Non-isocyanate polyurethanes (NIPU) from renewable resource have attracted much attention for significant benefit for sustainable development and green production. However, the low molar mass and poor mechanical properties of NIPU...

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Plant oils are becoming of high industrial importance due to the persisting challenges befalling with the utilization of fossil fuels. Thus, developing methodologies to produce multifunctional materials by taking advantage of the unique structure of plant oil is highly desired. In this study, castor oil served as a cross-linker and soft segments, by incorporating scalable rhodamine 6G derivatives, to systematically synthesize a series of smart polymers that possess self-toughening and multistimuli-responsive capabilities. The polyurethane elastomers showed 10 times and 60 times increases in tensile strength and toughness, respectively, in comparison with the unmodified polyurethane due to the existence of large amounts of hydrogen bonding, dynamic C−N spiro bonds, rigid benzene ring, and high cross-link densities. The novel polyurethane elastomers exhibited excellent reversible multichromic behaviors in response to light, pH, and mechanics. Notably, the resulting polyurethane elastomers exhibited ultrasensitive sustained photochromism with tunable white emission and rapid reversibility. This study provides a simple and effective strategy to utilize plant oil for multifunctional material preparation and paves the way to open access for application of plant oil-based products in a variety of industry applications, such as sensors, self-fitting tissue scaffolds, and switchable devices.

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