This study serves to combine two approaches into one single step, to achieve a significant improvement of the light-induced actuation capabilities. Graphene oxide (GO) is an inert material, from the electrical and thermal conductivity point of view, and is incompatible with the usually-used poly(dimethylsiloxane) (PDMS) matrix. During surface-modification by surface-initiated atom transfer radical polymerization, the GO was transformed into a conducting and compatible material with the PDMS showing enormous light-induced actuation capability. The GO surface-modification with poly(2-(trimethylsilyloxy)ethyl methacrylate) (PHEMATMS) chains was confirmed by transmission electron microscopy and thermogravimetric analysis, with an on-line monitoring of gasses using FTIR. The improved compatibility was elucidated using contact angle and dielectric properties measurements. The PHEMATMS shell was investigated using gel permeation chromatography and nuclear magnetic resonance. The improved electric conductivity was measured using the four-point probe method and by Raman spectroscopy. The very important mechanical properties were elucidated using dynamic mechanical analysis, and with the help of thermo-mechanic analysis for the light-induced actuation. The excellent actuation capabilities observed, with changes in the length of around 0.8% at 10% pre-strain, are very promising from the point of view of applications.

Centre for Advanced Materials Application Slovak Academy of Sciences Dubravska cesta 9 845 45 Bratislava Slovakia

Centre of Polymer Systems University Institute Tomas Bata University in Zlin Trida T Bati 5678 760 01 Zlin Czech Republic

Polymer Institute Slovak Academy of Sciences Dubravska cesta 9 845 41 Bratislava Slovakia

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Yetisen A.K., Martinez-Hurtado J.L., Uenal B., Khademhosseini A., Butt H. Wearables in medicine. Adv. Mater. 2018;30:1706910. doi: 10.1002/adma.201706910. PubMed DOI PMC

Bisoyi H.K., Urbas A.M., Li Q. Soft materials driven by photothermal effect and their applications. Adv. Opt. Mater. 2018;6:21. doi: 10.1002/adom.201800458. DOI

He K., Wen Q.K., Wang C.W., Wang B.X., Yu S.S., Hao C.C., Chen K.Z. A facile synthesis of hierarchical flower-like TiO2 wrapped with MoS2 sheets nanostructure for enhanced electrorheological activity. Chem. Eng. J. 2018;349:416–427. doi: 10.1016/j.cej.2018.05.102. DOI

Stejskal J., Bober P., Trchova M., Horsky J., Walterova Z., Filippov S.K., Plachy T., Mrlik M. Oxidation of pyrrole with p-benzoquinone to semiconducting products and their application in electrorheology. New J. Chem. 2018;42:10167–10176. doi: 10.1039/C8NJ01283K. DOI

Hu T., Xuan S.H., Ding L., Gong X.L. Stretchable and magneto-sensitive strain sensor based on silver nanowire-polyurethane sponge enhanced magnetorheological elastomer. Mater. Des. 2018;156:528–537. doi: 10.1016/j.matdes.2018.07.024. DOI

Cvek M., Mrlik M., Ilcikova M., Mosnacek J., Munster L., Pavlinek V. Synthesis of silicone elastomers containing silyl-based polymer grafted carbonyl iron particles: An efficient way to improve magnetorheological, damping, and sensing performances. Macromolecules. 2017;50:2189–2200. doi: 10.1021/acs.macromol.6b02041. DOI

Zhang W.Z., Wang L.F., Sun K., Luo T., Yu Z.Z., Pan K. Graphene-based janus film with improved sensitive response capacity for smart actuators. Sens. Actuators B Chem. 2018;268:421–429. doi: 10.1016/j.snb.2018.04.104. DOI

Wang T.P., Li M.T., Zhang H., Sun Y.Y., Dong B. A multi- responsive bidirectional bending actuator based on polypyrrole and agar nanocomposites. J. Mater. Chem. C. 2018;6:6416–6422. doi: 10.1039/C8TC00747K. DOI

