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Synthesis of crystalline materials is elemental in the field of coordination chemistry towards optical applications. In the present work, coordination between copper and benzene-1,3,5-tricarboxylic acid (BTC) is controlled by adjusting the pH scale of the reaction mixture at room temperature to synthesize two crystalline structures metal-organic framework HKUST-1 and coordination polymer Cu(BTC)·3H2O. The post-synthesis transformation of HKUST-1 into Cu(BTC)·3H2O is further demonstrated. Single crystals of both structures are studied by mu