Composition

Abstract

The present invention relates to compositions comprising polysiloxanes.

Description

[Technical Field]

[0001] The present invention relates to a composition containing at least a polysiloxane, and preferably to a composition for forming a protective layer, a method for producing a composition, a method for producing a layer, a layer, an electronic device, a method for using a sulfur-containing compound, and a method for using a composition as a protective layer. [Background technology]

[0002] U.S. Patent Application Publication No. 2010 / 0016488 discloses a method for producing organosiloxane polymers, comprising hydrolyzing trialkoxysilane and tetraalkoxysilane monomers in a hydrolysis step, and polymerizing the hydrolyzed monomers in a polymerization step by subjecting them to conditions that induce polymerization to form organosiloxane polymers, wherein the hydrolysis step is carried out in a reaction medium containing an organic compound having a hydroxy group. It also discloses the use of compositions produced by this process for optical coatings and electrical coatings. [Prior art documents] [Patent documents]

[0003] [Patent Document 1] U.S. Patent Application Publication No. 2010 / 0016488 Summary of the Invention

[0004] However, the present inventors have newly discovered that one or more important problems still remain that require improvement, as listed below: To obtain a polysiloxane-containing composition, preferably a composition for forming a protective layer, that exhibits an improved dielectric constant, such as that of a glass substrate of an electronic device, and preferably has the lowest haze characteristics; to obtain a layer or cured composition that exhibits an improved dielectric constant, such as that of a glass substrate of an electronic device, and preferably has the lowest haze characteristics; to obtain a polysiloxane-containing composition, preferably a composition for forming a protective layer, that allows a sufficient amount of thiol to be well dispersed in the composition; to obtain a layer or cured composition in which a sufficient amount of thiol is well dispersed in the layer or cured composition; to obtain a polysiloxane-containing composition, preferably a composition for forming a protective layer, that can be formed into a layer or cured composition with mild or lower temperature treatment, and that can form a smooth coating of the polysiloxane-containing composition on any substrate, i.e., PET, CPI, COP, or polarizer.

[0005] The inventors aimed to solve one or more of the above problems.

[0006] Thus, as claimed, a novel composition, preferably a composition for forming a protective layer, has been found, comprising, consisting essentially of, or consisting of at least: i) polysiloxane; and ii) A sulfur-containing compound represented by the following chemical formula (I), which is a dielectric constant improver preferably used in polysiloxane-containing compositions: XS-Y (I) where: X is a hydrogen atom or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, preferably a hydrogen atom; Y is one or more groups R a an unsubstituted or substituted alkyl group having 1 to 12 carbon atoms, an unsubstituted or substituted cyclic alkyl group having 3 to 22 carbon atoms, an unsubstituted or substituted aryl group having 3 to 22 carbon atoms, or an unsubstituted or substituted alkyl-aryl group having 4 to 22 carbon atoms, each of which may be substituted by R, wherein one or more non-adjacent CH groups in the alkyl group, cyclic alkyl group, aryl group, and / or alkyl-aryl group are each independently selected from the group consisting of Ra C=CR a , C≡C, Si(R a )2, Ge(R a )2, Sn(R a )2, C=O, C=S, C=Se, C=NR a , P(=O)(R a ), SO, CSR a , SO2, NR a , OS, or CONR a wherein one or more non-adjacent CH groups of said aryl group and / or said alkyl-aryl group may be substituted, independently of each other, by SiR a , GeR a , SnR a , CSR a , SO2, NR a , O, S, SO, or CONR a and one or more H atoms may be replaced by D, F, Cl, Br, I, CN, or NO2; R a are each the same or different and are H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, wherein an H atom may be replaced by D, F, Cl, Br, or I; a may also together form a monocyclic or polycyclic aliphatic, aromatic or heteroaromatic ring system.

[0007] In another aspect, the present invention relates to a method for producing a composition according to any one of the preceding claims, comprising at least the following steps: (I x ) polysiloxane; and A step of mixing a sulfur-containing compound represented by the following chemical formula (I): XS-Y (I)

[0008] In another aspect, the present invention relates to a composition obtained or obtainable by the method of the present invention.

[0009] In another aspect, the present invention relates to a method for producing a layer comprising, consisting essentially of, or consisting of at least the following steps: (I Y ) providing a composition of the present invention, preferably on a substrate, a support layer, or a layer of an electronic device; (II Y 2.) Heating the provided composition to form a layer, preferably removing any solvent in the composition.

[0010] In another aspect, the present invention relates to a layer obtained from the composition of the present invention by curing or obtained by the method of the present invention.

[0011] In another aspect, the present invention relates to a layer comprising, consisting essentially of, or consisting of at least: i) polymers made from polysiloxanes; and ii) A sulfur-containing compound represented by the following chemical formula (I): XS-Y (I)

[0012] In another aspect, the present invention relates to an electronic device comprising at least a layer of the present invention.

[0013] In another aspect, the present invention further relates to the use of the sulfur-containing compounds of formula (I) as dielectric constant enhancers in polysiloxane-containing compositions.

[0014] In another aspect, the present invention further relates to a method of using the composition of the present invention as a protective layer-forming composition for an electronic device.

[0015] Further advantages of the present invention will become apparent from the detailed description that follows. DETAILED DESCRIPTION OF THE INVENTION

[0016] Definition of Terms In this specification, unless otherwise specified, the symbols, units, abbreviations and terms have the following meanings: In this specification, unless otherwise specified, the singular includes the plural, and "one" and "the" mean "at least one." In this specification, unless otherwise specified, a conceptual element can be expressed by a plurality of species, and when an amount (e.g., mass % or mole %) is described, the amount means the sum of the plurality of species. "And / or" includes all combinations of elements and also includes the use of a single element. In this specification, when a numerical range is indicated using "to" or "-", it includes both endpoints and the units are the same. For example, 5 to 25 mol % means 5 mol % or more and 25 mol % or less. As used herein, "hydrocarbon" refers to a group containing carbon and hydrogen, and optionally oxygen or nitrogen. "Hydrocarbyl group" refers to a monovalent, divalent, or higher-valent hydrocarbon. As used herein, "aliphatic hydrocarbon" refers to a linear, branched, or cyclic aliphatic hydrocarbon, and "aliphatic hydrocarbon group" refers to a monovalent, divalent, or higher-valent aliphatic hydrocarbon. "Aromatic hydrocarbon" refers to a hydrocarbon containing an aromatic ring, which may optionally contain an aliphatic hydrocarbon group as a substituent, and which may be fused with a cycloaliphatic ring. "Aromatic hydrocarbon group" refers to a monovalent, divalent, or higher-valent aromatic hydrocarbon. Furthermore, "aromatic ring" refers to a hydrocarbon containing a conjugated unsaturated ring structure, and cycloaliphatic refers to a hydrocarbon having a ring structure but not a conjugated unsaturated ring structure. As used herein, "alkyl" refers to a group obtained by removing any one hydrogen from a linear or branched saturated hydrocarbon, and includes linear alkyl and branched alkyl. "cycloalkyl" refers to a group obtained by removing one hydrogen from a saturated hydrocarbon containing a cyclic structure, and optionally includes a linear or branched alkyl in the cyclic structure as a side chain. As used herein, "aryl" refers to a group obtained by removing any one hydrogen from an aromatic hydrocarbon. "Alkylene" refers to a group obtained by removing any two hydrogens from a linear or branched saturated hydrocarbon. "Arylene" refers to a hydrocarbon group obtained by removing any two hydrogens from an aromatic hydrocarbon. In the present specification, when a polymer has multiple types of repeating units, these repeating units are copolymerized. The copolymerization may be alternating copolymerization, random copolymerization, block copolymerization, graft copolymerization, or a mixture thereof. In this specification, the unit of temperature is Celsius. For example, 20°C means 20 degrees Celsius.

