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The bilayer compounds [n-CnH2n+1N(CH3)3]2ZnCl4 (n=16,18) exist the solid-solid phase transition in the temperatures range 310-340K.The low temperature crystal structures of the pure compounds are characteristic of the piling of sandwiches in which a two-dimensional macro-anion ZnCl42 is sandwiched between two alkylammonium layers.These layers become conformationally disordered in the high temperature phases.The structures can alternatively be viewed as a double layer of alkylammonium ions between ZnCl42-sheets and can be considered as crystalline models of lipid bilayers.The experimental subsolidus binary phase diagram of [n-C16H33N(CH3)3]2ZnCl4-[n-C18H37N(CH3)3]2ZnCl4 has been established over the whole composition range by Differential scanning calorimetry(DSC) and X-ray diffraction.In the phase diagram,one intermediate compound [n-C16H33N(CH3)3] [n-C18H37N(CH3)3]ZnCl4 at WC16C3Zn％=47.50％ and two eutectoid invariants points at WC16C3Zn％=35.10％ and WC16c3Zn％=75.70％ were observed,two eutectoids temperatures are about 320±1K.and 315±1K.There are three noticeable solid solution ranges (α,β,γ) at the left and right boundary and middle of the phase diagram.