Composition

Abstract

The present invention relates to compositions comprising polysiloxanes.

Description

[Technical Field]

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

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

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

[0004] However, the present inventors have newly discovered that there still exist one or more important problems that need to be improved, as listed below: To obtain a polysiloxane-containing composition, preferably a protective layer-forming composition, which exhibits an improved dielectric constant, such as for a glass substrate of an electronic device, and preferably has minimal haze characteristics; to obtain a layer or cured composition, which exhibits an improved dielectric constant, such as for a glass substrate of an electronic device, and preferably has minimal haze characteristics; to obtain a polysiloxane-containing composition, preferably a protective layer-forming composition, which allows for good dispersion of a sufficient amount of thiol in the composition; to obtain a layer or cured composition, which allows for good dispersion of a sufficient amount of thiol in the layer or cured composition; to obtain a polysiloxane-containing composition, preferably a protective layer-forming composition, which allows for the formation of a layer or cured composition in a mild or lower temperature process, and which allows for smooth coating of the polysiloxane-containing composition on any substrate, i.e., PET, CPI, COP, or polarizer.

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

[0006] There is then found a novel composition, preferably a protective layer-forming composition, as claimed, comprising, consisting essentially of, or consisting of at least: i) polysiloxane; and ii) A compound represented by the following formula (I): Preferably, the compound is a dielectric constant enhancer preferably used in polysiloxane-containing compositions: [ka] During the ceremony, Z X1 is selected from the group consisting of a direct bond, CH2, C=O, O, (C=O)2, (C=O)O, (C=O)3, (C=O)2O, (C=O)2CH2 and C=O(CH2)2, preferably selected from a direct bond, C=O, O, (C=O)2, (C=O)3; n is 0 or 1; R X1 is H, D, or OR X3 and; R X2 is H, D, or OR X3 and; R X3 is H, D, an unsubstituted or substituted linear alkyl group having 1 to 5 carbon atoms, an unsubstituted or substituted branched alkyl group having 3 to 5 carbon atoms, or Na + , Li + , K. + , Rb + , Cs + , Fr + , Cu + , Ag + , Au + , Ti + , Pd + , Ni + , Mn + , Cr + , V + Preferably, the monovalent metal cation is selected from the group consisting of Na + , Li + , K. + , Cu + , Ag + , Au + and more preferably Na + , Li + , K. + is.

[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 mixing a compound represented by formula (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 a layer 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) a polymer made from polysiloxane; and ii) A compound represented by formula (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 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 electronic devices.

[0015] Further advantages of the present invention will become apparent from the following detailed description.

[0016] Definition of Terms In this specification, symbols, units, abbreviations, and terms have the following meanings unless otherwise specified.

[0017] In this specification, unless otherwise stated, the singular includes the plural, and "one" or "that" means "at least one." In this specification, unless otherwise stated, elements of a concept may be expressed in terms of multiple species, and when amounts (e.g., mass % or mol %) are given, this refers to the sum of the multiple species. "And / or" includes all combinations of elements, including the use of elements singly.

[0018] In this specification, when a numerical range is indicated using "to" or "to," the numerical range 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.

[0019] As used herein, hydrocarbon refers to a group containing carbon and hydrogen, and optionally containing oxygen or nitrogen. Hydrocarbon (hydrocabyl) groups refer to monovalent or divalent or higher-valent hydrocarbons. As used herein, aliphatic hydrocarbons refer to linear, branched, or cyclic aliphatic hydrocarbons, and aliphatic hydrocarbon groups refer to monovalent or divalent or higher-valent aliphatic hydrocarbons. Aromatic hydrocarbons refer to hydrocarbons that not only optionally contain an aliphatic hydrocarbon group as a substituent, but also contain an aromatic ring that may be condensed with an alicyclic ring. Aromatic hydrocarbon groups refer to monovalent or divalent or higher-valent aromatic hydrocarbons. Furthermore, aromatic rings refer to hydrocarbons containing a conjugated unsaturated ring structure, and alicyclic rings refer to hydrocarbons that have a ring structure but do not contain a conjugated unsaturated ring structure.

[0020] In this specification, alkyl refers to a group obtained by removing any one hydrogen atom from a linear or branched saturated hydrocarbon, and includes linear alkyl and branched alkyl. Also, cycloalkyl refers to a group obtained by removing one hydrogen atom from a saturated hydrocarbon containing a cyclic structure, and optionally includes a linear or branched alkyl atom as a side chain in the cyclic structure.

[0021] In this specification, 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, and arylene refers to a hydrocarbon group obtained by removing any two hydrogens from an aromatic hydrocarbon.

[0022] In the present specification, when a polymer has multiple types of repeating units, these repeating units are copolymerized. The copolymerization may be any of alternating copolymerization, random copolymerization, block copolymerization, graft copolymerization, or any mixture thereof.

[0023] In this specification, the temperature unit is Celsius. For example, 20°C means 20 degrees Celsius. DETAILED DESCRIPTION OF THE INVENTION

[0024] According to the present invention, in one embodiment, the composition, which is preferably a protective layer-forming composition, comprises, consists essentially of, or consists of at least: i) polysiloxane; and ii) A compound represented by the following formula (I): Preferably, the compound is a dielectric constant enhancer preferably used in polysiloxane-containing compositions: [ka] During the ceremony, Z X1 is selected from the group consisting of a direct bond, CH2, C=O, O, (C=O)2, (C=O)O, (C=O)3, (C=O)2O, (C=O)2CH2 and C=O(CH2)2, preferably selected from a direct bond, C=O, O, (C=O)2, (C=O)3; n is 0 or 1; R X1 is H, D, or OR X3 and; R X2 is H, D, or OR X3 and; R X3 is H, D, an unsubstituted or substituted linear alkyl group having 1 to 5 carbon atoms, an unsubstituted or substituted branched alkyl group having 3 to 5 carbon atoms, or Na + , Li + , K. + , Rb + , Cs + , Fr + , Cu + , Ag + , Au + , Ti + , Pd + , Ni + , Mn + , Cr + , V + Preferably, the monovalent metal cation is selected from the group consisting of Na + , Li + , K. + , Cu + , Ag + , Au + and more preferably Na + , Li + , K. + is.

