Ionomer, composition, compact, glass laminate interlayer and glass laminate

Abstract

To provide an ionomer with improved performance balance of optical characteristics and moldability, a composition containing the ionomer, a compact obtained by molding the composition, a glass laminate interlayer, and a glass laminate.SOLUTION: An ionomer of an ethylene-unsaturated carboxylic acid copolymer satisfying the following requirements (i) to (iii). (i) When the total amount of structural units constituting the ethylene-unsaturated carboxylic acid copolymer is 100% by mass, the content of structural units derived from the unsaturated carboxylic acid is 17.0% by mass or more but less than 21.0% by mass. (ii) The degree of neutralization of the ionomer of the ethylene-unsaturated carboxylic acid copolymer is 35% or more and 50% or less. (iii) According to JIS K 7210:1999, the melt mass flow rate of the ethylene-unsaturated carboxylic acid copolymer before neutralization, measured under conditions of 190°C and a load of 2160 g, is 60 g / 10 min or more and 300 g / 10 min or less.SELECTED DRAWING: None

Description

[Technical Field]

[0001] The present invention relates to an ionomer, a composition, a molded article, a laminated glass interlayer, and a laminated glass. [Background technology]

[0002] Ionomer resins are ionic polymers in which a small amount of ionic groups have been introduced into the base polymer. Among ionomer resins, ethylene-based ionomer resins, which use ethylene-unsaturated carboxylic acid copolymers as the base polymer, are widely used as industrial and packaging materials.

[0003] Patent Document 1 discloses an ethylene acid copolymer resin composition for use in the production of transparent laminate articles, wherein (i) the composition consists essentially of 70 to 79 weight percent ethylene and 21 to 30 weight percent carboxylic acid monomers selected from the group consisting of α,β-unsaturated acids having 3 to 8 carbon atoms, in which 20 to 35% of the acid groups are neutralized, and (ii) the resin has a melt index of less than 55 g / 10 min before neutralization. It also discloses that the resin composition has improved adhesion, impact resistance, and toughness, as well as excellent optical transparency.

[0004] Patent Document 2 discloses a resin composition for laminated glass interlayer films used to form laminated glass interlayer films, the resin composition for laminated glass interlayer films containing an ionomer (A) of an ethylene-unsaturated carboxylic acid copolymer and an inorganic filler (B), wherein the inorganic filler (B) has a volume-based cumulative 10% diameter (D10) of 0.1 μm or more and 10 μm or less as measured by a laser diffraction scattering method. It also discloses that the resin composition for laminated glass interlayer films can provide a resin composition for laminated glass interlayer films with improved optical properties and adhesion to glass.

[0005] Patent Document 3 discloses a resin composition for use in forming a laminated glass interlayer, the resin composition comprising an ionomer (A) of an ethylene-unsaturated carboxylic acid copolymer and a silane coupling agent (B) having an amino group, wherein the metal ions constituting the ionomer (A) of the ethylene-unsaturated carboxylic acid copolymer include monovalent metal ions and polyvalent metal ions. It is described that this resin composition for a laminated glass interlayer can provide a resin composition for a glass interlayer that can improve optical properties and water resistance in a balanced manner and has improved adhesion to glass and the like. [Prior art documents] [Patent documents]

[0006] [Patent Document 1] Special Publication No. 2008-519104 [Patent Document 2] International Publication No. 2020 / 189335 [Patent Document 3] International Publication No. 2018 / 043236 Summary of the Invention [Problem to be solved by the invention]

[0007] The present invention provides an ionomer having an improved balance of optical properties and moldability, a composition containing the ionomer, and a molded article, laminated glass interlayer film, and laminated glass obtained by molding the composition. [Means for solving the problem]

[0008] The present inventors have found that, in an ionomer of an ethylene-unsaturated carboxylic acid copolymer, by adjusting the content of unsaturated carboxylic acid in the ethylene-unsaturated carboxylic acid copolymer, the degree of neutralization of the ionomer of the ethylene-unsaturated carboxylic acid copolymer, and the melt mass-flow rate of the ethylene-unsaturated carboxylic acid copolymer before neutralization within predetermined ranges, it is possible to provide an ionomer with an improved balance of optical properties and formability, a composition containing the ionomer, and a molded article, laminated glass interlayer film, and laminated glass obtained by molding the composition.

[0009] The present invention provides the following ionomer, composition, molded article, laminated glass interlayer film, and laminated glass.

