Exchangeable Liquid Crystalline Elastomers: Enabling Rapid Processing and Enhanced Actuation Stability through On-Demand Deactivation

Liu, Yumeng; Dong, Zhixiang; Wang, Yihai; Ding, Jian; Liu, Tuan; Long, Juan; Zhong, Tuhua; Pekol, Collin; Rios, Orlando; Keum, Jong; Xia, Min; Jiang, Naisheng; Li, Yuzhan

doi:10.1021/acs.macromol.4c00729

Exchangeable Liquid Crystalline Elastomers: Enabling Rapid Processing and Enhanced Actuation Stability through On-Demand Deactivation

Journal Article · Fri Oct 04 00:00:00 EDT 2024 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.4c00729· OSTI ID:2478335

Liu, Yumeng ^[1]; Dong, Zhixiang ^[2]; Wang, Yihai ^[1]; Ding, Jian ^[3]; ^[3]; Long, Juan ^[4]; ^[4]; ^[5]; Rios, Orlando ^[5]; ^[6]; Xia, Min ^[7]; ^[2]; ^[2]

Univ. of Science and Technology, Beijing (China)
Univ. of Science and Technology, Beijing (China); Liaoning Academy of Materials, Shenyang (China)
Shanghai Jiao Tong Univ. (China)
International Center for Bamboo and Rattan, Beijing (China)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Beijing Institute of Technology (China)

Exchangeable liquid crystalline elastomers (xLCEs) bearing dynamic covalent bonds are promising candidates for soft actuators due to their unique capability to adjust both network structure and liquid crystalline (LC) alignment after polymerization. While current xLCEs with low exchange temperatures are convenient for processing, they suffer from issues such as creep and loss of LC alignment during repeated thermal actuation. Herein, we present an effective solution using dynamic anhydride chemistry within a thiol-ene-based xLCE. This approach enables a catalyst-free, low-temperature bond exchange of the xLCE after polymerization, allowing for the adjustment of LC orientation under mild conditions. More importantly, it enables on-demand deactivation of the bond exchange via anhydride hydrolysis, effectively eliminating creep and enhancing actuation stability for over 100 cycles. Furthermore, the hydrolysis process results in the formation of carboxylic acid groups, which can be converted into carboxylates via alkali treatment, thereby providing the xLCE with humidity responsiveness. Finally, these findings highlight the use of dynamic anhydride bonds in the fabrication and optimization of xLCEs with enhanced durability and functionality, which is expected to facilitate significant advancements in their applications in soft actuators and robotics.

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This content will become publicly available on Sat Oct 04 00:00:00 EDT 2025

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: AC05-00OR22725; 52073025

OSTI ID:: 2478335

Journal Information:: Macromolecules, Vol. 57, Issue 20; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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