[0025] composition In a preferred embodiment of the present invention, the dielectric constant (ε r ) is 3.5 or more and 7 or less, the dielectric constant is preferably 3.9 or more and up to 6.5, more preferably 4.0 or more, and the dielectric constant is preferably 6.5 or less, more preferably 6 or less. 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.

[0026] According to the present invention, the dielectric constant (ε r ) is measured by the following method.

[0027] 1) Sample preparation and dielectric constant measurement coating the composition onto a conductive wafer selected from Al, Si, or Mo; Placing an electrode on the composition coated with Ag or Al by sputtering or vapor deposition to form a sample: Attaching a pin prober to the surface of the conductive wafer and the top electrode on the coated composition, respectively, to measure the dielectric constant of the sample. 2) Measurement conditions: The dielectric constant was measured at room temperature using an LCR meter (E4980A, Agilent, Korea / 6440B, Toyo Technical, Japan) by applying a specific frequency range (50-1 MHz) and reading the capacitance displayed on the LCR meter. The dielectric constant was calculated using the following formula: C = K / d (C = capacitance, K = dielectric constant, A = effective electrode area, d = distance between electrodes).

[0028] ii) a compound of formula (I) According to the present invention, any publicly available compound of formula (I) can be used.

[0029] Such compounds are believed to form two-dimensional structures within and / or on the surface of the film, providing a regular order of such compounds due to the effects of higher dielectric constants and / or strong hydrogen bonding conjugation.

[0030] Preferably, the molecular weight (Mw) of the compound is 250 or less, preferably in the range of 30-250, more preferably 100-200.

[0031] It is believed that the above-mentioned molecular weight can achieve improved dispersibility of the compound of formula (I) in the polysiloxane and good compatibility with the polysiloxane, which can result in lower haze values ​​of the composition and the layer obtained from the composition.

[0032] In a preferred embodiment of the present invention, the total amount of the compound of formula (I) based on the total amount of polysilazanes in the composition is in the range of 0.01 to 40% by weight, preferably 0.1 to 20% by weight, more preferably 0.5 to 5.0% by weight.

[0033] The above-mentioned total amount of the compound of formula (I) based on the total amount of polysiloxane in the composition is believed to enable further improved dispersibility of the compound of formula (I) in the composition, and to enable the resulting layer to have a lower haze value, such as on a glass substrate, and a layer obtained from the composition to have an optimally high value of the dielectric constant of the resulting layer.

[0034] According to the present invention, preferably, Z of formula (I) X1 is selected from a direct bond, C=O, O, (C=O)2, (C=O)3; n is 0 or 1; R X1 is H or OR X3 and; R X2 is H or OR X3 and; R X3 is H, an unsubstituted or substituted linear alkyl group having 1 to 3 carbon atoms, or Na + , Li + , K. + , Cu + , Ag + , Au + and more preferably, Na. + , Li + , K. + and; Preferably, the compound is an oxocarbonic acid selected from deltaic acid, squaric acid, croconic acid, rhodizonic acid, or heptagonic acid, preferably the oxocarbonic acid is squaric acid or croconynic acid; an oxocarbonic acid derivative, preferably the oxocarbonic acid derivative is 3,4-dihydroxy-3-cyclobutene-1,2-dione (squaric acid diethyl ester); 3,4-dibutoxy-3-cyclobutene-1,2-dione (squaric acid dibutyl ester), croconic acid disodium salt, potassium rhodizonate; maleic anhydride, or any combination thereof.

[0035] 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] During the ceremony, 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 or aromatic hydrocarbon group, each of which is unsubstituted or substituted with fluorine, hydroxy, or alkoxy; In the aliphatic and aromatic hydrocarbon groups, methylene is not replaced or one or more methylenes are replaced by oxy, imino or carbonyl, provided that R Ia is not hydroxy or alkoxy.

[0036] Here, the above methylene also includes terminal methyl. Furthermore, the above "substituted with fluorine, hydroxy or alkoxy" means that a hydrogen atom directly bonded to a carbon atom in an aliphatic hydrocarbon group or an aromatic hydrocarbon group is replaced with fluorine, hydroxy or alkoxy. The same applies to other similar descriptions in this specification.

[0037] In a more preferred embodiment of the present invention, a ), the repeating unit represented by R IaExamples 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 isocyanurate and amino, and (vii) oxygen-containing groups having an epoxy structure such as glycidyl, or an acryloyl structure or methacryloyl structure. Ia R is 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 the solvent and make the cured film less likely to crack.

[0038] 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 repeat unit represented by: [ka] During the ceremony, R Ib is a group obtained by removing multiple hydrogens from a nitrogen-containing and / or oxygen-containing cycloaliphatic hydrocarbon compound having an amino, imino, and / or carbonyl group.

[0039] In formula (Ib), 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 member. For example, R 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.

[0040] 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 repeat unit represented by: [ka]

[0041] Formula (I b ) and formula (I c If the mixing ratio of the repeating unit represented by the formula (I) is high, the compatibility with solvents and additives may decrease, the film stress may increase, and cracks may easily occur. Therefore, the mixing ratio of the repeating unit represented by the formula (I) is preferably 40 mol % or less, more preferably 20 mol % or less, based on the total number of repeating units of the polysiloxane.

[0042] 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 repeat unit represented by: [ka] During the ceremony, R Id are each independently hydrogen, C 1-30 (Preferably, C 1-10 ) linear, C 3-30 (Preferably, C 3-10 ) represents 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, and in the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is either 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 isocyanurate and amino, and (vii) oxygen-containing groups having an epoxy structure such as glycidyl, or an acryloyl structure or methacryloyl structure. Id R is 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 the solvent and make the cured film less likely to crack.

[0043] The above formula (I d ) repeating units, the polysiloxane according to the present invention can have a partially linear structure.

[0044] 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) are preferably 30 mol % or less, more preferably 5 mol % or less, based on the total number of repeating units of the polysiloxane. d ) is not present (0 mol %) in one embodiment of the present invention.

