium hydride intermediate, {[Tptm] CdH}.