[0017] Detailed Description of the Invention According to the present invention, in one embodiment, the composition, preferably the protective layer-forming composition, comprises, consists essentially of, or consists of at least: i) polysiloxane; and ii) A sulfur-containing compound represented by the following chemical formula (I), which is a dielectric constant improver preferably used in polysiloxane-containing compositions: XS-Y (I) where: X is a hydrogen atom or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, preferably a hydrogen atom; Y is one or more groups R a an unsubstituted or substituted alkyl group having 1 to 12 carbon atoms, an unsubstituted or substituted cyclic alkyl group having 3 to 22 carbon atoms, an unsubstituted or substituted aryl group having 3 to 22 carbon atoms, or an unsubstituted or substituted alkyl-aryl group having 4 to 22 carbon atoms, each of which may be substituted by R, wherein one or more non-adjacent CH groups in the alkyl group, cyclic alkyl group, aryl group, and / or alkyl-aryl group are each independently selected from the group consisting of R a C=CR a , C≡C, Si(R a )2, Ge(R a )2, Sn(R a )2, C=O, C=S, C=Se, C=NR a , P(=O)(R a ), SO, CSR a , SO2, NR a , OS, or CONR awherein one or more non-adjacent CH groups of said aryl group and / or said alkyl-aryl group may be substituted, independently of each other, by SiR a , GeR a , SnR a , CSR a , SO2, NR a , O, S, SO, or CONR a and one or more H atoms may be replaced by D, F, Cl, Br, I, CN, or NO2; R a are each the same or different and are H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, wherein an H atom may be replaced by D, F, Cl, Br, or I; a may also together form a monocyclic or polycyclic aliphatic, aromatic or heteroaromatic ring system.

[0018] composition In a preferred embodiment of the present invention, the dielectric constant (ε r ) is 3.5 to 7, more preferably 4 to 6.5, and even more preferably 4.5 to 6. Preferably, the dielectric constant (ε r ) is measured by the following method from the viewpoint of realizing a high dielectric constant of the composition and the resulting layer. According to the present invention, the dielectric constant (ε r ) is measured by the following method. 1) Sample preparation and dielectric constant measurement coating the composition onto a conductive wafer selected from Al, Si, or Mo; A sample is formed by placing an electrode on a composition coated with Ag or Al by sputtering or evaporation; The dielectric constant of the sample is measured by attaching a pin probe to each of the surface of the conductive wafer and the top electrode on the coated composition. 2) Measurement conditions: The dielectric constant was measured using an LCR meter (E4980A, Agilent, Korea / 6440B, Dongyang Technica, Japan) at room temperature. A specific frequency range (50-1 MHz) was applied, and the capacitance displayed on the LCR meter was read. The dielectric constant was calculated using the following formula: C = K A / d (C = capacitance, K = dielectric constant, A = effective electrode area, d = distance between electrodes).

[0019] ii) Sulfur-containing compounds According to the present invention, a compound of formula (I) or formula (I z Any publicly available sulfur-containing compound represented by chemical formula (I) can be used. Preferably, any publicly available sulfur-containing compound represented by chemical formula (I) is used. Preferably, the molecular weight (Mw) of the sulfur-containing compound is 600 or less, preferably 500 or less, more preferably 400 or less, even more preferably 80 to 400, and most preferably 100 to 210. When using a sulfur-containing compound represented by chemical formula (I), the molecular weight (Mw) of the sulfur-containing compound is preferably 400 or less, more preferably 80 to 400, and even more preferably 100 to 210. It is believed that the above molecular weight can improve the dispersibility of the sulfur-containing compound in the polysiloxane and achieve good compatibility with the polysiloxane, which can also lead to a lower haze value of the composition and the layer obtained from the composition.

[0020] In a preferred embodiment of the present invention, the total amount of sulfur-containing compounds based on the total amount of polysilazanes in the composition is 0.01 to 40 mass %, preferably 0.1 to 20 mass %, and more preferably 0.5 to 5.0 mass %. It is believed that the above total amount of the sulfur-containing compound based on the total amount of polysiloxane in the composition can achieve further improved dispersibility of the sulfur-containing compound in the composition and the resulting layer, can lower the haze value of the layer obtained from the composition, and can make the dielectric constant of the composition and the resulting layer optimally high, like a glass substrate.

[0021] According to the present invention, preferably, the sulfur-containing compound of formula (I) is represented by the following chemical formula (IIa) or (IIb): X a SY a -Z a (IIa) X a represents a hydrogen atom or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, and is preferably a hydrogen atom; Y a is one or more groups R a an unsubstituted or substituted linear alkylene group having 1 to 12 carbon atoms, or an unsubstituted or substituted branched alkylene group having 3 to 12 carbon atoms, optionally substituted by R, wherein one or more non-adjacent CH groups of the alkyl group, cyclic alkyl group, aryl group and / or alkyl-aryl group are each independently selected from the group consisting of R a C=CR a , C≡C, Si(R a )2, Ge(R a )2, Sn(R a )2, C=O, C=S, C=Se, C=NR a , P(=O)(R a ), SO, CSH, SO2, NR a , OS, or CONR a and one or more H atoms may be replaced by D, F, Cl, Br, I, CN, or NO2; R a are each the same or different and are H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, wherein an H atom may be replaced by D, F, Cl, Br, or I; a may also together form a monocyclic or polycyclic aliphatic, aromatic or heteroaromatic ring system; Z a teeth, * -CR a1 R a2 R a3 where R a1 , R a2and R a3 are each independently a hydrogen atom or a halogen atom selected from Cl, Br, F, or I, and R a1 , R a2 and R a3 At least one of R is a halogen atom, and preferably R a1 , R a2 and R a3 At least two of R are halogen atoms, and more preferably R a1 , R a2 and R a3 are all halogen atoms, preferably the halogen atoms are Cl or F, more preferably the halogen atom is F. X b SY b (IIb) X b represents a hydrogen atom or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, and is preferably a hydrogen atom; Y b is one or more groups R a an unsubstituted or substituted cyclic alkyl group having 3 to 22 carbon atoms, an unsubstituted or substituted aryl group having 3 to 22 carbon atoms, or an unsubstituted or substituted alkyl-aryl group having 4 to 22 carbon atoms, wherein one or more non-adjacent CH groups in the alkyl group, cyclic alkyl group, aryl group, and / or alkyl-aryl group are each independently selected from the group consisting of R a C=CR a , C≡C, Si(R a )2, Ge(R a )2, Sn(R a )2, C=O, C=S, C=Se, C=NR a , P(=O)(R a ), SO, CSR a , SO2, NR a , OS, or CONR a wherein one or more non-adjacent CH groups of said aryl group and / or said alkyl-aryl group may be substituted, independently of each other, by SiR a , GeR a , SnR a , CSR a , SO2, NR a, O, S, SO, or CONR a and one or more H atoms may be replaced by D, F, Cl, Br, I, CN, or NO2; R a are each the same or different and are H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, wherein an H atom may be replaced by D, F, Cl, Br, or I; a may also together form a monocyclic or polycyclic aliphatic, aromatic or heteroaromatic ring system.

[0022] For example, 1,2-mercaptobenzimidazole, 2-mercaptoimidazole, benzene-1,2-dithiol, cyclohexanethiol, 2,2,2-trifluoroethanethiol, 1-phenethyl-1H-benzo[d]imidazole-2-thiol, PEMP (pentaerythritol tetrakis(3-mercaptopropronate)), and TMMP (trimethylolpropane tris(3-mercaptopropionate)) can be preferably used.

