Additive composition, flame-retardant synthetic resin composition containing the same, and molded article thereof

The additive composition of ammonium polyphosphate and specific compounds enhances the heat resistance and flame retardancy of synthetic resins, addressing the inadequacies of current formulations in high-heat applications.

JP7811086B2Active Publication Date: 2026-02-04ADEKA CORP
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Patent Information

Application Number
JP2020535889
Authority / Receiving Office
JP · JP
Patent Type
Patents
Current Assignee / Owner
Priority Date
2018-08-10
Filing Date
2019-08-08
Publication Date
2026-02-04
Estimated Expiration
2039-08-08

AI Technical Summary

Technical Problem

Existing synthetic resins, particularly polyolefin resins, require improved heat resistance and flame retardancy, especially in applications near high heat sources like home appliances and automobile batteries, where current combinations of intumescent flame retardants and antioxidants may not provide sufficient performance.

Method used

An additive composition comprising ammonium polyphosphate and specific compounds, such as 1,3,5-tris(3,5-di-tert-butyl-4-hydroxybenzyl)isocyanurate, along with nitrogen-containing organic compounds like melamine cyanurate, is used to enhance the heat resistance and flame retardancy of synthetic resins.

Benefits of technology

The additive composition significantly improves the heat resistance and flame retardancy of synthetic resins, ensuring they meet the demanding requirements of applications near high heat sources.

✦ Generated by Eureka AI based on patent content.

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Abstract

The present invention provides an additive composition capable of imparting excellent heat resistance and flame retardancy to synthetic resins, a flame-retardant synthetic resin composition containing the same, and a molded article thereof. As the component (A), one or more ammonium polyphosphates are used, and as the component (B), a compound represented by the following general formula (1) and a compound represented by the following general formula (2): and at least one compound selected from the group consisting of compounds represented by general formula (1): 1 , R 2 and R 3 each independently represents a divalent hydrocarbon group having 1 to 3 carbon atoms, and in general formula (2), R 4 , R 5 and R 6 each independently represents a divalent hydrocarbon group having 1 to 3 carbon atoms; R 7 , R 8 and R 9 each independently represents a hydrogen atom or a monovalent hydrocarbon group having 1 to 4 carbon atoms.
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Description

[Technical Field]

[0001] The present invention relates to an additive composition, a flame-retardant synthetic resin composition containing the same (hereinafter also simply referred to as "synthetic resin composition"), and a molded article thereof, and more particularly to an additive composition that can impart excellent heat resistance and flame retardancy to a synthetic resin, a flame-retardant synthetic resin composition containing the same, and a molded article thereof. [Background technology]

[0002] Synthetic resins have advantages such as excellent moldability, heat resistance, and mechanical properties, as well as low specific gravity and light weight, and are therefore widely used for various molded products such as films, sheets, and structural parts. Furthermore, many attempts have been made to blend synthetic resins with other polymers to impart new physical properties such as impact resistance and elasticity.

[0003] However, because highly flammable synthetic resins such as polyolefin resins are widely used in a wide range of fields, it has become essential to blend flame retardants to impart flame retardancy to these resins. For example, Patent Documents 1 and 2 propose intumescent flame retardants, which contain ammonium polyphosphate and a nitrogen-containing compound as their main components and form a surface intumescent layer during combustion, thereby suppressing the diffusion of decomposition products and heat transfer, thereby exhibiting flame retardancy. [Prior art documents] [Patent documents]

[0004] [Patent Document 1] Japanese Patent Application Publication No. 11-236472 [Patent Document 2] Japanese Patent Application Laid-Open No. 2005-27574 Summary of the Invention [Problem to be solved by the invention]

[0005] Today, particularly in applications requiring high heat resistance and high flame retardancy, such as in home appliances and around automobile batteries, particularly high performance is required. Here, in order to achieve both heat resistance and flame retardancy in a synthetic resin, it is necessary to use an intumescent flame retardant in combination with an antioxidant. However, depending on the type of antioxidant used in combination, the heat resistance may be insufficient or a large amount may need to be added. Therefore, there is currently a demand for additive compositions with better heat resistance and flame retardancy than before.

[0006] Therefore, an object of the present invention is to provide an additive composition that can impart excellent heat resistance and flame retardancy to synthetic resins, a flame-retardant synthetic resin composition containing the same, and a molded article thereof. [Means for solving the problem]

[0007] As a result of extensive research into solving the above problems, the present inventors discovered that the above problems can be solved by using an ammonium polyphosphate salt and a compound having a specific structure, and thus completed the present invention.

[0008] That is, the additive composition of the present invention comprises one or more ammonium polyphosphates as component (A) and a compound represented by the following general formula (1) as component (B): and at least one compound selected from the group consisting of compounds represented by JPEG0007811086000001.jpg79166, Furthermore, the composition is characterized in that it contains, as component (C), one or more nitrogen-containing organic compounds other than the compound represented by general formula (1), the mass ratio of component (A) / component (C) is (A) / (C)=50 / 50 to 80 / 20, and the nitrogen-containing organic compound of component (C) is at least one or more triazine derivatives.

[0009] Here, in general formula (1), R 1 , R 2 and R 3 each independently represents a divalent hydrocarbon group having 1 to 3 carbon atoms.

[0011] The flame-retardant synthetic resin composition of the present invention is characterized by comprising a synthetic resin and the additive composition of the present invention blended therein.

[0012] In the flame-retardant synthetic resin composition of the present invention, the synthetic resin is preferably a polyolefin resin.

[0013] The molded article of the present invention is characterized by being obtained from the flame-retardant synthetic resin composition of the present invention. [Effects of the Invention]

[0014] According to the present invention, it is possible to provide an additive composition that can impart excellent heat resistance and flame retardancy to a synthetic resin, a flame-retardant synthetic resin composition containing the same, and a molded article thereof. DETAILED DESCRIPTION OF THE INVENTION

[0015] First, the additive composition of the present invention will be described. The additive composition of the present invention comprises one or more ammonium polyphosphates as component (A) and a compound represented by the following general formula (1): TIFF0007811086000002.tif79166 and a compound represented by the following general formula (2): and at least one compound selected from the group consisting of compounds represented by TIFF0007811086000003.tif79166.

[0016] First, component (A) will be described. The component (A) in the additive composition of the present invention is one or more ammonium polyphosphates, which function as a component that imparts flame retardancy to synthetic resins.

[0017] Component (A) according to the present invention is one or more ammonium polyphosphates. In the additive composition of the present invention, ammonium polyphosphates include ammonium orthophosphate, ammonium pyrophosphate, ammonium metaphosphate, and ammonium polyphosphate, all of which are included in ammonium polyphosphate. Component (A) may be one type or a mixture of two or more types. The degree of condensation of polyphosphoric acid in ammonium polyphosphate is, for example, 3 to 1000. Furthermore, ammonium polyphosphate may be a normal salt, an acid salt, or a basic salt.

[0018] Ammonium polyphosphate can be easily obtained, for example, by the following method: Using a phosphorus-containing compound such as phosphoric acid, polyphosphoric acid, urea phosphate, melamine phosphate, monoammonium phosphate, diammonium phosphate, or triammonium phosphate as raw materials, a condensing agent such as urea or phosphorus pentoxide and an ammoniating agent such as ammonia gas, ammonium carbonate, ammonium bicarbonate, or biuret are reacted at a temperature of 170 to 350°C for a sufficient period of time.

[0019] Alternatively, commercially available ammonium polyphosphates can be used, and examples of commercially available products include Exolit-422 (trade name, manufactured by Hoechst), Exolit-700 (trade name, manufactured by Hoechst), Phos-chek-P / 30 (trade name, manufactured by Monsanto), Phos-chek-P / 40 (trade name, manufactured by Monsanto), Sumisafe-P (trade name, manufactured by Sumitomo Chemical Co., Ltd.), TERRAJU (registered trademark, manufactured by Chisso Corporation)-S10, and TERRAJU (registered trademark, manufactured by Chisso Corporation)-S20.

[0020] Furthermore, since ammonium polyphosphate itself is susceptible to hydrolysis, ammonium polyphosphate coated or microencapsulated with a thermosetting resin, or ammonium polyphosphate particles coated with melamine monomer or other nitrogen-containing organic compounds, can also be suitably used. In addition, ammonium polyphosphate treated with a surfactant, a silane coupling agent, or a silicon compound such as silicone oil, or ammonium polyphosphate made insoluble by adding melamine or the like during the production process can also be used.

[0021] For example, ammonium polyphosphate microencapsulated with a thermosetting resin can be obtained by using a resin such as an epoxy resin, a urethane resin, an acrylic resin, a phenolic resin, an alkyd resin, a urea resin, a melamine resin, or a silicone resin, either alone or in combination, as the coating resin, and encapsulating the resin by a known method such as interfacial polymerization, in-situ polymerization, liquid curing, phase separation, liquid drying, melt-dispersion cooling, spray drying, or powder bed method.

[0022] Examples of methods for obtaining ammonium polyphosphate coated with melamine monomer include a sublimation coating method in which a predetermined amount of melamine monomer is added to ammonium polyphosphate preheated to 250°C to 300°C in a heating and stirring device, and heating is continued at the same temperature to add and / or adhere the sublimated melamine to the ammonium polyphosphate, and a so-called hybridization method in which a mixture of ammonium polyphosphate and melamine monomer is formed into a film in a powerful stirrer. Examples of methods for obtaining ammonium polyphosphate coated with silicone resin include a method disclosed in JP-A-3-131508 in which ammonium polyphosphate is suspended in an organic solvent and coated with a curable silicone resin, a curing accelerator, and water while stirring, followed by curing the silicone resin, as coated.

[0023] Examples of commercially available ammonium polyphosphate compounds with reduced hydrolysis properties include Exolit-462 (trade name, manufactured by Hoechst), Sumisafe-PM (trade name, manufactured by Sumitomo Chemical Co., Ltd.), TERRAJU (registered trademark, manufactured by Chisso Corporation)-C60, TERRAJU (registered trademark, manufactured by Chisso Corporation)-C70, TERRAJU (registered trademark, manufactured by Chisso Corporation)-C80, TERRAJU (registered trademark, manufactured by Chisso Corporation)-M30, and TERRAJU (registered trademark, manufactured by Chisso Corporation)-M40, and these commercially available products can also be suitably used.

[0024] Next, the component (B) will be described. Component (B) in the additive composition of the present invention is at least one selected from the group consisting of compounds represented by the following general formula (1) and compounds represented by the following general formula (2): The compounds represented by the following general formula (1) and the following general formula (2) function as components that impart heat resistance to synthetic resins.

[0025] TIFF0007811086000004.tif79166

[0026] TIFF0007811086000005.tif79166

[0027] Here, in general formula (1), R 1 , R 2 , R 3 each independently represents a divalent hydrocarbon group having 1 to 3 carbon atoms. 4 , R 5 and R 6 each independently represents a divalent hydrocarbon group having 1 to 3 carbon atoms, and R 7 , R 8 and R 9 each independently represents a hydrogen atom or a monovalent hydrocarbon group having 1 to 4 carbon atoms.

