EP2619821A1 - Boîtier de batterie ignifugé à résilience modifiée à base de polycarbonate ii - Google Patents

Boîtier de batterie ignifugé à résilience modifiée à base de polycarbonate ii

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Publication number
EP2619821A1
EP2619821A1 EP11764137.3A EP11764137A EP2619821A1 EP 2619821 A1 EP2619821 A1 EP 2619821A1 EP 11764137 A EP11764137 A EP 11764137A EP 2619821 A1 EP2619821 A1 EP 2619821A1
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EP
European Patent Office
Prior art keywords
parts
weight
sum
alkyl
components
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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Application number
EP11764137.3A
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German (de)
English (en)
Inventor
Thomas Eckel
Ulrich Grosser
Claus RÜDIGER
Achim Feldermann
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Bayer Intellectual Property GmbH
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Bayer Intellectual Property GmbH
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Publication of EP2619821A1 publication Critical patent/EP2619821A1/fr
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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/78—Cases; Housings; Encapsulations; Mountings
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L69/00—Compositions of polycarbonates; Compositions of derivatives of polycarbonates
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/204—Racks, modules or packs for multiple batteries or multiple cells
    • H01M50/207—Racks, modules or packs for multiple batteries or multiple cells characterised by their shape
    • H01M50/209—Racks, modules or packs for multiple batteries or multiple cells characterised by their shape adapted for prismatic or rectangular cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/204—Racks, modules or packs for multiple batteries or multiple cells
    • H01M50/207—Racks, modules or packs for multiple batteries or multiple cells characterised by their shape
    • H01M50/213—Racks, modules or packs for multiple batteries or multiple cells characterised by their shape adapted for cells having curved cross-section, e.g. round or elliptic
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/218—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by the material
    • H01M50/22—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by the material of the casings or racks
    • H01M50/222—Inorganic material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/218—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by the material
    • H01M50/22—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by the material of the casings or racks
    • H01M50/227—Organic material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/218—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by the material
    • H01M50/22—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by the material of the casings or racks
    • H01M50/229—Composite material consisting of a mixture of organic and inorganic materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/233—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by physical properties of casings or racks, e.g. dimensions
    • H01M50/24—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by physical properties of casings or racks, e.g. dimensions adapted for protecting batteries from their environment, e.g. from corrosion
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/233—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by physical properties of casings or racks, e.g. dimensions
    • H01M50/242—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by physical properties of casings or racks, e.g. dimensions adapted for protecting batteries against vibrations, collision impact or swelling
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/13—Energy storage using capacitors

Definitions

  • the present invention relates to flame retardant impact-modified polycarbonate-based battery cases containing a graft polymer containing a butadiene or acrylate rubber and a phosphorus flame retardant having good low-temperature impact strength combined with high Bmden absorbency and good flame retardancy and chemical resistance exhibit. Furthermore, the present invention relates to the use of the polycarbonate compositions according to the invention for the production of battery housings,
  • EP 0 363 608 describes polymer blends of aromatic polycarbonate, styrenic copolymer or graft copolymer and oligomeric phosphates as flame retardant additives.
  • the mechanical property level at low application temperatures, in particular the Bindenahtfestmaschine and the flow behavior is not sufficient.
  • EP 0 704 488 describes molding compositions of aromatic polycarbonate, styrene-containing copolymers and graft polymers with a specific graft base in specific proportions. If desired, these molding compositions can be rendered flame-resistant with phosphorus compounds. These molding compounds have a very good notched impact strength, but flow behavior, flame retardance and chemical resistance are not sufficient for certain applications.
  • EP 747 424 describes thermoplastic resins containing phosphate compounds having a molecular weight of 500 to 2000 and phosphate compounds having a molecular weight of 2300 to 11000 as a flame retardant, listing a variety of thermoplastic resins. Due to the high molecular weights of the phosphorus compounds, the flow behavior of the molding compositions is significantly impaired.
  • EP 754 531 describes reinforced PC ABS molding compositions which are suitable for precision parts. As flame retardants, among others, oligophosphates of the BPA type are used. The high filler contents have a very detrimental effect on the machanic properties, especially at low application temperatures and flow behavior.
  • EP 755 977 describes polymer blends of aromatic polycarbonate, graft copolymer having a rubber content of ⁇ 25% and oligomeric phosphates of ⁇ 8%. Due to the limited flame retardant content, the flow behavior and the flame resistance are not sufficient. In addition, there are no indications of the desired good toughness at low application temperatures.
  • EP 1 003 809 describes PC / ABS molding compositions containing oligomeric phosphorus compounds and graft polymers of a grafting base having a certain particle size. These molding compositions are characterized by good mechanical properties, in particular under increased elasticity stress. Their flow behavior and their flame retardancy are not sufficient for certain applications.
  • EP 0 983 315 describes molding compositions of aromatic polycarbonate, graft polymer and a flame retardant combination of a monomeric and an oligomeric phosphorus compound. These molding compositions have a high heat resistance and excellent mechanical properties (notched impact strength and Bindenahtfestmaschine), however, the flow behavior and flame retardancy are not sufficient, especially in the case of moldings with thin walls.
  • EP 1 165 680 describes flame-retardant PC / ABS molding compositions having good mechanical properties (tensile strength, weld line strength) containing oligomeric phosphates with a defined chain length.
