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Crystallization of Cd[S 2 CN(iPr)CH 2 CH 2 OH] 2  from ethanol yields the coordination polymer [{Cd[S 2 CN(iPr)CH 2 CH 2 OH] 2 }·EtOH] ∞  ( 1 ) within 3 h. When the solution is allowed to stand for another hour, the needles begin to dissolve and prisms emerge of the supramolecular isomer (SI), binuclear {Cd[S 2 CN(iPr)CH 2 CH 2 OH] 2 } 2 ·2EtOH ( 2 ). These have been fully characterized spectroscopically and by X-ray crystallography. Polymeric  1  has 2-fold symmetry and features dithiocarbamate ligands coordinating two octahedral Cd atoms in a  μ  2  κ  2 -tridentate mode. Binuclear  2  is centrosymmetric with two ligands being  μ  2  κ  2 -tridentate as for  1  but the other two being  κ  2 -chelating leading to square pyramidal geometries. The conversion of the kinetic crystallization product,  1 , to thermodynamic  2  is irreversible but transformations mediated by recrystallization (ethanol and acetonitrile) to related literature SI species, namely coordination polymer [{Cd[S 2 CN(iPr)CH 2 CH 2 OH] 2 } 3 ·MeCN] ∞  and binuclear {Cd[S 2 CN(iPr)CH 2 CH 2  OH] 2 } 2 ·2H 2 O·2MeCN, are demonstrated, some of which are reversible. Three other crystallization outcomes are described whereby crystal structures were obtained for the 1:2 co-crystal {Cd[S 2 CN(iPr)CH 2 CH 2 OH] 2 } 2 :2[3-(propan-2-yl)-1,3-oxazolidine-2-thione] ( 3 ), the salt co-crystal [iPrNH 2 (CH 2 CH 2 OH)] 4 [SO 4 ] 2 {Cd[S 2 CN(iPr)CH 2 CH 2 OH] 2 } 2  ( 4 ) and the salt [iPrNH 2 (CH 2 CH 2 OH)]{Cd[S 2 CN(iPr)CH 2 CH 2 OH] 3 } ( 5 ). These arise as a result of decomposition/oxidation of the dithiocarbamate ligands. In each of  3  and  4  the binuclear {Cd[S 2 CN(iPr)CH 2 CH 2 OH] 2 } 2  SI, as in  2 , is observed strongly suggesting a thermodynamic preference for this form.

Exploring the crystallization landscape of cadmium bis( N -hydroxyethyl, N -isopropyldithiocarbamate), Cd[S 2 CN(iPr)CH 2 CH 2 OH] 2