[0028] In general formula (1), R 1, R 2 and R 3 Examples of the divalent hydrocarbon group having 1 to 3 carbon atoms represented by the formula include a linear or branched alkylene group, a linear or branched alkenylene group, and an alkynylene group.

[0029] As a straight chain alkylene group, -(CH2) n -(n is an integer of 1 to 3), examples of the branched alkylene group include -CH(CH3)-, -CH2(CH2CH3)-, -CH(CH3)CH2-, and -CH2CH(CH3)-, examples of the straight-chain alkenylene group include -CH=CH-, -CH=CH-CH2-, and -CH2-CH=CH-, examples of the branched alkenylene group include -C(CH3)=CH- and -CH=C(CH3)-, and examples of the alkynylene group include -C≡C-, -CH2-C≡C-, and -C≡C-CH2-.

[0030] Examples of the compound represented by general formula (1) include 1,3,5-tris(3,5-di-tert-butyl-4-hydroxybenzyl)isocyanurate, 1,3,5-tris(3,5-di-tert-butyl-4-hydroxyphenylethyl)isocyanurate, and 1,3,5-tris(3,5-di-tert-butyl-4-hydroxyphenylpropyl)isocyanurate, which may be used alone or in combination of two or more. Among these, 1,3,5-tris(3,5-di-tert-butyl-4-hydroxybenzyl)isocyanurate is preferred.

[0031] In general formula (2), R 4 , R 5 and R 6 As the divalent hydrocarbon group having 1 to 3 carbon atoms represented by the formula 1 , R 2 and R 3 Examples of the divalent hydrocarbon group include the same groups as those having 1 to 3 carbon atoms and represented by the following formula:

[0032] R 7 , R 8 and R 9Examples of the monovalent hydrocarbon group having 1 to 4 carbon atoms represented by the formula (I) include a linear or branched alkyl group, a linear or branched alkenyl group, and a linear or branched alkynyl group. Examples of linear alkyl groups include CH3-, CH3CH2-, CH3CH2CH2-, and CH3CH2CH2CH2-. Examples of branched alkyl groups include CH3(CH3)CH-, CH3(CH3)CH2CH2-, CH3CH2(CH3)CH-, and (CH3)3C-. Examples of linear alkenyl groups include CH2=CH-, CH2=CHCH2-, CH3CH=CH-, and CH2=CHCH2C-. Examples of branched alkenyl groups include CH(CH)=CH-, CH=C(CH)-, CH=C(CH)CH-, and CHC(CH)=CH-, and examples of alkynyl groups include CH≡C-, CH≡CCH-, CHC≡C-, CH≡CCHCH-, CHC≡CCH-, and CHCHC≡CH-. Among these, linear or branched alkyl groups are preferred as hydrocarbon groups having 1 to 4 carbon atoms.

[0033] Examples of the compound represented by general formula (2) include 1,3,5-tris(3,5-di-tert-butyl-4-hydroxybenzyl)-2,4,6-trimethylbenzene, 1,3,5-tris(3,5-di-tert-butyl-4-hydroxyphenylethyl)-2,4,6-trimethylbenzene, 1,3,5-tris(3,5-di-tert-butyl-4-hydroxyphenylpropyl)-2,4,6-trimethylbenzene, 1,3,5-tris(3,5-di-tert-butyl- Examples of suitable hydroxybenzyl compounds include 1,3,5-tris(3,5-di-tert-butyl-4-hydroxybenzyl)-2,4,6-triethylbenzene, 1,3,5-tris(3,5-di-tert-butyl-4-hydroxybenzyl)-2,4,6-tripropylbenzene, 1,3,5-tris(3,5-di-tert-butyl-4-hydroxybenzyl)-2,4,6-tributylbenzene, and 1,3,5-tris(3,5-di-tert-butyl-4-hydroxybenzyl)benzene. These may be used alone or in combination of two or more. Among these, 1,3,5-tris(3,5-di-tert-butyl-4-hydroxybenzyl)-2,4,6-trimethylbenzene is preferred.

[0034] The compound represented by general formula (1) and the compound represented by general formula (2) may be used alone or in combination of two or more kinds, and when mixed, the ratio may be any value.

[0035] In the additive composition of the present invention, the content ratio (A) / (B) of the components (A) and (B) is, in terms of mass ratio, preferably (A) / (B)=99.95 / 0.05 to 75 / 25, more preferably (A) / (B)=99.8 / 0.2 to 85 / 15, and even more preferably (A) / (B)=99.7 / 0.3 to 92 / 8, from the viewpoints of heat resistance and flame retardancy.

[0036] The additive composition of the present invention can be obtained by mixing component (A) and component (B), but when blending them into a synthetic resin, they may be mixed in advance and then blended, or each component may be blended into the synthetic resin when blending it into the synthetic resin, or they may be blended as a masterbatch.

[0037] When mixing component (A) with component (B), or when mixing with component (C) or other optional components described below, various mixers can be used, such as a tumbler mixer, Henschel mixer, ribbon blender, V-type mixer, W-type mixer, Super mixer, and Nauta mixer.

[0038] The additive composition of the present invention preferably further contains, as component (C), one or more nitrogen-containing organic compounds other than the compound represented by general formula (1), from the viewpoint of heat resistance and flame retardancy.

[0039] The component (C) will be described below. Component (C) of the additive composition of the present invention is one or more nitrogen-containing organic compounds other than the compound represented by general formula (1). The nitrogen-containing organic compound of component (C), together with ammonium polyphosphate of component (A), functions as a component that imparts flame retardancy to the synthetic resin. The nitrogen-containing organic compound of component (C) is a compound that generates a non-flammable gas when ignited or ignited, or when exposed to heat such as flames, and also generates or promotes the generation of a carbonaceous residue, and specific examples thereof are listed below as (1) to (4).

[0040] (1) Triazine derivatives: melamine, melamine cyanurate, ammeline, phthalodiguanamine, butylenediguanamine, norbornenediguanamine, methylenediguanamine, ethylenedimelamine, trimethylenedimelamine, tetramethylenedimelamine, hexamethylenedimelamine, 1,3-hexylenedimelamine, methylolmelamine, and derivatives containing 1 to 6 methylol groups obtained by reacting melamine with formaldehyde in a molar ratio (former:latter) of 1:1 to 1:6. Methylol melamine, melamine resin obtained by heat-curing this methylol melamine in an acidic solution, modified melamine resin obtained by heat-curing this methylol melamine with the simultaneous addition of urea, phenol or alcohol when resinifying this methylol melamine, melamine phosphate, melamine orthophosphate, melamine pyrophosphate, melamine polyphosphate, melamine metaphosphate, melamine sulfate, reaction products of cyanuric acid halides with linear or branched alkylenediamines having 2 to 6 carbon atoms, especially cyanuric acid Benzoguanamine, a reaction product of an acid chloride with a linear or branched alkylenediamine having 2 to 6 carbon atoms, such as ethylenediamine, propylenediamine, 1,4-tetramethylenediamine, 1,5-pentamethylenediamine, or 1,6-hexamethylenediamine, in a molar ratio (former:latter) of 1:1 to 1:3; methylolated benzoguanamine obtained by reacting this benzoguanamine with formaldehyde in a molar ratio (former:latter) of 1:1 to 1:4; and A resinous substance obtained by heating and curing methylolated benzoguanamine in an acidic solution, acetoguanamine, a methylolated acetoguanamine obtained by reacting this acetoguanamine with formaldehyde in a molar ratio (former:latter) of 1:1 to 1:4, and a resinous substance obtained by heating and curing this methylolated acetoguanamine in an acidic solution, 3,9-bis[2-(3,5-diamino-2,4,6-triazaphenyl)ethyl]-2,4,8,10-tetraoxaspiro[5.5] A methylolated spiro compound obtained by reacting undecane or this spiro compound with formaldehyde in a molar ratio (former:latter) of 1:1 to 1:10, a resinous substance obtained by heat-curing this methylolated spiro compound in an acidic solution, and a homopolymer and / or copolymer having a repeating unit of a triazine derivative represented by the following general formula (3), wherein X in general formula (3) is 1Examples of the group include a monomethylamino group, a dimethylamino group, a methylethylamino group, a methylethylamino group, a monoethylamino group, a diethylamino group, a monopropylamino group, a dipropylamino group, a methylpropylamino group, an ethylpropylamino group, a diisopropylamino group, a mono-n-butylamino group, a di-n-propylamino group, a methyl-n-butylamino group, an ethyl-n-butylamino group, a propyl-n-butylamino group, an isopropyl-n-butylamino group, a monoisobutylamino group, a diisobutylamino group, a methylisobutylamino group, an ethylisobutylamino group, a propylisobutylamino group, an isopropylisobutylamino group, a monopentylamino group, a dipentylamino group, a methylpentylamino group, an ethylpentylamino group, a propylpentylamino group, an isopropylpentylamino group, an n-butylpentylamino group, an isobutylpentylamino group, an isobutylpentylamino group, an Examples thereof include an ethylamino group, a monohexylamino group, a dihexylamino group, a methylhexylamino group, an ethylhexylamino group, a propylhexylamino group, an isopropylhexylamino group, an n-butylhexylamino group, an isobutylhexylamino group, a pentylhexylamino group, a monohydroxyethylamino group, a dihydroxyethylamino group, a monohydroxypropylamino group, a dihydroxypropylamino group, a monohydroxyisopropylamino group, a dihydroxypropylamino group, a monohydroxy-n-butylamino group, a dihydroxy-n-butylamino group, a monohydroxyisobutylamino group, a dihydroxyisobutylamino group, a monohydroxypentylamino group, a dihydroxypentylamino group, a monohydroxyhexylamino group, a dihydroxyhexylamino group, an N-methylhydroxyethylamino group, a morpholino group, and a piperidino group. Examples of the group Y in general formula (3) include an ethylenediamine residue, an N,N'-dimethylethylenediamine residue, an N-N'-diethylethylenediamine residue, a 1,3-diaminopropane residue, a tetramethylenediamine residue, a pentamethylenediamine residue, a hexamethylenediamine residue, a piperazine residue, and a trans-2,5-dimethylpiperazine residue.

[0041] TIFF0007811086000006.tif37166

[0042] Here, in the general formula (3), X 1 and Y are groups bonded to the triazine ring via a nitrogen atom, and X 1 Ga-NHR 10 or -NR 11 R 12 R is an alkylamino group, a morpholino group, or a piperidino group represented by the formula 10 , R 11 and R 12 are each a hydrogen atom or a straight-chain or branched alkyl group containing 1 to 6 carbon atoms (R 11 and R 12 may be the same group or different groups), or X 1 Ga-NHR 13 or -NR 14 R 15 is a hydroxyalkylamino group represented by R 13 , R 14 and R 15 are straight-chain or branched hydroxyalkyl groups containing 2 to 6 carbon atoms (R 14 and R 15 may be the same or different groups). Y is a divalent piperazine radical, formula -HN(CH2) m a divalent group represented by NH- (where m is a number from 2 to 6) or -NR 16 (CH2) p R 17 is a group represented by N-, and R 16 and R 17 is a straight or branched alkyl or hydroxyalkyl group containing 1 to 6 carbon atoms).