[0045] Polysiloxanes are represented by the chemical formula (I e ) repeating units. [ka] During the ceremony, R Ieis a linear alkyl group having 1 to 5 carbon atoms or a branched alkyl group having 3 to 7 carbon atoms, wherein one or more non-adjacent CH groups of the linear alkyl group or the branched alkyl group can be replaced by C=CH2, C=O, or OH, or the terminal CH3 of the linear alkyl group having 1 to 5 carbon atoms or the branched alkyl group having 3 to 7 carbon atoms can be replaced by C=CH3, and preferably R Ie is a linear alkyl group having 1 to 4 carbon atoms, a branched alkyl group having 3 to 5 carbon atoms, more preferably a branched alkyl group having 3 to 5 carbon atoms. Even more preferably, R Ie is a branched alkyl group having 3 carbon atoms. More preferably, at least one of the CH2 groups of the linear alkyl group having 1 to 5 carbon atoms or the branched alkyl group having 3 to 7 carbon atoms may be replaced by C=CH2, or the terminal CH3 group of the linear alkyl group having 1 to 5 carbon atoms or the branched alkyl group having 3 to 7 carbon atoms may be replaced by C=CH3, and even more preferably, R Ie is C=CH3 or C=CH2-CH3, Most preferably, the compound of formula (I e )teeth; [ka] or [ka] and each ma is independently an integer of 1 to 6, preferably 2 to 5, and more preferably 3.

[0046] It is believed that such acrylic functional group substituted siloxane polymers may provide higher dielectric constants. e Siloxane polymers containing repeating units of formula (I) can provide higher dielectric constants. eAs the siloxane polymer containing the repeating unit of (III), publicly available polymers can be preferably used. For example, siloxane polymers manufactured by Torey Fine Chemical Co., Ltd., siloxane polymers manufactured by Merck Co., Ltd., etc.

[0047] The polysiloxane used in the present invention may contain two or more of the above-mentioned repeating units. For example, RI a is methyl or phenyl a ) and a repeating unit represented by formula (I c and three types of repeating units having the repeating units represented by

[0048] In addition, the polysiloxane used in the composition of the present invention preferably has silanol. Here, the silanol is a silanol in which an OH group is directly bonded to the Si skeleton of the polysiloxane, and is represented by the above formula (I a )~(I d In other words, silanol refers to a compound in which hydroxy is directly bonded to a silicon atom in a polysiloxane containing a repeating unit such as the above formula (l a ) to (I d The silanol content in polysiloxane varies depending on the conditions for synthesizing the polysiloxane, such as the mixing ratio of the monomers and the type of reaction catalyst.

[0049] The silanol content can be quantitatively evaluated by infrared absorption spectroscopy. The absorption band attributed to silanol (SiOH) is 900±100 cm -1 The intensity of this absorption band increases when the silanol content is high.

[0050] It is believed that the high silanol residual siloxane polymer is effective in providing good dispersion of the compound of formula (I) in the composition / resulting film.

[0051] In the present invention, in order to quantitatively evaluate the silanol content, the intensity of the absorption band attributed to Si—O is used as the standard. -1 An absorption band having a peak in this range is adopted as the peak attributed to Si—O. The silanol content can be relatively evaluated by the ratio S2 / S1 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, the ratio S2 / S1 is preferably 0.003 to 0.15, and more preferably 0.01 to 0.10.

[0052] Considering the noise in the infrared absorption spectrum, the integrated intensity of the absorption band is determined. In a typical infrared absorption spectrum of polysiloxane, the band intensity is 900±100 cm -1 and an absorption band assigned to Si-OH with a peak in the range of 1100±100 cm -1 Absorption bands attributable to Si-O, with peaks in the range of 1000 to 10000, are identified. The integrated intensities of these absorption bands can be measured as the region in which the baseline is taken into account, taking noise and other factors into consideration. It is possible for the foot of the absorption band attributable to Si-OH and the foot of the absorption band attributable to Si-O to overlap. In such cases, the wavenumber corresponding to the minimum point between the two absorption bands in the spectrum is set as their boundary. The same applies when the foot of another absorption band overlaps with the foot of an absorption band attributable to Si-OH or Si-O.

[0053] 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 improved the coating properties tend to be. On the other hand, the lower the molecular weight, the easier the synthesis because the synthesis conditions are not limited, and it is difficult to synthesize polysiloxanes with significantly high molecular weights. 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, which can be measured by gel permeation chromatography based on polystyrene.

[0054] As mentioned above, publicly available polysiloxanes that meet the above definition can be preferably used in the embodiments described in WO 2021 / 099236 and EP 3717966.

[0055] solvent In a preferred embodiment of the present invention, the composition can further comprise a solvent to improve handling, coating, and coating of the composition when stringing or producing layers. Alternatively, to provide a solvent-free composition, the composition contains 5 wt. % or less of a solvent based on the total amount of polysiloxane in the composition, and preferably the composition contains no solvent at all.

[0056] Preferably, the solvent is selected from one or more members of the group consisting of propylene glycol monomethyl ether acetate, propylene glycol monomethyl ether, propylene glycol diacetate, diethylene glycol monohexyl ether, and methyl 3-methoxypropionate, methyl isobutyl ketone, and methyl ethyl ketone, and is preferably an amine-type solvent selected from one or more members of the group consisting of N-methylpyrrlidone (NMP), 3-methoxy-N,N-dimethylpropanamide, N,N-dimethylacetamide (DMA), N,N-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), hexamethylphosphoric triamide (HMPA), and acetonitrile, and is more preferably N-methylpyrrolidon (NMP) or 3-methoxy-N,N-dimethylpropanamide.

[0057] 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 lower temperature manufacturing of the layer, and / or provide easy manufacturing.

[0058] The amine-type solvent, preferably an aprotic polar solvent, is preferably selected from one or more members of the group consisting of N-methylpyrrolidone (NMP), 3-methoxy-N,N-dimethylpropanamide, N,N-dimethylacetamide (DMA), N,N-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), hexamethylphosphoric triamide (HMPA), acetonitrile, more preferably N-methylpyrrolidone (NMP) or 3-methoxy-N,N-dimethylpropanamide; it is believed that this can improve the dispersibility of the compound of formula (I) in the polymer composition and / or in the resulting layer.

