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Crystals of L-leucylglycine (L-Leu–Gly) 0.67-hydrate, C8H16N2O3·0.67H2O, (I), were obtained from an aqueous solution. There are three symmetrically independent dipeptide zwitterionic mol­ecules in (I) and they are parallel to one another. The hydrogen-bond network composed of carboxyl­ate and amino groups and water mol­ecules extends parallel to the ab plane. Hydro­philic regions composed of main chains and hydro­phobic regions composed of the isobutyl groups of the leucyl residues are aligned alternately along the c axis. An imidazolidinone derivative was obtained from L-Leu–Gly and acetone, viz. [(4S)-2,2-dimethyl-4-(2-methyl­prop­yl)-5-oxo­imid­azolidin-3-ium-1-yl]acetate, C11H20N2O3, (II), and was crystallized from a methanol–acetone solution of L-Leu–Gly. The unit-cell parameters coincide with those reported previously for L-Leu–Gly dihydrate revealing that the previously reported values should be assigned to the structure of (II). One of the imidazolidine N atoms is protonated and the ring is nearly planar, except for the protonated N atom. Protonated N atoms and deprotonated carb­oxy groups of neighbouring mol­ecules form hydrogen-bonded chains. The ring carbonyl group is not involved in hydrogen bonding.
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