[0043] Further, specific examples of triazine derivatives include poly-[2,4-(piperazin-1,4-yl)-6-(morpholino-4-yl)-1,3,5-triazine] (CAS No. 93058-67-4, CAS No. 1078142-02-5).

[0044] (2) (Iso)cyanuric acid derivatives: melamine cyanurate obtained by the neutralization reaction of cyanuric acid and melamine, derivatives having an unsaturated double bond such as triallyl cyanurate, triallyl isocyanurate, and trimethallyl isocyanurate, as well as resinous substances obtained by crosslinking these derivatives having an unsaturated double bond, such as trisepoxypropyl isocyanurate and tris-(2-hydroxyethyl)isocyanurate.

[0045] (3) Imidazolidinone derivatives: Examples include resinous substances obtained by heat-condensing a methylolated product obtained by reacting ethyleneurea or ethylenethiourea with formaldehyde in a molar ratio (former:latter) of 1:1 to 1:2 in an acidic solution.

[0046] (4) Piperazine derivatives: piperazine, piperazine phosphate, piperazine orthophosphate, piperazine pyrophosphate, piperazine polyphosphate, and piperazine metaphosphate.

[0047] In the additive composition of the present invention, the nitrogen-containing organic compound of component (C) may be a commercially available product.

[0048] Among the nitrogen-containing organic compounds of component (C), triazine derivatives are preferred from the viewpoints of heat resistance and flame retardancy, with melamine cyanurate and poly-[2,4-(piperazin-1,4-yl)-6-(morpholino-4-yl)-1,3,5-triazine] (CAS No. 93058-67-4, CAS No. 1078142-02-5) being more preferred, and poly-[2,4-(piperazin-1,4-yl)-6-(morpholino-4-yl)-1,3,5-triazine] (CAS No. 93058-67-4, CAS No. 1078142-02-5) being even more preferred.

[0049] The content ratio (A) / (C) of the components (A) and (C) in the additive composition of the present invention is preferably (A) / (C)=30 / 70 to 95 / 5 by mass, more preferably (A) / (C)=40 / 60 to 85 / 15, and even more preferably (A) / (C)=50 / 50 to 80 / 20.

[0050] The component (C) may be blended in advance with the additive composition of the present invention, or may be blended with the synthetic resin when blending with the synthetic resin.

[0051] The additive composition of the present invention preferably further contains one or more dialkylphosphinic acids or salts thereof, which are preferably dialkylphosphinic acids or salts thereof represented by the following general formula (4) from the viewpoints of heat resistance and flame retardancy:

[0052] TIFF0007811086000007.tif36166

[0053] Here, in general formula (4), R 19 , R 20 are the same or different and are linear or branched alkyl groups having 1 to 6 carbon atoms; M is Mg, Ca, Al, Sb, Sn, Ge, Ti, Fe, Zr, Zn, Ce, Bi, Sr, Mn, Li, Na, K, H, and / or a protonated nitrogen base; and m is 1 to 4.

[0054] R 19 , R 20 Examples of the alkyl group having 1 to 6 carbon atoms include methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, sec-butyl, tert-butyl, n-pentyl, isopentyl, neopentyl, tert-amyl, 1,2-dimethylpropyl, n-hexyl, 1,3-dimethylbutyl, 1-isopropylpropyl, 1,2-dimethylbutyl, cyclopropyl, cyclobutyl, cyclopentyl, and cyclopropyl.

[0055] R 19 , R 20From the viewpoints of heat resistance and flame retardancy, M is preferably an alkyl group having 1 to 4 carbon atoms, and most preferably an ethyl group. From the viewpoints of heat resistance and flame retardancy, M is preferably zinc or aluminum, and more preferably aluminum. From the viewpoints of heat resistance and flame retardancy, the dialkylphosphinic acid or a salt thereof is preferably compound (4-1) or compound (4-2) of the following structural formula, and more preferably compound (4-1).

[0056] TIFF0007811086000008.tif42166

[0057] The dialkylphosphinic acid or a salt thereof may be blended in advance with the additive composition of the present invention, or may be blended with the synthetic resin when blending with the synthetic resin.

[0058] When blended into a synthetic resin, the amount of dialkylphosphinic acid or a salt thereof is preferably 1 to 100 parts by mass, more preferably 5 to 60 parts by mass, and more preferably 10 to 40 parts by mass, per 100 parts by mass of the synthetic resin.

[0059] The additive composition of the present invention may contain a metal oxide as a flame retardant aid, if necessary, within a range that does not impair the effects of the present invention. Examples of metal oxides include zinc oxide, titanium oxide, magnesium oxide, and silicon oxide, with zinc oxide being preferred. The metal oxide may be surface-treated. Commercially available zinc oxide products may be used, such as Zinc Oxide Type 1 (manufactured by Mitsui Mining & Smelting Co., Ltd.), partially coated zinc oxide (manufactured by Mitsui Mining & Smelting Co., Ltd.), Nanofine 50 (ultrafine zinc oxide particles with an average particle size of 0.02 μm: manufactured by Sakai Chemical Industry Co., Ltd.), and Nanofine K (ultrafine zinc oxide particles coated with zinc silicate with an average particle size of 0.02 μm: manufactured by Sakai Chemical Industry Co., Ltd.).

[0060] When a metal oxide is contained, the content thereof is preferably 0.01 to 10 parts by mass, more preferably 0.5 to 10 parts by mass, and even more preferably 1.0 to 7.5 parts by mass, based on 100 parts by mass of the total amount of components (A) and (C) contained in the additive composition, from the viewpoint of flame retardancy. If the content is less than 0.01 part by mass, the flame retardant auxiliary effect is insufficient, and if it exceeds 10 parts by mass, the properties of the resin may be deteriorated. The metal oxide may be blended in advance with the additive composition of the present invention, or may be blended with the synthetic resin when blending the synthetic resin.

[0061] The additive composition of the present invention may also contain an anti-drip agent, if necessary, within the range that does not impair the effects of the present invention. Examples of the anti-drip agent include fluorine-based anti-drip agents, silicone rubbers, and layered silicates.

[0062] Examples of layered silicates include smectite clay minerals such as montmorillonite, saponite, hectorite, beidellite, stevensite, and nontronite, as well as vermiculite, halloysite, swelling mica, and talc, and organic cations, quaternary ammonium cations, and phosphonium cations may be intercalated between the layers.

[0063] Fluorine-based anti-drip agents are particularly preferred as the anti-drip agent, and specific examples of fluorine-based anti-drip agents include fluorine-based resins such as polytetrafluoroethylene, polyvinylidene fluoride, and polyhexafluoropropylene, as well as alkali metal salt compounds of perfluoroalkanesulfonic acids or alkaline earth metal salts of perfluoroalkanesulfonic acids such as sodium perfluoromethanesulfonate, potassium perfluoro-n-butanesulfonate, potassium perfluoro-t-butanesulfonate, sodium perfluorooctanesulfonate, and calcium perfluoro-2-ethylhexanesulfonate. Among anti-drip agents, polytetrafluoroethylene is most preferred from the viewpoint of drip prevention.

[0064] When an anti-drip agent is contained, the content of the anti-drip agent is preferably 0.005 to 5 parts by mass, more preferably 0.01 to 5 parts by mass, more preferably 0.05 to 3 parts by mass, and even more preferably 0.1 to 1 part by mass, per 100 parts by mass of the total amount of components (A) and (C) contained in the additive composition. If the content is less than 0.005 parts by mass, the anti-drip effect is insufficient, and if the content exceeds 5 parts by mass, the properties of the resin may be reduced. The anti-drip agent may be blended into the additive composition of the present invention in advance, or may be blended into the synthetic resin when blending with the synthetic resin.

[0065] In addition, within the scope that does not impair the effects of the present invention, silicone oil can be blended into the additive composition of the present invention as necessary to suppress secondary aggregation during blending and improve water resistance.Examples of silicone oil include dimethyl silicone oil, in which the side chain and terminal of polysiloxane are all methyl groups; methylphenyl silicone oil, in which part of the side chain of polysiloxane is phenyl group; methylhydrogen silicone oil, in which part of the side chain of polysiloxane is hydrogen, etc., and copolymers thereof.In addition, organic groups can be introduced into part of these side chains and / or terminals, and the modified silicone oils that are amine-modified, epoxy-modified, alicyclic epoxy-modified, carboxyl-modified, carbinol-modified, mercapto-modified, polyether-modified, long-chain alkyl-modified, fluoroalkyl-modified, higher fatty acid ester-modified, higher fatty acid amide-modified, silanol-modified, diol-modified, phenol-modified and / or aralkyl-modified can be used.

[0066] Specific examples of silicone oils include dimethyl silicone oils such as KF-96 (manufactured by Shin-Etsu Chemical Co., Ltd.), KF-965 (manufactured by Shin-Etsu Chemical Co., Ltd.), and KF-968 (manufactured by Shin-Etsu Chemical Co., Ltd.), methyl hydrogen silicone oils or silicone oils having a methyl hydrogen polysiloxane structure such as KF-99 (manufactured by Shin-Etsu Chemical Co., Ltd.), KF-9901 (manufactured by Shin-Etsu Chemical Co., Ltd.), HMS-151 (manufactured by Gelest), HMS-071 (manufactured by Gelest), HMS-301 (manufactured by Gelest), and DMS-H21 (manufactured by Gelest), and examples of methyl phenyl silicone oils such as KF-50 (manufactured by Shin-Etsu Chemical Co., Ltd.), KF-53 (manufactured by Shin-Etsu Chemical Co., Ltd.), and KF-54 (manufactured by Shin-Etsu Chemical Co., Ltd.). Examples of epoxy-modified products include X-22-343 (Shin-Etsu Chemical Co., Ltd.), X-22-2000 (Shin-Etsu Chemical Co., Ltd.), KF-101 (Shin-Etsu Chemical Co., Ltd.), KF-102 (Shin-Etsu Chemical Co., Ltd.), KF-100 Examples of the carboxyl-modified products include X-22-3701E (Shin-Etsu Chemical Co., Ltd.), examples of the carbinol-modified products include X-22-4039 (Shin-Etsu Chemical Co., Ltd.) and X-22-4015 (Shin-Etsu Chemical Co., Ltd.), and examples of the amine-modified products include KF-393 (Shin-Etsu Chemical Co., Ltd.).

[0067] When silicone oil is contained, the content of silicone oil is preferably 0.01 to 10 parts by mass, more preferably 0.1 to 5 parts by mass, and even more preferably 0.5 to 3 parts by mass, per 100 parts by mass of the total amount of components (A) and (C) contained in the additive composition. If the content is less than 0.01 part by mass, the suppression of secondary aggregation and water resistance may be insufficient, while if it exceeds 10 parts by mass, the properties of the resin may be deteriorated. The silicone oil may be blended into the additive composition of the present invention in advance, or may be blended into the synthetic resin when blending it with the synthetic resin.

