Two novel metal-organic frameworks with different structures were obtained by reactions of PbI2 with N,N′-bis(3-pyridylmethyl)-1,4-biphenylenedimethyleneimine (L) under different M/L ratios. When the M/L ratio is 1:1, L bridges [PbI2]n chains to form a layered organic–inorganic hybrid compound with the empirical formula [Pb(L)I2] (1). When changing the M/L ratio to 2:1, L bridges the double chains [Pb2I4]n to form networks [Pb2(L)I4] (2), which are further linked by C–H···I hydrogen bonds to give a 3D structure.
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