Fabrication of High-Strength, Highly Transparent and Reprocessable Bio-Based Itaconate Polymeric Glass via Constructing a Dual Dynamic Cross-Linked Network

Abstract

Conventional plastics are widely used, but they rely on nonrenewable petrochemical feedstocks. Although existing biobased plastics are derived from sustainable sources, their performance is often inferior to that of petroleum-based plastics. Introducing cross-linked networks can improve the mechanical properties of biobased plastics, but it also renders them nonrecyclable, thereby undermining their sustainability. Therefore, inexpensive biobased dimethyl itaconate was used to prepare biobased itaconate organic glass, and a dual dynamic cross-linked network (hydrogen bonds/hindered urea bonds) was constructed by introducing dynamic hindered urea bonds into the system. This structure not only achieves simultaneous strengthening and toughening of the biobased plastic, but also overcomes challenges in existing studies, such as the difficulty of balancing mechanical strength and transparency, high preparation costs, and poor recyclability. This material exhibited excellent properties: a maximum tensile strength of 33.5 MPa and an elongation at break of 13.9%, representing an increase of 782% in tensile strength and 1831% in elongation at break compared with the sample without dynamic urea bonds. The visible light transmittance exceeds 90%. After one reprocessing cycle, approximately 70% of the mechanical strength and more than 90% of the optical performance were retained, outperforming most existing recyclable biobased plastics. This work provides a feasible strategy for the design of high-performance biobased polymers integrating “function, strength, and recyclability”.