[0023] In another aspect, the present invention also relates to a composition, preferably a protective layer-forming composition, comprising, consisting essentially of, or consisting of at least: i) polysiloxane; and ii) a compound of the following chemical formula (I z ), which is a dielectric constant improver preferably used in polysiloxane-containing compositions: (X z SY z ) n -A z (I z ) X zrepresents a hydrogen atom or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, and is preferably a hydrogen atom; Y z is R z -C=O; R z is an unsubstituted or substituted linear alkylene group having 1 to 5 carbon atoms, or an unsubstituted or substituted branched alkylene group having 3 to 5 carbon atoms, wherein one or more non-adjacent CH groups of the alkylene group are each independently selected from R a C=CR a , C≡C, Si(R a )2, Ge(R a )2, Sn(R a )2, C=O, C=S, C=Se, C=NR a , P(=O)(R a ), SO, CSH, SO2, NR a , OS, or CONR a and one or more H atoms may be replaced by D, F, Cl, Br, I, CN, or NO2; A z is a polyol group selected from pentaerythritol, trimethylolpropane, glycerin, ethylene glycol, and propylene, wherein the oxygen atom of each hydroxy group of the polyol group is represented by —COO—, and Y z directly bonded to the carbon atom of C=O, or z is a nitrogen-containing heterocyclic compound selected from a 3-membered ring containing 1 to 3 nitrogen atoms, a 4-membered ring containing 1 to 4 nitrogen atoms, a 5-membered ring containing 1 to 4 nitrogen atoms, a 6-membered ring containing 1 to 4 nitrogen atoms, and a 7-membered ring containing 1 to 4 nitrogen atoms as ring-constituting atoms, and is preferably an isocyanurate; n is an integer from 1 to 4, and A z Number of functional groups or A z is the same as the molecular charge number of

[0024] Chemical formula (I zAs the sulfur-containing compound represented by the formula (I), pentaerythritol tetrakis(3-mercaptobutanate), tris(3-mercaptobutyloxyethyl)isocyanurate, trimethylolpropane tris(3-mercaptobutyrate), and pentaerythritol tetra(3-mercaptopropionate) can be preferably used.

[0025] i) Polysiloxane According to the present invention, any publicly available polysiloxane can be used. Preferably, the polysiloxane has the chemical formula (I): a ) repeating units. [ka] where: R Ia is hydrogen, C 1-30 (Preferably C 1-10 ) linear, C 3-30 (Preferably C 3-10 ) a branched or cyclic saturated or unsaturated aliphatic hydrocarbon group or aromatic hydrocarbon group, wherein the aliphatic hydrocarbon group and the aromatic hydrocarbon group are each unsubstituted or substituted with fluorine, hydroxy, or alkoxy; In the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is not substituted or one or more methylenes are substituted with oxy, imino or carbonyl, provided that R Ia is neither hydroxy nor alkoxy. Here, the above methylene also includes a terminal methyl. Furthermore, the above-mentioned "substituted with fluorine, hydroxy or alkoxy" means that a hydrogen atom directly bonded to a carbon atom of an aliphatic hydrocarbon group or an aromatic hydrocarbon group is substituted with fluorine, hydroxy or alkoxy. In this specification, this also applies to other similar descriptions.

[0026] In a more preferred embodiment of the present invention,a ) in the repeating unit represented by R Ia Examples of R include (i) alkyls such as methyl, ethyl, propyl, butyl, pentyl, hexyl, heptyl, octyl, and decyl; (ii) aryls such as phenyl, tolyl, and benzyl; (iii) fluoroalkyls such as trifluoromethyl, 2,2,2-trifluoroethyl, and 3,3,3-trifluoropropyl; (iv) fluoroaryls; (v) cycloalkyls such as cyclohexyl; (vi) nitrogen-containing groups having an amino or imide structure such as isocyanate or amino; and (vii) oxygen-containing groups having an epoxy structure such as glycidyl, or an acryloyl or methacryloyl structure. Preferred are methyl, ethyl, propyl, butyl, pentyl, hexyl, and phenyl. Ia Compounds in which R is methyl are preferred because the raw materials are easily available, the hardness of the film after curing is high, and the chemical resistance is high. Ia Compounds in which is phenyl are preferred because they increase the solubility of the polysiloxane in a solvent and make the cured film less likely to crack.

[0027] In a preferred embodiment of the present invention, the polysiloxane used in the present invention is represented by the formula (I b ) may further comprise a repeating unit represented by: [ka] where: R Ib is a group obtained by removing multiple hydrogens from a nitrogen- and / or oxygen-containing alicyclic hydrocarbon compound having an amino, imino, and / or carbonyl group. Formula (I b ) in R Ib is preferably a group obtained by removing multiple hydrogen atoms, preferably two or three hydrogen atoms, from a nitrogen-containing aliphatic hydrocarbon ring having an imino and / or carbonyl group, more preferably a five- or six-membered ring containing nitrogen as a ring member. For example, it is a group obtained by removing two or three hydrogen atoms from piperidine, pyrrolidine, or isocyanurate. Ib connects Si atoms contained in multiple repeating units together.

[0028] In a preferred embodiment of the present invention, the polysiloxane used in the present invention is represented by the formula (I c ) may further comprise a repeating unit represented by: [ka] Formula (I b ) and (I c If the mixing ratio of the repeating unit represented by the formula (I) is high, the compatibility with solvents and additives will decrease, film stress will increase, and cracks may easily occur. Therefore, the mixing ratio is preferably 40 mol % or less, and more preferably 20 mol % or less, based on the total number of repeating units of the polysiloxane.

[0029] According to the present invention, in some embodiments, the polysiloxane used in the present invention is represented by the formula (I d ) may further comprise a repeating unit represented by: [ka] where: R Id are each independently hydrogen, C 1-30 (Preferably C 1-10 ) linear, C 3-30 (Preferably C 3-10 ) a branched or cyclic saturated or unsaturated aliphatic hydrocarbon group or aromatic hydrocarbon group, the aliphatic hydrocarbon group and the aromatic hydrocarbon group are each unsubstituted or substituted with fluorine, hydroxy, or alkoxy; In the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is unsubstituted or substituted with oxy, imido or carbonyl. Formula (I d ) in the repeating unit represented by R IdExamples of R include (i) alkyls such as methyl, ethyl, propyl, butyl, pentyl, hexyl, heptyl, octyl, and decyl; (ii) aryls such as phenyl, tolyl, and benzyl; (iii) fluoroalkyls such as trifluoromethyl, 2,2,2-trifluoroethyl, and 3,3,3-trifluoropropyl; (iv) fluoroaryls; (v) cycloalkyls such as cyclohexyl; (vi) nitrogen-containing groups having an amino or imide structure such as isocyanate or amino; and (vii) oxygen-containing groups having an epoxy structure such as glycidyl, or an acryloyl or methacryloyl structure. Preferred are methyl, ethyl, propyl, butyl, pentyl, hexyl, and phenyl. Id Compounds in which R is methyl are preferred because the raw materials are easily available, the hardness of the film after curing is high, and the chemical resistance is high. Id Compounds in which is phenyl are preferred because they increase the solubility of the polysiloxane in a solvent and make the cured film less likely to crack.

[0030] The above formula (I d ) repeating units, the polysiloxane of the present invention can have a partially linear structure.

[0031] However, since the heat resistance is reduced, it is preferable that the linear structure portion is small. d The repeating units of the formula (I) preferably account for 30 mol % or less, more preferably 5 mol % or less, based on the total number of repeating units of the polysiloxane. d ) repeating unit (0 mol %) is also an embodiment of the present invention.

[0032] The polysiloxane used in the present invention may contain two or more types of repeating units. For example, R Ia is methyl or phenyl a ) and a repeating unit represented by formula (I c and a repeating unit represented by

[0033] The polysiloxane used in the composition of the present invention preferably has silanol. Here, silanol refers to a polysiloxane in which an OH group is directly bonded to the Si skeleton, and is represented by the above formula (I a )~(I d In other words, silanol is a compound in which a hydroxyl group is directly bonded to the silicon atom of a polysiloxane containing a repeating unit such as the above formula (I a )~(I d ), it is formed by bonding -O0.5H to -O0.5-. The silanol content in polysiloxane varies depending on the synthesis conditions of polysiloxane, such as the mixing ratio of monomers and the type of reaction catalyst.