  • the quantitative ranges for flame retardants and graft polymer are very broad. Therefore, the property combination according to the invention of good mechanical properties at low application temperatures and good flame retardancy is not described.
  • EP-A 635547 discloses flame-retardant polycarbonate compositions containing polycarbonate, a copolymer gel, an acrylate or diene rubber-based toughening modifier, a flame retardant such as oligophosphate and optionally an impact modifier having a diene rubber, acrylate rubber or EPDM rubber backbone.
  • EP-A 635547 does not disclose battery housings having the property combination according to the invention of good impact strength at elevated temperatures in combination with high weld line strength and good flame retardancy and excellent chemical resistance.
  • the object of the present invention was therefore to provide polycarbonate compositions for the manufacture of battery cases as well as the battery cases themselves, which have a good impact strength at low temperatures in combination with a high Bindenahtfestmaschine and a good flame retardancy and excellent chemical resistance.
  • battery housing in the sense The present invention also includes housings for stationary and mobile rechargeable power sources such as accumulators and capacitors.
  • Maleic anhydride C 1 -C 4 alkyl- or -phenyi-N-substituted maleimides or
  • B.2 5 to 95, preferably 20 to 70 parts by weight of a rubbery grafting would be based on butadiene or acrylate.
  • thermoplastic Vmyi (co) polymer E.I.
  • / or polyalkylene terephthalate E.2
  • the composition is free of thermoplastic vinyl (co) polymers (E.I.) and / or polyalkylene terephthalates (E.2), and
  • compositions 0 to 20.0 parts by weight, preferably 0, 1 to 10.0 parts by weight, particularly preferably 0.2 to 5.0 parts by weight (based on the sum of the parts by weight of the components A + B + C) further additives, wherein the compositions are preferably free of rubber-free Polyalky! (A! Kyi) acrylate, and wherein all parts by weight in the present application are normalized so that the sum of theDSsstei le of the components A + B + C in the composition 100, have the desired property profile.
  • Aromatic polycarbonates and / or aromatic polyester carbonates according to component A which are suitable according to the invention are known from the literature or can be prepared by processes known from the literature (for example, see Schnell, Chemistry and Physics of Polycarbonates, Interscience Publishers, 1964 and DE-AS 1 495 626, for the preparation of aromatic polycarbonates.
  • the preparation of aromatic polycarbonates z. B.
  • Diphenoie for the preparation of the aromatic polycarbonates and / or aromatic polyester carbonates are preferably those of the formula (I)
  • Heteroatom-containing rings may be condensed
  • B are each C, to C-alkyl, preferably methyl, halogen, preferably chlorine and / or bromine
  • x each independently 0, 1 or 2
  • R 7 and R s are individually selectable for each X 1 , independently of one another hydrogen or C 3 to C -
  • Alkyl preferably hydrogen, methyl or ethyl
  • m is an integer from 4 to 7, preferably 4 or 5, with the proviso that on at least one atom X 3 , R 'and R 8 are simultaneously alkyl.
  • Preferred diphenols are hydrohionone, resorcinol, dihydroxydiphenols, bis (hydroxyphenyl) C 1 -C 4 alkanes, bis (hydroxyphenyl) C 5 -C 8 -cycloalkanes, bis (hydroxyphenyl) ethers, bis (hydroxyphenyl) sulfoxides, bis (hydroxyphenyl) ketones, bis (hydroxyphenyl) sulfones and oc, a-bis (hydroxyphenyl) diisopropyl-benzenes and their nuclear-brominated and / or ring-chlorinated derivatives.
  • Particularly preferred diphenols are 4,4'-dihydroxydiphenyl, bisphenol -A, 2,4-bis (4-hydroxyphenyl) -2-methylbutane, 1, bis (4-hydroxyphenyl) cyclohexane, 1, 1 -Bis - (4-hydroxyphenyl) -3.3, 5-trimethylcyclohexane, 4,4'-dihydroxydiphenylsulfide, 4,4'-dihydroxydiphenylsulfone and their di- and tetrabrominated or chlorinated derivatives such as 2,2-bis (3-chloro-4-hydroxyphe - nyi) -propane, 2,2-bis (3,5-dichloro-4-hydroxyphenyl) -propane or 2,2-bis (3,5-dibromo-4-hydroxyphenyl) -propane.
  • 2,2-bis (4-hydroxyphenyl) propane bisphenol A
  • the diphenols can be used individually or as any mixtures.
  • the diphenols are known from the literature or obtainable by literature methods.
  • Chain terminators which are suitable for the preparation of the thermoplastic, aromatic polycarbonates are, for example, phenol, p-chlorophenol, p-tert-butylphenol or 2,4,6-tribromophenol, but also long-chain alkylphenols, such as 4- [2- (2,4,4 -Trimethylpentyi)] - phenol, 4- (l, 3-tetramethyl-butyl) -phenol according to DE-A 2,842,005 or monoalkylphenol or dialkylphenols having a total of 8 to 20 carbon atoms in the alkyl substituents such as 3,5-di-tert.
  • the amount of chain terminators to be used is generally between 0.5 mol% and 10 mol%, based on the molar sum of the diphenols used in each case.
  • thermoplastic aromatic polycarbonates have weight average molecular weight (M w , measured for example by GPC, ultracentrifuge or scattered light measurement) of 10,000 to 200,000 g / mol, preferably 15,000 to 80,000 g / mol, particularly preferably 24,000 to 32,000 g / mol.