[0010] [1] An ionomer of an ethylene-unsaturated carboxylic acid copolymer that satisfies the following requirements (i) to (iii): (i) When the total amount of structural units constituting the ethylene-unsaturated carboxylic acid copolymer is taken as 100% by mass, the content of structural units derived from unsaturated carboxylic acid is 17.0% by mass or more and less than 21.0% by mass. (ii) The degree of neutralization of the ionomer of the ethylene-unsaturated carboxylic acid copolymer is 35% or more and 50% or less. (iii) The melt mass flow rate of the ethylene-unsaturated carboxylic acid copolymer before neutralization, measured in accordance with JIS K 7210:1999 at 190°C under a load of 2160 g, is 60 g / 10 min or more and 300 g / 10 min or less. [2] [1] The ionomer according to [1], wherein the melt mass flow rate of the ionomer of the ethylene-unsaturated carboxylic acid copolymer after neutralization is 1.0 g / 10 min or more, as measured in accordance with JIS K 7210:1999 under conditions of 190°C and a load of 2160 g. [3] The ionomer according to [1] or [2], wherein the metal ions constituting the ionomer of the ethylene-unsaturated carboxylic acid copolymer include one or more ions selected from the group consisting of sodium ions, lithium ions, potassium ions, silver ions, mercury ions, calcium ions, magnesium ions, zinc ions, aluminum ions, barium ions, beryllium ions, strontium ions, copper ions, cadmium ions, tin ions, lead ions, iron ions, cobalt ions, and nickel ions. [4] A composition comprising an ionomer of the ethylene-unsaturated carboxylic acid copolymer according to any one of [1] to [3]. [5] The composition according to [4], further comprising a silane coupling agent. [6] A molded article obtained by molding the composition according to [4] or [5]. [7] [4] or [5]. A laminated glass interlayer film comprising the composition according to [4] or [5]. [8] [7] A laminated glass comprising the laminated glass interlayer film according to [7] and transparent plate-like members provided on both sides of the laminated glass interlayer film. [Effects of the Invention]

[0011] The present invention can provide an ionomer having an improved balance of optical properties and moldability, a composition containing the ionomer, and a molded article, laminated glass interlayer film, and laminated glass obtained by molding the composition. DETAILED DESCRIPTION OF THE INVENTION

[0012] DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS Hereinafter, embodiments of the present invention will be described with reference to the accompanying drawings. In this specification, "A to B" indicating a range of values ​​means A or more and B or less unless otherwise specified.

[0013] <Ionomer of ethylene-unsaturated carboxylic acid copolymer> The ionomer of the ethylene-unsaturated carboxylic acid copolymer of this embodiment satisfies the following requirements (i) to (iii). (i) When the total amount of structural units constituting the ethylene-unsaturated carboxylic acid copolymer is taken as 100% by mass, the content of structural units derived from unsaturated carboxylic acid is 17.0% by mass or more and less than 21.0% by mass. (ii) The degree of neutralization of the ionomer of the ethylene-unsaturated carboxylic acid copolymer is 35% or more and 50% or less. (iii) The melt mass flow rate of the ethylene-unsaturated carboxylic acid copolymer before neutralization, measured in accordance with JIS K 7210:1999 at 190°C under a load of 2160 g, is 60 g / 10 min or more and 300 g / 10 min or less.

[0014] Ionomers, which are copolymers of ethylene and unsaturated carboxylic acids, exhibit unique solid and melt properties not found in base polymers, and are therefore used in laminated glass interlayers, cosmetic containers, golf ball covers, food packaging, etc. In particular, for applications requiring high aesthetics and design, such as laminated glass interlayers and cosmetic containers, excellent transparency and formability are required.

[0015] The mechanism by which the ionomer of the ethylene-unsaturated carboxylic acid copolymer of this embodiment can improve the balance of optical properties such as transparency and moldability is believed to be as follows. Ionomers of ethylene-unsaturated carboxylic acid copolymers have a three-phase structure consisting of a crystalline polyethylene phase, an amorphous phase, and ionic associates, and the more the crystal growth of polyethylene is suppressed, the more transparent they become. Here, it is believed that by increasing the content of unsaturated carboxylic acid in the ethylene-unsaturated carboxylic acid copolymer to a predetermined value or more and by increasing the degree of neutralization of the ionomer of ethylene-unsaturated carboxylic acid copolymer to a predetermined value or more, the crystal growth of polyethylene can be suppressed, thereby improving transparency. On the other hand, when an ethylene-unsaturated carboxylic acid copolymer with a certain level of unsaturated carboxylic acid is neutralized with metal ions to form an ionomer, the fluidity of the ionomer deteriorates and its moldability deteriorates. However, we have found that by increasing the melt mass-flow rate of the ethylene-unsaturated carboxylic acid copolymer before neutralization to a certain level, the fluidity of the ionomer after neutralization can be improved, thereby improving its moldability.

