Deep eutectic solvent inclusions for high-k composite dielectric elastomers

Abstract

Recent advances in novel electroactive devices have placed new requirements on material development. High-performance dielectric elastomers with good mechanical stretchability and high dielectric constant are under high demand. However, the current strategy for fabricating these materials suffers from high cost or low thermal stability, which greatly hinders large-scale industrial production. Herein, we have successfully developed a novel strategy for improving the dielectric constant of polymeric elastomers via deep eutectic solvent inclusion by taking advantage of the low cost, convenient and environmentally benign synthesis process and high ionic conductivity from deep eutectic solvents. The as-prepared composite elastomers showed good stretchability and a greatly enhanced dielectric constant with a negligible increase in dielectric dissipation. Moreover, we have proven the universality of our strategy by using different types of deep eutectic solvents. It is believed that low-cost, easy-synthesis and environmentally friendly deep eutectic solvents including composite elastomers are highly suitable for large-scale industrial production and can greatly broaden the application fields of dielectric elastomers.

Key words： composite materials; deep eutectic solvent; dielectric elastomer; high dielectric constant

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant No. 22078276), the Program for Guangdong Introducing Innovative and Entrepreneurial Teams (Grant No. 2017ZT07C291), Shenzhen Science and Technology Program (Grant No. KQTD20170810141424366), Shenzhen Key Laboratory of Advanced Materials Product Engineering (Grant No. ZDSYS20190911164401990). Qi Zhang thanks the Presidential Fund (Grant No. PF01000949) for supporting his research at CUHK-Shenzhen. Dr. Yifeng Sheng is thanked for the advice on emulsion preparation. Prof. Xilin Wang and Ms. Jinfeng Peng from Tsinghua Shenzhen International Graduate School, Prof. Zhijun Dong and Ms. Lili Wu from Shenzhen Institute of Information Technology are thanked for their support in sample testing.

References

1 Shian S, Bertoldi K, Clarke D R. Dielectric elastomer based “grippers” for soft robotics. Advanced Materials, 2015, 27( 43): 6814– 6819

2 Rafsanjani A, Zhang Y, Liu B, Rubinstein S M, Bertoldi K. Kirigami skins make a simple soft actuator crawl. Science Robotics, 2018, 3( 15): eaar7555

3 Duduta M, Wood R J, Clarke D R. Multilayer dielectric elastomers for fast, programmable actuation without prestretch. Advanced Materials, 2016, 28( 36): 8058– 8063

4 Poulin A, Rosset S, Shea H R. Printing low-voltage dielectric elastomer actuators. Applied Physics Letters, 2015, 107( 24): 244104

5 Hajiesmaili E, Clarke D R. Reconfigurable shape-morphing dielectric elastomers using spatially varying electric fields. Nature Communications, 2019, 10( 1): 1– 7

6 Shi L, Yang R, Lu S, Jia K, Xiao C, Lu T, Wang T, Wei W, Tan H, Ding S. Dielectric gels with ultra-high dielectric constant, low elastic modulus, and excellent transparency. NPG Asia Materials, 2018, 10( 8): 821– 826

7 Ke Y, Chen J, Lin G, Wang S, Zhou Y, Yin J, Lee P S, Long Y. Smart windows: electro-, thermo-, mechano-, photochromics, and beyond. Advanced Energy Materials, 2019, 9( 39): 1902066

8 Kim H N, Yang S. Responsive smart windows from nanoparticle–polymer composites. Advanced Functional Materials, 2020, 30( 2): 1902597

9 Kim H N, Ge D, Lee E, Yang S. Multistate and on-demand smart windows. Advanced Materials, 2018, 30( 43): 1803847

10 Xu C, Stiubianu G T, Gorodetsky A A. Adaptive infrared-reflecting systems inspired by cephalopods. Science, 2018, 359( 6383): 1495– 1500

11 Pelrine R, Kornbluh R, Pei Q, Joseph J. High-speed electrically actuated elastomers with strain greater than 100%. Science, 2000, 287( 5454): 836– 839

12 Mannsfeld S C, Tee B C, Stoltenberg R M, Chen C V H, Barman S, Muir B V, Sokolov A N, Reese C, Bao Z. Highly sensitive flexible pressure sensors with microstructured rubber dielectric layers. Nature Materials, 2010, 9( 10): 859– 864

13 Carpi F, Bauer S, De Rossi D. Stretching dielectric elastomer performance. Science, 2010, 330( 6012): 1759– 1761

14 Carpi F, Frediani G, Turco S, De Rossi D. Bioinspired tunable lens with muscle-like electroactive elastomers. Advanced Functional Materials, 2011, 21( 21): 4152– 4158

15 Quinsaat J E Q, Alexandru M, Nüesch F A, Hofmann H, Borgschulte A, Opris D M. Highly stretchable dielectric elastomer composites containing high volume fractions of silver nanoparticles. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 2015, 3( 28): 14675– 14685

16 Biggs J, Danielmeier K, Hitzbleck J, Krause J, Kridl T, Nowak S, Orselli E, Quan X, Schapeler D, Sutherland W, Wagner J. Electroactive polymers: developments of and perspectives for dielectric elastomers. Angewandte Chemie International Edition, 2013, 52( 36): 9409– 9421

17 Sun W, Mao J, Wang S, Zhang L, Cheng Y. Review of recent advances of polymer based dielectrics for high-energy storage in electronic power devices from the perspective of target applications. Frontiers of Chemical Science and Engineering, 2021, 15( 1): 18– 34

