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We report about the synthesis and crystal structure determination of Hg 2 (NCN)Cl 2  (P2 1 /c (No. 14), Z = 4, a = 806.7(1), b = 907.1(2), c = 788.0(1) pm, β = 106.446(3)°, 1374 independent reflections, 67 variables, R 1  = 0.0463) and Hg 3 (NCN) 2 Cl 2  (Pca2 1  (No. 29), Z = 4, a = 702.0(2), b = 1078.5(2), c = 1050.3(2) pm, 1977 independent reflections, 71 variables, R 1  = 0.0380). Both compounds contain infinite -Hg-NCN-Hg- zigzag chains which are linked by additional Hg atoms to result in two-dimensional frameworks characterized by 20-membered rings sharing edges. The remarkably flexible structural backbone [Hg 3 (NCN) 2 ] 2+  hosts additional Cl! anions and HgCl 2  molecules in Hg 2 (NCN)Cl2 but only Cl -  anions in Hg 3 (NCN) 2 Cl 2 , by that reaching a high packing efficiency in both cases.While Hg 2 (NCN)Cl 2  exclusively contains carbodiimide N=C=N 2-  species, Hg 3 (NCN) 2 Cl 2  is the first structural example of an inorganic network built up from both carbodiimide N=C=N 2-  and cyanamide N-C≡N 2-  groups.

Mercury Cyanamide / Carbodiimide Networks: Synthesis and Crystal Structures of Hg 2 (NCN)Cl 2 and Hg 3 (NCN) 2 Cl 2