[0016] Regarding requirement (i), when the total amount of constituent units constituting the ethylene-unsaturated carboxylic acid copolymer in the ionomer of the ethylene-unsaturated carboxylic acid copolymer of the present embodiment is taken as 100 mass%, the content of constituent units derived from unsaturated carboxylic acid is 17.0 mass% or more and less than 21.0 mass%, and preferably 17.5 mass% or more and 20.5 mass% or less. When the content of unsaturated carboxylic acid-derived structural units in the ionomer of ethylene-unsaturated carboxylic acid copolymer is equal to or greater than the above lower limit, transparency can be improved. On the other hand, when the content of unsaturated carboxylic acid-derived structural units in the ionomer of ethylene-unsaturated carboxylic acid copolymer is equal to or less than the above upper limit, the balance of performance such as heat resistance, mechanical strength, water resistance, and processability can be further improved.

[0017] In the ionomer of the ethylene-unsaturated carboxylic acid copolymer of the present embodiment, when the total amount of structural units constituting the ethylene-unsaturated carboxylic acid copolymer is taken as 100% by mass, the content of structural units derived from ethylene is preferably more than 79.0% by mass and not more than 83.0% by mass, more preferably 79.5% by mass or more and 82.5% by mass or less, from the viewpoint of further improving the balance of performance such as heat resistance, mechanical strength, water resistance, processability, and productivity.

[0018] The ionomer of the ethylene-unsaturated carboxylic acid copolymer may contain other copolymerizable monomers in addition to ethylene and unsaturated carboxylic acid. Other copolymerizable monomers include unsaturated esters, for example, vinyl esters such as vinyl acetate and vinyl propionate; and (meth)acrylic acid esters such as methyl (meth)acrylate, ethyl (meth)acrylate, isobutyl (meth)acrylate, n-butyl (meth)acrylate, and 2-ethylhexyl (meth)acrylate. In order to further improve flexibility and optical properties, the content of structural units derived from other copolymerizable monomers in the ionomer of the ethylene-unsaturated carboxylic acid copolymer is preferably from 0 to 30% by mass, more preferably from 0 to 25% by mass, when the total amount of structural units constituting the ethylene-unsaturated carboxylic acid copolymer is taken as 100% by mass.

[0019] Here, the content of ethylene-derived structural units, the content of unsaturated carboxylic acid-derived structural units, and the content of other copolymerizable monomer-derived structural units in the ionomer of an ethylene-unsaturated carboxylic acid copolymer can be measured, for example, by Fourier transform infrared absorption spectroscopy (FT-IR).

[0020] Regarding the requirement (ii), the degree of neutralization of the ionomer in the ethylene-unsaturated carboxylic acid copolymer of the present embodiment is 35% or more and 50% or less, and preferably 38% or more and 48% or less. When the degree of neutralization of the ionomer of the ethylene-unsaturated carboxylic acid copolymer is equal to or greater than the above lower limit, the optical properties are improved, and when the degree of neutralization of the ionomer of the unsaturated carboxylic acid copolymer is equal to or less than the above upper limit, the moldability is improved. The degree of neutralization of an ionomer of an ethylene-unsaturated carboxylic acid copolymer is the ratio (mol%) of the number of moles of carboxyl groups neutralized by metal ions to the total number of moles of carboxyl groups contained in the ethylene-unsaturated carboxylic acid copolymer. The degree of neutralization of an ionomer of an ethylene-unsaturated carboxylic acid copolymer can be measured, for example, by incineration residue analysis.

[0021] Regarding requirement (iii), the melt mass flow rate (MFR) of the ethylene-unsaturated carboxylic acid copolymer before neutralization is 60 g / 10 min or more and 300 g / 10 min or less, preferably 70 g / 10 min or more and 250 g / 10 min or less, more preferably 80 g / 10 min or more and 200 g / 10 min or less, and even more preferably 90 g / 10 min or more and 180 g / 10 min or less. The ethylene-unsaturated carboxylic acid copolymer before neutralization refers to the ethylene-unsaturated carboxylic acid copolymer before it is neutralized to form an ionomer of the ethylene-unsaturated carboxylic acid copolymer.