  • the thermoplastic, aromatic Polvcarbonate may be branched in a known manner, preferably by the incorporation of 0.05 to 2.00 mol%, based on the sum of the diphenols used, of three functional or more than trifunctional compounds, for example those with three and more phenolic groups. Both homopolycarbonates and copolycarbonates are suitable.
  • copolycarbonates of component A For the preparation of copolycarbonates of component A according to the invention, 1.0 to 25.0% by weight, preferably 2.5 to 25.0% by weight, based on the total amount of diphenols to be used, of hydroxyaryloxy endblocked polydiorganosiloxanes. These are known (US Pat. No. 3,419,634) and can be obtained by literature methods. The preparation of polydiorganosiloxane-containing copolycarbonates is described in DE-A 3 334 782.
  • Preferred polycarbonates are, in addition to the bisphenol A homopolycarbonates, the copolycarbonates of bisphenol A with up to 15 mol%, based on the molar sums of diphenols, other than preferred or particularly preferred diphenols, in particular 2,2-bis (3,5 dibromo-4-hydroxyphenyl) -propane.
  • Aromatic dicarboxylic acid dihalides for preparing aromatic polyester carbonates are preferably the diacid dichlorides of isophthalic acid, terephthalic acid, diphenyl ether-4,4'-dicarboxylic acid and naphthalene-2,6-dicarboxylic acid. Be particularly preferred mixtures of the Diklaredichiori de of isophthalic acid and terephthalic acid in the ratio between 1:20 and 20: 1.
  • a carbonic acid halide preferably phosgene
  • phosgene is used as bifunctional acid derivative in the production of polyester-carbonates.
  • the amount of chain terminators is in each case from 0.1 to 10.0 mol%, based on moles of diphenol in the case of the phenolic chain terminators and on moles of dicarboxylic acid dichloride in the case of monocarboxylic acid chloride chain terminators.
  • the aromatic polyester carbonates may also contain incorporated aromatic hydroxy carboxylic acids.
  • the aromatic polyester carbonates can be branched both linearly and in a known manner (see DE-A 2 940 024 and DE-A 3 007 934).
  • branching agents are trifunctional or polyfunctional carboxylic acid chlorides, such as trimesic acid trichloride, cyanuric trichloride, 3,3 ', 4,4'-benzophenone tetracarboxylic acid tetrachloride, 1,4,5,8-naphthalamide tetracarboxylic acid tetrachloride or pyromellitic acid tetrachloride Amounts of from 0.01 to 1.0 mol% (based on the dicarboxylic acid dichlorides used) or difunctional or polyfunctional phenols, such as phloroglucinol, 4,6-dimethyl-2,4,6-tri- (4-hydroxyphenyl) heptane 2-ene, 4,6-dimethyl-2,4,6-tri- (4-hydroxyphenyl) -heptane, l, 3,5-tri- (4-hydroxyphenyl) -benzene, 1, 1, 1-tri (4-hydroxyphenyl) ethane, tri-
  • the proportion of carbonate structural units can vary as desired.
  • the proportion of carbonate groups is preferably up to 100 mol%, in particular up to 80 mol%, particularly preferably up to 50 mol%, based on the sum of ester groups and carbonate groups.
  • Both the ester and the carbonate of the aromatic Polvestercarbonate may be present in the form of blocks or randomly distributed in the polycondensate.
  • the relative solution viscosity ( ⁇ ⁇ ) of the aromatic polycarbonates and Polvestercarbonate is in the range 1.18 to 1.40, preferably 1.20 to 1.32 (measured on solutions of 0.5 g of polycarbonate or polyester in 100 ml of methylene chloride solution 25 ° C).
  • thermoplastic, aromatic polycarbonates and Polvestercarbonate can be used alone or in any mixture.
  • the graft polymers B are prepared by free-radical polymerization, e.g. by emulsion, suspension, solution or bulk polymerization, preferably by emulsion polymerization.
  • the graft polymers B comprise, for example, Graft polymers having elastomeric properties which are essentially obtainable from at least 2 of the following monomers: chloroprene, butadiene-1,3-isoprene, styrene, acrylonitrile, ethylene, propylene, vinyl acetate and (meth) acrylic esters having from 1 to 18 carbon atoms in the alcohol component; So polymers, such as in "Methods of Organic Chemistry” (Houben-Weyl), Vol. 14/1, Georg Thieme-Verlag, Stuttgart 1961, pp. 393-406 and in CB Bucknall, "Toughened Plastics", Appl. Science Publishers, London 1977.
  • Preferred polymers B are partially crosslinked and have gel contents (measured in toluene) of more than 20% by weight, preferably more than 40% by weight, in particular more than 60% by weight.
  • Preferred graft polymers B include graft polymers of:
  • B. l. l 50 to 95 parts by weight of styrene, ⁇ -methylstyrene, methylene-substituted styrene,
  • the graft base has a glass transition temperature below -10 ° C.
  • a graft base based on a polybutadiene rubber is particularly preferred.
  • the glass transition temperatures are determined by means of dynamic differential thermal analysis (DSC) according to the standard DIN EN 61006 at a heating rate of 10 K / min with definition of T g as the midpoint temperature (tangent method).