[0068] Furthermore, the additive composition of the present invention may contain a silane coupling agent, if necessary, to prevent aggregation of the additive powder, improve storage stability, and impart water resistance and heat resistance, within a range that does not impair the effects of the present invention.

[0069] Examples of the silane coupling agent include silane coupling agents having an alkenyl group, such as vinyltrimethoxysilane, vinyltriethoxysilane, vinyltriacetoxysilane, vinyltris(2-methoxyethoxy)silane, vinylmethyldimethoxysilane, octenyltrimethoxysilane, allyltrimethoxysilane, and p-styryltrimethoxysilane; silane coupling agents having an acrylic group, such as 3-acryloxypropyltrimethoxysilane and 3-acryloxypropyltriethoxysilane; and silane coupling agents having a methacryl group, such as 3-methacryloxypropylmethyldimethoxysilane, 3-methacryloxypropyltrimethoxysilane, 3-methacryloxypropylmethyldiethoxysilane, 3-methacryloxypropyltriethoxysilane, and methacryloxyoctyltrimethylsilane. Examples of silane coupling agents having an epoxy group include 2-(3,4-epoxycyclohexyl)ethyltrimethoxysilane, 3-glycidoxypropylmethyldimethoxysilane, 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropylmethyldiethoxysilane, 3-glycidoxypropyltriethoxysilane, and glycidoxyoctyltrimethoxysilane. Examples of silane coupling agents having an amino group include N-2-(aminoethyl)-3-aminopropylmethyldimethoxysilane, N-2-(aminoethyl)-3-aminopropyltrimethoxysilane, 3-aminopropyltrimethoxysilane, 3-aminopropyltriethoxysilane, 3-triethoxysilyl-N-(1,3-dimethyl-butylidene)propylamine, N-phenyl-3-aminopropyltrimethoxysilane, N,Examples of silane coupling agents having an isocyanurate group include tris-(trimethoxysilylpropyl)isocyanurate. Examples of silane coupling agents having a mercapto group include 3-mercaptopropylmethyldimethoxysilane, 3-mercaptopropyltrimethoxysilane, and 3-mercaptopropyltriethoxysilane. Examples of silane coupling agents having a ureido group include silane coupling agents having an isocyanurate group, tris-(trimethoxysilylpropyl)isocyanurate. Examples of silane coupling agents having an isocyanurate group include 3-mercaptopropylmethyldimethoxysilane, 3-mercaptopropyltrimethoxysilane, and 3-mercaptopropyltriethoxysilane. Examples of silane coupling agents include 3-ureidopropyltrimethoxysilane and 3-ureidopropyltriethoxysilane. Examples of silane coupling agents having a sulfide group include bis(triethoxysilylpropyl)tetrasulfide. Examples of silane coupling agents having a thioester group include 3-octanoylthio-1-propyltriethoxysilane. Examples of silane coupling agents having an isocyanate group include 3-isocyanatepropyltriethoxysilane and 3-isocyanatepropyltrimethoxysilane.

[0070] Among these silane coupling agents, a silane coupling agent having an epoxy group is preferred from the viewpoints of preventing aggregation of the additive powder, improving storage stability, water resistance, and heat resistance.

[0071] Commercially available silane coupling agents can be used. Examples of vinyltrimethoxysilanes include KBM-1003 manufactured by Shin-Etsu Chemical Co., Ltd., A-171 manufactured by Montiv Performance Materials Japan LLC, Z-6300 manufactured by Toray Dow Corning Co., Ltd., GENIOSIL XL10 manufactured by Asahi Kasei Silicone Co., Ltd., and Sila Ace S210 manufactured by Nichibi Shoji Co., Ltd.; examples of vinyltriethoxysilanes include KBE-1003 manufactured by Shin-Etsu Chemical Co., Ltd., A-151 manufactured by Montiv Performance Materials Japan LLC, Z-6519 manufactured by Toray Dow Corning Co., Ltd., GENIOSIL GF56 manufactured by Asahi Kasei Silicone Co., Ltd., and Sila Ace S220 manufactured by Nichibi Shoji Co., Ltd.; and examples of vinyltriacetoxysilanes include GENIOSIL XL10 manufactured by Asahi Kasei Silicone Co., Ltd. Examples of vinyltris(2-methoxyethoxy)silane include A-172 manufactured by Montive Performance Materials Japan LLC, examples of vinylmethyldimethoxysilane include A-2171 manufactured by Montive Performance Materials Japan LLC, and GENIOSIL manufactured by Wacker Asahi Kasei Silicone Co., Ltd. Examples of octenyltrimethoxysilane include KBM-1083 manufactured by Shin-Etsu Chemical Co., Ltd., examples of allyltrimethoxysilane include Z-6825 manufactured by Dow Corning Toray Co., Ltd., examples of p-styryltrimethoxysilane include KBM-1403 manufactured by Shin-Etsu Chemical Co., Ltd., examples of 3-acryloxypropyltrimethoxysilane include KBM-5103, examples of 3-methacryloxypropylmethyldimethoxysilane include KBM-502 manufactured by Shin-Etsu Chemical Co., Ltd. and Z-6033 manufactured by Dow Corning Toray Co., Ltd., and examples of 3-methacryloxypropyltrimethoxysilane include KBM-503 manufactured by Shin-Etsu Chemical Co., Ltd., A-174 manufactured by Montive Performance Materials Japan LLC, Z-6030 manufactured by Dow Corning Toray Co., Ltd., and GENIOSIL manufactured by Wacker Asahi Kasei Silicone Co., Ltd. GF31, Sila Ace S710 manufactured by Nitto Shoji Co., Ltd., and the like. 3-methacryloxypropylmethyldiethoxysilane is,Examples of 3-methacryloxypropyltriethoxysilane include KBE-503 manufactured by Shin-Etsu Chemical Co., Ltd. and Y-9936 manufactured by Montive Performance Materials Japan LLC. Examples of methacryloxyoctyltrimethoxysilane include KBM-5803 manufactured by Shin-Etsu Chemical Co., Ltd. Examples of 2-(3,4-epoxycyclohexyl)ethyltrimethoxysilane include KBM-303 manufactured by Shin-Etsu Chemical Co., Ltd. and A-186 manufactured by Montive Performance Materials Japan LLC. Examples of 2-(3,4-epoxycyclohexyl)ethyltrimethoxysilane include KBM-303 manufactured by Shin-Etsu Chemical Co., Ltd. and A-186 manufactured by Montive Performance Materials Japan LLC. Examples of 3-glycidoxypropylmethyldimethoxysilane include KBM-402 manufactured by Shin-Etsu Chemical Co., Ltd., Z-6044 manufactured by Dow Corning Toray Co., Ltd., and Sila Ace S520 manufactured by Dow Corning Toray Co., Ltd. Examples of 3-glycidoxypropyltrimethoxysilane include KBM-403 manufactured by Shin-Etsu Chemical Co., Ltd., A-187 manufactured by Montiv Performance Materials Japan LLC, Z-6040 manufactured by Dow Corning Toray Co., Ltd., and GENIOSIL manufactured by Wacker Asahi Kasei Silicone Co., Ltd. Examples of 3-glycidoxypropylmethyldiethoxysilane include KBE-402 manufactured by Shin-Etsu Chemical Co., Ltd. Examples of 3-glycidoxypropyltriethoxysilane include KBE-403 manufactured by Shin-Etsu Chemical Co., Ltd., A-1871 manufactured by Montiv Performance Materials Japan LLC, and GENIOSIL GF82 manufactured by Wacker Asahi Kasei Silicone Co., Ltd. Examples of glycidoxyoctyltrimethoxysilane include KBM-4803 manufactured by Shin-Etsu Chemical Co., Ltd. Examples of N-2-(aminoethyl)-3-aminopropylmethyldimethoxysilane include KBM-602 manufactured by Shin-Etsu Chemical Co., Ltd., A-2120 manufactured by Montiv Performance Materials Japan LLC, and GENIOSIL GF82 manufactured by Wacker Asahi Kasei Silicone Co., Ltd. Examples of N-2-(aminoethyl)-3-aminopropyltrimethoxysilane include KBM-603 manufactured by Shin-Etsu Chemical Co., Ltd., and Sila-Ace S310 manufactured by Nitto Shoji Co., Ltd.Examples of the silane include A-1120 manufactured by Montiv Performance Materials Japan LLC, A-1122 manufactured by Montiv Performance Materials Japan LLC, Z-6020 manufactured by Dow Corning Toray Co., Ltd., Z-6094 manufactured by Dow Corning Toray Co., Ltd., GENIOSIL GF-91 manufactured by Wacker Asahi Kasei Silicone Co., Ltd., and Sila Ace S320 manufactured by Nichibi Shoji Co., Ltd. Examples of the 3-aminopropyltrimethoxysilane include KBM-903 manufactured by Shin-Etsu Chemical Co., Ltd., A-1110 manufactured by Montiv Performance Materials Japan LLC, Z-6610 manufactured by Dow Corning Toray Co., Ltd., and Sila Ace S360 manufactured by Nichibi Shoji Co., Ltd. Examples of the 3-aminopropyltriethoxysilane include KBE-903, Montiv Performance Examples of 3-triethoxysilyl-N-(1,3-dimethyl-butylidene)propylamine include KBE-9103 and Sila Ace S340 manufactured by Nichimi Shoji Co., Ltd. Examples of N-phenyl-3-aminopropyltrimethoxysilane include KBM-573 and Montiv manufactured by Shin-Etsu Chemical Co., Ltd. Examples of N,N'-bis[3-(trimethoxysilyl)propyl]ethylenediamine include Sila-Ace XS1003 manufactured by Nitto Shoji Co., Ltd. Examples of N-(vinylbenzyl)-2-aminoethyl-3-aminopropyltrimethoxysilane hydrochloride include KBM-575 manufactured by Shin-Etsu Chemical Co., Ltd. and Z-6883 manufactured by Toray Dow Corning Co., Ltd. Examples of the tris-(trimethoxysilylpropyl)isocyanurate include KBM-9659 manufactured by Shin-Etsu Chemical Co., Ltd. Examples of the 3-mercaptopropylmethyldimethoxysilane include KBM-802 manufactured by Shin-Etsu Chemical Co., Ltd. and Z-6852 manufactured by Dow Corning Toray Co., Ltd. Examples of the 3-mercaptopropyltrimethoxysilane include KBM-803 manufactured by Shin-Etsu Chemical Co., Ltd.Examples of 3-mercaptopropyltriethoxysilane include A-189 manufactured by Montiv Performance Materials Japan LLC, Z-6062 manufactured by Dow Corning Toray Co., Ltd., and Sila Ace S810 manufactured by Nichibi Shoji Co., Ltd. Examples of 3-mercaptopropyltriethoxysilane include A-1891 manufactured by Montiv Performance Materials Japan LLC and Z-6911 manufactured by Dow Corning Toray Co., Ltd. Examples of 3-ureidopropyltriethoxysilane include A-1160 manufactured by Montiv Performance Materials Japan LLC, and examples of 3-ureidopropyltrialkoxysilane include KBE-585 manufactured by Shin-Etsu Chemical Co., Ltd. Examples of bis(triethoxysilane) include A-1891 manufactured by Montiv Performance Materials Japan LLC and Z-6911 manufactured by Dow Corning Toray Co., Ltd. Examples of 3-octanoylthio-1-propyltriethoxysilane include KBE-846 manufactured by Shin-Etsu Chemical Co., Ltd., examples of 3-octanoylthio-1-propyltriethoxysilane include A-LINK599 manufactured by Montive Performance Materials Japan LLC, examples of 3-isocyanatepropyltriethoxysilane include KBE-9007 manufactured by Shin-Etsu Chemical Co., Ltd. and A-1310 manufactured by Montive Performance Materials Japan LLC, and examples of 3-isocyanatepropyltrimethoxysilane include Y-5187 manufactured by Montive Performance Materials Japan LLC and GENIOSIL GF40 manufactured by Wacker Asahi Kasei Silicone Co., Ltd.

