A series of optically transparent composites were made by using tunicate cellulose membranes, in which the naturally organized cellulose microfibrillar network structure of tunicate tunics was preserved and used as the template and a solution of glycerol and citric acid at different molar ratios was used as the matrix. Polymerization through ester bond formation occurred at elevated temperatures without any catalyst, and water was released as the only byproduct. The obtained composites had a uniform and dense structure. Thus, the produced glycerol citrate polyester improved the transparency of the tunicate cellulose membrane while the cellulose membrane provided rigidity and strength to the prepared composite. The interaction between cellulose and polyester afforded the composites high thermal stability. Additionally, the composites were optically transparent and their shape, strength, and flexibility were adjustable by varying the formulation and reaction conditions. These composites of cellulose, glycerol, and citric acid are renewable and biocompatible and have many potential applications as structural materials in packaging, flexible displays, and solar cells.
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