  • graft polymers B are graft polymers obtained by grafting of
  • I. 10 to 70 preferably 15 to 50, in particular 20 to 40 wt .-%, based on graft, of at least one (meth) acrylic acid ester or 10 to 70, preferably 15
  • the gel content of this graft II is preferably at least 70 wt .-% (measured in toluene), the degree of grafting G 0, 15 to 0.55 and the average Teiichen graspmesser d ⁇ Q of
  • graft polymer B 0.05 to 2, preferably 0, 1 to 0.6 ⁇ .
  • (Meth) acrylic esters I are esters of aeryic acid or methacrylic acid and monohydric alcohols having 1 to 18 carbon atoms. Particularly preferred are methyl methacrylate, ethyl ester and propyl ester.
  • the graft base II in addition to Butadienresten up to 50 wt .-%, based on II, residues of other ethylenically unsaturated monomers such as styrene, acrylonitrile, esters of acrylic or methacrylic acid having 1 to 4 carbon atoms in the alcohol component (such as methyl acrylate, ethyl acrylate , Methyimethacryiat, Ethyimethacryiat), vinyl esters and / or vinyl ethers.
  • the preferred graft layer II consists of pure polybutadiene.
  • graft polymers B are also those products which are obtained by polymerization of the graft monomers in the presence of the graft.
  • the molding compositions according to the invention preferably have a total amount of the polymer formed from graft monomers or added free, not chemically bound to the graft, eg free SAN, of less than 2.0 wt.%, Preferably less than 35 1, 5 wt.% (Ie from 0.0-2.0% by weight, preferably 0.0-1.5% by weight), based on the Total molding composition. With an increase of this proportion, the erfmdungsfaben properties deteriorate drastically.
  • Graft degree G denotes the weight ratio of grafted graft monomers to the graft base and is dimensionless.
  • the mean particle size d ⁇ Q is the diameter, above and below each
  • 50 wt .-% of the particles are. It can be determined by ultracentrifuge measurements (W. Schoitan, H. Lange, Kolloid, Z. and Z. Polymere 250 (1972), 782-796).
  • graft polymers B are e.g. also graft polymers
  • the graft base of acrylate rubber has a glass transition temperature of less than -20 ° C, preferably less than -30 ° C.
  • the acrylate rubbers (a) of the polymers B are preferably polymers of acrylic acid alkyl esters, optionally with up to 40% by weight, based on (a), of other polymerizable, ethylenically unsaturated monomers.
  • Preferred polymerizable acrylic esters include C j -Cg alkyl esters, for example, methyl, ethyl, n-butyl, n-octyl, and 2-
  • crosslinking monomers having more than one polymerizable double bond can be copolymerized.
  • Preferred examples of crosslinking monomers are esters of unsaturated monocarboxylic acids having 3 to 8 C atoms and unsaturated monohydric alcohols having 3 to 12 C-30 atoms or saturated polyols having 2 to 4 OH groups and 2 to 20 C atoms, such as e.g.
  • Preferred crosslinking monomers are allyl methacrylate, ethylene glycol dimethacrylate, diallyl phthalate and heterocyclic compounds having at least 3 ethylenically unsaturated groups.
  • crosslinking monomers are the cyclic monomers triallyl cyanurate, triallyl isocyanurate, trivinyl cyanurate, triacryloyl hexahydro-s-triazine, triallyl benzenes.
  • the amount of the crosslinking monomers is preferably 0.02 to 5.00, in particular 0.05 to 2.00 wt .-%, based on the graft (a).
  • graft base (a) In the case of cyclic crosslinking monomers having at least 3 ethylenically unsaturated groups, it is advantageous to limit the amount to less than 1% by weight of the graft base (a).
  • Preferred "other" polymerizable, ethylenically unsaturated monomers which may optionally be used in addition to the acrylic esters for the preparation of the graft base (a) are, for example, acrylonitrile, styrene, ⁇ -methylstyrene, acrylamides, vinyl-C 1 -C -alkyl ethers, methyl methacrylate,
  • Preferred acrylate rubbers as the graft base (a) are emulsion polymers which have a gel content of at least 60% by weight.
  • compositions of the invention also contain Flammtikmitte !, which are preferably selected from the group comprising the phosphorus-containing flame retardants and halogenated flame retardants.
  • phosphorus-containing flame retardants are selected from the Gmppen the mono- and oligomeric phosphoric and phosphonic acid esters, Phosphonatamine, phosphazenes and phosphinic, wherein mixtures of several components selected from one or more of these Gmppen as flame retardants are used can.
  • Other halogen-free phosphorus compounds which are not specifically mentioned here can also be used alone or in any desired combination with other halogen-free phosphorus compounds.
  • Preferred mono- and oligomeric phosphoric or phosphonic acid esters are phosphorus compounds of the general formula (V)
  • R 1, R 2, R 3 and R 4 independently of one another are each optionally halogenated C 1 -C 8 -alkyl, in each case optionally substituted by alkyl, preferably C 1 -C 4 -alkyl, and / or halogen, preferably chlorine, bromine, substituted C 5 -C 6 -cycloalkyl, C6 to C20 aryl or C7 to C12 aralkyl,
  • n independently, 0 or 1
  • X is a mononuclear or polynuclear aromatic radical having 6 to 30 C atoms, or a linear or branched aliphatic radical having 2 to 30 C atoms, which may be OH-substituted and may contain up to eight ether bonds.