[0072] When a silane coupling agent is blended into the additive composition of the present invention, the content thereof is preferably 0.01 to 5.0 parts by mass, more preferably 0.05 to 3.0 parts by mass, and even more preferably 0.1 to 2.0 parts by mass, relative to 100 parts by mass of the total amount of components (A) and (C) contained in the additive composition. The silane coupling agent may be blended into the additive composition of the present invention in advance, or may be blended into the synthetic resin when blending with the synthetic resin.

[0073] The additive composition of the present invention may contain a hydrotalcite compound, if necessary, to improve heat resistance, reduce the risk of corrosion in processing machines, and improve weather resistance, as long as the effects of the present invention are not impaired. In the additive composition of the present invention, the hydrotalcite compound refers to a carbonate double salt compound of magnesium and / or zinc with aluminum. The hydrotalcite compound may be a natural product or a synthetic product. Examples of methods for synthesizing synthetic products include known methods described in Japanese Patent Publication Nos. 46-2280, 50-30039, 51-29129, and 61-174270. Furthermore, the additive composition of the present invention can be used without any restrictions on the crystal structure, crystalline particle system, or the presence and amount of water of crystallization of the hydrotalcite compound.

[0074] Furthermore, the hydrotalcite compound can be treated with perchloric acid, and the surface thereof can be coated with a higher fatty acid such as stearic acid, a higher fatty acid metal salt such as an alkali metal salt of oleic acid, an organic sulfonic acid metal salt such as an alkali metal salt of dodecylbenzenesulfonic acid, a higher fatty acid amide, a higher fatty acid ester, or a wax, or the like.

[0075] The hydrotalcite compound is preferably a compound represented by the following general formula (5).

[0076] Mg x1 Zn x2 Al2(OH) 2(X1+X2)+4 CO₃mH₂O (5)

[0077] In the general formula (5), x1 and x2 each represent a number that satisfies the conditions expressed by the following formula, and m represents a real number: 0≦x2 / x1<10, 2≦x1+x2<20

[0078] Commercially available hydrotalcite compounds can be used, such as DHT-4 (hydrotalcite: manufactured by Kyowa Chemical Industry Co., Ltd.), DHT-4A (hydrotalcite: manufactured by Kyowa Chemical Industry Co., Ltd.), Magcera-1 (hydrotalcite: manufactured by Kyowa Chemical Industry Co., Ltd.), Alkamiser 1 (hydrotalcite: manufactured by Kyowa Chemical Industry Co., Ltd.), Alkamiser 2 (hydrotalcite: manufactured by Kyowa Chemical Industry Co., Ltd.), Alkamiser 4 (Alkamiser P-93) (zinc-modified hydrotalcite: manufactured by Kyowa Chemical Industry Co., Ltd.), Alkamiser 7 (zinc-modified hydrotalcite: manufactured by Kyowa Chemical Industry Co., Ltd.), Alkamiser 5 (perchloric acid-treated hydrotalcite: manufactured by Kyowa Chemical Industry Co., Ltd.), and the like, and DHT-4A (hydrotalcite: manufactured by Kyowa Chemical Industry Co., Ltd.) is particularly preferred.

[0079] When a hydrotalcite-based compound is contained, the content thereof is preferably 0.01 to 5 parts by mass relative to 100 parts by mass of the total amount of components (A) and (C) contained in the additive composition, and from the viewpoints of heat resistance, reduced corrosion risk of processing machines, and weather resistance, is more preferably 0.05 to 4 parts by mass, and even more preferably 0.1 to 2 parts by mass. The hydrotalcite compound may be blended in advance with the additive composition of the present invention, or may be blended with the synthetic resin when blending with the synthetic resin.

[0080] Furthermore, the additive composition of the present invention may contain, if necessary, a flame retardant aid other than the above-mentioned metal oxides, as long as the effect of the present invention is not impaired. Examples of the flame retardant aid include polyhydric alcohol compounds.

[0081] A polyhydric alcohol compound is a compound having multiple hydroxyl groups bonded thereto, and although it may overlap with the above-mentioned polyhydric alcohol compounds, it is a compound added as a flame retardant aid to improve flame retardancy. Examples of polyhydric alcohol compounds as flame retardant aids include pentaerythritol, dipentaerythritol, tripentaerythritol, polypentaerythritol, neopentyl glycol, trimethylolpropane, ditrimethylolpropane, 1,3,5-tris(2-hydroxyethyl)isocyanurate, polyethylene glycol, glycerin, diglycerin, mannitol, maltitol, lactitol, sorbitol, erythritol, xylitol, xylose, sucrose, trehalose, inositol, fructose, maltose, and lactose. Among these, pentaerythritol or pentaerythritol condensates such as pentaerythritol, dipentaerythritol, tripentaerythritol, and polypentaerythritol are preferred, pentaerythritol condensates are more preferred, and dipentaerythritol is particularly preferred. 1,3,5-tris(2-hydroxyethyl)isocyanurate and sorbitol can also be suitably used.

[0082] The pentaerythritol condensate may be a mixture of pentaerythritol and pentaerythritol condensates. When a polyhydric alcohol compound is contained, the content thereof is preferably 0.5 to 15 parts by mass, more preferably 2 to 12 parts by mass, and even more preferably 5 to 10 parts by mass, based on 100 parts by mass of the total amount of components (A) and (C) contained in the additive composition, from the viewpoint of flame retardancy. The polyhydric alcohol compound may be blended in advance with the additive composition of the present invention, or may be blended with the synthetic resin when blending with the synthetic resin.

[0083] Furthermore, the additive composition of the present invention may contain a lubricant, if necessary, within the range that does not impair the effects of the present invention. Examples of such lubricants include pure hydrocarbon-based lubricants such as liquid paraffin, natural paraffin, microwax, synthetic paraffin, low-molecular-weight polyethylene, and polyethylene wax; halogenated hydrocarbon-based lubricants; fatty acid-based lubricants such as higher fatty acids and oxyfatty acids; fatty acid amide-based lubricants such as fatty acid amides and bisfatty acid amides; ester-based lubricants such as lower alcohol esters of fatty acids, polyhydric alcohol esters of fatty acids such as glycerides, polyglycol esters of fatty acids, and fatty alcohol esters of fatty acids (ester waxes); lubricants based on metal soaps, fatty alcohols, polyhydric alcohols, polyglycols, polyglycerols, partial esters of fatty acids and polyhydric alcohols, partial esters of fatty acids and polyglycols or polyglycerols, silicone oils, mineral oils, and the like. Two or more types of lubricants may be used.

[0084] When a lubricant is contained, the content thereof is preferably 0.05 to 10 parts by mass, and more preferably 0.1 to 5 parts by mass, relative to 100 parts by mass of the total amount of components (A) and (C) contained in the additive composition. The lubricant may be blended in advance with the additive composition of the present invention, or may be blended with the synthetic resin when blending with the synthetic resin.

[0085] The additive composition of the present invention may further contain one or more organic or inorganic flame retardants or flame retardant auxiliaries, as needed, to the extent that the effects of the present invention are not impaired. Examples of such flame retardants or flame retardant auxiliaries include metal hydroxides, phosphate ester flame retardants, condensed phosphate ester flame retardants, inorganic phosphorus-based flame retardants, silicone-based flame retardants, metal oxides, boric acid compounds, expandable graphite, other inorganic flame retardant auxiliaries, and other organic flame retardants. These flame retardants or flame retardant auxiliaries may be blended into the additive composition of the present invention in advance, or may be blended into the synthetic resin when blending the synthetic resin with the additive composition.

[0086] Examples of metal hydroxides include magnesium hydroxide, aluminum hydroxide, calcium hydroxide, barium hydroxide, zinc hydroxide, and Kismer 5A (a trademark of magnesium hydroxide manufactured by Kyowa Chemical Industry Co., Ltd.).

[0087] Examples of phosphate ester-based flame retardants include trimethyl phosphate, triethyl phosphate, tributyl phosphate, tributoxyethyl phosphate, trischloroethyl phosphate, trisdichloropropyl phosphate, triphenyl phosphate, tricresyl phosphate, cresyl diphenyl phosphate, trixylenyl phosphate, octyl diphenyl phosphate, xylenyl diphenyl phosphate, trisisopropylphenyl phosphate, 2-ethylhexyl diphenyl phosphate, t-butylphenyl diphenyl phosphate, bis-(t-butylphenyl)phenyl phosphate, tris-(t-butylphenyl)phosphate, isopropylphenyl diphenyl phosphate, bis-(isopropylphenyl)diphenyl phosphate, and tris-(isopropylphenyl)phosphate.

[0088] Examples of condensed phosphate ester flame retardants include 1,3-phenylenebis(diphenyl phosphate), 1,3-phenylenebis(dixylenyl phosphate), bisphenol A bis(diphenyl phosphate), naphthalene-2,5-diyl-tetraphenyl bis(phosphate), [1,1'-biphenyl]-4,4'-diyl-tetraphenyl bis(phosphate), [1,1'-biphenyl]-4,4'-diyl-tetrakis(2,6-dimethylphenyl)bis(phosphate), tetraphenyl(thiobis(4,1-phenylene))bis(phosphate), and tetraphenyl(sulfonylbis(4,1-phenylene))bis(phosphate).

[0089] An example of an inorganic phosphorus-based flame retardant is red phosphorus.

[0090] Other inorganic flame retardant aids include inorganic compounds such as titanium oxide, aluminum oxide, magnesium oxide, and hydrotalcite, and surface-treated products thereof. Specific examples include various commercially available products such as TIPAQUE R-680 (titanium oxide trademark manufactured by Ishihara Sangyo Kaisha, Ltd.), Kyowamag 150 (magnesium oxide trademark manufactured by Kyowa Chemical Industry Co., Ltd.), DHT-4A (hydrotalcite: manufactured by Kyowa Chemical Industry Co., Ltd.), and Alkamiser 4 (zinc-modified hydrotalcite trademark manufactured by Kyowa Chemical Industry Co., Ltd.).