[0022] By ensuring that the melt mass flow rate of the ethylene-unsaturated carboxylic acid copolymer before neutralization is equal to or greater than the above lower limit, the melt mass flow rate of the ionomer of the ethylene-unsaturated carboxylic acid copolymer described below can be improved, thereby improving the moldability and processing stability of the ionomer. Here, in order to improve the fluidity and formability of the ionomer of the ethylene-unsaturated carboxylic acid copolymer, it is conceivable to increase the molding temperature during molding. On the other hand, when the ionomer of the ethylene-unsaturated carboxylic acid copolymer of this embodiment is used in a laminated glass interlayer, a silane coupling agent may be blended, as described below, to further improve adhesion to the glass. However, if the molding temperature is too high, the silane coupling agent may react during molding, which poses a problem when the molding temperature is too high. As described above, by setting the melt mass flow rate of the ethylene-unsaturated carboxylic acid copolymer before neutralization to the above-mentioned lower limit or higher, the formability of the ionomer can be improved even when the molding temperature is within a moderate range. Furthermore, by ensuring that the melt mass flow rate of the ethylene-unsaturated carboxylic acid copolymer before neutralization is equal to or less than the above upper limit, the performance balance of the ionomer of the ethylene-unsaturated carboxylic acid copolymer, such as heat resistance and mechanical strength, can be improved. The melt mass flow rate of the ethylene-unsaturated carboxylic acid copolymer before neutralization is measured in accordance with JIS K 7210:1999 under conditions of 190°C and a load of 2160 g.

[0023] The melt mass flow rate (MFR) of the ionomer of the ethylene-unsaturated carboxylic acid copolymer after neutralization according to the present embodiment is preferably 1.0 g / 10 min or more and 10.0 g / 10 min or less, more preferably 1.3 g / 10 min or more and 8.0 g / 10 min or less, even more preferably 1.5 g / 10 min or more and 6.0 g / 10 min or less, and still more preferably 1.7 g / 10 min or more and 5.5 g / 10 min or less. When the melt mass flow rate of the ionomer of the ethylene-unsaturated carboxylic acid copolymer after neutralization is equal to or greater than the above lower limit, the performance balance of moldability and processing stability can be improved, and when the melt mass flow rate of the ionomer of the ethylene-unsaturated carboxylic acid copolymer after neutralization is equal to or less than the above upper limit, the performance balance of heat resistance, mechanical strength, etc. can be further improved. The melt mass flow rate (MFR) of the ionomer of the neutralized ethylene-unsaturated carboxylic acid copolymer is measured in accordance with JIS K 7210:1999 under the conditions of 190°C and a load of 2160g.

[0024] The density of the ionomer of the ethylene-unsaturated carboxylic acid copolymer of this embodiment is preferably 900 kg / m from the viewpoint of further improving the balance of mechanical strength and processability. 3 More than 980kg / m 3 Less than or equal to 910 kg / m 3 More than 970kg / m 3 or less, more preferably 920 kg / m 3 More than 970kg / m 3 or less, more preferably 930 kg / m 3 More than 960kg / m 3 The following is the result. The density of the ionomer of ethylene-unsaturated carboxylic acid copolymer is measured in accordance with JIS K 7112:1999.

[0025] The metal ions constituting the ionomer of ethylene-unsaturated carboxylic acid copolymer are preferably one or more selected from the group consisting of sodium ions, lithium ions, potassium ions, silver ions, mercury ions, calcium ions, magnesium ions, zinc ions, aluminum ions, barium ions, beryllium ions, strontium ions, copper ions, cadmium ions, tin ions, lead ions, iron ions, cobalt ions, and nickel ions. From the viewpoint of easier availability of industrially produced products, the metal ions are more preferably one or more selected from the group consisting of sodium ions, lithium ions, potassium ions, calcium ions, magnesium ions, zinc ions, aluminum ions, and barium ions. From the viewpoint of further improving transparency, the metal ions are even more preferably one or more selected from the group consisting of sodium ions, potassium ions, magnesium ions, and zinc ions. These metal ions may be used alone or in combination.

[0026] In addition to the above metal ions, the ionomer of the ethylene-unsaturated carboxylic acid copolymer may also contain amino compounds such as ammonia, methylamine, dimethylamine, trimethylamine, ethylamine, diethylamine, triethylamine, ethylenediamine, diethylenetriamine, triethylenetetramine, and 1,3-dimethylaminocyclohexane.