[0059] Thus, in a preferred embodiment of the present invention, the solvent comprises at least one amine-type solvent selected from one or more members of the group consisting of N-methylpyrrolidone (NMP), 3-methoxy-N,N-dimethylpropanamide, N,N-dimethylacetamide (DMA), N,N-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), hexamethylphosphoric triamide (HMPA), acetonitrile, and preferably the amine-type solvent is N-methylpyrrolidone (NMP) or 3-methoxy-N,N-dimethylpropanamide.

[0060] Preferably, the solvent may further contain another solvent selected from one or more members of the group consisting of propylene glycol monomethyl ether acetate, propylene glycol monomethyl ether, propylene glycol diacetate, diethylene glycol monohexyl ether, and methyl 3-methoxypropionate, methyl isobutyl ketone, methyl ethyl ketone, and γ-butyrolactone.

[0061] 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 weight. When the composition contains a solvent, the amount is preferably 0.1 to 150% by weight, more preferably 10 to 90% by weight.

[0062] 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 members of the group consisting of surfactants, adhesion promoters, silane coupling agents, thermal acid generators, thermal base generators, crosslinking monomers, and polymerization initiators. Preferably, publicly available additives, such as those described in EP 3717966 or WO 2021 / 099236, can be used. Since such additives are not essential to the present invention, the amount of additive in the composition or layer based on the total amount of polysiloxane is preferably 5 wt.% or less, more preferably 1 wt.% or less. The composition and / or layer obtained from the composition may not contain any such additives.

[0063] In another aspect, the present invention further relates to a method for making the composition of the present invention comprising, consisting essentially of, or consisting of at least the following steps: (I x ) polysiloxane; and a compound represented by the following chemical formula (I): The compound is preferably a dielectric constant enhancer preferably used in polysiloxane-containing compositions, [ka] During the ceremony, Z X1 is selected from the group consisting of a direct bond, CH2, C=O, O, (C=O)2, (C=O)O, (C=O)3, (C=O)2O, (C=O)2CH2 and C=O(CH2)2, preferably selected from a direct bond, C=O, O, (C=O)2, (C=O)3; n is 0 or 1; R X1 is H, D, or OR X3 and; R X2 is H, D, or OR X3 and; R X3is H, D, an unsubstituted or substituted linear alkyl group having 1 to 5 carbon atoms, an unsubstituted or substituted branched alkyl group having 3 to 5 carbon atoms, or Na + , Li + , K. + , Rb + , Cs + , Fr + , Cu + , Ag + , Au + , Ti + , Pd + , Ni + , Mn + , Cr + , V + Preferably, the monovalent metal cation is selected from the group consisting of Na + , Li + , K. + , Cu + , Ag + , Au + and more preferably Na + , Li + , K. + is.

[0064] A detailed description of the compounds and polysiloxanes, including preferred amounts, is provided above in the sections ii) Compounds of Formula (I) and i) Polysiloxanes.

[0065] In another aspect, the present invention further relates to a composition obtained or obtainable by the method for producing the composition described above.

[0066] 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, the heating being preferably carried out at a temperature in the range of 60 to 140°C, more preferably in the range of 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 is light having a peak light wavelength in the range of 250 to 450 nm.

[0067] 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 described above. Preferably, the layer is a protective layer for an electronic device. Preferably, the curing is thermal curing and / or UV light curing.

[0068] In another aspect, the present invention further relates to a layer comprising, consisting essentially of, or consisting of at least: i) a polymer made from polysiloxane; and A compound represented by the following chemical formula (I): The compound is preferably a dielectric constant enhancer preferably used in polysiloxane-containing compositions, [ka] During the ceremony, Z X1 is selected from the group consisting of a direct bond, CH2, C=O, O, (C=O)2, (C=O)O, (C=O)3, (C=O)2O, (C=O)2CH2 and C=O(CH2)2, preferably selected from a direct bond, C=O, O, (C=O)2, (C=O)3; n is 0 or 1; R X1 is H, D, or OR X3 and; R X2 is H, D, or OR X3 and; R X3is H, D, an unsubstituted or substituted linear alkyl group having 1 to 5 carbon atoms, an unsubstituted or substituted branched alkyl group having 3 to 5 carbon atoms, or Na + , Li + , K. + , Rb + , Cs + , Fr + , Cu + , Ag + , Au + , Ti + , Pd + , Ni + , Mn + , Cr + , V + Preferably, the monovalent metal cation is selected from the group consisting of Na + , Li + , K. + , Cu + , Ag + , Au + and more preferably Na + , Li + , K. + is.

[0069] A detailed description of the compound of formula (I) and the polysiloxane, including preferred amounts, is provided above in the sections ii) Compound of formula (I) and i) Polysiloxane.

[0070] In a preferred embodiment of the present invention, the dielectric constant (ε r ) is 3.5 or more and 7 or less, the dielectric constant is preferably 3.9 or more and up to 6.5, more preferably 4.0 or more, and the dielectric constant is preferably 6.5 or less, more preferably 6 or less. The dielectric constant is preferably in the range of 3.5 to 7, more preferably 3.6 to 6.5, and even more preferably 4 to 6.

[0071] The dielectric constant (ε r ) is believed to provide improved touch sensitivity of layers such as glass substrates 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 in the composition section above. In a preferred embodiment of the present invention, the haze value of the layer is less than 100%, preferably in the range of 0.01 to 10%, more preferably 0.1 to 5%.

[0072] 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. In particular, the thickness of the sample is 700 μm. Overview of the integrating sphere for transmission and haze measurements, total transmittance (T T )T T =T P +T D , Haze (H) H=T D / T T . Parallel transmittance (T P ) is determined by measuring the light intensity at a point on the sphere opposite the sample, and by measuring the light passing through the sample, the equation T T =T P +T D Using the D ) and T P Total transmittance (T T The degree of light scattering in the sample, i.e., the haze (H) is calculated as H = T D / T T The transmittance and haze are measured.

[0073] In another aspect, the present invention further relates to an electronic device comprising at least the layer of the present invention, preferably the electronic device comprising a light-modulating layer or a light-emitting layer, preferably the layer being disposed on the outermost surface of the electronic device, more preferably on the light-extraction side (viewing side) of the electronic device. Preferably, the electronic device does not comprise a cover glass substrate, and the layer is used in place of the cover glass substrate, achieving a cover glass-free electronic device with good touch sensitivity, preferably with the lowest haze value.