[0091] The additive composition of the present invention may contain, as needed, a phosphorus-based antioxidant, a thioether-based antioxidant, an ultraviolet absorber, a hindered amine-based light stabilizer, an antiaging agent, etc. These components may be blended into the additive composition of the present invention in advance, or may be blended into the synthetic resin when blending with the synthetic resin. It is preferable to stabilize the synthetic resin by blending these components.

[0092] Examples of phosphorus-based antioxidants include trisnonylphenyl phosphite, tris[2-tert-butyl-4-(3-tert-butyl-4-hydroxy-5-methylphenylthio)-5-methylphenyl]phosphite, tridecyl phosphite, octyldiphenyl phosphite, di(decyl)monophenyl phosphite, di(tridecyl)pentaerythritol diphosphite, di(nonylphenyl)pentaerythritol diphosphite, bis(2,4-ditert-butylphenyl)pentaerythritol diphosphite, bis(2,6-ditert-butyl-4-methylphenyl)pentaerythritol diphosphite, bis(2,4,6-tritert-butylphenyl)pentaerythritol diphosphite, bis(2,4-dicumylphenyl)pentaerythritol diphosphite, tetra(tridecyl)isopropylidenediphenol diphosphite, tetra(tridecyl)-4,4'-n-butylidenebis(2- tert-butyl-5-methylphenol) diphosphite, hexa(tridecyl)-1,1,3-tris(2-methyl-4-hydroxy-5-tert-butylphenyl)butane triphosphite, tetrakis(2,4-ditert-butylphenyl) biphenylene diphosphonite, 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide, 2,2'-methylenebis(4,6-tert-butylphenyl)-2-ethylhexyl phosphite, 2 Examples of suitable phosphorus-based antioxidants include 2'-methylenebis(4,6-tert-butylphenyl)octadecyl phosphite, 2,2'-ethylidenebis(4,6-di-tert-butylphenyl)fluorophosphite, tris(2-[(2,4,8,10-tetrakis-tert-butyldibenzo[d,f][1,3,2]dioxaphosphepin-6-yl)oxy]ethyl)amine, and phosphite of 2-ethyl-2-butylpropylene glycol and 2,4,6-tri-tert-butylphenol. The amount of these phosphorus-based antioxidants blended into the synthetic resin is preferably 0.001 to 10 parts by mass, and more preferably 0.05 to 5 parts by mass, per 100 parts by mass of the synthetic resin.

[0093] Examples of thioether-based antioxidants include dialkylthiodipropionates such as dilauryl thiodipropionate, dimyristyl thiodipropionate, and distearyl thiodipropionate, and pentaerythritol tetra(β-alkylthiopropionic acid) esters. The amount of these thioether-based antioxidants added to a synthetic resin is preferably 0.001 to 10 parts by mass, and more preferably 0.05 to 5 parts by mass, per 100 parts by mass of the synthetic resin.

[0094] Examples of the ultraviolet absorber include 2-hydroxybenzophenones such as 2,4-dihydroxybenzophenone, 2-hydroxy-4-methoxybenzophenone, 2-hydroxy-4-octoxybenzophenone, and 5,5'-methylenebis(2-hydroxy-4-methoxybenzophenone); 2-(2'-hydroxy-5'-methylphenyl)benzotriazole, 2-(2'-hydroxy-3',5'-di-tert-butylphenyl)-5-chlorobenzotriazole, and 2-(2'-hydroxy-3',5'- 2-(2'-hydroxyphenyl)benzotriazoles such as 2-(tert-butyl-5'-methylphenyl)-5-chlorobenzotriazole, 2-(2'-hydroxy-5'-tert-octylphenyl)benzotriazole, 2-(2'-hydroxy-3',5'-dicumylphenyl)benzotriazole, 2,2'-methylenebis(4-tert-octyl-6-(benzotriazolyl)phenol), and 2-(2'-hydroxy-3'-tert-butyl-5'-carboxyphenyl)benzotriazole; phenyl Benzoates such as ricinate, resorcinol monobenzoate, 2,4-ditert-butylphenyl-3,5-ditert-butyl-4-hydroxybenzoate, 2,4-ditert-amylphenyl-3,5-ditert-butyl-4-hydroxybenzoate, hexadecyl-3,5-ditert-butyl-4-hydroxybenzoate; substituted oxanilides such as 2-ethyl-2'-ethoxyoxanilide, 2-ethoxy-4'-dodecyloxanilide; ethyl-α-cyano-β,β-diphenylacrylate, methyl and triaryltriazines such as 2-(2-hydroxy-4-octoxyphenyl)-4,6-bis(2,4-di-tert-butylphenyl)-s-triazine, 2-(2-hydroxy-4-methoxyphenyl)-4,6-diphenyl-s-triazine, and 2-(2-hydroxy-4-propoxy-5-methylphenyl)-4,6-bis(2,4-di-tert-butylphenyl)-s-triazine. The amount of these ultraviolet absorbers blended in a synthetic resin is preferably 0.001 to 30 parts by mass, and more preferably 0.05 to 10 parts by mass, per 100 parts by mass of the synthetic resin.

[0095] Examples of the hindered amine light stabilizer include 2,2,6,6-tetramethyl-4-piperidyl stearate, 1,2,2,6,6-pentamethyl-4-piperidyl stearate, 2,2,6,6-tetramethyl-4-piperidyl benzoate, bis(2,2,6,6-tetramethyl-4-piperidyl)sebacate, bis(1,2,2,6,6-pentamethyl-4-piperidyl)sebacate, bis(1-octoxy-2,2,6,6-tetramethyl-4-piperidyl)sebacate, tetrakis(2,2,6,6-tetramethyl-4-piperidyl)- 1,2,3,4-Butanetetracarboxylate, Tetrakis(1,2,2,6,6-pentamethyl-4-piperidyl)-1,2,3,4-butanetetracarboxylate, Bis(2,2,6,6-tetramethyl-4-piperidyl)·bis(tridecyl)-1,2,3,4-butanetetracarboxylate, Bis(1,2,2,6,6-pentamethyl-4-piperidyl)·bis(tridecyl)-1,2,3,4-butanetetracarboxylate, Bis(1,2,2,6,6-pentamethyl-4-piperidyl)·bis(tridecyl)-1,2,3,4-butanetetracarboxylate, Bis(1,2,2,6,6-pentamethyl-4-piperidyl)-2-butyl-2-(3,5-di-tert-butyl) (4-hydroxybenzyl)malonate, 1,2,2,6,6-pentamethyl-4-piperidyl methacrylate, poly[{6-(1,1,3,3-tetramethylbutyl)amino-1,3,5-triazine-2,4-diyl}{(2,2,6,6-tetramethyl-4-piperidyl)imino}hexamethylene{(2,2,6,6-tetramethyl-4-piperidyl)imino}], 1,2,3,4-butanecarboxylic acid / 2,2-bis(hydroxymethyl)-1,3-propanediol / 3-hydroxy-2,2-dimethylpropanal / 1,2,2,6,6 -Pentamethyl-4-piperidinyl ester polycondensate, bis(1,2,2,6,6-pentamethyl-4-piperidyl) decanedioate / methyl 1,2,2,6,6-pentamethyl-4-piperidyl sebacate mixture, 2,2,6,6-tetramethyl-4-piperidyl methacrylate, 1-(2-hydroxyethyl)-2,2,6,6-tetramethyl-4-piperidinol / diethyl succinate polycondensate, 1,6-bis(2,2,6,6-tetramethyl-4-piperidylamino)hexane / dibromoethane polycondensate, 1,6-bis(2,2,6,6-tetramethyl-4-piperidylamino)hexane / 2,4-dichloro-6-morpholino-s-triazine polycondensate, 1,6-bis(2,2,6,6-tetramethyl-4-piperidylamino)hexane / 2,4-dichloro-6-tert-octylamino-s-triazine polycondensate, 1,5,8,12-tetrakis[2,4-bis(N-butyl-N-(2,2,6,6-tetramethyl-4-piperidyl)amino)-s-triazine-6-yl ]-1,5,8,12-tetraazadodecane, 1,5,8,12-tetrakis[2,4-bis(N-butyl-N-(1,2,2,6,6-pentamethyl-4-piperidyl)amino)-s-triazin-6-yl]-1,5,8,12-tetraazadodecane, 1,6,11-tris[2,4-bis(N-butyl-N-(2,2,6,6-tetramethyl-4-piperidyl)amino)-s-triazin-6-ylamino]undecane, 1,6,1 1-Tris[2,4-bis(N-butyl-N-(1,2,2,6,6-pentamethyl-4-piperidyl)amino)-s-triazin-6-ylamino]undecane, 3,9-bis[1,1-dimethyl-2-{tris(2,2,6,6-tetramethyl-4-piperidyloxycarbonyl)butylcarbonyloxy}ethyl]-2,4,8,10-tetraoxaspiro[5.5]undecane, 3,9-bis[1,1-dimethyl-2-{tris(2,2,6,6-tetramethyl-4-piperidyloxycarbonyl)butylcarbonyloxy}ethyl]-2,4,8,10-tetraoxaspiro[5.5]undecane, Examples of suitable hindered amine light stabilizers include (1,2,2,6,6-pentamethyl-4-piperidyloxycarbonyl)butylcarbonyloxy}ethyl)-2,4,8,10-tetraoxaspiro[5.5]undecane, bis(1-undecyloxy-2,2,6,6-tetramethylpiperidin-4-yl)carbonate, 2,2,6,6-tetramethyl-4-piperidylhexadecanoate, and 2,2,6,6-tetramethyl-4-piperidyloctadecanoate. The amount of these hindered amine light stabilizers blended into a synthetic resin is preferably 0.001 to 30 parts by mass, and more preferably 0.05 to 10 parts by mass, per 100 parts by mass of the synthetic resin.

[0096] Examples of antioxidants include naphthylamines, diphenylamines, p-phenyldiamines, quinolines, hydroquinone derivatives, monophenols, thiobisphenols, hindered phenols, phosphite esters, etc. The amount of these antioxidants added to a synthetic resin is preferably 0.001 to 10 parts by mass, and more preferably 0.05 to 5 parts by mass, per 100 parts by mass of the synthetic resin.

[0097] It is possible to blend phenolic antioxidants other than component (B) in the additive composition of the present invention, but the phenolic antioxidants cannot exhibit excellent heat resistance and flame retardancy unless used in combination with component (B). Of course, there is no problem with using them in combination with component (B).