[0027] The method for producing the ethylene-unsaturated carboxylic acid copolymer of this embodiment is not particularly limited, and it can be produced by a known method. For example, it can be obtained by radical copolymerization of each polymerization component under high temperature and high pressure. Furthermore, an ionomer of the ethylene-unsaturated carboxylic acid copolymer of this embodiment can be obtained by reacting the ethylene-unsaturated carboxylic acid copolymer with a metal compound. Furthermore, commercially available ionomers of the ethylene-unsaturated carboxylic acid copolymer may be used.

[0028] <Composition> The composition of the present embodiment contains an ionomer of the ethylene-unsaturated carboxylic acid copolymer of the present embodiment. In the composition of the present embodiment, the content of the ionomer of the ethylene-unsaturated carboxylic acid copolymer is preferably 70% by mass or more and 100.0% by mass or less, more preferably 80% by mass or more and 99.9% by mass or less, and even more preferably 90% by mass or more and 99.9% by mass or less, when the entire composition is taken as 100% by mass.

[0029] The composition of the present embodiment preferably further contains a silane coupling agent, which can further improve film-forming properties and adhesiveness. Examples of silane coupling agents include alkoxysilanes having an amino group, a glycidyl group, or an epoxy group. More specifically, examples include γ-glycidoxypropyltrimethoxysilane, 3-glycidoxypropylmethyldimethoxysilane, 3-glycidoxypropylmethyldiethoxysilane, N-2-(aminoethyl)-3-aminopropylmethyldimethoxysilane, N-2(aminoethyl)3-aminopropyltrimethoxysilane, N-2(aminoethyl)3-aminopropylmethyldiethoxysilane, 3-aminopropyltrimethoxysilane, 3-aminopropyltriethoxysilane, N-phenyl-3-aminopropyltrimethoxysilane, and N-phenyl-3-aminopropyltriethoxysilane. These silane coupling agents may be used alone or in combination of two or more. Among these, when the composition of the present embodiment is used for a laminated glass interlayer film, from the viewpoints of achieving a better balance of optical properties, water resistance, and adhesion to glass, and stabilizing film-formability during sheet processing, silane coupling agents having an amino group, a glycidyl group, or an epoxy group are preferred, and silane coupling agents having an amino group are more preferred. In the composition of this embodiment, when the composition of this embodiment is used as an interlayer film for laminated glass, the content of the silane coupling agent is preferably from 0.001 to 5% by mass, more preferably from 0.005 to 2% by mass, and even more preferably from 0.01 to 1% by mass, based on 100% by mass of the entire composition, from the viewpoint of achieving a better balance of optical properties, water resistance, and adhesion to glass.

[0030] The composition of this embodiment may contain various additives within the scope of the present invention. The various additives are not particularly limited, but examples thereof include plasticizers, antioxidants, ultraviolet absorbers, wavelength conversion agents, antistatic agents, surfactants, colorants, light stabilizers, foaming agents, lubricants, crystal nucleating agents, crystallization accelerators, crystallization retarders, catalyst deactivators, heat absorbers, heat reflectors, heat dissipation agents, thermoplastic resins other than ionomers of ethylene-unsaturated carboxylic acid copolymers, thermosetting resins, inorganic fillers, organic fillers, impact modifiers, slip agents, crosslinking agents, crosslinking aids, tackifiers, processing aids, mold release agents, hydrolysis inhibitors, heat stabilizers, antiblocking agents, antifogging agents, flame retardants, flame retardant aids, light diffusing agents, antibacterial agents, antifungal agents, dispersants, and other resins. The various additives may be used alone or in combination of two or more.

[0031] <Molded body> The molded article of the present embodiment can be obtained by molding the composition of the present embodiment. The molding method is not limited, and known molding methods such as extrusion molding, injection molding, compression molding, and blow molding can be used, and the molded article can be obtained by molding into various shapes such as a sheet shape, a film shape, a plate shape, and other three-dimensional shapes. The molded article of this embodiment may be made solely of the composition of this embodiment, or may be made of the composition of this embodiment and other components. The molded article of this embodiment may be a part or the whole of a member.

[0032] Furthermore, the surface of the molded article of this embodiment may be subjected to a flame treatment, a corona treatment, a plasma treatment, a hard coat treatment with an inorganic or organic compound, an antistatic treatment, an antireflection treatment, an electromagnetic shielding treatment, etc., within the scope of not impairing the effects of the present invention. These treatments can be performed on the surface of the molded article by vapor deposition, sputtering, dipping, thermal transfer, etc.

[0033] The molded article of the present embodiment is not particularly limited, and can be used in a wide range of fields, such as optical materials, electronic components, various mechanical components, foams, sheets, films, pipes, tubes, toys, and daily necessities.

