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DE1210189B - Process for the production of mixed polymers of methacrylic acid methyl ester - Google Patents

Process for the production of mixed polymers of methacrylic acid methyl ester

Info

Publication number
DE1210189B
DE1210189B DE1960R0029241 DER0029241A DE1210189B DE 1210189 B DE1210189 B DE 1210189B DE 1960R0029241 DE1960R0029241 DE 1960R0029241 DE R0029241 A DER0029241 A DE R0029241A DE 1210189 B DE1210189 B DE 1210189B
Authority
DE
Germany
Prior art keywords
production
methyl ester
methacrylic acid
acid methyl
acid imide
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.)
Pending
Application number
DE1960R0029241
Other languages
German (de)
Inventor
Dr Adolf Wohnhas
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Roehm GmbH Darmstadt
Original Assignee
Roehm and Haas GmbH
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Roehm and Haas GmbH filed Critical Roehm and Haas GmbH
Priority to DE1960R0029241 priority Critical patent/DE1210189B/en
Publication of DE1210189B publication Critical patent/DE1210189B/en
Pending legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08FMACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F220/00Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical or a salt, anhydride ester, amide, imide or nitrile thereof
    • C08F220/02Monocarboxylic acids having less than ten carbon atoms; Derivatives thereof
    • C08F220/10Esters
    • C08F220/12Esters of monohydric alcohols or phenols
    • C08F220/14Methyl esters, e.g. methyl (meth)acrylate
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08FMACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F212/00Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by an aromatic carbocyclic ring
    • C08F212/02Monomers containing only one unsaturated aliphatic radical
    • C08F212/04Monomers containing only one unsaturated aliphatic radical containing one ring
    • C08F212/06Hydrocarbons
    • C08F212/12Monomers containing a branched unsaturated aliphatic radical or a ring substituted by an alkyl radical
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08FMACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F226/00Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a single or double bond to nitrogen or by a heterocyclic ring containing nitrogen
    • C08F226/06Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a single or double bond to nitrogen or by a heterocyclic ring containing nitrogen by a heterocyclic ring containing nitrogen

Landscapes

  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Addition Polymer Or Copolymer, Post-Treatments, Or Chemical Modifications (AREA)

Description

Verfahren zur Herstellung von Mischpolymerisaten des Methacrylsäuremethylesters Thermoplastische Formmassen, d. h. Kunststoffe, die nach dem Preß-, Preßspritz-, Spritzguß-, Strangpreß- oder nach dem Walzverfahren verarbeitet werden, sollen eine hohe Wärmeformbeständigkeit, die z. B. durch die Vicat-Erweichungstemperatur bestimmt wird, bei möglichst guter Verarbeitbarkeit aufweisen. Die Verarbeitbarkeit hängt außer vom Fließverhalten auch von der Thermostabilität ab.Process for the production of copolymers of methyl methacrylate Thermoplastic molding compounds, d. H. Plastics that are produced after compression molding, compression molding, Injection molding, extrusion or by the rolling process are to be processed high heat resistance, the z. B. determined by the Vicat softening temperature will have, with the best possible processability. The workability depends apart from the flow behavior, it also depends on the thermal stability.

Darunter versteht man, daß das Material bei der Verarbeitungstemperatur noch nicht depolymerisiert.This means that the material is at the processing temperature not yet depolymerized.

Erwünscht ist ein möglichst großer Spielraum in der Verarbeitungstemperatur, um auch schwierige Teile herstellen, vornehmlich spritzen zu können.The greatest possible latitude in the processing temperature is desirable, in order to be able to manufacture even difficult parts, primarily to be able to inject.

Mischpolymerisate aus Methacrylsäuremethylester und a-Methylstyrol zeichnen sich durch einen hohen Erweichungspunkt aus, d. h., die daraus hergestellten Formkörper sind z. B. in kochendem Wasser formbeständig. Die Thermostabilität dieser Mischpolymerisate ist jedoch unbefriedigend; sie beginnen bei der für die Verarbeitung erforderlichen Temperatur zu depolymerisieren. Dieser Abbau kann beim Verspritzen zu Schlieren- und Blasenbildung im Formteil führen. Copolymers of methyl methacrylate and α-methylstyrene are characterized by a high softening point, i. i.e., those made from it Shaped bodies are z. B. dimensionally stable in boiling water. The thermostability of this Copolymers are unsatisfactory, however; they start with for processing required temperature to depolymerize. This breakdown can occur when splashing lead to streaking and blistering in the molded part.

Es ist auch bereits bekannt, Methacrylsäuremethylester zusammen mit a-Methylstyrol und einem weiteren Monomeren, wie Acrylnitril, Styrol oder Acrylsäureester, zu polymerisieren. It is also already known to use methyl methacrylate together with a-methylstyrene and another monomer, such as acrylonitrile, styrene or acrylic acid ester, to polymerize.

