Towards Tailored Dialdehyde Cellulose Derivatives: A Strategy for Tuning the Glass Transition Temperature

The derivatization of dialdehyde cellulose (DAC) has received increasing attention in the development of sustainable thermoplastics. In this study, a series of dialcohol celluloses were generated by borohydride reduction, which exhibited glass transition temperature (Tg) values ranging from 23 to 109 degrees C, depending on the initial degree of oxidation (DO) of the DAC intermediate. However, the DAC derivatives did not exhibit thermoplastic behavior when the DO of the modified DAC was below 26 %. The influence of introduced side chains was highlighted by comparing DAC-based thermoplastic materials obtained by either oximation or borohydride reduction. Our results provide insights into the generation of DAC-based thermoplastics and highlight a strategy for tailoring the Tg by adjusting the DO during the periodate oxidation step and selecting appropriate substituents in subsequent modifications. Precise control over the glass transition temperature (Tg) is a critical aspect when developing sustainable thermoplastics for a wide range of applications. The present study highlights a strategy to tailor Tg of dialdehyde cellulose derivatives by adjusting the ratio of modified and unoxidized glucopyranose units and by introducing different side chains along the polymer backbone.image