[0074] In another aspect, the present invention further relates to the use of a compound of formula (I) as a dielectric constant enhancer in a polysiloxane-containing composition.

[0075] 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 the electronic device.

[0076] Preferred Embodiments 1. A composition, preferably a protective layer-forming composition, comprising, consisting essentially of, or consisting of at least: i) polysiloxane; and ii) A compound represented by the following chemical formula (I): The compound is preferably a dielectric constant enhancer preferably used in polysiloxane-containing compositions, [ka] During the ceremony, Z X1 is selected from the group consisting of a direct bond, CH2, C=O, O, (C=O)2, (C=O)O, (C=O)3, (C=O)2O, (C=O)2CH2 and C=O(CH2)2, preferably selected from a direct bond, C=O, O, (C=O)2, (C=O)3; n is 0 or 1; R X1 is H, D, or OR X3 and; R X2 is H, D, or OR X3 and; R X3 is H, D, an unsubstituted or substituted linear alkyl group having 1 to 5 carbon atoms, an unsubstituted or substituted branched alkyl group having 3 to 5 carbon atoms, or Na + , Li + , K. + , Rb + , Cs + , Fr+ , Cu + , Ag + , Au + , Ti + , Pd + , Ni + , Mn + , Cr + , V + Preferably, the monovalent metal cation is selected from the group consisting of Na + , Li + , K. + , Cu + , Ag + , Au + and more preferably Na + , Li + , K. + is.

[0077] 2. The composition according to embodiment 1, wherein the molecular weight (Mw) of the compound is 250 or less, preferably in the range of 30 to 250, more preferably 100 to 200.

[0078] 3. The composition according to embodiment 1 or 2, wherein the total amount of the compound of formula (I) based on the total amount of polysilazanes in the composition is in the range of 0.01 to 40% by weight, preferably 0.1 to 20% by weight, more preferably 0.3 to 5.0% by weight.

[0079] 4. Dielectric constant of the solid content of the composition (ε r ) is greater than or equal to 3.5 and less than or equal to 7, the dielectric constant is preferably greater than or equal to 3.9 and up to 6.5, more preferably greater than or equal to 4.0, and the dielectric constant is preferably less than or equal to 6.5, more preferably less than or equal to 6.

[0080] Preferably, 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; Placing an electrode on the composition coated with Ag or Al by sputtering or vapor deposition to form a sample: Attaching a pin prober to the surface of the conductive wafer and the top electrode on the coated composition, respectively, to measure the dielectric constant of the sample. 2) Measurement conditions: The dielectric constant was measured at room temperature using an LCR meter (E4980A, Agilent, Korea / 6440B, Toyo Technical, Japan) by applying a specific frequency range (50-1 MHz) and reading the capacitance displayed on the LCR meter. The dielectric constant was calculated using the following formula: C = K / d (C = capacitance, K = dielectric constant, A = effective electrode area, d = distance between electrodes).

[0081] 5. Z X1 is selected from a direct bond, C=O, O, (C=O)2, (C=O)3; n is 0 or 1; R X1 is H or OR X3 and; R X2 is H or OR X3 and; R X3 is H, an unsubstituted or substituted linear alkyl group having 1 to 3 carbon atoms, or Na + , Li + , K. + , Cu + , Ag + , Au + and more preferably, Na. + , Li + , K. + and; The composition of any one of the preceding embodiments, wherein the compound is an oxocarbonic acid selected from deltaic acid, squaric acid, croconic acid, rhodizonic acid, or heptagonic acid, preferably, the oxocarbonic acid is squaric acid or croconic acid; an oxocarbonic acid derivative, preferably, the oxocarbonic acid derivative is 3,4-dihydroxy-3-cyclobutene-1,2-dione (squaric acid diethyl ester); 3,4-dibutoxy-3-cyclobutene-1,2-dione (squaric acid dibutyl ester), croconic acid disodium salt, potassium rhodizonate; maleic anhydride, or any combination thereof.

[0082] 6. The polysiloxane is represented by the chemical formula (I a ) repeat units. [ka] During the ceremony, 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 or aromatic hydrocarbon group, each of which is unsubstituted or substituted with fluorine, hydroxy, or alkoxy; In the aliphatic and aromatic hydrocarbon groups, methylene is not replaced or one or more methylenes are replaced by oxy, imino or carbonyl, provided that R Ia is not hydroxy or alkoxy.

[0083] 7. The polysiloxane is represented by the chemical formula (I b ) repeat units. [ka] During the ceremony, RIb is a group obtained by removing multiple hydrogens from a nitrogen- and / or oxygen-containing alicyclic hydrocarbon compound having amino, imino, and / or carbonyl groups. 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 from a five- or six-membered ring containing nitrogen as one member. For example, R 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.

[0084] 8. The polysiloxane is represented by the chemical formula (I c ) repeat units. [ka]

[0085] 9. The polysiloxane is represented by the chemical formula (I d ) repeat units. [ka] During the ceremony, R Id are each independently hydrogen, C 1-30 (Preferably, C 1-10 ) linear, C 3-30 (Preferably, C 3-10 ) represents a branched or cyclic, saturated or unsaturated, aliphatic or aromatic hydrocarbon group; The aliphatic hydrocarbon group and the aromatic hydrocarbon group are each unsubstituted or substituted with fluorine, hydroxy, or alkoxy, and in the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is either unsubstituted or substituted with oxy, imido, or carbonyl.