[0098] Examples of phenolic antioxidants other than component (B) include 2,6-di-tert-butyl-p-cresol, 2,6-diphenyl-4-octadecyloxyphenol, distearyl (3,5-di-tert-butyl-4-hydroxybenzyl) phosphonate, 1,6-hexamethylenebis[(3,5-di-tert-butyl-4-hydroxyphenyl)propionic acid amide], 4,4'-thiobis(6-tert-butyl-m-cresol), 2,2'-methylenebis(4-methyl-6-tert-butylphenol), 2,2'-methylenebis(4-ethyl-6-tert-butylphenol), 4,4'-butylidenebis(6-tert-butyl-m-cresol), 2,2'-ethylidenebis(4,6-di-tert-butylphenol), 2,2'-ethylidenebis(4-sec-butyl-6-tert-butylphenol), 1,1,3-tris(2-methyl-4-hydroxy-5-tert-butylphenyl)butane, 2-tert-butyl-4-methyl-6-(2-acryloyloxy-3-tert-butyl-5-methylbenzyl)phenol methyl 3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate, stearyl (3,5-di-tert-butyl-4-hydroxyphenyl)propionate, tetrakis[methyl 3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate]methane, thiodiethylene glycol bis[(3,5-di-tert-butyl-4-hydroxyphenyl)propionate], 1,6-hexamethylene bis[(3,5-di-tert-butyl-4-hydroxyphenyl)propionate], bis[3,3-bis(4-hydroxy-3-tert-butylphenyl)butyric acid bis[2-tert-butyl-4-methyl-6-(2-hydroxy-3-tert-butyl-5-methylbenzyl)phenyl]terephthalate, 3,9-bis[1,1-dimethyl-2-{(3-tert-butyl-4-hydroxy-5-methylphenyl)propionyloxy}ethyl]-2,4,8,10-tetraoxaspiro[5,5]undecane, triethylene glycol bis[(3-tert-butyl-4-hydroxy-5-methylphenyl)propionate], and the like.

[0099] The additive composition of the present invention may contain a reinforcing material as an optional component, provided that the effects of the present invention are not impaired. These components may be blended into the synthetic resin when the additive composition of the present invention is blended with the synthetic resin. The reinforcing material may be in the form of a fiber, plate, granule, or powder, which is typically used to reinforce synthetic resins. Specific examples of the reinforcing material include inorganic fibrous reinforcing materials such as glass fiber, asbestos fiber, carbon fiber, graphite fiber, metal fiber, potassium titanate whisker, aluminum borate whisker, magnesium whisker, silicon whisker, wollastonite, sepiolite, asbestos, slag fiber, zonolite, elestadite, gypsum fiber, silica fiber, silica-alumina fiber, zirconia fiber, boron nitride fiber, silicon nitride fiber, and boron fiber; polyester fiber, nylon fiber, acrylic fiber, regenerated cellulose fiber, acetate fiber, kenaf, ramie, cotton, jute, hemp, rhinoceros fiber, and the like. Examples of suitable reinforcing materials include organic fibrous reinforcing materials such as colander, flax, linen, silk, Manila hemp, sugarcane, wood pulp, wastepaper, recycled paper, and wool, as well as plate-like and granular reinforcing materials such as glass flakes, non-swelling mica, graphite, metal foil, ceramic beads, clay, mica, sericite, zeolite, bentonite, dolomite, kaolin, finely powdered silicic acid, feldspar powder, potassium titanate, silicic acid balloons, calcium carbonate, magnesium carbonate, barium sulfate, calcium oxide, aluminum oxide, titanium oxide, aluminum silicate, silicon oxide, gypsum, novaculite, dawsonite, and clay. These reinforcing materials may be coated or bundled with a thermoplastic resin such as ethylene / vinyl acetate copolymer or a thermosetting resin such as epoxy resin, or may be treated with a coupling agent such as aminosilane or epoxysilane.

[0100] The additive composition of the present invention may further contain a nucleating agent as an optional component, as long as it does not impair the effects of the present invention. As the nucleating agent, those generally used as nucleating agents for polymers can be used appropriately, and in the present invention, both inorganic nucleating agents and organic nucleating agents can be used. These components may be added to the synthetic resin when the additive composition of the present invention is added to the synthetic resin.

[0101] Specific examples of inorganic crystal nucleating agents include kaolinite, synthetic mica, clay, zeolite, silica, graphite, carbon black, magnesium oxide, titanium oxide, calcium sulfide, boron nitride, calcium carbonate, barium sulfate, aluminum oxide, neodymium oxide, and metal salts such as phenylphosphonate, etc. These inorganic crystal nucleating agents may be modified with an organic substance to enhance dispersibility in the composition.

[0102] Specific examples of organic crystal nucleating agents include sodium benzoate, potassium benzoate, lithium benzoate, calcium benzoate, magnesium benzoate, barium benzoate, lithium terephthalate, sodium terephthalate, potassium terephthalate, calcium oxalate, sodium laurate, potassium laurate, sodium myristate, potassium myristate, calcium myristate, sodium octacosanoate, calcium octacosanoate, sodium stearate, potassium stearate, lithium stearate, calcium stearate, magnesium stearate, barium stearate, sodium montanate, calcium montanate, sodium toluate, sodium salicylate, potassium salicylate, zinc salicylate, Examples of suitable organic carboxylic acid metal salts include aluminum dibenzoate, potassium dibenzoate, lithium dibenzoate, sodium β-naphthalate, and sodium cyclohexanecarboxylate; organic sulfonates such as sodium p-toluenesulfonate and sodium sulfoisophthalate; carboxylic acid amides such as stearic acid amide, ethylene bislauric acid amide, palmitic acid amide, hydroxystearic acid amide, erucic acid amide, and trimesic acid tris(t-butylamide); benzylidene sorbitol and derivatives thereof; metal salts of phosphorus compounds such as sodium 2,2'-methylenebis(4,6-di-t-butylphenyl)phosphate; and 2,2-methylbis(4,6-di-t-butylphenyl)sodium.

[0103] Furthermore, the additive composition of the present invention may contain, as an optional component, a known neutralizing agent to neutralize residual catalyst in the synthetic resin, provided that the effects of the present invention are not impaired. Examples of neutralizing agents include fatty acid metal salts such as calcium stearate, lithium stearate, and sodium stearate, and fatty acid amide compounds such as ethylene bis(stearamide), ethylene bis(12-hydroxystearamide), and stearic acid amide. These neutralizing agents may be used in combination.

[0104] Furthermore, the additive composition of the present invention may further contain an acrylic processing aid as an optional component, provided that the effects of the present invention are not impaired. The acrylic processing aid may be a polymerized (meth)acrylic acid ester or a copolymerized (meth)acrylic acid ester of two or more. These components may be added to a synthetic resin when the flame retardant composition of the present invention is blended with the synthetic resin. Examples of the (meth)acrylic acid ester to be polymerized or copolymerized include (meth)acrylic acid esters such as methyl acrylate, methyl methacrylate, ethyl acrylate, ethyl methacrylate, n-propyl acrylate, isopropyl acrylate, n-propyl methacrylate, isopropyl methacrylate, n-butyl acrylate, isobutyl acrylate, t-butyl methacrylate, n-hexyl acrylate, n-hexyl methacrylate, 2-ethylhexyl acrylate, 2-ethylhexyl methacrylate, dodecyl methacrylate, and tridecyl methacrylate. In addition to these, (meth)acrylic acid and (meth)acrylic acid esters containing a hydroxy group are also included.

[0105] The additive composition of the present invention may contain a plasticizer as an optional component, provided that the effects of the present invention are not impaired. Plasticizers generally used as plasticizers for polymers can be used as appropriate, and examples thereof include polyester-based plasticizers, glycerin-based plasticizers, polycarboxylic acid ester-based plasticizers, polyalkylene glycol-based plasticizers, ether ester-based plasticizers, and epoxy-based plasticizers. These components may be added to a synthetic resin when the additive composition of the present invention is added to the synthetic resin.

[0106] In addition, the additive composition of the present invention may contain additives commonly used in synthetic resins, such as crosslinking agents, antistatic agents, metal soaps, fillers, antifogging agents, antiplate-out agents, surface treatment agents, fluorescent agents, antifungal agents, bactericides, foaming agents, metal deactivators, release agents, pigments, processing aids other than acrylic processing aids, etc., as long as the effects of the present invention are not impaired. These components may be blended into the synthetic resin when the additive composition of the present invention is blended into the synthetic resin.

[0107] When mixing the components of the additive composition of the present invention or when mixing with other compounding components, various mixers can be used. Heat may be applied during mixing. Examples of mixers that can be used include a tumbler mixer, Henschel mixer, ribbon blender, V-type mixer, W-type mixer, Super mixer, Nauta mixer, etc.

[0108] The additive composition of the present invention can impart excellent heat resistance and flame retardancy to synthetic resins, and is therefore preferably blended with synthetic resins to form flame-retardant synthetic resin compositions having excellent heat resistance. The flame-retardant synthetic resin compositions of the present invention can be used to obtain molded articles having excellent heat resistance and flame retardancy.

[0109] Next, the flame-retardant synthetic resin composition of the present invention will be described. The flame-retardant synthetic resin composition of the present invention is obtained by blending the additive composition of the present invention with a synthetic resin.

[0110] Specific examples of synthetic resins that can be made flame retardant by the additive composition of the present invention include α-olefin polymers such as polypropylene, high-density polyethylene, low-density polyethylene, linear low-density polyethylene, cross-linked polyethylene, ultra-high molecular weight polyethylene, polybutene-1, and poly-3-methylpentene; polyolefins such as ethylene-vinyl acetate copolymer, ethylene-ethyl acrylate copolymer, and ethylene-propylene copolymer, and copolymers thereof; polyvinyl chloride, polyvinylidene chloride, chlorinated polyethylene, chlorinated polypropylene, polyvinylidene fluoride, chlorinated rubber, vinyl chloride-vinyl acetate copolymer, vinyl chloride-ethylene copolymer, vinyl chloride-vinylidene chloride copolymer, vinyl chloride-vinylidene chloride-vinyl acetate terpolymer, vinyl chloride-acrylic acid ester copolymer, and vinyl chloride-maleic acid ester copolymer. halogen-containing resins such as vinyl chloride-cyclohexylmaleimide copolymers; petroleum resins, coumarone resins, polystyrene, polyvinyl acetate, acrylic resins, polymethyl methacrylate, polyvinyl alcohol, polyvinyl formal, polyvinyl butyral; aromatic polyesters such as polyalkylene terephthalates such as polyethylene terephthalate, polybutylene terephthalate, and polycyclohexanedimethylene terephthalate, polyalkylene naphthalates such as polyethylene naphthalate and polybutylene naphthalate, and linear polyesters such as polytetramethylene terephthalate; degradable aliphatic polyesters such as polyhydroxybutyrate, polycaprolactone, polybutylene succinate, polyethylene succinate, polylactic acid resin, polymalic acid, polyglycolic acid, polydioxane, and poly(2-oxetanone);Examples of the resin include polyamides such as polyphenylene oxide, polycaprolactam, and polyhexamethylene adipamide, thermoplastic resins such as polycarbonate, branched polycarbonate, polyacetal, polyphenylene sulfide, polyurethane, and cellulose-based resins, and blends thereof; thermosetting resins such as phenolic resin, urea resin, melamine resin, epoxy resin, and unsaturated polyester resin; fluorine-based resins, silicone resins, silicone rubber, polyethersulfone, polysulfone, polyphenylene ether, polyether ketone, polyether ether ketone, and liquid crystal polymers. Further examples include isoprene rubber, butadiene rubber, acrylonitrile-butadiene copolymer rubber, styrene-butadiene copolymer rubber, fluororubber, and silicone rubber.