[0034] <Laminated glass interlayer film> The laminated glass interlayer film of this embodiment is composed of the composition of this embodiment, and specifically includes a layer composed of the composition of this embodiment. The laminated glass interlayer film of this embodiment may have a single-layer structure or a multi-layer structure of two or more layers. More specifically, the laminated glass interlayer film of this embodiment may be a single-layer film consisting of one layer made of the composition of this embodiment, a multilayer film consisting of two or more layers made of the composition of this embodiment, or a multilayer film having at least one layer made of the composition of this embodiment and at least one layer other than the layer made of the composition of this embodiment.

[0035] The thickness of the laminated glass interlayer film of this embodiment is preferably 0.1 mm or more and 10 mm or less, more preferably 0.2 mm or more and 5 mm or less, and even more preferably 0.3 mm or more and 3 mm or less. When the thickness of the laminated glass interlayer is at least the above lower limit, the mechanical strength of the laminated glass interlayer can be further improved. When the thickness of the laminated glass interlayer is at most the above upper limit, the performance balance between the optical properties and interlayer adhesion of the resulting laminated glass can be further improved.

[0036] The method for producing the laminated glass interlayer film according to this embodiment is not limited, and any conventionally known production method can be used. The laminated glass interlayer film according to this embodiment can be produced by, for example, press molding, extrusion molding, T-die molding, injection molding, compression molding, cast molding, calendar molding, inflation molding, etc. The laminated glass interlayer film according to this embodiment can be obtained by supplying the composition according to this embodiment from a hopper and extruding it into a sheet.

[0037] <Laminated glass> The laminated glass of this embodiment includes the laminated glass interlayer film of this embodiment and transparent plate-like members provided on both sides of the laminated glass interlayer film. More specifically, the laminated glass may have a configuration of transparent plate-like member / laminated glass interlayer film / transparent plate-like member, for example. The laminated glass of this embodiment has excellent optical properties due to the inclusion of the laminated glass interlayer film of this embodiment.

[0038] The transparent plate-like member is not particularly limited, and examples thereof include commonly used transparent plate glass, such as inorganic glass, including float plate glass, polished plate glass, patterned plate glass, wired plate glass, striped plate glass, colored plate glass, heat-absorbing plate glass, heat-reflecting plate glass, and green glass. Also usable are organic plastic plates, such as polycarbonate plates, poly(meth)acrylate plates, polymethyl(meth)acrylate plates, polystyrene plates, cyclic polyolefin plates, polyethylene terephthalate plates, polyethylene naphthalate plates, and polyethylene butyrate plates. The transparent plate-like member may be subjected to a surface treatment such as corona treatment, plasma treatment, or flame treatment as appropriate.

[0039] The thickness of the transparent plate-like member is not particularly limited, but is preferably 20 mm or less, more preferably 10 mm or less. There is no lower limit to the thickness of the transparent plate-like member, but it is usually 0.1 mm or more, preferably 0.5 mm or more. In the laminated glass of this embodiment, the transparent plate-like members provided on both sides of the laminated glass interlayer film may be the same, or different plate-like members may be used in combination.

[0040] In order to maintain the transparency of the laminated glass in an appropriate range, the haze of the laminated glass of this embodiment, measured by the following method, is preferably less than 1.5%, more preferably 1.3% or less, even more preferably 1.1% or less, and still more preferably 0.9% or less. There is no particular lower limit for the haze of the laminated glass of this embodiment, but it may be, for example, 0.1% or more, or 0.3% or more. Furthermore, from the viewpoint of ensuring that the transparency of the laminated glass is within an appropriate range, the total light transmittance of the laminated glass of this embodiment, measured by the following method, is preferably 89.0% or more, more preferably 89.3% or more, even more preferably 89.5% or more, and still more preferably 89.7% or more. There is no particular upper limit to the total light transmittance of the laminated glass of this embodiment, but it may be, for example, 99.0% or less, 95.0% or less, or 93.0% or less. Furthermore, in order to ensure that the transparency of the laminated glass is within an appropriate range, the laminated glass of this embodiment preferably has a haze of less than 1.5% and a total light transmittance of 89.0% or more. (Evaluation method for haze and total light transmittance) A laminated glass interlayer film of 120 mm × 75 mm × 400 μm thick composed of the composition of this embodiment is obtained. Next, four of the obtained laminated glass interlayer films are stacked, sandwiched between two glass plates of 120 mm × 75 mm × 3.2 mm, and pressed in a vacuum heating laminator at 140 °C and 1 atm (gauge pressure) for 20 minutes to obtain a laminated glass. Next, the haze (%) of the obtained laminated glass is measured according to JIS K7136:2000 and the total light transmittance (%) according to JIS K7361-1:1997 using a haze meter.