[0086] 10. The polysiloxane is represented by the chemical formula (I e The composition of any one of the preceding embodiments, further comprising a repeat unit of: [ka] During the ceremony, R Ie is a linear alkyl group having 1 to 5 carbon atoms or a branched alkyl group having 3 to 7 carbon atoms, wherein one or more non-adjacent CH groups of the linear alkyl group or the branched alkyl group can be replaced with C=CH2, C=O, or OH, or the terminal CH3 of the linear alkyl group having 1 to 5 carbon atoms or the branched alkyl group having 3 to 7 carbon atoms can be replaced with C=CH3; R Ie is preferably a linear alkyl group having 1 to 4 carbon atoms, a branched alkyl group having 3 to 5 carbon atoms, more preferably a branched alkyl group having 3 to 5 carbon atoms, and even more preferably a branched alkyl group having 3 carbon atoms, More preferably, at least one of the CH2 groups of the linear alkyl group having 1 to 5 carbon atoms or the branched alkyl group having 3 to 7 carbon atoms may be replaced with C=CH2, or the terminal CH3 group of the linear alkyl group having 1 to 5 carbon atoms or the branched alkyl group having 3 to 7 carbon atoms may be replaced with C=CH3, and even more preferably, R Ie is C=CH3 or C=CH2-CH3, Most preferably, the compound of formula (I e )teeth; [ka] or [ka] and each ma is independently an integer of 1 to 6, preferably 2 to 5, and more preferably 3.

[0087] 11. The composition of any one of the preceding embodiments, wherein the composition further comprises an additive.

[0088] 12. The composition of any one of the preceding embodiments, further comprising a solvent, preferably selected from one or more members of the group consisting of propylene glycol monomethyl ether acetate, propylene glycol monomethyl ether, propylene glycol diacetate, diethylene glycol monohexyl ether, and methyl 3-methoxypropionate, methyl isobutyl ketone, methyl ethyl ketone, preferably an amine-type solvent selected from one or more members of the group consisting of N-methylpyrrolidone (NMP), 3-methoxy-N,N-dimethylpropanamide, N,N-dimethylacetamide (DMA), N,N-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), acetonitrile, more preferably N-methylpyrrolidone (NMP) or 3-methoxy-N,N-dimethylpropanamide.

[0089] 13. A method of making a composition according to any one of the preceding embodiments, comprising, consisting essentially of, or consisting of at least the following steps: (I x ) polysiloxane; and a compound represented by the following chemical formula (I): The compound is preferably a dielectric constant enhancer preferably used in polysiloxane-containing compositions, [ka] During the ceremony, Z X1 is selected from the group consisting of a direct bond, CH2, C=O, O, (C=O)2, (C=O)O, (C=O)3, (C=O)2O, (C=O)2CH2 and C=O(CH2)2, preferably selected from a direct bond, C=O, O, (C=O)2, (C=O)3; n is 0 or 1; R X1 is H, D, or ORX3 and; R X2 is H, D, or OR X3 and; R X3 is H, D, an unsubstituted or substituted linear alkyl group having 1 to 5 carbon atoms, an unsubstituted or substituted branched alkyl group having 3 to 5 carbon atoms, or Na + , Li + , K. + , Rb + , Cs + , Fr + , Cu + , Ag + , Au + , Ti + , Pd + , Ni + , Mn + , Cr + , V + The monovalent metal cation is preferably selected from the group consisting of Na + , Li + , K. + , Cu + , Ag + , Au + and more preferably Na + , Li + , K. + is.

[0090] 14. A composition obtained or obtainable by the method according to embodiment 13.

[0091] 15. A method for producing a layer comprising at least the following steps: (I Y ) providing a composition according to any one of embodiments 1 to 12 and 14, 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 to remove the solvent in the composition, the heating being preferably carried out at a temperature in the range of 60 to 140°C, more preferably in the range of 80 to 130°C.

[0092] 16. A layer obtained by curing the composition of any one of embodiments 1 to 12 and 14, or by the method of embodiment 15. Preferably, the layer is a protective layer for an electrical device. Preferably, the curing is thermal curing.

[0093] 17. A layer containing at least the following: i) a polymer made from polysiloxane; and ii) A compound represented by the following chemical formula (I): The compound is preferably a dielectric constant enhancer preferably used in polysiloxane-containing compositions, [ka] During the ceremony, Z X1 is selected from the group consisting of a direct bond, CH2, C=O, O, (C=O)2, (C=O)O, (C=O)3, (C=O)2O, (C=O)2CH2 and C=O(CH2)2, preferably selected from a direct bond, C=O, O, (C=O)2, (C=O)3; n is 0 or 1; R X1 is H, D, or OR X3 and; R X2 is H, D, or OR X3 and; R X3 is H, D, an unsubstituted or substituted linear alkyl group having 1 to 5 carbon atoms, an unsubstituted or substituted branched alkyl group having 3 to 5 carbon atoms, or Na + , Li + , K. + , Rb + , Cs + , Fr + , Cu + , Ag + , Au + , Ti + , Pd + , Ni + , Mn + , Cr + , V +The monovalent metal cation is preferably selected from the group consisting of Na + , Li + , K. + , Cu + , Ag + , Au + and more preferably Na + , Li + , K. + is.

[0094] 18. Dielectric constant of the solid content of the layer (ε r ) is 3.5 or more and 7 or less, the dielectric constant is preferably 3.9 or more and up to 6.5, more preferably 4.0 or more, and the dielectric constant is preferably 6.5 or less, more preferably 6 or less. The dielectric constant is preferably in the range of 3.5 to 7, more preferably 3.6 to 6.5, even more preferably 4 to 6.

[0095] 19. The layer of any one of embodiments 16 to 18, wherein the haze value of the layer is less than 100%, preferably in the range of 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). Overview of the integrating sphere for transmission and haze measurements, total transmittance (T T )T T =T P +T D , Haze (H) H=T D / T T . Parallel transmittance (T P ) is determined by measuring the light intensity at a point on the sphere opposite the sample, and by measuring the light passing through the sample, the equation T T =T P +T D Using the D ) and T P Total transmittance (T TThe degree of light scattering in the sample, i.e., the haze (H) is calculated as H = T D / T T The transmittance and haze are measured.

[0096] 20. The electronic device preferably comprises a light-modulating layer or a light-emitting layer, the layer preferably being disposed on the outermost surface of the electronic device, more preferably on the light extraction side (viewing side) of the electronic device, comprising at least one layer according to any one of embodiments 16 to 19.

[0097] 21. Use of a compound of formula (I) as a dielectric constant enhancer in a polysiloxane-containing composition.

[0098] 22. A method of using the composition described in any one of embodiments 1 to 12 and 14 as a composition for forming a protective layer of an electronic device, preferably using the composition in place of the upper glass substrate of the electronic device.

