Sustainable Multiple- and Multistimulus-Shape-Memory and Self-Healing Elastomers with Semi-interpenetrating Network Derived from Biomass via Bulk Radical Polymerization

Abstract

Sustainable shape-memory and self-healing elastomers with semi-interpenetrating network were prepared by a simple, efficient, and green bulk radical polymerization of ethyl cellulose, furfural, and fatty-acid-derived monomers. This approach could in situ one-pot form a semi-interpenetrating network elastomer with properties combining multiple-shape-memory and self-healing under solvent-free conditions. These elastomers were found to possess excellent multiple-shape-memory properties toward temperature, water, THF, and methanol. Moreover, the multiple-shape-memory properties could assist the self-healing of these elastomers, which was triggered by heating. Self-healing behavior studies showed that the presence of linear polymers in these elastomers could significantly improve the self-healing performance. This work provides a facile, efficient, and green approach in a solvent-free system to design new-generation sustainable, green, and functional materials.

Two‐Step 3 D‐Printing Approach toward Sustainable, Repairable, Fluorescent Shape‐Memory Thermosets Derived from Cellulose and Rosin

“…The freezing of these molecular chains stored the energy and endowed the material with internal stress. When the thermoset was reheated above the T g , the hydrogen bonds were broken again, the molecular long chain became flexible and started to release the potential stored energy, and the internal stresses drove the thermosets to finish the recovery process …”

“…Ethyl cellulose macromonomer (ECM) and rosin‐based monomer (DAGMA) were synthesized according to previously reported methods. Hexamethylene diisocyanate (HDI), 2‐hydroxyethyl acrylate (HEA), and diphenyl(2,4,6‐trimethylbenzoyl)phosphine oxide were purchased from Macklin Inc. and used as received.…”

“…Recently, we developed a series of forestry‐based monomers derived from cellulose and rosin. From cellulose, we synthesized a methacrylated ethyl cellulose macromonomer (ECM) bearing the hydroxy group, which was used as a crosslinker for the fabrication of crosslinked polymers by free‐radical bulk polymerization . Additionally, we also converted rosin, obtained by tapping pine trees, into a novel acrylate monomer (DAGMA) that consists of characteristic hydrophobic hydrophenanthrene rings with acrylate and hydroxy groups .…”

Arbitrarily 3D Configurable Hygroscopic Robots with a Covalent–Noncovalent Interpenetrating Network and Self‐Healing Ability

“…Figure c demonstrates ultimate tensile strength and healing efficiency comparison of various soft actuator materials (details are in Table S3, Supporting Information) . Thanks to the reversible hydrogen bonding and covalent bonding crosslinking networks (Figure a), our actuator material has two distinctive advantages: i) it exhibits relatively high mechanical ultimate strength (3 MPa) and stretchability, which make it more robust than other soft actuators for further applications . ii) It is able to repeatedly heal itself at low ambient temperature (≤35 °C) with great self‐healing efficiency, which makes it much more suitable for the maintenance of complicated 3D structured actuators.…”

Sustainable self‐healing elastomers with thermoreversible network derived from biomass via emulsion polymerization

“…Furfuryl methacrylate (FMA) is a monomer derived from a biomass feedstock, furfural, and a promising monomer due to its potential availability from different carbohydrates, inulin, and agricultural or forestry waste . FMA can be synthesized from methacrylic acid of bio‐origin from the oil of roman chamomile plant.…”