[0034] The silanol content can be evaluated by quantitative infrared absorption spectroscopy. The absorption band attributed to silanol (SiOH) is 900±100 cm in the infrared absorption spectrum. -1 The higher the silanol content, the stronger the intensity of this absorption band.

[0035] In the present invention, the intensity of the absorption band attributed to Si—O is used as the standard for quantitatively evaluating the silanol content. -1 An absorption band having a peak in this range is taken as the peak attributed to Si-O. The silanol content can be relatively evaluated by S2 / S1, which is the ratio of the integrated intensity S2 of the absorption band attributed to SiOH to the integrated intensity S1 of the absorption band attributed to Si-O. In the present invention, S2 / S1 is preferably 0.003 to 0.15, and more preferably 0.01 to 0.10.

[0036] The integrated intensity of the absorption band is determined by taking into account noise in the infrared absorption spectrum. In a typical infrared absorption spectrum of polysiloxane, the band intensity is 900±100 cm -1 and an absorption band attributable to Si-OH with a peak in the range of 1100 ± 100 cm -1An absorption band attributed to Si-O is confirmed, with a peak in the range. The integrated intensities of these absorption bands can be measured as a region taking into account a baseline that takes noise and other factors into account. Note that the tail of the absorption band attributed to Si-OH and the tail of the absorption band attributed to Si-O may overlap. In this case, the wavenumber corresponding to the minimum point between the two absorption bands in the spectrum is used as the boundary. The same applies when the tail of another absorption band overlaps with the tail of the absorption band attributed to Si-OH or Si-O.

[0037] The weight-average molecular weight of the polysiloxane used in the present invention is not particularly limited. However, the higher the molecular weight, the more likely it is that coating properties will be improved. On the other hand, the lower the molecular weight, the easier the synthesis is because synthesis conditions are less limited, while synthesizing polysiloxanes with significantly higher molecular weights is difficult. For these reasons, from the viewpoint of solubility in organic solvents, the weight-average molecular weight of the polysiloxane is usually 500 to 25,000, preferably 1,000 to 20,000. Here, the weight-average molecular weight refers to the weight-average molecular weight in terms of polystyrene, and can be measured by gel permeation chromatography based on polystyrene.

[0038] As mentioned above, publicly available polysiloxanes that fall within the above definition, such as those described in WO 2021 / 099236 and EP 3717966, can be preferably used.

[0039] solvent In a preferred embodiment of the present invention, the composition may further comprise a solvent in order to improve handling, application, and coating of the composition when threading or producing layers thereon. Alternatively, in order to provide a solvent-free composition, the composition contains 5% by weight or less of a solvent based on the total amount of polysiloxane in the composition, and preferably the composition is solvent-free.

[0040] Preferably, the solvent is selected from one or more of the group consisting of propylene glycol monomethyl ether acetate, propylene glycol monomethyl ether, γ-butyrolactone, propylene glycol diacetate, diethylene glycol monohexyl ether, methyl 3-methoxypropionate, methyl isobutyl ketone, methyl ethyl ketone, more preferably γ-butyrolactone, propylene glycol monomethyl ether acetate, or a mixture of γ-butyrolactone and propylene glycol monomethyl ether acetate.

[0041] The selected solvents are believed to have good compatibility with the composition, boiling point, viscosity, and / or vapor pressure, provide better handling of the composition, are suitable for producing layers at lower temperatures, and / or provide easy production.

[0042] In a preferred embodiment of the present invention, the total amount of solvents based on the total amount of polysiloxanes is 0 to 300% by mass. When the composition contains a solvent, it is preferably 0.1 to 150% by mass, more preferably 50 to 90% by mass.

[0043] additives In some embodiments of the present invention, the composition may optionally further contain one or more additives. Such additives may be selected from, for example, one or more of the group consisting of surfactants, adhesion promoters, silane coupling agents, thermal acid generators, thermal base generators, crosslinking monomers, and polymerization initiators. Publicly available additives, such as those described in EP 3717966 or WO 2021 / 099236, are preferably used. Since the additives are not essential to the present invention, the amount of the additive in the composition or layer based on the total amount of polysiloxane is preferably 5% by weight or less, more preferably 1% by weight or less. The composition and / or layer obtained from the composition may not contain the additive.

[0044] In another aspect, the present invention further relates to a method for making a composition of the present invention comprising, consisting essentially of, or consisting of at least the following steps: (I x ) polysiloxane; and The following chemical formula (I) or chemical formula (I z ), preferably a sulfur-containing compound represented by the following chemical formula (I), optionally together with a solvent and / or other additives. XS-Y (I) A detailed description of the sulfur-containing compound and polysiloxane (including preferred amounts) is provided above in the sections ii) Sulfur-containing compound and i) Polysiloxane.

[0045] In another aspect, the present invention further relates to a composition obtained or obtainable by the process for producing the composition described above.

[0046] In another aspect, the present invention further relates to a method for producing a layer comprising, consisting essentially of, or consisting of at least the following steps: (I Y ) providing a composition of the present invention, preferably on a substrate, a support layer, or a layer of an electronic device; (II Y ) heating the provided composition to form a layer, preferably to remove the solvent in the composition, preferably at a temperature of 60 to 140°C, more preferably 80 to 130°C; (III Y ) Optionally, exposing the provided composition to ultraviolet (UV) light to cure it. According to the present invention, the UV light has a peak light wavelength in the range of 250 to 450 nm.

[0047] In another aspect, the present invention further relates to a layer obtained from the composition of the present invention by curing or by the method for producing a layer as described above. Preferably, said layer is a protective layer for an electrical device. Preferably, said curing is thermal curing and / or UV light curing.

[0048] In another aspect, the present invention further relates to a layer comprising, consisting essentially of, or consisting of at least: i) polymers made from polysiloxanes; and ii) a compound represented by the following chemical formula (I) or chemical formula (I z ) a sulfur-containing compound represented by the following chemical formula (I), preferably a sulfur-containing compound represented by the following chemical formula (I): XS-Y (I) A detailed description of the sulfur-containing compound and polysiloxane (including preferred amounts) is provided above in the sections ii) Sulfur-containing compound and i) Polysiloxane.

[0049] In a preferred embodiment of the present invention, the dielectric constant (ε r ) is 3.5 to 10, more preferably 3.6 to 8, even more preferably 4 to 7, and even more preferably 4.5 to 6.

[0050] The dielectric constant (ε r ) is believed to provide improved touch sensitivity of the layer, like a glass substrate, when used as a protective layer in devices, i.e., electronic devices such as OLEDs, LCDs, etc. The dielectric constant of the layer is measured as described above in the composition section.

[0051] In a preferred embodiment of the present invention, the haze value of the layer is less than 100%, preferably 0.01 to 10%, and more preferably 0.1 to 5%. According to the present invention, the haze value is measured in air at room temperature using a haze measurement system equipped with an integrating sphere (NDH-7000, Nippon Denshoku, Japan, light source: white LED 3W, wavelength range: 380-780 nm). The thickness of the sample is 2 μm-700 μm, particularly 700 μm. In the schematic diagram of the integrating sphere for measuring transmittance and haze, the total light transmittance (T T )T T =T P +T D , Haze (H) H=TD / T T is. Parallel light transmittance (T P ) is determined by measuring the light intensity at a position facing the sample inside the integrating sphere, and the diffracted light transmittance (T D ) and T P Total light transmittance (T T ) is the formula T T =T P +T D The degree of light scattering in the sample, i.e., haze (H), is calculated by H=T D / T T The transmittance and haze are measured.

