Free Volume Effect Via Various Chemical Structured Monomers On
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polymers Article Free Volume Effect via Various Chemical Structured Monomers on Adhesion Property and Relative Permittivity in Acrylic Pressure Sensitive Adhesives Jung-Hun Lee 1,2, Ji-Soo Kim 2 , Hyun-Joong Kim 2,3,* , Kyujong Park 4, Jungwoo Moon 4, Jinyoung Lee 4 and Youngju Park 4 1 Carbon Composite Materials Research Center, Institute of Advanced Composite Materials, Korea Institute of Science and Technology, Jeonbuk 55324, Korea; [email protected] 2 Lab. of Adhesion and Bio-Composites, Program in Environmental Materials Science, Department of Agriculture, Forestry and Bioresources Seoul National University, Seoul 08826, Korea; [email protected] 3 Research Institute of Agriculture and Life Sciences, College of Agriculture and Life Sciences, Seoul National University, Seoul 08826, Korea 4 Samsung Display Co., Ltd., Yongin 17113, Korea; [email protected] (K.P.); [email protected] (J.M.); [email protected] (J.L.); [email protected] (Y.P.) * Correspondence: [email protected]; Tel.: +82-2-880-4783 Received: 12 October 2020; Accepted: 5 November 2020; Published: 10 November 2020 Abstract: Acrylic pressure-sensitive adhesives (PSAs) are used as fixatives between layers of a display. PSAs’ function is an important factor that determines the performance of the display. Of the various display types available, the touch screen panel (TSP) of smart devices is firmly related to the relative permittivity of the elementals. Therefore, adjusting the relative permittivity of the PSA is indispensable for driving the TSP. Accordingly, selected acrylic pre-polymers were polymerized and the pre-polymer was blended and cross-linked with monomers with different chemical structure to adjust the relative permittivity. The monomers were hexametyldisiloxane (HMDS), N-vinylcaprolactam (NVC), tert-butyl acrylate (TBA), and isooctadecyl acrylate (ISTA). The gel fraction and transmittance as a function of the monomers show a similar result to the pure acrylic PSA. However, the gel fraction value decreased to about 90% and the transmittance decreased to about 85%, due to the immiscibility between nonpolar HMDS and acrylic PSA. On the other hand, the adhesion properties were improved when NVC was added because of the polarity of the nitrogen group. In addition, the relative permittivity of the PSA decreased regardless of the monomer chosen. There was, however, a difference in the optimal content of each monomer, and NVC decreased from 4 phr content to about 3.4 in reducing relative permittivity. Through the above results, it was confirmed that NVC having a nitrogen group is most advantageous in lowering adhesion properties and relative permittivity, and necessitates further research based on the findings. Keywords: acrylic pressure-sensitive adhesive; monomer; adhesion performance; relative permittivity; free volume 1. Introduction Pressure-sensitive adhesives (PSAs) are widely used in various industrial fields, such as medical products, aircraft, space shuttles, electrical devices, optical products, and automobiles. In particular, the demand for functional PSAs is rapidly increasing in the display market [1]. Displays are composed of a plurality of layer types and PSAs play an important fixative role. The PSA can fix the base material by applying slight pressure and becomes easy to adjust, Polymers 2020, 12, 2633; doi:10.3390/polym12112633 www.mdpi.com/journal/polymers Polymers 2020, 12, 2633 2 of 14 Polymers 2020, 12, x FOR PEER REVIEW 2 of 14 basewhile material the processing by applying rate slight can be pressure increased and [2 ].becomes Recently, easy to imto proveadjust, the while technological the processing development rate can beof increased displays, br[2].oader Recently, properties to improve of the PSA the technolo functiongical are required development including of displays, transparency broaderhigh properties elongation, ofhigh the recovery,PSA function and heatare required dissipation including [3]. transparency high elongation, high recovery, and heat dissipationOptical [3]. clarity means a transmittance of 90% or more in the range of 400 to 800 nm and PSA satisfies thisOptical criteria definingclarity means the utility a transmittance of optical clear of adhesives90% or more (OCAs). in the PSA range includes of 400 rubber, to 800 acrylic, nm and silicone, PSA satisfiesand urethane, this criteria and acrylic defining PSA the is widelyutility of used optical in terms clear of adhesives their optical (OCAs). clarity. PSA Mo reover,includes the rubber, process acrylic,time can silicone, be significantly and urethane, reduced, and andacrylic UV crosslinkingPSA is widely is considerablyused in terms economical of their optical as a techni clarity.que. Moreover,As