[0111] Specific examples of synthetic resins to be flame-retarded include olefin-based thermoplastic elastomers, styrene-based thermoplastic elastomers, polyester-based thermoplastic elastomers, nitrile-based thermoplastic elastomers, nylon-based thermoplastic elastomers, vinyl chloride-based thermoplastic elastomers, polyamide-based thermoplastic elastomers, and polyurethane-based thermoplastic elastomers. These synthetic resins may be used alone or in combination. The synthetic resins may also be alloyed.

[0112] The synthetic resin used in the synthetic resin composition of the present invention can be used regardless of molecular weight, degree of polymerization, density, softening point, proportion of solvent-insoluble matter, degree of stereoregularity, presence or absence of catalyst residue, types and blending ratios of raw material monomers, type of polymerization catalyst (e.g., Ziegler catalyst, metallocene catalyst, etc.), etc. Among these synthetic resins, polyolefin-based resins are preferred because they can impart excellent flame retardancy.

[0113] Examples of polyolefin resins include polyethylene, low-density polyethylene, linear low-density polyethylene, high-density polyethylene, polypropylene, homopolypropylene, random copolymer polypropylene, block copolymer polypropylene, impact copolymer polypropylene, high-impact copolymer polypropylene, isotactic polypropylene, syndiotactic polypropylene, hemiisotactic polypropylene, maleic anhydride-modified polypropylene, polybutene, cycloolefin polymer, stereoblock polypropylene, α-olefin polymers such as poly-3-methyl-1-butene, poly-3-methyl-1-pentene, and poly-4-methyl-1-pentene; ethylene / propylene block or random copolymers; and α-olefin copolymers such as ethylene-methyl methacrylate copolymer and ethylene-vinyl acetate copolymer.

[0114] In the synthetic resin composition of the present invention, the total amount of components (A) and (C) contained in the additive composition is preferably 10% by mass or more and less than 70% by mass, more preferably 15% by mass or more and less than 60% by mass, and even more preferably 20% by mass or more and less than 50% by mass, from the viewpoints of heat resistance and flame retardancy. If it is less than 10% by mass, sufficient flame retardancy may not be exhibited, and if it is 70% by mass or more, the inherent physical properties of the resin may be impaired.

[0115] Next, the molded article of the present invention will be described. The molded article of the present invention is obtained from the flame-retardant synthetic resin composition of the present invention. By molding the synthetic resin composition of the present invention, a molded article having excellent heat resistance and flame retardancy can be obtained. The molding method is not particularly limited, and examples thereof include extrusion processing, calendar processing, injection molding, roll molding, compression molding, blow molding, etc., and molded articles of various shapes such as resin plates, sheets, films, and irregular shapes can be produced.

[0116] The synthetic resin composition of the present invention and its molded article can be used for housings (frames, enclosures, covers, exteriors) and parts for electric vehicles, machines, electric and electronic equipment, office automation equipment, etc., and for automobile interior and exterior materials, etc.

[0117] The synthetic resin composition of the present invention and its molded article can be used in a wide range of industrial fields, including electricity, electronics, and communications, agriculture, forestry, and fisheries, mining, construction, food, textiles, clothing, medicine, coal, petroleum, rubber, leather, automobiles, precision instruments, wood, building materials, civil engineering, furniture, printing, and musical instruments. More specifically, they are used in office and office equipment such as printers, personal computers, word processors, keyboards, PDAs (personal digital assistants), telephones, copiers, facsimiles, ECRs (electronic cash registers), calculators, electronic organizers, cards, holders, stationery, etc.; home appliances such as washing machines, refrigerators, vacuum cleaners, microwave ovens, lighting fixtures, game consoles, irons, kotatsu table, etc.; audio-visual equipment such as TVs, VCRs, video cameras, radio cassette players, tape recorders, minidiscs, CD players, speakers, and LCD displays; electrical and electronic components such as connectors, relays, capacitors, switches, printed circuit boards, coil bobbins, semiconductor encapsulation materials, LED encapsulation materials, electric wires, cables, transformers, deflection yokes, distribution boards, and clocks; and communication equipment, housings (frames, enclosures, covers, exteriors) and parts for office equipment, etc.; and automotive interior and exterior materials.

[0118] Furthermore, the synthetic resin composition of the present invention and its molded article can be used for seats (padding, surface, etc.), belts, ceiling coverings, convertible tops, armrests, door trims, rear package trays, carpets, mats, sun visors, wheel covers, mattress covers, airbags, insulating materials, hand straps, hand straps, wire covering materials, electrical insulating materials, paints, coating materials, covering materials, flooring materials, corner walls, carpets, wallpaper, wall covering materials, exterior materials, interior materials, roofing materials, deck materials, wall materials, pillar materials, and paving materials. It is used for a variety of purposes, including boards, fence materials, frames and moldings, window and door profiles, shingles, paneling, terraces, balconies, soundproofing boards, heat insulating boards, window materials, etc. for automobiles, hybrid cars, electric cars, vehicles, ships, aircraft, buildings, houses and construction materials, civil engineering materials, clothing, curtains, sheets, plywood, synthetic fiber boards, carpets, entrance mats, sheets, buckets, hoses, containers, eyeglasses, bags, cases, goggles, skis, rackets, tents, musical instruments and other daily necessities and sporting goods. [Example]

[0119] [Preparation of Additive Compositions 1 to 12] Additive compositions 1 to 12 of the present invention were produced using the blending ratios (parts by mass) shown in Tables 1 and 2. The following compounds B-1 and B-2 were used as component (B).

[0120] TIFF0007811086000009.tif68169

[0121] [Preparation of Comparative Additive Compositions 1 to 12] Comparative additive compositions 1 to 12 were produced at the blending ratios (parts by mass) shown in the following Tables 3 and 4. In the comparative additive compositions 1 to 12, comparative phenolic antioxidants 1 to 3 were used in place of component (B).

[0122] [Table 1] *1: Ammonium polyphosphate (degree of polymerization 1000) *2: Poly-[2,4-(piperazin-1,4-yl)-6-(morpholino-4-yl)-1,3,5-triazine] *3: Melamine cyanurate *4: Tetrakis[3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionic acid methyl]methane *5: 1,1,3-tris(2-methyl-4-hydroxy-5-tert-butylphenyl)butane *6: 3,9-bis[1,1-dimethyl-2-{(3-tert-butyl-4-hydroxy-5-methylphenyl)propionyloxy}ethyl]-2,4,8,10-tetraoxaspiro[5,5]undecane

[0123] [Table 2]

[0124] [Table 3]

[0125] [Table 4]

[0126] [Examples 1 to 6, Reference Examples 1 to 8, and Comparative Examples 1 to 14] To a polypropylene resin composition prepared by blending 0.1 part by mass of calcium stearate (lubricant), 0.1 part by mass of tris(2,4-di-tert-butylphenyl) phosphite (phosphorus antioxidant), and 0.3 part by mass of glycerin monostearate (lubricant) in the amounts (parts by mass) shown in Tables 5 and 6, additive compositions 1 to 12 were added in the amounts (parts by mass) shown in Tables 5 and 6 to obtain synthetic resin compositions of Examples 1 to 6 and Reference Examples 1 to 8. These were extruded at 200 to 220°C to produce pellets, which were then injection-molded at 200 to 220°C to obtain two types of test pieces measuring 60 × 30 × 2 mm and 127 × 12.7 × 1.6 mm, as well as test pieces for tensile strength measurement. These test pieces were used to conduct the various tests described below. The results are shown in Tables 5 and 6.

[0127] Furthermore, synthetic resin compositions of Comparative Examples 1 to 14 were obtained by adding Comparative Additive Compositions 1 to 12 in the amounts (parts by mass) shown in Tables 7 and 8. Test pieces were obtained in the same manner and subjected to the following various tests. The results are also shown in Tables 7 and 8.

[0128] <Flame retardancy UL-94V test method> A 127 x 12.7 x 1.6 mm test specimen was held vertically, and a burner flame was applied to the bottom edge for 10 seconds. The flame was then removed, and the time it took for the flame to extinguish was measured. Next, as soon as the flame extinguished, a second flame was applied for 10 seconds, and the time it took for the flame to extinguish was measured in the same manner as the first. The test specimen was also evaluated for ignition of the cotton underneath by the falling embers. A flammability rating was assigned according to the UL-94V standard based on the first and second burning times and whether or not the cotton ignited. V-0 is the highest flammability rating, with flame retardancy decreasing as the ratings progress from V-1 to V-2. However, specimens not meeting any of the V-0 to V-2 ratings were classified as NR. In this invention, specimens with a rating of V-2 or lower are not suitable for practical use.

[0129] <Cracks> A test piece of 60 × 30 × 2 mm was placed in an oven at 150 ° C. and visually inspected every 24 hours for cracks. The time until cracks appeared was measured. The longer the time until cracks appeared, the better the heat resistance, and the shorter the time until cracks appeared, the worse the heat resistance. In the present invention, a test piece that had been left standing for less than 800 hours was not suitable for practical use.

[0130] <Tensile strength> The test was conducted in accordance with ISO 527. Specifically, the test piece for tensile strength was placed in an oven at 150°C, and the tensile strength was measured every 48 hours. The time until the tensile strength value fell to 70% or less of the initial value before being placed in the oven was measured. The longer the time until the value fell to 70% or less, the better the heat resistance, and the shorter the time until the value fell to 70% or less, the poorer the heat resistance.

[0131] [Table 5]

[0132] [Table 6]

[0133] [Table 7]

[0134] [Table 8]

[0135] From the results in Tables 1 to 8, it is clear that the present invention can provide an additive composition that can impart excellent heat resistance and flame retardancy to a synthetic resin. It is also clear from the results in Tables 1 to 8 that the present invention can provide a flame-retardant synthetic resin composition that is excellent in heat resistance and flame retardancy. It is also clear from the results in Tables 1 to 8 that the present invention can provide a molded article that is excellent in heat resistance and flame retardancy.

Claims

1. The composition contains, as component (A), one or more ammonium polyphosphates, and as component (B), at least one compound selected from the group consisting of compounds represented by the following general formula (1): An additive composition characterized in that it further contains, as component (C), one or more nitrogen-containing organic compounds other than the compound represented by general formula (1), the mass ratio of component (A) / component (C) is (A) / (C)=50 / 50 to 80 / 20, and the nitrogen-containing organic compound of component (C) is at least one or more triazine derivatives. In general formula (1), R 1 , R 2 and R 3 each independently represents a divalent hydrocarbon group having 1 to 3 carbon atoms.

2. 10. A flame-retardant synthetic resin composition comprising a synthetic resin and the additive composition according to claim 1 blended therewith.

3. 3. The flame-retardant synthetic resin composition according to claim 2, wherein the synthetic resin is a polyolefin resin.

4. A molded article obtained from the flame-retardant synthetic resin composition according to claim 2 or 3.

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