[0052] In another aspect, the present invention further relates to an electronic device comprising at least the layer of the present invention, preferably said electronic device comprises a light modulating layer or a light emitting layer, preferably said layer is disposed on the outermost surface of the electronic device. More preferably, it is the light extraction side (viewing side) of the electronic device. Preferably, said electronic device does not comprise a cover glass substrate, and the layer is used in place of the cover glass substrate to achieve a cover glass-free electronic device with good touch sensitivity and preferably with a lower haze value.

[0053] In another aspect, the present invention further relates to the use of the sulfur-containing compounds of formula (I) as dielectric constant enhancers in polysiloxane-containing compositions.

[0054] In another aspect, the present invention further relates to a method of using the composition of the present invention as a protective layer forming composition for an electronic device, preferably by using the composition in place of the top glass substrate of said electronic device.

[0055] Preferred Embodiments 1. A composition comprising, consisting essentially of, or consisting of at least the following, preferably a composition for forming a protective layer: i) polysiloxane; and ii) a compound represented by the following chemical formula (I) or chemical formula (I z), preferably a sulfur-containing compound represented by the following chemical formula (I), which is a dielectric constant improver preferably used in polysiloxane-containing compositions: XS-Y (I) where: X is a hydrogen atom or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, preferably a hydrogen atom; Y is one or more groups R a an unsubstituted or substituted alkyl group having 1 to 12 carbon atoms, an unsubstituted or substituted cyclic alkyl group having 3 to 22 carbon atoms, an unsubstituted or substituted aryl group having 3 to 22 carbon atoms, or an unsubstituted or substituted alkyl-aryl group having 4 to 22 carbon atoms, each of which may be substituted by R, wherein one or more non-adjacent CH groups in the alkyl group, cyclic alkyl group, aryl group, and / or alkyl-aryl group are each independently selected from the group consisting of R a C=CR a , C≡C, Si(R a )2, Ge(R a )2, Sn(R a )2, C=O, C=S, C=Se, C=NR a , P(=O)(R a ), SO, CSR a , SO2, NR a , OS, or CONR a wherein one or more non-adjacent CH groups of said aryl group and / or said alkyl-aryl group may be substituted, independently of each other, by SiR a , GeR a , SnR a , CSR a , SO2, NR a , O, S, SO, or CONR a and one or more H atoms may be replaced by D, F, Cl, Br, I, CN, or NO2; R aare each the same or different and are H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, wherein an H atom may be replaced by D, F, Cl, Br, or I; a may also together form a monocyclic or polycyclic aliphatic, aromatic or heteroaromatic ring system. 2. The composition according to embodiment 1, wherein the molecular weight (Mw) of the sulfur-containing compound is 600 or less, preferably 500 or less, more preferably 400 or less, even more preferably 80 to 400, and most preferably 100 to 210. 3. The composition according to embodiment 1 or 2, wherein the total amount of the sulfur-containing compounds based on the total amount of the polysilazanes in the composition is 0.01 to 40 mass%, preferably 0.1 to 20 mass%, and more preferably 0.5 to 5.0 mass%. 4. The dielectric constant (ε r The composition according to any one of the above embodiments, wherein the dielectric constant (ε ) of the solid content of the composition is 3.5 to 7, more preferably 4 to 6.5, and even more preferably 4.5 to 6. Preferably, r ) is measured by the following method. 1) Sample preparation and dielectric constant measurement coating the composition onto a conductive wafer selected from Al, Si, or Mo; A sample is formed by placing an electrode on a composition coated with Ag or Al by sputtering or evaporation; The dielectric constant of the sample is measured by attaching a pin probe to each of the surface of the conductive wafer and the top electrode on the coated composition. 2) Measurement conditions: The dielectric constant was measured using an LCR meter (E4980A, Agilent, Korea / 6440B, Dongyang Technica, Japan) at room temperature. A specific frequency range (50-1 MHz) was applied, and the capacitance displayed on the LCR meter was read. The dielectric constant was calculated using the following formula: C = K A / d (C = capacitance, K = dielectric constant, A = effective electrode area, d = distance between electrodes). 5. The composition of any one of the preceding embodiments, wherein the sulfur-containing compound (I) is represented by the following chemical formula (IIa) or (IIb): X a SY a -Z a (IIa) X a represents a hydrogen atom or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, and is preferably a hydrogen atom; Y a is one or more groups R a an unsubstituted or substituted linear alkylene group having 1 to 12 carbon atoms, or an unsubstituted or substituted branched alkylene group having 3 to 12 carbon atoms, optionally substituted by R, wherein one or more non-adjacent CH groups of the alkyl group, cyclic alkyl group, aryl group and / or alkyl-aryl group are each independently selected from the group consisting of R a C=CR a , C≡C, Si(R a )2, Ge(R a )2, Sn(R a )2, C=O, C=S, C=Se, C=NR a , P(=O)(R a ), SO, CSH, SO2, NR a , OS, or CONR a and one or more H atoms may be replaced by D, F, Cl, Br, I, CN, or NO2; R aare each the same or different and are H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, wherein an H atom may be replaced by D, F, Cl, Br, or I; a may also together form a monocyclic or polycyclic aliphatic, aromatic or heteroaromatic ring system; Z a teeth, * -CR a1 R a2 R a3 where R a1 , R a2 and R a3 are each independently a hydrogen atom or a halogen atom selected from Cl, Br, F, or I, and R a1 , R a2 and R a3 At least one of R is a halogen atom, and preferably R a1 , R a2 and R a3 At least two of R are halogen atoms, and more preferably R a1 , R a2 and R a3 are all halogen atoms, preferably the halogen atoms are Cl or F, more preferably the halogen atom is F. X b SY b (IIb) X b represents a hydrogen atom or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, and is preferably a hydrogen atom; Y b is one or more groups R a an unsubstituted or substituted cyclic alkyl group having 3 to 22 carbon atoms, an unsubstituted or substituted aryl group having 3 to 22 carbon atoms, or an unsubstituted or substituted alkyl-aryl group having 4 to 22 carbon atoms, wherein one or more non-adjacent CH groups in the alkyl group, cyclic alkyl group, aryl group, and / or alkyl-aryl group are each independently selected from the group consisting of R a C=CRa , C≡C, Si(R a )2, Ge(R a )2, Sn(R a )2, C=O, C=S, C=Se, C=NR a , P(=O)(R a ), SO, CSR a , SO2, NR a , OS, or CONR a wherein one or more non-adjacent CH groups of said aryl group and / or said alkyl-aryl group may be substituted, independently of each other, by SiR a , GeR a , SnR a , CSR a , SO2, NR a , O, S, SO, or CONR a and one or more H atoms may be replaced by D, F, Cl, Br, I, CN, or NO2; R a are each the same or different and are H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, wherein an H atom may be replaced by D, F, Cl, Br, or I; a may also together form a monocyclic or polycyclic aliphatic, aromatic or heteroaromatic ring system. 6. The polysiloxane is represented by the chemical formula (I a The composition of any one of the preceding embodiments, comprising a repeat unit of: [ka] where: R Ia is hydrogen, C 1-30 (Preferably C 1-10 ) linear, C 3-30 (Preferably C 3-10) a branched or cyclic saturated or unsaturated aliphatic hydrocarbon group or aromatic hydrocarbon group, wherein the aliphatic hydrocarbon group and the aromatic hydrocarbon group are each unsubstituted or substituted with fluorine, hydroxy, or alkoxy; In the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is not substituted or one or more methylenes are substituted with oxy, imino or carbonyl, provided that R Ia is neither hydroxy nor alkoxy. 7. The polysiloxane is represented by the chemical formula (I b The composition of any one of the preceding embodiments, comprising a repeat unit of: [ka] where: R Ib is a group obtained by removing multiple hydrogen atoms from a nitrogen-containing and / or oxygen-containing alicyclic hydrocarbon compound having amino, imino, and / or carbonyl; R Ib is preferably a group obtained by removing multiple hydrogen atoms, preferably two or three hydrogen atoms, from a nitrogen-containing aliphatic hydrocarbon ring having an imino and / or carbonyl group, more preferably a five- or six-membered ring containing nitrogen as a ring member; for example, it is a group obtained by removing two or three hydrogen atoms from piperidine, pyrrolidine, or isocyanurate; R Ib connects Si atoms contained in multiple repeating units together. 