  • R 1, R 2, R 3 and R 4 independently of one another are C 1 - to C 4 -alkyl, phenyl, naphthyl or phenyl-C 1 -C 4 -alkyl.
  • the aromatic groups R 1, R 2, R 3 and R 4 may in turn be substituted by halogen and / or alkyl groups, preferably chlorine, bromine and / or C 1 to C 4 alkyl.
  • Particularly preferred aryl radicals are Kresyi, phenyl, xylenyl, propylphenyi or butyiphenyl and the corresponding brominated and chlorinated derivatives thereof.
  • X in the formula (V) is preferably a mononuclear or polynuclear aromatic radical having 6 to 30 carbon atoms. This is preferably derived from diphenols of the formula (1).
  • n in the formula (V) may independently be 0 or 1, preferably n is equal to 1.
  • q (also in formula VT) stands for integer values of 0 to 30, preferably 0 to 20, particularly preferably 0 to 10, in the case of mixtures for average values of 0.8 to 5.0, preferably 1.0 to 3.0 , more preferably 1.05 to 2.00, and more preferably from 1.08 to 1.60.
  • X is particularly preferred for
  • X is derived from resorcinol, hydroquinone, bisphenol A or diphenyiphenol.
  • X is particularly preferably derived from bisphenol A.
  • Phosphorus compounds of the formula (V) are, in particular, tributyl phosphate, triphenyl phosphate, tricresyl phosphate, diphenyl cresyl phosphate, diphenyl octyl phosphate, diphenyl 2-ethyl cresyl phosphate, tri (isopropyiphenyl) phosphate, resorcinol bridged oligophosphate and bisphenol A-containing oligophosphate.
  • oligomeric phosphoric acid esters of the formula (V) derived from bisphenol A is particularly preferred.
  • component C is bisphenol A-based oligophosphate according to formula (Va)
  • component C is resorcinol-based oligophosphate according to formula (Vb)
  • the phosphorus compounds according to component C are known (cf., for example, EP-A 0 363 608, EP-A 0 640 655) or can be prepared by known methods in an analogous manner (for example, Ulimanns Enzyklopadie der ischen Chemie, Vol ff. 1979; Houben-Weyi, Methods of Organic Chemistry, Vol. 12/1, p. 43; Beilstein, Vol. 6, p. 177).
  • component C it is also possible to use mixtures of phosphates with different chemical structure and / or with the same chemical structure and different molecular weight. Preference is given to using mixtures having the same structure and different chain length, the stated q value being the mean q value.
  • the mean q value can be determined by determining the composition of the phosphorus compound (molecular weight distribution) by means of a suitable method (gas chromatography (GC), high pressure liquid chromatography (HPLC), gel permeation chromatography (GPC)) and from this the mean values for q are calculated.
  • GC gas chromatography
  • HPLC high pressure liquid chromatography
  • GPC gel permeation chromatography
  • phosphonatoms and phosphazenes as described in WO 00/00541 and WO 01/18105, can be used as flame retardants.
  • the flame retardants can be used alone or in any mixture with each other or in mixture with other flame retardants.
  • Further preferred flameproofing agents in the sense of the invention are salts of a phosphinic acid with any desired metal cations. It is also possible to use mixtures of salts that differ in their metal cation.
  • the metal cations are the cations metals of the 1st main group (alkali metals, preferably Li + , Na + , K + ), the 2nd main group (alkaline earth metals, preferably Mg 2+ , Ca 2 "1 , Sr 2+ , Ba 2+ , more preferably Ca 2+ ) or the 3, main group (elements of the boron group, preferably Al 3 " ) and / or the second, 7th or 8th subgroup (preferably Zn 2" , Mn ' T , Fe 2+ , Fe 3 " ) of the periodic table.
  • a salt or a mixture of salts of a phosphinic acid of the formula (IV) is used.
  • the average particle size d 50 of the Phosphinklaresaizes (component C) is less than 80 ⁇ , preferably less than 60 ⁇ , more preferably d 50 is between 10 ⁇ and 55 ⁇ .
  • the mean particle size d 50 is the diameter, above and below which each 50% by weight of the particles are. It is also possible to use mixtures of salts which differ in their mean particle size d 50 .
  • the phosphinic acid salt can be used either alone or in combination with other phosphorus flame retardants.
  • compositions according to the invention may preferably contain fluorinated polyolefins D.
  • Fluorinated polyolefins are generally known (cf., for example, EP-A 640 655).
  • a commercially available product is, for example, Teflon® 30 N from DuPont.
  • the fluorinated polyolefms may also be used in the form of a coagulated mixture of emulsions of the fluorinated polyolefins with emulsions of graft polymers B) or an emulsion of a copolymer E.I) preferably based on styrene / acrylonitrile or polymethyimetharylate, the fluorinated polyolefin being an emulsion is mixed with an emulsion of the graft polymer or copolymer and then coagulated.
  • the fluorinated polyolefins can be used as a precompound with the graft polymer B) or a copolymer E, 1) based preferably on styrene / acrylonitrile or polymethyl methacrylate.
  • the fluorinated polyolefins are mixed as a powder with a powder or granules of the graft polymer or copolymer and melt compounded generally at temperatures of 200 to 330 ° C in conventional units such as internal mixers, extruders or twin-screw.
