Permanently Mechanically Adjustable Photothermal Catalytic Spontaneous Double Cross‐Linking Network Enables Durable and Stretchable Plant Skin‐Like Materials

Abstract

In cellulose‐based plastics, as a type of thermoplastic and thermosetting materials, the excellent balance of mechanical strength and ductility poses a large challenge. To tackle this problem, a novel approach is devised to introduce reversible non‐covalent ester cross‐linking into dynamic covalent hydrogen‐bonded polymer networks. However, the formation of ester bonds typically requires excess reactants and dehydrating agents, which is energy‐intensive, environmentally harmful, and costly. To address these concerns, inspired by polyester‐rich plant bark, a supramolecular composite material is developed. It can be dissolved and regenerated using a binary solvent system (choline hexanoate/choline chloride‐oxalic acid). In water, this supramolecular composite material underwent self‐healing and ester exchange reactions to form double‐cross‐linked networks, interfaced with photo‐thermal catalysis promoting the reaction due to its high photo‐thermal conversion efficiency (86.7%) and water evaporation rate (1.38 kg m−2 h−1). This enables the rapid and repeatable construction of durable and stretchable biomaterials. The mechanical properties of the supramolecular plastic can be adjusted by solar photo‐thermal conditions of the synthesis environment. These materials exhibit high performance in solar water evaporation and have self‐healing properties and are degradable, recyclable, and capable of eliminating their own adhesions.

A Tough Monolithic‐Integrated Triboelectric Bioplastic Enabled by Dynamic Covalent Chemistry

“…The thin films of polyethylene, RC, cellulose nanopaper, and triboelectric bioplastic were buried in the soil at 1 cm below the ground surface (summer, average temperature 30 °C), and their changes were monitored over time. Due to the presence of natural bacteria, fungi, and other microorganisms in the soil, which directly attack and digest the macromolecular network (cellulose) of bioplastics, [ 30 ] these macromolecules are completely biodegraded after being buried for 20 days. Unlike commercially available polyethylene plastics, which retain their shape after 20 days of soil burial, the triboelectric bioplastic completely degraded and vanished within 45 days.…”

Transforming wastes into functional materials: natural cork-based physical structural components and polymers

“…14d), formed thin films with antimicrobial properties against Escherichia coli and Staphylococcus aureus. 158 Additionally, the dissolution and regeneration of cork using a binary solvent system (choline caproate/choline chloride–oxalic acid) facilitated the formation of a supramolecular complex exhibiting self-healing properties and ester exchange reactions, culminating in the production of durable and stretchable biomaterials with excellent mechanical properties 159 (Fig. 15a).…”

“…Fig.15(a) Schematic diagram of bioplastics prepared under photothermal catalysis. The structural linkages between regenerated suberin, lignin, and cellulose 159. Copyright 2023, Wiley-VCH.…”

Research on Toughening Polylactic Acid by an Epoxy Soybean Oil Curing Network Based on Dynamic Cross-Linking

“…In recent years, there has been a growing interest in the utilization of biobased environmentally friendly materials and the exploration of reversible dynamic networks to address the performance deficiencies in materials. − Notably, in 2011, Leibler successfully synthesized an epoxy resin material known as “Vitrimer” through a reversible ester-exchange reaction, catalyzed by zinc acetate. “Vitrimer” represents an epoxy resin material founded on a covalently adaptive network established through ester exchange reactions and remains one of the most extensively studied reversible reactions in the field. ,− The ester exchange reaction involves ester groups and hydroxyl groups undergoing a reaction, catalyzed by heat and catalysts, resulting in the formation of new ester and hydroxyl groups .…”