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By means of microgravimetry, UV–Vis spectroscopy and optic microscopy, sorption of pyridine, primary aliphatic amines and benzylamine by the Langmuir–Blodgett (LB) films of tetra-4-
tert-butyl- and tetra-(3-nitro-5-
tert-butyl)-substituted cobalt phthalocyanines (CoPc’ and CoPc*, respectively) was studied over a broad concentration range. In general, sorption occurs as stepwise intercalation of the sorbate molecules into the supramolecular 3D structure of the phthalocyanine assembly followed by formation of the donor–acceptor complexes. Both intercalation depth and stoichiometry of the complexes are determined by the molecular structure of amines. The supramolecular factor allows discrimination between amines in air but not in aqueous solutions because of concurrent intercalation of water.