  • the fluorinated polyolefins may also be employed in the form of a masterbatch prepared by emulsion polymerization of at least one monoethylenically unsaturated monomer in the presence of an aqueous dispersion of the fluorinated polyoefin.
  • Preferred monomer components are styrene, acrylonitrile and mixtures thereof.
  • the polymer is used after acid precipitation and subsequent drying as a free-flowing powder.
  • the coagulates, pre-compounds or masterbatches usually have solids contents of fluorinated polyolefin of 5 to 95 wt .-%, preferably 7 to 60 wt .-%.
  • Component E comprises one or more thermoplastic vinyl (co) polymers E.I. and / or polyalkylene terephthalates E.2.
  • Suitable as vinyl (co) polymers E. l polymers of at least one monomer from the group of vinyl aromatics, vinyl cyanides (unsaturated nitriles), unsaturated carboxylic acids and derivatives (such as esters, anhydrides and imides) of unsaturated carboxylic acids. Particularly suitable are (co) polymers of
  • E. L 50 to 99, preferably 60 to 80 parts by weight of vinylaromatics and / or ring-substituted
  • Vinyl aromatics such as styrene, ⁇ -methylstyrene, p-methylstyrene, p-chlorostyrene
  • E.1.2 1 to 50, preferably 20 to 40 parts by weight of vinyl cyanides (unsaturated nitriles, such as acrylonitrile and methacrylonitrile) and / or unsaturated carboxylic acids (such as acrylic acid and maleic acid) and / or derivatives (such as anhydrides and imides) of unsaturated carboxylic acids
  • the Vinyi (co) polymers E.I are resinous, thermoplastic and rubber free. Particularly preferred is the copolymer of E. i .1 styrene and E. i .2 acrylonitrile.
  • the (co) polymers according to E. 1 are known and can be prepared by free-radical polymerization, in particular by emulsion, suspension, solution or bulk polymerization.
  • the (co) polymers preferably have average molecular weights Mw (weight average, determined by light scattering or sedimentation) of between 15,000 and 200,000.
  • the polyalkylene terephthalates of component E, 2 are reaction products of aromatic dicarboxylic acids or their reactive derivatives, such as dimethyl esters or anhydrides, and aliphatic, cycloaliphatic or aliphatic diols and mixtures of these reaction products.
  • Preferred polyalkylene terephthalates contain at least 80% by weight, preferably at least 90% by weight, based on the dicarboxylic acid component, of terephthalic acid residues and at least 80% by weight, preferably at least 90% by mole, based on the diol component of ethylene glycol and / or butanediol , 4-residues.
  • the preferred polyalkylene terephthalates may contain, in addition to terephthalic acid residues, up to 20 mole%, preferably up to 10 mole%, of other aromatic or cycloaliphatic dicarboxylic acids having 8 to 14 carbon atoms or aliphatic dicarboxylic acids having 4 to 12 carbon atoms, e.g. Residues of phthalic acid, isophthalic acid, naphthalene-2,6-dicarboxylic acid, 4,4'-diphenyidicarboxylic acid, succinic acid, adipic acid, sebacic acid, azelaic acid, cyclohexanediacetic acid.
  • the preferred polyalkylene terephthalates may contain up to 20 mol%, preferably up to 10 mol%, other aliphatic diols having 3 to 12 carbon atoms or cycloaliphatic diols having 6 to 21 carbon atoms.
  • Contain atoms eg Residues of 1,3-propanediol, 2-ethylpropanediol-1, 3, neopentiglycol, pentanediol-1, 5, hexanediol-1, 6, cyclohexane-dimethanol-1, 4, 3-ethylpentanediol-2,4, 2-methylpentanediol 2,4,2,2,4-trimethylpentanediol-1,3,2-ethylhexanediol-1,3,2,2-diethylpropanediol-1,3-hexanediol-2,5,1,4-di ( ⁇ -hydroxyethoxy ) benzene, 2,2-bis (4-hydroxycyclohexyl) propane, 2,4-dihydroxy-l, 1,3,3-tetramethylcyclobutane, 2,2-bis (4-.beta.-hydroxyethoxy-phenyl )
  • the polyalkylene terephthalates can be prepared by incorporation of relatively small amounts of trihydric or trihydric alcohols or 3- or 4-basic carboxylic acids, e.g. according to DE-A 1 900 270 and US-PS
  • branching agents are trime sinic acid, trimellitic acid, trimethylolethane and -propane and pentaerythritol.
  • polyalkylene terephthalates which have been prepared solely from terephthalic acid and its reactive derivatives (for example their dialkyl esters) and ethylene glycol and / or butanediol-1, 4, and mixtures of these polyalkylene terephthalates.
  • Mixtures of polyalkylene terephthalates contain from 1 to 50% by weight, preferably from 1 to 30% by weight, of polyethylene terephthalate and from 50 to 99% by weight, preferably from 70 to 99% by weight, of polybutylene terephthalate.
  • the preferably used Polvalkylenenterephthalate generally have an intrinsic viscosity of 0.4 to 1.5 dl / g, preferably 0.5 to 1.2 dl / g, as measured in phenol / o-dichlorobenzene (1: 1 parts by weight) at 25 ° C. in the Ubbelohde viscometer.
  • the polyalkylene terephthalates can be prepared by known methods (see, for example, Kunststoff-Handbuch, Volume VIII, pp. 695 et seq., Carl Hanser Verlag, Kunststoff 1973).