[0041] The method for producing the laminated glass of the present embodiment is not particularly limited, and can be a conventionally known production method such as a nip roll method, an autoclave method, a vacuum bag method, a vacuum laminator method, etc. One of these methods may be used for production, or two or more production methods may be combined. The laminated glass of this embodiment can be produced, for example, by sandwiching a laminated glass interlayer between two sheets of glass and thermocompression bonding them under heat and pressure. The heating temperature is preferably about 100°C to 250°C, the pressure is preferably about 10 kPa to 3 MPa (0.98 atm to 29.6 atm), and the time is preferably 10 minutes to 60 minutes. These laminated glasses can be used for various purposes, such as architectural laminated glass, automotive laminated glass, general buildings, agricultural buildings, railway windows, etc., but are not limited to these uses.

[0042] Although the embodiments of the present invention have been described above, these are merely examples of the present invention, and various other configurations can also be adopted. Furthermore, the present invention is not limited to the above-described embodiment, and modifications and improvements within the scope of achieving the object of the present invention are included in the present invention. [Example]

[0043] The present embodiment will be described in detail below with reference to examples, etc. However, the present embodiment is not limited to the descriptions of these examples.

[0044] [material] The components used were as follows:

[0045] <Ionomer of ethylene-unsaturated carboxylic acid copolymer> Ionomer A: Ionomer of ethylene-methacrylic acid copolymer (ethylene content: 80% by mass, methacrylic acid content: 20% by mass) (metal ion: sodium ion, neutralization degree: 40%) Ionomer B: Ionomer of ethylene-methacrylic acid copolymer (ethylene content: 80% by mass, methacrylic acid content: 20% by mass) (metal ion: sodium ion, neutralization degree: 30%) Ionomer C: Ionomer of ethylene-methacrylic acid copolymer (ethylene content: 80% by mass, methacrylic acid content: 20% by mass) (metal ion: sodium ion, neutralization degree: 40%) Ionomer D: Ionomer of ethylene-methacrylic acid copolymer (ethylene content: 80% by mass, methacrylic acid content: 20% by mass) (metal ion: sodium ion, neutralization degree: 47%) Ionomer E: Ionomer of ethylene-methacrylic acid copolymer (ethylene content: 80% by mass, methacrylic acid content: 20% by mass) (metal ion: sodium ion, neutralization degree: 40%) Ionomer F: Ionomer of ethylene-methacrylic acid copolymer (ethylene content: 80% by mass, methacrylic acid content: 20% by mass) (metal ion: sodium ion, neutralization degree: 40%) Ionomer G: Ionomer of ethylene-methacrylic acid copolymer (ethylene content: 82.5% by mass, methacrylic acid content: 17.5% by mass) (metal ion: sodium ion, neutralization degree: 40%) Ionomer H: Ionomer of ethylene-methacrylic acid copolymer (ethylene content: 85% by mass, methacrylic acid content: 15% by mass) (metal ion: sodium ion, neutralization degree: 40%) Ionomer I: Ionomer of ethylene-methacrylic acid copolymer (ethylene content: 85% by mass, methacrylic acid content: 15% by mass) (metal ion: sodium ion, degree of neutralization: 54%)

[0046] <Silane coupling agent> Silane coupling agent 1: N-2-(aminoethyl)-3-aminopropylmethyldimethoxysilane, KBM-602, manufactured by Shin-Etsu Chemical Co., Ltd.

[0047] [Melt mass flow rate measurement] For each ionomer, the melt mass-flow rate (MFR) (g / 10 min) was measured at 190°C and a load of 2160 g using a melt indexer (product name: F-B01) manufactured by Toyo Seiki Co., Ltd., in accordance with JIS K7210:1999. Sheet formability was also evaluated according to the following criteria. The results are shown in Table 1. (Standards for sheet formability) A (Good): Ionomer MFR is 1.0 g / 10 min or more B (poor): MFR of ionomer is less than 1.0 g / 10 min

[0048] [Forming sheets for laminated glass interlayers] The ionomer of each example was impregnated with a silane coupling agent according to the formulation shown in Table 1, and then extrusion sheet molding was carried out under the following conditions using a 40 mmφ single-screw extruder (manufactured by Nakatani Machinery Co., Ltd.) equipped with a 400 mm wide T-die coat hanger, to obtain a 400 μm thick sheet for use as an interlayer film in laminated glass. <Molding conditions> Equipment: 40mmφ single screw extruder (with 400mm wide T-die coat hanger) Cylinder temperature: 170℃ Adapter and die temperature: 170°C Screw rotation speed: 50 rpm