the transmittance the process of time PSA can is a verybe significantly important factorreduced, in dis andplay UV qua crosslinlity, a lokingw transmittance is considerably may economicallimit its application as a technique. in the displayAs the transmittance industry [4,5]. of PSA is a very important factor in display quality, a low Atransmittance touch screen may panel limit (TSP) its isapplication a major technology in the display for increasing industry [4,5]. input convenience and reducing productA touch weight screen by panel replacing (TSP) theis a keyboardmajor technology in the display for increasing of electronic input convenience devices. The and demand reducing for productTSP has weight soared by owing replacing to the the spread keyboard of smart in the phones display and of tabletelectronic PCs, devices. and it is The essential demand to improvefor TSP hastouch soared sensitivity. owing to A the capacitive spread touchof smart screen phones panel and is tablet composed PCs, and of a topit is andessential bottom to improve plate, on touch which sensitivity.a transparent A capacitive electrode touch (indium screen tin oxide,panel ITO)is composed is deposited of a andtop and each bottom layer isplate, fixed on using which PSAs a transparent(see Figure 1electrode). As part (indium of the capacitive tin oxide, method,ITO) is deposited a current flowand operateseach layer through is fixed ITO using on onePSAs side (see of Figurethe glass 1). orAs apart transparent of the capacitive film and amethod, touch operation a current is flow recognized operates by through sensing ITO a change on one in side capacitance of the glassthat occursor a transparent when a finger film orand a toucha touch pen operation touches theis recognized touch screen by surface. sensing a change in capacitance that occurs when a finger or a touch pen touches the touch screen surface. FigureFigure 1. 1. StructureStructure of of capacitance capacitance type type touch touch screen screen pa panelnel (TSP). (TSP). PSA, PSA, pressu pressure-sensitivere-sensitive adhesive; adhesive; ITO,ITO, indium indium tin tin oxide. oxide. TheThe relative relative permittivity isis aa measuremeasure of of the the degree degree of polarizationof polarizati ofon electric of electric charges charges inside inside when whenan electric an electric field isfield applied is applied to the to non-conductor the non-conduc surfacetor surface from from the outside. the outside. From From this pointthis point of vie ofw, view,the non-cond the non-conductoructor is called is called the dielectric the dielectric ("). The (ε relative). The relative permittivity permittivity ("γ, dielectric (ɛγ, dielectric constant) constant) refers to refersthe ratio to the of theratio permittivity of the permittivity of the material of the base material relative base to therelative permittivity to the permittivity in a vacuum. in I na vacuum. other wo rds,In otherthe relative words, permittivitythe relative ispermittivi determinedty is bydetermined the permittivity by the ofpermittivity a substance of (see a substance Figure2)[ (see6] andFigure can 2) be [6]expressed and can bybe expressed the following by the equation: following equation: "γ = "/"0 (1) ɛγ = ɛ/ɛ0 (1) Over the past decade, the performance of microelectronic integrated circuits (ICs) that make-up Over the past decade, the performance of microelectronic integrated circuits (ICs) that make-up electronic devices has been improved owing to an increase in transistor speed and a decrease in size. electronic devices has been improved owing to an increase in transistor speed and a decrease in size. ICs have become faster and more complex because smaller transistors run faster. However, these efforts ICs have become faster and more complex because smaller transistors run faster. However, these are causing a decrease in the speed of signal propagation. The signal delay can increase with the size efforts are causing a decrease in the speed of signal propagation. The signal delay can increase with of the electronic device, which can degrade the performance of the final product. In other words, the size of the electronic device, which can degrade the performance of the final product. In other continuous shrinkage increases the speed of the transistor, but decreases the interconnection between words, continuous shrinkage increases the speed of the transistor, but decreases the interconnection the transistors. A way to improve this is to use a non-conductor with a low dielectric constant [7]. between the transistors. A way to improve this is to use a non-conductor with a low dielectric Non-conductors with a relative permittivity of 4.2 or less are called low-k dielectrics [8]. In addition, constant [7]. Non-conductors with a relative permittivity of 4.2 or less are called low-k