  • the molding compositions of the invention may contain at least one other of the usual additives, e.g. Lubricants and mold release agents, nucleating agents, antistatic agents, stabilizers, dyes and pigments as well as fillers and reinforcing materials.
  • additives e.g. Lubricants and mold release agents, nucleating agents, antistatic agents, stabilizers, dyes and pigments as well as fillers and reinforcing materials.
  • the component F also comprises very finely divided inorganic compounds which are distinguished by an average particle diameter of less than or equal to 200 nm, preferably less than or equal to 150 nm, in particular from 1 to 100 nm.
  • Suitable finely divided inorganic compounds preferably consist of at least one polar compound of one or more metals of the 1st to 5th main group or 1st to 8th subgroup of the Periodic Table, preferably the 2nd to 5th main gland or 4th to 8th subgroup, especially preferably the 3rd to 5th main group or 4th to 8th subgroup, or compounds of these metals with at least one element selected from oxygen, hydrogen, sulfur, phosphorus, boron, carbon, nitrogen or silicon.
  • Examples of preferred compounds are oxides, hydroxides, hydrous oxides, sulfates, sulfites, sulfides, carbonates, carbides, nitrates, nitrites, nitrides, borates, silicates, phosphates, hydrides, phosphites or phosphonates.
  • the finely divided inorganic compounds of oxides, phosphates, hydroxides preferably (from Ti0 2, Si0 2, Sn0 2, ZnO, ZnS, boehmite, Zr0 2, A1 2 0 3, aluminum phosphates, iron oxides, further TiN, WC, AlO OH ), Fe 2 O 3 iron oxides, NaSO 4 , vanadium oxides, zinc borate, silicates such as Al silicates, Mg silicates, one-, two-, three-dimensional silicates and talc. Mixtures and doped compounds are also useful. Furthermore, these very finely divided inorganic compounds can be surface-modified with organic molecules in order to achieve better compatibility with the polymers. In this way, hydrophobic or hydrophilic surfaces can be obtained. witness. Hydrate-containing aluminum oxides (eg boehmite) or TiO 2 are particularly preferred.
  • Particle size and particle diameter of the inorganic particles means the average particle diameter d 0 , z. B. determined by S e dimentationsme sungen about the settling velocity of the particles, for example, in a Sedigraph.
  • the inorganic compounds may be present as powders, pastes, brine dispersions or suspensions. By precipitation, powders can be obtained from dispersions, sols or suspensions.
  • the inorganic compounds can be incorporated into the thermoplastic molding compositions by conventional methods, for example by direct kneading or extrusion of molding compositions and the very finely divided inorganic compounds.
  • Preferred methods make the preparation of a masterbatch, e.g. in flame retardant additives and at least one component of the molding compositions according to the invention in monomers or solvents, or the co-precipitation of a thermoplastic component and the very finely divided inorganic compounds, for. by co-precipitation of an aqueous emulsion and the very finely divided inorganic compounds, optionally in the form of dispersions, suspensions, pastes or sols of the very finely divided inorganic materials.
  • compositions according to the present invention are prepared by mixing the respective ingredients in a known manner and melt-compounding and melt-extruding at temperatures of 200 ° C to 300 ° C in conventional aggregates such as internal mixers, extruders and double shear screws.
  • the mixing of the individual components can be carried out in a known manner both successively and simultaneously, both at about 20 ° C. (room temperature) and at a higher temperature.
  • thermoplastic compositions and molding compositions according to the present invention are suitable for the production of battery housings according to the invention because of their excellent balance of good low temperature impact strength combined with high weld line strength and good flame retardancy and chemical resistance.
  • the invention also provides methods for producing the battery housing and the use of the molding compositions for the production of battery housings.
  • the molding compounds can be processed by injection molding to battery housings.
  • Another object of the invention is the manufacture of battery casings by thermoforming from prefabricated sheets or foils.
  • the battery cases are suitable for the following applications: vehicle battery and accumulators, battery cases for automobiles, buses, trucks, campers, rail vehicles, aircraft, watercraft or other vehicles, stationary batteries, e.g. in buildings for emergency power supply, storage of solar power from photovoltaic systems.
  • the battery cases preferably meet the requirements of the UN 3480 transport test.
  • FIGS. 1 and 2 Examples of battery housing according to the invention are shown in FIGS. 1 and 2.
  • FIG. 1A shows a battery housing for flat battery cells, which has a spacing between the insertion slots for the flat cells, in which a coolant can be arranged or in which a coolant circulates.
  • Figure 1B shows a plan view of the battery housing for flat battery lines.
  • Figure IC shows a sectional view (section AA) through the battery case for flat
  • FIG. 2A shows a battery case for cylindrical battery cells, which has a distance between the insertion slots for the cylindrical lines, in which a coolant may be arranged or in which a coolant circulates.
  • FIG. 2B shows a plan view of the battery housing for cylindrical battery lines.
  • Figure 2C shows a sectional view (section DD) through the battery case for cylindrical battery cells.
  • the battery housing has channels for cooling the individual cells, preferably water / glycol cooling or air cooling.
  • the battery housing consists of an outer housing and an inner insert for receiving the individual cells, wherein the outer housing may optionally have an insulation, for example by a double wall.
  • the outer housing and the receptacle of the cells (insertion slots) are preferably made of a material and, more preferably, of a component (in one piece).
