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  1. Biomass-based polymers show promise for the mitigation of environmental issues associated with petroleum-derived commodity polymers; however, due to poor entanglement, many of these polymers typically lack mechanical strength and toughness. Herein, we report a facile approach to utilizing metal–ligand coordination to create physical crosslinking, and thus chain entanglements for plant oil-derived polymers. A series of soybean oil-derived copolymers containing a pendant acid group can be easily synthesized using free radical polymerization. The resulting chain architecture can be controlled through supramolecular interactions to produce bioplastics with enhanced thermomechanical properties. The metal–ligand coordination in this work can be varied by changing the metal lability and the density of metal–ligand bonds, allowing for further control of properties. The final bioplastics remain reprocessable and feature good thermoplastic and stimuli-responsive properties. 
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  2. Abstract

    Advanced templating techniques have enabled delicate control of both nano‐ and microscale structures and have helped thrust functional materials into the forefront of society. Cellulose nanomaterials are derived from natural polymers and show promise as a templating source for advanced materials. Use of cellulose nanomaterials in templating combines nanoscale property control with sustainability, an attribute often lacking in other templating techniques. Use of cellulose nanofibers for templating has shown great promise in recent years, but previous reviews on cellulose nanomaterial templating techniques have not provided extensive analysis of cellulose nanofiber templating. Cellulose nanofibers display several unique properties, including mechanical strength, porosity, high water retention, high surface functionality, and an entangled fibrous network, all of which can dictate distinctive aspects in the final templated materials. Many applications exploit the unique aspects of templating with cellulose nanofibers that help control the final properties of the material, including, but not limited to, applications in catalysis, batteries, supercapacitors, electrodes, building materials, biomaterials, and membranes. A detailed analysis on the use of cellulose nanofibers templating is provided, addressing specifically how careful selection of templating mechanisms and methodologies, combined toward goal applications, can be used to directly benefit chosen applications in advanced functional materials.

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