8. The polysiloxane is represented by the chemical formula (I c The composition of any one of the preceding embodiments, comprising a repeat unit of: [ka] 9. The polysiloxane is represented by the chemical formula (I d The composition of any one of the preceding embodiments, comprising a repeat unit of: [ka] where: R Idare each independently hydrogen, C 1-30 (Preferably C 1-10 ) linear, C 3-30 (Preferably C 3-10 ) a branched or cyclic saturated or unsaturated aliphatic hydrocarbon group or aromatic hydrocarbon group, the aliphatic hydrocarbon group and the aromatic hydrocarbon group are each unsubstituted or substituted with fluorine, hydroxy, or alkoxy; In the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is unsubstituted or substituted with oxy, imido or carbonyl. 10. The composition of any one of the previous embodiments, further comprising an additive. 11. The composition of any one of the preceding embodiments, further comprising a solvent, preferably selected from one or more of the group consisting of propylene glycol monomethyl ether acetate, propylene glycol monomethyl ether, gamma-butyrolactone, propylene glycol diacetate, diethylene glycol monohexyl ether, methyl 3-methoxypropionate, methyl isobutyl ketone, methyl ethyl ketone, more preferably gamma-butyrolactone, propylene glycol monomethyl ether acetate, or a mixture of gamma-butyrolactone and propylene glycol monomethyl ether acetate. 12. A method of making a composition according to any one of the preceding embodiments, comprising at least the following steps: (I x ) polysiloxane; and The following chemical formula (I) or chemical formula (I z ), preferably a sulfur-containing compound represented by the following chemical formula (I): XS-Y (I) where: X is a hydrogen atom or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, preferably a hydrogen atom; Y is one or more groups R aan unsubstituted or substituted alkyl group having 1 to 12 carbon atoms, an unsubstituted or substituted cyclic alkyl group having 3 to 22 carbon atoms, an unsubstituted or substituted aryl group having 3 to 22 carbon atoms, or an unsubstituted or substituted alkyl-aryl group having 4 to 22 carbon atoms, each of which may be substituted by R, wherein one or more non-adjacent CH groups in the alkyl group, cyclic alkyl group, aryl group, and / or alkyl-aryl group are each independently selected from the group consisting of R a C=CR a , C≡C, Si(R a )2, Ge(R a )2, Sn(R a )2, C=O, C=S, C=Se, C=NR a , P(=O)(R a ), SO, CSR a , SO2, NR a , OS, or CONR a wherein one or more non-adjacent CH groups of said aryl group and / or said alkyl-aryl group may be substituted, independently of each other, by SiR a , GeR a , SnR a , CSR a , SO2, NR a , O, S, SO, or CONR a and one or more H atoms may be replaced by D, F, Cl, Br, I, CN, or NO2; R a are each the same or different and are H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, wherein an H atom may be replaced by D, F, Cl, Br, or I; a may also together form a monocyclic or polycyclic aliphatic, aromatic or heteroaromatic ring system. 13. A composition obtained or obtainable by the method of embodiment 12. 14. A method for producing a layer comprising at least the following steps: (I Y) providing the composition of any one of embodiments 1 to 11 and 13, preferably on a substrate, a support layer, or a layer of an electronic device; preferably, the substrate is selected from a glass substrate, a plastic substrate, or a polarizer; (II Y ) a step of heating the provided composition to form a layer, preferably to remove the solvent in the composition, and preferably the heating is carried out at a temperature of 60 to 140°C, more preferably 80 to 130°C. 15. A layer obtained from the composition according to any one of embodiments 1 to 13 by curing or by the method according to embodiment 14. Preferably, the layer is a protective layer for an electrical device. Preferably, the curing is thermal curing. 16. A layer comprising at least: i) polymers made from polysiloxanes; and ii) a compound represented by the following chemical formula (I) or chemical formula (I z ), preferably a sulfur-containing compound represented by the following chemical formula (I): XS-Y (I) where: X is a hydrogen atom or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, preferably a hydrogen atom; Y is one or more groups R a an unsubstituted or substituted alkyl group having 1 to 12 carbon atoms, an unsubstituted or substituted cyclic alkyl group having 3 to 22 carbon atoms, an unsubstituted or substituted aryl group having 3 to 22 carbon atoms, or an unsubstituted or substituted alkyl-aryl group having 4 to 22 carbon atoms, each of which may be substituted by R, wherein one or more non-adjacent CH groups in the alkyl group, cyclic alkyl group, aryl group, and / or alkyl-aryl group are each independently selected from the group consisting of R a C=CR a , C≡C, Si(R a )2, Ge(R a )2, Sn(R a )2, C=O, C=S, C=Se, C=NR a , P(=O)(R a ), SO, CSR a , SO2, NR a, OS, or CONR a wherein one or more non-adjacent CH groups of said aryl group and / or said alkyl-aryl group may be substituted, independently of each other, by SiR a , GeR a , SnR a , CSR a , SO2, NR a , O, S, SO, or CONR a and one or more H atoms may be replaced by D, F, Cl, Br, I, CN, or NO2; R a are each the same or different and are H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, wherein an H atom may be replaced by D, F, Cl, Br, or I; a may also together form a monocyclic or polycyclic aliphatic, aromatic or heteroaromatic ring system. 17. The dielectric constant (ε r ) is from 3.5 to 10, more preferably from 3.6 to 8, even more preferably from 4 to 7, and still more preferably from 4.5 to 6. 18. The layer of any one of embodiments 15 to 17, wherein the haze value of the layer is less than 100%, preferably 0.01 to 10%, more preferably 0.1 to 5%. Here, the haze value is measured in air at room temperature using a haze measurement system equipped with an integrating sphere (NDH-7000, Nippon Denshoku, Japan, light source: white LED 3W, wavelength range: 380 to 780 nm). In the schematic diagram of the integrating sphere for measuring transmittance and haze, the total light transmittance (T T )T T =T P +T D , Haze (H) H=T D / T T is. Parallel light transmittance (T P) is determined by measuring the light intensity at a position facing the sample inside the integrating sphere, and the diffracted light transmittance (T D ) and T P Total light transmittance (T T ) is the formula T T =T P +T D The degree of light scattering in the sample, i.e., haze (H), is calculated by H=T D / T T The transmittance and haze are measured. 19. An electronic device comprising at least a layer according to any one of embodiments 15 to 18. Preferably, said electronic device comprises a light modulating layer or a light emitting layer, and preferably said layer is disposed on the outermost surface of the electronic device. More preferably, it is the light extraction side (viewing side) of the electronic device. 20. A compound of formula (I) or formula (I) as a dielectric constant enhancer in a polysiloxane-containing composition. z ) a method using a sulfur-containing compound. 21. A method of using the composition according to any one of embodiments 1 to 11 and 13 as a composition for forming a protective layer for an electronic device, preferably by using the composition in place of the upper glass substrate of the electronic device.

[0056] Technical effect of the invention The present invention provides one or more of the following technical advantages: To obtain a polysiloxane-containing composition, preferably a composition for forming a protective layer, that exhibits an improved dielectric constant, such as that of a glass substrate of an electronic device, and preferably has the lowest haze characteristics; to obtain a layer or cured composition that exhibits an improved dielectric constant, such as that of a glass substrate of an electronic device, and preferably has the lowest haze characteristics; to obtain a polysiloxane-containing composition, preferably a composition for forming a protective layer, that allows a sufficient amount of thiol to be well dispersed in the composition; to obtain a layer or cured composition in which a sufficient amount of thiol is well dispersed in the layer or cured composition; to obtain a polysiloxane-containing composition, preferably a composition for forming a protective layer, that can be formed into a layer or cured composition with mild or lower temperature treatment, and that can form a smooth coating of the polysiloxane-containing composition on any substrate, i.e., PET, CPI, COP, or polarizer. [Example]

[0057] The following Examples 1 to 10 provide an explanation of the present invention and detailed descriptions of their preparation, but the present invention is not limited to these examples.

