Abstract

A promising way to induce shape transformation in soft materials is via spatial variation in the orientation of the alignment of liquid crystalline elastomers (LCEs). Here, we improve the nascent thermomechanial shape transformation in main-chain LCEs prepared via aza-Michael addition reactions. Specifically, increasing the alkyl length in the n-alkylamine chain extender effectively reduces the actuation temperature by destabilizing the nematic phase as well as reduces the glass transition temperature (Tg) by increasing the free volume. In addition, incorporating a hydroxyl end-group in the amine chain extender (i.e., n-alkanolamine) increases the actuation strain and improves the film quality by preventing side-chain aggregates of n-alkylamine-functionalized LCEs. Interestingly, uniaxially aligned n-alkanolamine-functionalized LCEs exhibit an unprecedentedly large elongation and an enhanced toughness even along the loading direction likely due to hydrogen bonding between chains. Thus, our study highlight...

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