Preparation of shape memory polyurethane/modified cellulose nanocrystals composites with balanced comprehensive performances

Abstract

AbstractIn this work, we first synthesized modified cellulose nanocrystals (MCNC) with 2,4‐toluene diisocyanate and 9,10‐dihydro‐9‐oxa‐10‐phosphaphenanthrene‐10‐oxide via a two‐step in‐situ polymerization method, and then incorporated it with shape memory polyurethane (SMPU) to fabricate composite. It was found that the urethane chains and phosphorus‐containing flame retardant were covalently grafted onto the cellulose nanocrystals surface, and the MCNC exhibited good dispersion level in the SMPU matrix. Due to the crystallization‐induced and flame retardant effects of the prepared MCNC, it could be acted as a multifunctional reinforcer in SMPU composites. Noticeably, the most balanced improvements in crystallization, shape memory, mechanical, thermal stability, and flame retardancy properties of composites were observed with the incorporation of 3 wt% MCNC. Shape memory experiment demonstrated that the SMPU‐MCNC3 composite exhibited admirable thermal induced shape memory behavior, and its shape fixity and shape recovery ratios were maintained above 90% after five cycles. More importantly, the SMPU‐MCNC3 composite showed well balanced mechanical (σb = 13.1 MPa, εb = 189.3%), limiting oxygen index (23.8%), and UL‐94 rating (V‐2) among the prepared polyurethane films. In addition, the representative SMPU‐MCNC3 showed obviously reductions in heat and smoke production during combustion as compared to the neat SMPU. The present work offers a promising route to fabricate shape memory polyurethane composites with versatile functions.