[0058] Example 1: Mixed sample preparation A polysiloxane polymer (Merck) represented by the following chemical formula was mixed with 1% or 5% by weight of 1,2-mercaptobenzimidazole (based on the total weight of the polysiloxane) as a thiol-containing compound in the presence of a mixture of propylene glycol monomethyl ether acetate and gamma-butyrolactone (total weight of the siloxane polymer and thiol-containing compound:solvent mixture = 3:7). After mixing, the above compounds were separately coated onto Al-deposited silicon wafers by spin coating to obtain samples (Sample 1-1 contains 1% 1,2-mercaptobenzimidazole, and Sample 1-2 contains 5% 1,2-mercaptobenzimidazole). The solvent mixture was then evaporated at 120°C during the curing process to obtain Samples 1-1 (1%) and 1-2 (5%). [ka]

[0059] Examples 2 to 9: Mixed sample preparation Examples 2 to 9 were carried out in the same manner as in Example 1, except that the thiol-containing compounds listed below were used instead of 1,2-mercaptobenzimidazole. In this manner, 1% thiol-containing compound samples (Samples 2-1, 3-1, 4-1, 5-1, 6-1, 7-1, 8-1, and 9-1) and 5% thiol-containing compound samples (Samples 2-2, 3-2, 4-2, 5-2, 6-2, 7-2, 8-2, and 9-2) were obtained in each example.

[0060] Thiol-containing compounds used in Examples 1 to 9 Comparative Example 1: No thiol-containing compound is used Example 1: 1,2-mercaptobenzimidazole Example 2: 2-mercaptoimidazole Example 3: Benzene-1,2-dithiol Example 4: Cyclohexanethiol Example 5: 2,2,2-trifluoroethanethiol Example 6: Pentaerythritol tetrakis(3-mercaptobutanate) Example 7: Tris(3-mercaptobutyloxyethyl) isocyanurate Example 8: Trimethylolpropane tris(3-mercaptobutyrate) Example 9: Pentaerythritol tetra(3-mercaptopropionate) Other thiol-containing compounds such as 1-phenethyl-1H-benzo[d]imidazole-2-thiol can also be preferably used.

[0061] Comparative Example 1: Reference Sample Preparation A reference sample is prepared in the same manner as described in Example 1, except that no thiol-containing compound is added / mixed with the siloxane polymer. In this way, a reference sample is obtained.

[0062] Example 10: Measurement of the dielectric constant of the samples of Examples 1 to 6 and Comparative Example 1 The haze values of the samples of Examples 1 to 6 and Comparative Example 1 were measured independently in air at room temperature using a haze measurement system equipped with an integrating sphere (NDH-7000, Nippon Denshoku, Japan, light source: white LED 3W, wavelength range: 380 to 780 nm). The thickness of the samples was 2 μm to 700 μm, and in particular 700 μm. In the schematic diagram of the integrating sphere for measuring transmittance and haze, the total light transmittance (T T )T T =T P +T D , Haze (H) H=T D / T T is. Parallel light transmittance (T P ) is determined by measuring the light intensity at a position facing the sample inside the integrating sphere, and the diffracted light transmittance (T D ) and T P Total light transmittance (T T ) is the formula T T =T P +T D The degree of light scattering in the sample, i.e., haze (H), is calculated by H=T D / T T The transmittance and haze are measured.

[0063] Table 1 below shows the measurement results.

[0064] [Table 1]

[0065] As shown in Table 1 above, the thiol-containing compounds, preferably those used in Samples 1-5, dramatically increase the dielectric constant of the polysiloxane compositions, which is believed to aid in the touch sensitivity of glass-free electronic devices, such as the touch-glass-free OLED concept.

Claims

1. A composition comprising at least the following, preferably a protective layer forming composition: i) Polysiloxanes; and ii) Sulfur-containing compounds represented by the following chemical formula (I): XS-Y (I) Here, X is a hydrogen atom, or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, preferably a hydrogen atom; Y is an unsubstituted or substituted alkyl group having 1 to 12 carbon atoms, an unsubstituted or substituted cycloalkyl group having 3 to 22 carbon atoms, an unsubstituted or substituted aryl group having 3 to 22 carbon atoms, or an unsubstituted or substituted alkyl-aryl group having 4 to 22 carbon atoms, which may be substituted with one or more groups R ａ wherein one or more non-adjacent CH groups of the alkyl group, cycloalkyl group, aryl group and / or the alkyl-aryl group are independently of each other, R ２ C═CR ａ C≡C, Si(R ａ ), Ge(R ａ ), Sn(R ２ ), C═O, C═S, C═Se, C═NR ａ ), P(═O)(R ２ ), SO, CSR ａ ), SO ２ ), NR ａ ), OS, or CONR ａ ), and one or more non-adjacent CH groups of the aryl group and / or the alkyl-aryl group are independently of each other, SiR ａ ), GeR ２ ), SnR ａ ), CSR ａ ), SO ａ ), NR ａ ), O, S, SO, or CONR ａ ), and one or more H atoms may be substituted with D, F, Cl, Br, I, CN, or NO ａ ); ２ ); ａ ); ａ ); ２ ; R ａ Each of these is either the same or different, and is H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, where the H atom may be substituted with D, F, Cl, Br, or I; and two or more adjacent substituents R ａ They may also form monocyclic or polycyclic aliphatic, aromatic, or heteroaromatic ring systems with respect to each other.

2. The composition according to claim 1, wherein the molecular weight (Mw) of the sulfur-containing compound is 600 or less.

3. The composition according to claim 1 or 2, wherein the total amount of the sulfur-containing compound based on the total amount of the polysilazane in the composition is 0.01 to 40% by mass.

4. The dielectric constant of the solid content of the composition (ε ｒ The composition according to claim 1 or 2, wherein ) is 3.5 to 7.