18 Li P, Wang Y, Gupta U, Liu J, Zhang L, Du D, Foo C C, Ouyang J, Zhu J. Transparent soft robots for effective camouflage. Advanced Functional Materials, 2019, 29( 37): 1901908

19 Zhalmuratova D, Chung H J. Reinforced gels and elastomers for biomedical and soft robotics applications. ACS Applied Polymer Materials, 2020, 2( 3): 1073– 1091

20 Ilami M, Bagheri H, Ahmed R, Skowronek E O, Marvi H. Materials, actuators, and sensors for soft bioinspired robots. Advanced Materials, 2021, 33( 19): 2003139

21 Ning N, Ma Q, Liu S, Tian M, Zhang L, Nishi T. Tailoring dielectric and actuated properties of elastomer composites by bioinspired poly(dopamine) encapsulated graphene oxide. ACS Applied Materials & Interfaces, 2015, 7( 20): 10755– 10762

22 Panahi M, Zahiri B, Noroozi M. Graphene-based composite for dielectric elastomer actuator: a comprehensive review. Sensors and Actuators. A, Physical, 2019, 293 : 222– 241

23 Cakmak E, Fang X, Yildiz O, Bradford P D, Ghosh T K. Carbon nanotube sheet electrodes for anisotropic actuation of dielectric elastomers. Carbon, 2015, 89 : 113– 120

24 Zhao H, Zhang L, Yang M H, Dang Z M, Bai J. Temperature-dependent electro-mechanical actuation sensitivity in stiffness-tunable BaTiO₃/polydimethylsiloxane dielectric elastomer nanocomposites. Applied Physics Letters, 2015, 106( 9): 092904

25 Luo S, Yu S, Sun R, Wong C P. Nano Ag-deposited BaTiO₃ hybrid particles as fillers for polymeric dielectric composites: toward high dielectric constant and suppressed loss. ACS Applied Materials & Interfaces, 2014, 6( 1): 176– 182

26 Bartlett M D, Fassler A, Kazem N, Markvicka E J, Mandal P, Majidi C. Stretchable, high-k dielectric elastomers through liquid-metal inclusions. Advanced Materials, 2016, 28( 19): 3726– 3731

27 Pan C, Markvicka E J, Malakooti M H, Yan J, Hu L, Matyjaszewski K, Majidi C. A liquid-metal-elastomer nanocomposite for stretchable dielectric materials. Advanced Materials, 2019, 31( 23): e1900663

28 Ankit T N, Ho F, Krisnadi F, Kulkarni M R, Nguyen L L, Koh S J A, Mathews N. High-k, ultrastretchable self-enclosed ionic liquid-elastomer composites for soft robotics and flexible electronics. ACS Applied Materials & Interfaces, 2020, 12( 33): 37561– 37570

29 Shi L, Zhang C, Du Y, Zhu H, Zhang Q, Zhu S. Improving dielectric constant of polymers through liquid electrolyte inclusion. Advanced Functional Materials, 2021, 31( 8): 2007863

30 Zhong M, Tang Q F, Zhu Y W, Chen X Y, Zhang Z J. An alternative electrolyte of deep eutectic solvent by ChCl and EG for wide temperature range supercapacitors. Journal of Power Sources, 2020, 452 : 227847

31 Zhao J, Zhang J, Yang W, Chen B, Zhao Z, Qiu H, Dong S, Zhou X, Cui G, Chen L. “Water-in-deep eutectic solvent” electrolytes enable zinc metal anodes for rechargeable aqueous batteries. Nano Energy, 2019, 57 : 625– 634

32 Parnham E R, Drylie E A, Wheatley P S, Slawin A M, Morris R E. Ionothermal materials synthesis using unstable deep-eutectic solvents as template-delivery agents. Angewandte Chemie International Edition, 2006, 118( 30): 5084– 5088

33 García-Argüelles S, Serrano M, Gutiérrez M C, Ferrer M L, Yuste L, Rojo F, del Monte F. Deep eutectic solvent-assisted synthesis of biodegradable polyesters with antibacterial properties. Langmuir, 2013, 29( 30): 9525– 9534

34 Zhang C, Ding Y, Zhang L, Wang X, Zhao Y, Zhang X, Yu G. A sustainable redox-flow battery with an aluminum-based, deep-eutectic-solvent anolyte. Angewandte Chemie International Edition, 2017, 56( 26): 7454– 7459

35 Wu J, Liang Q, Yu X, Lü Q F, Ma L, Qin X, Chen G, Li B. Deep eutectic solvents for boosting electrochemical energy storage and conversion: a review and perspective. Advanced Functional Materials, 2021, 31( 22): 2011102

36 Tadros T F. Fundamental principles of emulsion rheology and their applications. Colloids and Surfaces. A, Physicochemical and Engineering Aspects, 1994, 91 : 39– 55

37 Style R W, Boltyanskiy R, Allen B, Jensen K E, Foote H P, Wettlaufer J S, Dufresne E R. Stiffening solids with liquid inclusions. Nature Physics, 2015, 11( 1): 82– 87

38 Nan C W, Birringer R, Clarke D R, Gleiter H. Effective thermal conductivity of particulate composites with interfacial thermal resistance. Journal of Applied Physics, 1997, 81( 10): 6692– 6699