[0099] Technical effects of the invention: The present invention provides one or more of the following technical advantages: To obtain a polysiloxane-containing composition, preferably a protective layer-forming composition, which exhibits an improved dielectric constant, such as for a glass substrate of an electronic device, and preferably has minimal haze characteristics; to obtain a layer or cured composition, which exhibits an improved dielectric constant, such as for a glass substrate of an electronic device, and preferably has minimal haze characteristics; to obtain a polysiloxane-containing composition, preferably a protective layer-forming composition, which allows for good dispersion of a sufficient amount of thiol in the composition; to obtain a layer or cured composition, which allows for good dispersion of a sufficient amount of thiol in the layer or cured composition; to obtain a polysiloxane-containing composition, preferably a protective layer-forming composition, which allows for the formation of a layer or cured composition in a mild or lower temperature process, and which allows for smooth coating of the polysiloxane-containing composition on any substrate, i.e., PET, CPI, COP, or polarizer. [Example]

[0100] The following examples provide an explanation of the present invention as well as detailed descriptions of their preparation, but the present invention is not limited to these examples.

[0101] Example 1: Mixed sample preparation A polysiloxane polymer manufactured by Merck, represented by the following chemical formula, was mixed with 0.5 wt% (Sample 1-1), 1 wt% (Sample 1-2), and 2 wt% (Sample 1-3) of squaric acid as the compound of Formula (I) based on the total weight of the polysiloxane, in the presence of a mixture of propylene glycol monomethyl ether acetate and NMP (N-methylpyrrolidone) (total weight of the siloxane polymer and the compound of Formula (I):solvent mixture = 3:7). After mixing, the above compounds were separately coated on an Al-deposited silicon wafer by spin coating to obtain the samples. The solvent mixture was then evaporated in a curing process at 120 °C to obtain Samples 1-1 (0.5 wt% squaric acid), 1-2 (1 wt% squaric acid), and 1-3 (2 wt% squaric acid). [ka]

[0102] Examples 2 to 4: Mixed sample preparation Examples 2 to 4 were carried out in the same manner as in Example 1, except that the compounds described below were used instead of squaric acid. Then, in each example, samples containing 0.5 wt% of the compound (Samples 2-1, 3-1, and 4-1), 1 wt% of the compound (Samples 2-2, 3-2, and 4-2), and 2 wt% of the compound (Samples 2-3, 3-3, and 4-3) were obtained.

[0103] Compounds of formula (I) used in Examples 1 to 4 Comparative Example 1: A non-thiol containing compound is used. Example 1: Squaric acid. Example 2: 3,4-Dihydroxy-3-cyclobutene-1,2-dione. Example 3: Croconic acid. Example 4: Maleic anhydride.

[0104] Comparative Example 1: Reference sample preparation. The reference sample is prepared in the same manner as in Example 1, except that the compound of formula (I) is not added / mixed into the siloxane polymer, and the following polymer is used as the siloxane polymer: Reference Sample 1 is then obtained. [ka]

[0105] Comparative Example 2: Reference sample preparation. A reference sample is prepared in the same manner as described in Example 1, except that no compound of formula (I) is added / mixed to the siloxane polymer. Reference sample 2 is then obtained.

[0106] Example 5: Measurement of the dielectric constants of the samples of Examples 1 to 4 and Comparative Example 1. The dielectric constant was measured at room temperature using an LCR meter (E4980A, Agilent, Korea / 6440B, Toyo Technical, Japan) by applying a specific frequency range (50-1 MHz) and reading the capacitance displayed on the LCR meter. The dielectric constant was calculated using the following formula: C = K A / d (C = capacitance, K = dielectric constant, A = effective area of ​​the electrodes, d = distance between the electrodes).

[0107] Table 1 below shows the measurement results. [Table 1]

[0108] As shown in Table 1 above, the compounds of formula (I), preferably those used in Samples 1-4, dramatically increase the dielectric constant of the polysiloxane composition, which is believed to be beneficial for the touch sensitivity of glass-free electronic devices, such as the touch-glass-free OLED concept.

Claims

1. The composition, preferably a protective layer-forming composition, comprises at least: i) a polysiloxane; ii) a compound represented by the following chemical formula (I): and preferably, the compound is a dielectric constant enhancer preferably used in polysiloxane-containing compositions, 【Chemical 1】 During the ceremony, Z Ｘ１ is a direct bond, CH ２ , C=O, O, (C=O) ２ , (C=O)O, (C=O) ３ , (C=O) ２ O, (C=O) ２ CH ２ and C=O(CH ２ ) ２ and preferably a direct bond, C=O, O, (C=O) ２ , (C=O) ３ Selected from: n is 0 or 1; R Ｘ１ is H, D, or OR Ｘ３ and R Ｘ２ is H, D, or OR Ｘ３ and R Ｘ３ is H, D, an unsubstituted or substituted linear alkyl group having 1 to 5 carbon atoms, an unsubstituted or substituted branched alkyl group having 3 to 5 carbon atoms, or Na ＋ , Li ＋ , K. ＋ , Rb ＋ , Cs ＋ , Fr ＋ , Cu ＋ , Ag ＋ , Au ＋ , Ti ＋ , Pd ＋ , Ni ＋ , Mn ＋ , Cr ＋ , V ＋ and the monovalent metal cation is preferably selected from the group consisting of Na ＋ , Li ＋ , K. ＋ , Cu ＋ , Ag ＋ , Au ＋ and more preferably Na ＋ , Li ＋ , K. ＋ The composition.

2. 2. The composition of claim 1, wherein the molecular weight (Mw) of the compound is 250 or less.

3. 3. The composition according to claim 1, wherein the total amount of said compounds based on the total amount of polysilazanes in said composition is in the range of 0.01 to 40% by weight.

4. The dielectric constant (ε ｒ 4. The composition according to claim 1, wherein the dielectric constant is preferably 3.9 or more and up to 6.5, more preferably 4.0 or more, and the dielectric constant is preferably 6.5 or less, more preferably 6 or less.