Zahoranova A., Mrlik M., Tomanova K., Kronek J., Luxenhofer R. Aba and bab triblock copolymers based on 2-methyl-2-oxazoline and 2-n-propyl-2-oxazoline: Synthesis and thermoresponsive behavior in water. Macromol. Chem. Phys. 2017;218:12. doi: 10.1002/macp.201700031. DOI

Shah A., Malik M.S., Khan G.S., Nosheen E., Iftikhar F.J., Khan F.A., Shukla S.S., Akhter M.S., Kraatz H.B., Aminabhavi T.M. Stimuli-responsive peptide-based biomaterials as drug delivery systems. Chem. Eng. J. 2018;353:559–583. doi: 10.1016/j.cej.2018.07.126. DOI

Li M., Wang Y., Chen A.P., Naidu A., Napier B.S., Li W.Y., Rodriguez C.L., Crooker S.A., Omenetto F.G. Flexible magnetic composites for light-controlled actuation and interfaces. Proc. Natl. Acad. Sci. USA. 2018;115:8119–8124. doi: 10.1073/pnas.1805832115. PubMed DOI PMC

Toshchevikov V., Petrova T., Saphiannikova M. Kinetics of ordering and deformation in photosensitive azobenzene lc networks. Polymers. 2018;10:20. doi: 10.3390/polym10050531. PubMed DOI PMC

Ilcikova M., Mrlik M., Sedlacek T., Slouf M., Zhigunov A., Koynov K., Mosnacek J. Synthesis of photoactuating acrylic thermoplastic elastomers containing diblock copolymer-grafted carbon nanotubes. ACS Macro Lett. 2014;3:999–1003. doi: 10.1021/mz500444m. PubMed DOI

Hu Y., Wu G., Lan T., Zhao J.J., Liu Y., Chen W. A graphene-based bimorph structure for design of high performance photoactuators. Adv. Mater. 2015;27:7867–7873. doi: 10.1002/adma.201502777. PubMed DOI

Yang Y.K., Zhan W.J., Peng R.G., He C.G., Pang X.C., Shi D., Jiang T., Lin Z.Q. Graphene-enabled superior and tunable photomechanical actuation in liquid crystalline elastomer nanocomposites. Adv. Mater. 2015;27:6376–6381. doi: 10.1002/adma.201503680. PubMed DOI

Pennacchio F.A., Fedele C., De Martino S., Cavalli S., Vecchione R., Netti P.A. Three-dimensional microstructured azobenzene-containing gelatin as a photoactuable cell confining system. Acs Appl. Mater. Interfaces. 2018;10:91–97. doi: 10.1021/acsami.7b13176. PubMed DOI

Li C., Yun J.H., Kim H., Cho M. Light propagation and photoactuation in densely cross-linked azobenzene-functionalized liquid-crystalline polymers: Contribution of host and concerted isomerism. Macromolecules. 2016;49:6012–6020. doi: 10.1021/acs.macromol.6b01002. DOI

Osicka J., Ilcikova M., Mrlik M., Minarik A., Pavlinek V., Mosnacek J. The impact of polymer grafting from a graphene oxide surface on its compatibility with a pdms matrix and the light-induced actuation of the composites. Polymers. 2017;9:14. doi: 10.3390/polym9070264. PubMed DOI PMC

Ilcikova M., Mrlik M., Sedlacek T., Doroshenko M., Koynov K., Danko M., Mosnacek J. Tailoring of viscoelastic properties and light-induced actuation performance of triblock copolymer composites through surface modification of carbon nanotubes. Polymer. 2015;72:368–377. doi: 10.1016/j.polymer.2015.03.060. DOI

Loomis J., King B., Burkhead T., Xu P., Bessler N., Terentjev E., Panchapakesan B. Graphene-nanoplatelet-based photomechanical actuators. Nanotechnology. 2012;23:10. doi: 10.1088/0957-4484/23/4/045501. PubMed DOI

Koerner H., Price G., Pearce N.A., Alexander M., Vaia R.A. Remotely actuated polymer nanocomposites—Stress-recovery of carbon-nanotube-filled thermoplastic elastomers. Nat. Mater. 2004;3:115–120. doi: 10.1038/nmat1059. PubMed DOI