  • a plurality of battery housings can be modulatively extended to larger units.
  • the battery housing contains a receptacle for control electronics.
  • Component B is a compound having Component B:
  • the Gelgehait is 72%.
  • F-l pentaerythritol tetrastearate as slip-release agent
  • F-2 phosphite stabilizer, phosphite stabilizer, Irganox® B900 (blend of 80% Irgafos® 168 and 20% Irganox® 1076; BASF AG; Ludwigshafen / Irgafos® 168 (tris (2,4-di-tert-butyl-phenyl) - phosphite) / Irganox® 1076 (2,6-di-tert-butyl-4- (octadecanoxycarbonylethyl) phenol).
  • Irganox® B900 blend of 80% Irgafos® 168 and 20% Irganox® 1076; BASF AG; Ludwigshafen / Irgafos® 168 (tris (2,4-di-tert-butyl-phenyl) - phosphite) / Irganox® 1076 (2,6-di-tert-buty
  • the feedstocks listed in Table 1 are compounded at a speed of 225 rpm and a throughput of 20 kg / h at a machine temperature of 260 ° C and granulated.
  • the finished granules are processed on an injection molding machine to the corresponding test specimens (melt temperature 240 ° C, mold temperature 80 ° C, flow front speed 240 mm / s).
  • the flowability was determined according to ISO 11443 (melt viscosity).
  • the impact toughness ak was measured according to ISO I 80 / 1A on a single-sided sprayed test rod of dimension 80x10x4 mm at the indicated measuring temperatures.
  • the heat resistance was measured in accordance with DIN ISO 306 (Vicat softening temperature, method B with 50 N load and a heating rate of 120 K / h) on a single-side molded test rod of dimension 80x10x4 mm.
  • the fire behavior is measured according to UL 94V on rods measuring 127 x 12.7 x 1.5 mm.

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Abstract

L'invention concerne un boîtier de batterie comprenant des compositions contenant A) entre 70,0 et 90,0 parties en poids (rapporté à la somme des parties en poids des composants A + B + C) de polycarbonate aromatique ramifié et/ou de polyester carbonate aromatique, B) entre 6,0 et 15,0 parties en poids (rapporté à la somme des parties en poids des composants A + B + C) d'au moins un polymère greffé avec B.I) entre 5 et 95 parties en poids, de préférence entre 30 et 80 parties en poids, d'un mélange de B. I. I) entre 50 et 95 parties en poids des composés suivants: styrène, α-méthyle styrène, styrène substitué par noyau méthyle, alkylméthacrylate C1-C8, en particulier méthylméthacrylate, alkylacrylate C1-C8, en particulier méthylacrylate, ou des mélanges de ces composés et de B. I. 2) entre 5 et 50 parties en poids des composés suivants: acrylnitrile, méthacrylnitrile alkylméthacrylates C1-C8, en particulier méthylméthacrylate, alkylacrylate C1-C8, en particulier méthylacrylate, anhydre de l'acide maléique, alkyle C1-C4 ou maléinimides alkyle C1-C4-N-substitués ou phényl-N-substitués ou des mélanges de ces composés sur B. 2) entre 5 et 95 parties en poids, de préférence entre 20 et 70 parties en poids d'une base de greffage à base de butadiène ou d'acrylate, C) entre 2,0 et 15,0 parties en poids (rapporté à la somme des parties en poids des composants A + B + C) de composés phosphore sélectionnés dans les groupes comprenant les esters de monoacide et les esters d'acide phosphorique et phosphonique oligomères, les phosphonatamines, les phosphazènes et les phosphinates, ainsi que des mélanges de ces composés, D) entre 0 et 3,0 parties en poids (rapporté à la somme des parties en poids des composants A + B + C) d'agents anti-gouttes, E) entre 0 et 3,0 parties en poids (rapporté à la somme des parties en poids des composants A + B + C) de (co) polymère de vinyle (E.1) et/ou de polyalkylène térephtalate (E.2) thermoplastiques, et F) entre 0 et 20,0 parties en poids (rapporté à la somme des parties en poids des composants A + B + C) d'autres additifs, lesdites compositions étant exemptes polyalkyl/alkyl)acrylate exempt de caoutchouc et toutes les données relatives aux parties en poids de la présente demande étant normalisées de sorte que la somme des parties en poids des composants A + B + C dans la composition soit égale à 100.
EP11764137.3A 2010-09-24 2011-09-20 Boîtier de batterie ignifugé à résilience modifiée à base de polycarbonate ii Withdrawn EP2619821A1 (fr)

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DE102010041388A DE102010041388A1 (de) 2010-09-24 2010-09-24 Flammgeschützte schlagzähmodifizierte Batteriegehäuse auf Polycarbonatbasis II
PCT/EP2011/066310 WO2012038419A1 (fr) 2010-09-24 2011-09-20 Boîtier de batterie ignifugé à résilience modifiée à base de polycarbonate ii

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KR20130102077A (ko) 2013-09-16
DE102010041388A1 (de) 2012-03-29
CA2812249A1 (fr) 2012-03-29
CN103180995A (zh) 2013-06-26
US20120074036A1 (en) 2012-03-29
MX2013003239A (es) 2013-05-22
BR112013006614A2 (pt) 2016-06-21
TW201229130A (en) 2012-07-16
WO2012038419A1 (fr) 2012-03-29

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