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Asymmetric Janus Adhesive Tape Prepared by Interfacial Wan et al. NPG Asia Materials (2019) 11:49 https://doi.org/10.1038/s41427-019-0150-x NPG Asia Materials ARTICLE Open Access Asymmetric Janus adhesive tape prepared by interfacial hydrosilylation for wet/dry amphibious adhesion Xizi Wan1,2,ZhenGu1,3,4, Feilong Zhang2,DezhaoHao1,2,XiLiu1,2,BingDai1,2, Yongyang Song1,2 and Shutao Wang1,2,4 Abstract Janus films with asymmetric properties on opposite sides have been widely used to facilitate energy storage, ion transport, nanofiltration, and responsive bending. However, studies on Janus films rarely involve controlling surface adhesion, either dry or wet adhesion. Herein, we report Janus adhesive tape with an asymmetrically crosslinked polydimethylsiloxane (PDMS) network prepared through an interfacial hydrosilylation strategy, realizing wet/dry amphibious adhesion on various solid surfaces. The lightly crosslinked side of the Janus adhesive tape acts as an adhesive layer with high adhesion, and the highly crosslinked side functions as a supporting layer with high mechanical strength. This Janus adhesive tape with good adhesion and mechanical properties can be dyed different colors and can act as an underwater adhesive and a skin adhesive for wearable electronic devices. This study provides a promising design model for next-generation adhesive materials and related applications. Introduction fi 1234567890():,; 1234567890():,; 1234567890():,; 1234567890():,; studies on Janus lms rarely involve controlling surface Janus films with asymmetric features on opposite sides adhesion, either dry or wet adhesion. have been emerging as important functional materials that Many unique adhesion phenomena in nature, such as – strongly affect various applications in energy storage1, ion dry adhesion of geckos16 19 and wet adhesion of mus- – – transport2,3,nanofiltration4, and responsive bending5 7. sels20 23, barnacles24, and octopi25, have inspired the Many unique methods have been developed to prepare a rational design of functional adhesive materials. Gecko- series of functional Janus films with asymmetric properties inspired dry adhesion26 and octopus-inspired wet such as wettability, surface charge, and morphology8,9. For adhesion25,27 are often based on elaborate replicating example, hydrophilic–hydrophobic Janus films were fab- templates with unique structures. Mussel- and barnacle- ricated by electrospinning as materials for excess biofluid inspired wet adhesion is based on molecular design, such removal10 or as battery separators1. Electrostatic hetero- as graft28 or block29,30 copolymerization. By synergistically structure Janus films were fabricated by spin-coating and combining the salient elements of both gecko and mussel microphase separation for ion rectification3,11,12. Hydro- adhesives, PDMS micro-/nanopillar arrays coated with a gel-elastomer/organogel Janus films were fabricated by thin layer of synthetic catechol-based polymers have been interfacial polymerization for mechanical robustness, fabricated to achieve adhesion in both dry and wet antifouling13,14, or responsive bonding5,15. However, environments31,32. However, the elaborate preconstruc- tion of surface micro-/nanostructures or the introduction of catechol groups into adhesive polymers greatly restricts Correspondence: Shutao Wang ([email protected]) 1CAS Key Laboratory of Bioinspired Materials and Interfacial Science, CAS the practical applications of these functional adhesives. It Center for Excellence in Nanoscience, Technical Institute of Physics and is still a great challenge to develop wet/dry amphibious Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China adhesive materials without laborious replicating structure 2University of Chinese Academy of Sciences, Beijing 100049, P. R. China Full list of author information is available at the end of the article. preparation and molecular design. These authors contributed equally: Xizi Wan, Zhen Gu © The Author(s) 2019 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a linktotheCreativeCommons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. Wan et al. NPG Asia Materials (2019) 11:49 Page 2 of 9 a b Adhesive layer: low crosslinked PDMS 518 nm 2.5 2.0 1.5 Interfacial hydrosilylation 1.0 0.5 Absorbance (a.u.) Supporting layer: highly crosslinked PDMS 0 Wavelength (nm) Hydrosilylation reaction: Silicon base Curing agent Crosslinking point c d e 300 In air 1.0 /cm) Under water 250 N 0.8 200 force ( force 0.6 Janus tape 150 0.4 Stress (kPa) 100 adhesion 0.2 50 50:1 10 mm Crack 20:1 20:1 0 Peeling 0 Janus tape 50:1 01234 Strain Fig. 1 Design and characterization of asymmetric Janus adhesive tape. a Schematic of Janus adhesive tape with an asymmetrically crosslinked network prepared through an interfacial