5. Z Ｘ１ is a direct bond, C=O, O, (C=O) ２ , (C=O) ３ Selected from: n is 0 or 1; R Ｘ１ is H or OR Ｘ３ and R Ｘ２ is H or OR Ｘ３ and R Ｘ３ is H, an unsubstituted or substituted linear alkyl group having 1 to 3 carbon atoms, or Na ＋ , Li ＋ , K. ＋ , Cu ＋ , Ag ＋ , Au ＋ and more preferably, Na. ＋ , Li ＋ , K. ＋ and The composition of any one of claims 1 to 4, wherein the compound is an oxocarbonic acid selected from deltaic acid, squaric acid, croconic acid, rhodizonic acid or heptagonic acid, preferably the oxocarbonic acid is squaric acid or croconic acid; an oxocarbonic acid derivative, preferably the oxocarbonic acid derivative is 3,4-dihydroxy-3-cyclobutene-1,2-dione (squaric acid diethyl ester); 3,4-dibutoxy-3-cyclobutene-1,2-dione (squaric acid dibutyl ester), croconic acid disodium salt, potassium rhodizonate; maleic anhydride, or any combination thereof.

6. The polysiloxane has the chemical formula (I) ａ ) repeating units, 【Chemistry 2】 During the ceremony, 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 replaced or one or more methylenes are replaced by oxy, imino or carbonyl, provided that R Ｉａ The composition of any one of claims 1 to 5, wherein is not hydroxy or alkoxy.

7. The polysiloxane has the chemical formula (I) ｂ ) repeating units, 【Chemistry 3】 During the ceremony, R Ｉｂ is a group obtained by removing multiple hydrogen atoms from a nitrogen-containing and / or oxygen-containing cycloaliphatic hydrocarbon compound having amino, imino, and / or carbonyl groups, R Ｉｂ is preferably a group obtained by removing a plurality of hydrogen atoms, preferably two or three hydrogen atoms, from a nitrogen-containing aliphatic hydrocarbon ring having an imino and / or carbonyl group, more preferably from a five- or six-membered ring containing nitrogen as a member, for example, a group obtained by removing two or three hydrogen atoms from piperidine, pyrrolidine or isocyanurate, and R Ｉｂ The composition according to any one of claims 1 to 6, wherein connects Si atoms contained in a plurality of repeating units together.

8. The composition of any one of claims 1 to 7, further comprising a solvent.

9. A method for producing the composition according to any one of claims 1 to 8, comprising at least (I ｘ ) polysiloxane; a compound represented by the following chemical formula (I); wherein the compound is a dielectric constant enhancer preferably used in polysiloxane-containing compositions; 【Chemistry 4】 During the ceremony, Z Ｘ１ is a direct bond, CH ２ , C=O, O, (C=O) ２ , (C=O)O, (C=O) ３ , (C=O) ２ O, (C=O) ２ CH ２ and C=O(CH ２ ) ２ and preferably a direct bond, C=O, O, (C=O) ２ , (C=O) ３ Selected from: n is 0 or 1; R Ｘ１ is H, D, or OR Ｘ３ and R Ｘ２ is H, D, or OR Ｘ３ and R Ｘ３ is H, D, an unsubstituted or substituted linear alkyl group having 1 to 5 carbon atoms, an unsubstituted or substituted branched alkyl group having 3 to 5 carbon atoms, or Na ＋ , Li ＋ , K. ＋ , Rb ＋ , Cs ＋ , Fr ＋ , Cu ＋ , Ag ＋ , Au ＋ , Ti ＋ , Pd ＋ , Ni ＋ , Mn ＋ , Cr ＋ , V ＋ and the monovalent metal cation is preferably selected from the group consisting of Na ＋ , Li ＋ , K. ＋ , Cu ＋ , Ag ＋ , Au ＋ and more preferably Na ＋ , Li ＋ , K. ＋ That's the method.

10. A method for producing a layer, comprising at least: (I Ｙ 10.) Providing a composition according to any one of claims 1 to 8; (II Ｙ ) heating the provided composition to form a layer, preferably to remove solvent in the composition, the heating being preferably carried out at a temperature in the range of 60 to 140°C, more preferably in the range of 80 to 130°C; A method comprising:

11. A layer obtained from a composition according to any one of claims 1 to 8 by curing, or a layer obtained by the method according to claim 10.

12. at least; i) a polymer made from polysiloxane; ii) a compound represented by the following chemical formula (I): wherein preferably said compound is a dielectric constant enhancer preferably used in polysiloxane-containing compositions, 【Chemistry 5】 During the ceremony, Z Ｘ１ is a direct bond, CH ２ , C=O, O, (C=O) ２ , (C=O)O, (C=O) ３ , (C=O) ２ O, (C=O) ２ CH ２ and C=O(CH ２ ) ２ and preferably a direct bond, C=O, O, (C=O) ２ , (C=O) ３ Selected from: n is 0 or 1; R Ｘ１ is H, D, or OR Ｘ３ and R Ｘ２ is H, D, or OR Ｘ３ and R Ｘ３ is H, D, an unsubstituted or substituted linear alkyl group having 1 to 5 carbon atoms, an unsubstituted or substituted branched alkyl group having 3 to 5 carbon atoms, or Na ＋ , Li ＋ , K. ＋ , Rb ＋ , Cs ＋ , Fr ＋ , Cu ＋ , Ag ＋ , Au ＋ , Ti ＋ , Pd ＋ , Ni ＋ , Mn ＋ , Cr ＋ , V ＋ and the monovalent metal cation is preferably selected from the group consisting of Na ＋ , Li ＋ , K. ＋ , Cu ＋ , Ag ＋ , Au ＋ and more preferably Na ＋ , Li ＋ , K. ＋ That is, layer.

13. The dielectric constant (ε ｒ 13. The layer according to claim 11 or 12, wherein the dielectric constant is ≧3.5 and ≦7, said dielectric constant is preferably ≧3.9 and up to 6.5, more preferably ≧4.0, said dielectric constant is preferably ≦6.5, more preferably ≦6, said dielectric constant is preferably in the range of 3.5 to 7, more preferably 3.6 to 6.5, even more preferably 4 to 6.

14. The layer according to any one of claims 11 to 13, wherein the haze value of said layer is less than 100%.

15. An electronic device comprising at least a layer according to any one of claims 11 to 14.

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