Self-healing and shape-memory polymers based on cellulose acetate matrix

The creation of self-healing polymers with superior strength and stretchability from biodegradable materials is attracting increasing attention. In this study, we synthesized new biomass-derived cellulose acetate (CA) derivatives by ring-opening graft polymerization of δ-valerolactone followed by the introduction of ureidopyrimidinone (Upy) groups in the polymer side chains. Due to the semicrystalline aliphatic characteristics of the side chain poly(δ-valerolactone) (PVL) and quadruple hydrogen bonds formed by the Upy groups, the stretchability of the resulting polymers was significantly enhanced. Moreover, the shape memory ability and self-healing property (58.3% of self-healing efficiency) were successfully imparted to the polymer. This study demonstrates the great significance of using biomass sources to create self-healing polymers. This paper describes the first successful demonstration of self-healing polymers with superior strength and stretchability from a biodegradable material, cellulose acetate (CA). We initially introduced the ureidopyrimidinone (Upy) groups in the side chains of CA. However, the resulting polymer was not soluble and processable. In order to solve this issue, a new strategy based on the ring-opening graft polymerization of δ-valerolactone followed by the introduction of ureidopyrimidinone (Upy) groups was adopted. Due to the semicrystalline aliphatic characteristics of the side chain poly(δ-valerolactone) (PVL), the resulting polymers were soluble and processable. In addition, the quadruple hydrogen bonds formed by the Upy groups enhanced the stretchability of the resulting polymers. Moreover, the shape memory ability and self-healing property were successfully achieved due to the presence of PVL and Upy. The developed new strategy can be applied to a variety of polymers including biomass-based polymers and materials.</p