Mechanically Robust, Self-Repairable, Shape Memory and Recyclable Ionomeric Elastomer Composites with Renewable Lignin via Interfacial Metal–Ligand Interactions

Lignin, the most abundant aromatic polymer in nature, is one of the most promising renewable feedstocks for value-added polymer products. However, it is challenging to prepare high-performance and multifunctional polymer materials with renewable lignin because of its poor compatibility with the elastomer matrix. In fact, lignin often requires solvent fractionation, chemical modification, or prohibitively expensive additives. This work develops a cost-effective strategy to prepare ionomeric elastomer composites based on a commercial carboxyl elastomer and a high content of lignin without purification or chemical modification. The compatibility between the elastomer and lignin is improved by the incorporation of zinc oxide which creates metal-ligand coordination at the interfaces between the carboxyl groups of the elastomer and the oxygen-bearing groups of the lignin. This results in fine dispersion of the lignin in the elastomer matrix, even when its content reaches 50 wt %. The lignin/elastomer composites show excellent mechanical properties, which are attributed to the reinforcing effect of the lignin domains and the presence of abundant sacrificial coordination bonds. Moreover, ionic bonds and ionic aggregates created by the neutralization of the zinc ions with the carboxyl groups of the elastomer behave as physical crosslinks which endow the composites with excellent recyclability; namely, their mechanical properties are retained or even improved after multiple reprocessing cycles. They also show good self-repairability and shape memory. Hence, this work may open up new avenues to utilize lignin as a renewable alternative to petroleum derivatives for designing and fabricating high-performance and multifunctional elastomer materials.