Afzal A., Kausar A., Siddiq M. Review highlighting physical prospects of styrenic polymer and styrenic block copolymer reinforced with carbon nanotube. Polym. Plast. Technol. Eng. 2017;56:573–593. doi: 10.1080/03602559.2016.1233276. DOI

Ilcikova M., Mrlik M., Sedlacek T., Chorvat D., Krupa I., Slouf M., Koynov K., Mosnacek J. Viscoelastic and photo-actuation studies of composites based on polystyrene-grafted carbon nanotubes and styrene-b-isoprene-b-styrene block copolymer. Polymer. 2014;55:211–218. doi: 10.1016/j.polymer.2013.11.031. DOI

Feng Y.Y., Qin M.M., Guo H.Q., Yoshino K., Feng W. Infrared-actuated recovery of polyurethane filled by reduced graphene oxide/carbon nanotube hybrids with high energy density. Acs Appl. Mater. Interfaces. 2013;5:10882–10888. doi: 10.1021/am403071k. PubMed DOI

Czanikova K., Torras N., Esteve J., Krupa I., Kasak P., Pavlova E., Racko D., Chodak I., Omastova M. Nanocomposite photoactuators based on an ethylene vinyl acetate copolymer filled with carbon nanotubes. Sens. Actuators B. 2013;186:701–710. doi: 10.1016/j.snb.2013.06.054. DOI

Mrlik M., Ilcikova M., Sedlacik M., Mosnacek J., Peer P., Filip P. Cholesteryl-coated carbonyl iron particles with improved anti-corrosion stability and their viscoelastic behaviour under magnetic field. Colloid Polym. Sci. 2014;292:2137–2143. doi: 10.1007/s00396-014-3245-5. DOI

Osicka J., Mrlik M., Ilcikova M., Hanulikova B., Urbanek P., Sedlacik M., Mosnacek J. Reversible actuation ability upon light stimulation of the smart systems with controllably grafted graphene oxide with poly (glycidyl methacrylate) and pdms elastomer: Effect of compatibility and graphene oxide reduction on the photo-actuation performance. Polymers. 2018;10:832. doi: 10.3390/polym10080832. PubMed DOI PMC

Mrlik M., Cvek M., Osicka J., Moucka R., Sedlacik M., Pavlinek V. Surface-initiated atom transfer radical polymerization from graphene oxide: A way towards fine tuning of electric conductivity and electro-responsive capabilities. Mater. Lett. 2018;211:138–141. doi: 10.1016/j.matlet.2017.09.107. DOI

Mrlik M., Ilcikova M., Plachy T., Moucka R., Pavlinek V., Mosnacek J. Tunable electrorheological performance of silicone oil suspensions based on controllably reduced graphene oxide by surface initiated atom transfer radical polymerization of poly(glycidyl methacrylate) J. Ind. Eng. Chem. 2018;57:104–112. doi: 10.1016/j.jiec.2017.08.013. DOI

Yoon J.T., Lee S.C., Jeong Y.G. Effects of grafted chain length on mechanical and electrical properties of nanocomposites containing polylactide-grafted carbon nanotubes. Compos. Sci. Technol. 2010;70:776–782. doi: 10.1016/j.compscitech.2010.01.011. DOI

Ilcikova M., Mrlik M., Spitalsky Z., Micusik M., Csomorova K., Sasinkova V., Kleinova A., Mosnacek J. A tertiary amine in two competitive processes: Reduction of graphene oxide vs. Catalysis of atom transfer radical polymerization. Rsc Adv. 2015;5:3370–3376. doi: 10.1039/C4RA12915F. DOI

Ma C.X., Le X.X., Tang X.L., He J., Xiao P., Zheng J., Xiao H., Lu W., Zhang J.W., Huang Y.J., et al. A multiresponsive anisotropic hydrogel with macroscopic 3d complex deformations. Adv. Funct. Mater. 2016;26:8670–8676. doi: 10.1002/adfm.201603448. DOI

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