5. The composition according to claim 1 or 2, wherein the sulfur-containing compound is represented by the following chemical formula (IIa) or (IIb): X ａ S-Y ａ -Z ａ (IIa) Here, X ａ is a hydrogen atom, or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, preferably a hydrogen atom; Y ａ is one or more base R ａ An unsubstituted or substituted linear alkylene group having 1 to 12 carbon atoms, or an unsubstituted or substituted branched alkylene group having 3 to 12 carbon atoms, wherein one or more non-adjacent CH groups of the alkyl group, cyclic alkyl group, aryl group and / or alkyl-aryl group. ２ The bases are independent of each other, R ａ C=CR ａ , C≡C, Si(R ａ ) ２ , Ge(R ａ ) ２ , Sn(R ａ ) ２ , C=O, C=S, C=Se, C=NR ａ , P(=O)(R ａ ), SO, CSH, SO ２ , NR ａ OS, or CONR ａ They may be substituted by D, F, Cl, Br, I, CN, or NO. ２ It may be replaced by; R ａ Each of these is either the same or different, and is H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, where the H atom may be substituted with D, F, Cl, Br, or I; and two or more adjacent substituents R ａ They may also form monocyclic or polycyclic aliphatic, aromatic, or heteroaromatic ring systems with respect to each other; Z ａ teeth, ＊ -CR ａ１ R ａ２ R ａ３ And here, R ａ１ , R ａ２ and R ａ３ R is a hydrogen atom or a halogen atom selected from Cl, Br, F, or I, independently of each other. ａ１ , R ａ２ and R ａ３ At least one of them is a halogen atom, preferably R ａ１ , R ａ２ and R ａ３ At least two of them are halogen atoms, more preferably R ａ１ , R ａ２ and R ａ３ all of these are halogen atoms, preferably the halogen atoms are Cl or F, and more preferably the halogen atoms are F; X ｂ S-Y ｂ (Ib) Here, Xb is a hydrogen atom, or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, preferably a hydrogen atom; Y b is an unsubstituted or substituted cyclic alkyl group having 3 to 22 carbon atoms, an unsubstituted or substituted aryl group having 3 to 22 carbon atoms, or an unsubstituted or substituted alkyl-aryl group having 4 to 22 carbon atoms, which may be substituted with one or more groups Ra, where one or more non-adjacent CH2 groups of the alkyl group, cyclic alkyl group, aryl group and / or the alkyl-aryl group may be independently substituted with Ra C=CR a, C≡C, Si(Ra)2, Ge(Ra)2, Sn(Ra)2, C=O, C=S, C=Se, C=NR a, P(=O)(Ra), SO, CSR a, SO2, NR a, OS, or CONR a, and one or more non-adjacent CH groups of the aryl group and / or the alkyl-aryl group may be independently substituted with SiRa They may be substituted with GeR a, SnR a, CSR a, SO 2, NR a, O, S, SO, or CONR a, and one or more H atoms may be substituted with D, F, Cl, Br, I, CN, or NO 2; Each of the R a atoms may be the same or different, and may be H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, where the H atom may be substituted with D, F, Cl, Br, or I; two or more adjacent substituents R a may also form monocyclic or polycyclic aliphatic, aromatic, or heteroaromatic ring systems with respect to each other.

6. The aforementioned polysiloxane has the chemical formula (I ａ The composition according to claim 1 or 2, comprising a repeating unit of ): 【Chemistry 1】 Here, R Ｉａ is hydrogen, C １－３０ (Preferably C １－１０ ) Linear chain, C ３－３０ (Preferably C ３－１０ ) A branched or cyclic saturated or unsaturated aliphatic hydrocarbon group or an aromatic hydrocarbon group, wherein the aliphatic hydrocarbon group and the aromatic hydrocarbon group are either unsubstituted or substituted with fluorine, hydroxyl, or alkoxy, In the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is either unsubstituted or one or more methylene is substituted with oxy, imino, or carbonyl, provided that R Ｉａ It is neither hydroxyl nor alkoxy.

7. The aforementioned polysiloxane has the chemical formula (I ｂ The composition according to claim 1 or 2, comprising a repeating unit of ): 【Chemistry 2】 Here, R Ｉｂ This is a group obtained by removing multiple hydrogen atoms from a nitrogen-containing and / or oxygen-containing alicyclic hydrocarbon compound having amino, imino, and / or carbonyl groups; R Ｉｂ R is a group obtained by removing several hydrogens, preferably two or three, from a nitrogen-containing aliphatic hydrocarbon ring having an imino and / or carbonyl, more preferably a five-membered or six-membered ring containing nitrogen as a ring member; for example, a group obtained by removing two or three hydrogens from piperidine, pyrrolidine, or isocyanurate; R Ｉｂ This connects the Si elements contained within multiple repeating units.

8. The composition according to claim 1 or 2, further comprising a solvent.

9. A method for producing the composition according to claim 1 or 2, comprising at least the following steps: (I ｘ ) Polysiloxane; and The process involves mixing a sulfur-containing compound represented by the following chemical formula (I): XS-Y (I) Here, X is a hydrogen atom, or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, preferably a hydrogen atom; Y is an unsubstituted or substituted alkyl group having 1 to 12 carbon atoms, an unsubstituted or substituted cycloalkyl group having 3 to 22 carbon atoms, an unsubstituted or substituted aryl group having 3 to 22 carbon atoms, or an unsubstituted or substituted alkyl-aryl group having 4 to 22 carbon atoms, which may be substituted with one or more groups R ａ wherein one or more non-adjacent CH groups of the alkyl group, cycloalkyl group, aryl group and / or the alkyl-aryl group are independently of each other R ２ C═CR ａ C≡C, Si(R ａ ), Ge(R ａ ), Sn(R ２ ), C═O, C═S, C═Se, C═NR ａ ), P(═O)(R ２ ), SO, CSR ａ ), SO ２ ), NR ａ ), OS, or CONR ａ ), and one or more non-adjacent CH groups of the aryl group and / or the alkyl-aryl group are independently of each other SiR ａ ), GeR ２ ), SnR ａ ), CSR ａ ), SO ａ ), NR ａ ), O, S, SO, or CONR ａ ), and one or more H atoms may be substituted with D, F, Cl, Br, I, CN, or NO ａ ); ２ ), NR ａ ), O, S, SO, or CONR ａ ), and one or more H atoms may be substituted with D, F, Cl, Br, I, CN, or NO ２ ); R ａ Each of these is either the same or different, and is H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, where the H atom may be substituted with D, F, Cl, Br, or I; and two or more adjacent substituents R ａ They may also form monocyclic or polycyclic aliphatic, aromatic, or heteroaromatic ring systems with respect to each other.

10. A method for producing layers comprising at least the following steps: (I Ｙ ) A step of providing the composition according to claim 1 or 2; (II Ｙ ) A step of heating the provided composition to form a layer, preferably removing the solvent in the composition, preferably carrying out the heating at a temperature of 60 to 140°C, more preferably 80 to 130°C.

11. A layer obtained by curing from the composition according to claim 1 or 2.

12. Layers that include at least the following: i) Polymers produced from polysiloxanes; and ii) Sulfur-containing compounds represented by the following chemical formula (I): XS-Y (I) Here, X is a hydrogen atom, or an unsubstituted or substituted alkyl group having 1 to 4 carbon atoms, preferably a hydrogen atom; Y is one or more base R ａ An unsubstituted or substituted alkyl group having 1 to 12 carbon atoms, an unsubstituted or substituted cyclic alkyl group having 3 to 22 carbon atoms, an unsubstituted or substituted aryl group having 3 to 22 carbon atoms, or an unsubstituted or substituted alkyl-aryl group having 4 to 22 carbon atoms, wherein one or more non-adjacent CH groups of the alkyl group, cyclic alkyl group, aryl group and / or alkyl-aryl group ２ The bases are independent of each other, R ａ C=CR ａ , C≡C, Si(R ａ ) ２ , Ge(R ａ ) ２ , Sn(R ａ ) ２ , C=O, C=S, C=Se, C=NR ａ , P(=O)(R ａ ), SO, CSR ａ SO ２ , NR ａ OS, or CONR ａ They may be substituted with, and one or more non-adjacent CH groups of the aryl group and / or the alkyl-aryl group are independently of each other, SiR ａ , GeR ａ SnR ａ CSR ａ SO ２ , NR ａ , O, S, SO, or CONR ａ They may be substituted with D, F, Cl, Br, I, CN, or NO. ２ It may be replaced with; R ａ Each of these is either the same or different, and is H, D, or an alkyl group having 1 to 10 carbon atoms, a cyclic alkyl group having 3 to 10 carbon atoms, an aryl group having 3 to 10 carbon atoms, an aryl-alkyl group having 4 to 10 carbon atoms, or a heteroaryl group having 3 to 10 carbon atoms, where the H atom may be substituted with D, F, Cl, Br, or I; and two or more adjacent substituents R ａ They may also form monocyclic or polycyclic aliphatic, aromatic, or heteroaromatic ring systems with respect to each other.

13. The dielectric constant of the solid content of the aforementioned layer (ε ｒ The layer according to claim 12, wherein the value is 3.5 to 10.

14. The layer according to claim 12 or 13, wherein the haze value of the layer is less than 100%.

15. An electronic device comprising at least the layer described in claim 12 or 13.

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