[0049] [Making laminated glass] Using a vacuum heating laminator (double vacuum chamber laminator LM-50×50-S, manufactured by NPC Corporation), four sheets of the resulting 400 μm-thick laminated glass interlayer film sheet were laminated with glass in the following configuration to produce laminated glass for evaluating optical properties. The glass used was high-transparency white float glass (dimensions: length 120 mm x width 75 mm x thickness 3.2 mm) manufactured by AGC Fabritech Co., Ltd. Laminated glass composition: 3.2mm thick glass / laminated glass interlayer sheet (400μm thick x 4 sheets = 1600μm) / 3.2mm thick glass Lamination conditions: temperature 140°C, pressure 1 atm, time 20 minutes After lamination, the laminated glass was wrapped in bleached cloth, sandwiched between cardboard boxes, and cooled slowly in an environment of 23°C.

[0050] [Evaluation of optical properties of laminated glass] The obtained laminated glass was measured for haze (%) in accordance with JIS K7136:2000 and total light transmittance (%) in accordance with JIS K7361-1:1997 using a haze meter HZ-V3 (manufactured by Suga Test Instruments Co., Ltd.). The optical properties were also evaluated according to the following criteria. The results are shown in Table 1. (Optical characteristics standard) A (Good): Haze less than 1.5% and total light transmittance 89.0% or more B (Poor): Haze 1.5% or more or total light transmittance less than 89.0%

[0051] [Table 1]

[0052] The laminated glasses of Examples 1 to 6, which were made of an ionomer with an ethylene-methacrylic acid copolymer containing 17.5% by mass or more and 20% by mass or less of methacrylic acid, had improved optical properties compared to the laminated glasses of Comparative Examples 1 and 2, which were made of an ionomer with a methacrylic acid content of 15% by mass. Furthermore, the laminated glasses of Examples 1 to 6, which were made of an ionomer with a neutralization degree of 35 to 50%, had improved optical properties compared to the laminated glass of Comparative Example 3, which was made of an ionomer with a neutralization degree of 30%. On the other hand, the laminated glass of Comparative Example 2, which was made of an ionomer with a neutralization degree of more than 50%, had an MFR of less than 1.0 g / 10 min and was poor in sheet formability.

Claims

1. An ionomer of an ethylene-unsaturated carboxylic acid copolymer that satisfies the following requirements (i) to (iii): (i) When the total amount of structural units constituting the ethylene-unsaturated carboxylic acid copolymer is taken as 100% by mass, the content of structural units derived from unsaturated carboxylic acid is 17.0% by mass or more and less than 21.0% by mass. (ii) The degree of neutralization of the ionomer of the ethylene-unsaturated carboxylic acid copolymer is 35% or more and 50% or less. (iii) The melt mass flow rate of the ethylene-unsaturated carboxylic acid copolymer before neutralization, measured in accordance with JIS K 7210:1999 at 190°C under a load of 2160 g, is 60 g / 10 min or more and 300 g / 10 min or less.

2. 2. The ionomer according to claim 1, wherein the melt mass flow rate of the ionomer of the ethylene-unsaturated carboxylic acid copolymer after neutralization is 1.0 g / 10 min or more, as measured in accordance with JIS K 7210:1999 under conditions of 190°C and a load of 2160 g.

3. 3. The ionomer according to claim 1 or 2, wherein the metal ions constituting the ionomer of the ethylene-unsaturated carboxylic acid copolymer include one or more ions selected from the group consisting of sodium ions, lithium ions, potassium ions, silver ions, mercury ions, calcium ions, magnesium ions, zinc ions, aluminum ions, barium ions, beryllium ions, strontium ions, copper ions, cadmium ions, tin ions, lead ions, iron ions, cobalt ions, and nickel ions.

4. A composition comprising an ionomer of the ethylene-unsaturated carboxylic acid copolymer according to any one of claims 1 to 3.

5. The composition of claim 4 further comprising a silane coupling agent.

6. A molded article obtained by molding the composition according to claim 4 or 5.

7. A laminated glass interlayer film comprising the composition according to claim 4 or 5.

8. A laminated glass comprising the laminated glass interlayer film according to claim 7 and transparent plate-like members provided on both sides of the laminated glass interlayer film.

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