hydrosilylation strategy. The lightly crosslinked PDMS acts as an adhesive layer with high adhesion, and the highly crosslinked PDMS acts as a supporting layer with high mechanical strength. b Visible spectra at the interfacial transitional region of the Janus adhesive tape. The gradual increase in the absorption peak at 518 nm (probed by Oil Red) indicates the gradient diffusion of the curing agent across the interface. Note that the supporting layer (20:1) was kept transparent and that the adhesive layer (50:1) was dyed with Oil Red. c The mechanical and d adhesion properties of the Janus adhesive tape, with HCPDMS tape and LCPDMS tape used as controls. e The Janus PDMS tape shows apparent asymmetric adhesion performance of its two sides and can withstand large deformations Herein, we present an interfacial hydrosilylation strat- Procedures egy to fabricate asymmetric Janus adhesive tape by curing Fabrication of Janus adhesive tape lightly crosslinked PDMS on partially cured highly Different ratios of the silicone base and curing agent crosslinked PDMS. The lightly crosslinked side exhibiting (Sylgard 184, Dow corning) were well mixed by a high adhesion force acts as an adhesive layer, and the mechanical agitator in a plastic cup for 5 min at 500 highly crosslinked side exhibiting high mechanical rounds per min. The mixture was vacuumed in a vacuum strength functions as a supporting layer (Fig. 1a). This pump for 30 min to remove air bubbles. Highly cross- asymmetric Janus adhesive tape simultaneously possesses linked PDMS (20:1) was cured at 80 °C for 15 min to make good wet/dry adhesion performance and good mechanical it partially cured. Then, the same amount of lightly properties and can adhere to different kinds of substrates. crosslinked PDMS precursor (50:1) (dyed with Oil Red) This study provides a new concept for designing next- was poured on top of the precured 20:1 PDMS, and the generation adhesive materials with wet/dry amphibious two components were subsequently cured at 80 °C for adhesion properties. 1.5 h to make them completely joined together through an interfacial hydrosilylation reaction. Experimental procedure Materials PDMS-based elastomer Sylgard 184 (Dow Corning, Mechanical property testing United States), which consists of silicone base and a The tensile test (stress, strain, and elongation at break) crosslinking agent. was performed with a dynamometer (M5-2; Mark-10 Wan et al. NPG Asia Materials (2019) 11:49 Page 3 of 9 Corporation). The stroke speed in the tensile test was The contact state test between the Janus adhesive tape and 100 mm/min. a glass substrate In the CLSM observation experiment, Janus adhesive ′ ′ ′ Adhesion force testing tape was labeled with 1,1 -dioctadecyl-3,3,3 ,3 -tetra- ≥ The adhesion test of the Janus adhesive tape was per- methylindocarbocyanine perchlorate (DiI) ( 98%; Alad- formed with a dynamometer (M5-2; Mark-10 Corpora- din) in red, and H2O was labeled with Rhodamine 110 ≥ tion). The precursor mixtures were wiped on a polymeric ( 98%; Aladdin) in green. The concentration of the fl support membrane (fluoroalkylsilane-modified poly- uorescent dyes is 10 nM. ethylene terephthalate film), and the samples for mea- Results and discussion surements were tailored to 10 mm wide, 1 mm thick, and 60 mm long. For the peeling adhesion force test, the As a widely used elastomer, PDMS often acts as a soft fl 33,34 peeling speed was 500 mm/min, and the maximum and sticky sealant in micro uidic and wearable elec- tronic devices35,36 at a low crosslinking degree and as a adhesion force was read while peeling off the rest of the 37,38 sample from the substrate. All the tests were repeated at hard and less sticky stamp for microscopic patterning least three times. at a high crosslinking degree. Its crosslinking degree can be regulated by changing the proportion of two pre- cursors, silicone base and curing agent. In our design, we Surface modification of substrates integrated LCPDMS (wsilicone base:wcuring agent = 50:1) and The silanization reactions were performed at a tempera- HCPDMS (w :w = 20:1) together ≈ silicone base curing agent ture of 80 °C under reduced pressure ( 0.2atm)for5h by through an interfacial hydrosilylation reaction39. Briefly, placing samples in a closed chamber. The silanes chosen to we first prepared a partially crosslinked PDMS layer by modify the substrates are (3-aminopropyl)trimethoxysilane, curing a 20:1 mixture of silicone base and curing agent at (CH3O)3Si(CH2)3NH2 (C3NH); ethyltrimethoxysilane, 80 °C for 15 min. Then, we wiped a layer of 50:1 silicone (CH3O)3SiCH2CH3 (C2); n-butyltrimethoxysilane, (CH3O)3 base and curing agent on the precured 20:1 PDMS layer Si(CH2)3CH3 (C4); n-octyltrimethoxysilane, (CH3O)3Si(CH2)7 and cured them together at 80 °C for 1.5 h.
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