Es wurde nun gefunden, daß bei einem Verfahren zur Herstellung von Mischpolymerisaten durch Block-oder Perlpolymerisation von überwiegenden Mengen an Methacrylsäuremethylester und 5 bis 30 Gewichtsprozent a-Methylstyrol zusammen mit anderen polymerisierbaren Monomeren in Gegenwart von Beschleunigern, gegebenenfalls von Reglern, bei Temperaturen von 50 bis 130"C dann neben der Erhöhung der Erweichungstemperatur gleichzeitig eine Verbesserung der Thermostabilität erzielt wird, wenn man als anderes polymerisierbares Monomeres 2 bis 20 Gewichtsprozent N-Vinylbernsteinsäureimid oder N-Vinylphthalsäureimid einsetzt. It has now been found that in a process for the production of Copolymers by block or bead polymerization in predominant amounts of methyl methacrylate and 5 to 30 percent by weight of α-methylstyrene with other polymerizable monomers in the presence of accelerators, if appropriate of regulators, at temperatures from 50 to 130 "C then in addition to increasing the softening temperature at the same time an improvement in thermal stability is achieved if one as another polymerizable monomer 2 to 20 weight percent N-vinyl succinic acid imide or N-vinylphthalic acid imide is used.

Die Mischpolymerisate, gemäß dem Verfahren der Erfindung hergestellt, erlauben den Spritzguß auch von komplizierten Formteilen. Sie bringen also im Hinblick auf ihre technische Verwertbarkeit deutliche Vorteile. The copolymers produced according to the process of the invention allow the injection molding of complex molded parts. So you bring in view clear advantages in terms of their technical usability.

Die Herstellung der Mischpolymerisate erfolgt in an sich bekannter Weise durch Block- oder Perlpolymerisation in Gegenwart eines Beschleunigers bei 50 bis 130"C. Als Beschleuniger sind Verbindungen wie Azodiisobuttersäurenitril oder Peroxyde geeignet. Im besonderen Maße haben sich Kombinationen aus Azodiisobuttersäurenitril mit einem eine hohe Zerfallstemperatur besitzenden Peroxyd, wie tert.Butylhydroperoxyd oder tert.Butylperbenzoat, bewährt. The copolymers are produced in a manner known per se Way by block or bead polymerization in the presence of an accelerator 50 to 130 "C. Compounds such as azodiisobutyronitrile are used as accelerators or peroxides suitable. Combinations of azodiisobutyronitrile have proven to be particularly good with a peroxide that has a high decomposition temperature, such as tert-butyl hydroperoxide or tert-butyl perbenzoate, proven.

Außerdem haben sich Kombinationen aus einem niedrig- und einem hochzerfallenden Peroxyd, wie aus Dilauroylperoxyd zusammen mit tert.Butylhydroperoxyd, als zweckmäßig erwiesen. In addition, there are combinations of a low-decay and a high-decay Peroxide, such as from dilauroyl peroxide together with tert-butyl hydroperoxide, is useful proven.

Mit besonderem Vorteil kann man die Polymerisation mit Schwefelreglern, wie Mercaptanen, leiten. The polymerization with sulfur regulators, like mercaptans, conduct.

Ein weiterer Vorteil des erfindungsgemäßen Verfahrens besteht darin, daß durch die Mitverwendung von N-Vinylbernsteinsäureimid oder N-Vinylphthalsäureimid die Polymerisationsgeschwindigkeit der radikalisch initiierten Methylmethacrylat-a-Methylstyrol-Mischpolymerisation gesteigert wird. Another advantage of the method according to the invention is that that by using N-vinyl succinic acid imide or N-vinyl phthalic acid imide the polymerization rate of the radical initiated methyl methacrylate-α-methylstyrene copolymerization is increased.

Man erhält glasklare Polymerisate, die praktisch ungefärbt sind. Crystal-clear polymers which are practically uncolored are obtained.

Außer den bereits genannten guten Eigenschaften der neuen Mischpolymerisate, nämlich außer einem hohen Erweichungspunkt und einer guten Thermostabilität, verdient ihre Wasserunempfindlichkeit hervorgehoben zu werden. In addition to the already mentioned good properties of the new copolymers, namely, apart from a high softening point and good thermal stability, deserves their insensitivity to water to be emphasized.

In der nachstehenden Tabelle ist die Vicat-Erweichungstemperatur von bekannten Polymerisaten mit der von erfindungsgemäß hergestellten Mischpolynerisaten zum Vergleich angeführt. Die Anteile sind Gewichtsprozente. Vicat- a-Methyi- Weiteres Monomeres Erweichungs- acrylat Y temperatur 01o 01o °/o "C 100 - - 120 75 25 - 132 72 25 3 Acrylnitril 134 70 25 5 Styrol 133 70 10 20 N-Vinylbern- 136 steinsäureimid 65 25 10 N-Vinylbern- 145 steinsäureimid Beispiel Ein Monomerengemisch, bestehend aus 10g Methylmethacrylat, 1,45 g os-Methylstyrol und 2,9 g N-Vinylbernsteinsäureimid, wird im Reagenzglas bei 85° C in Gegenwart von 20 mg Dilauroylperoxyd und 10 mg tert.Butylhydroperoxyd sow,ie 20 mg tert.-Dodecylmercaptan 5 Tage polymerisiert.In the table below, the Vicat softening temperature of known polymers is given for comparison with that of copolymers prepared according to the invention. The proportions are percentages by weight. Vicat a-methyi- other monomer softening acrylate Y temperature 01o 01o ° / o "C 100 - - 120 75 25-132 72 25 3 acrylonitrile 134 70 25 5 styrene 133 70 10 20 N-vinyl amber 136 stinic acid imide 65 25 10 N-vinyl amber 145 stinic acid imide EXAMPLE A monomer mixture consisting of 10 g of methyl methacrylate, 1.45 g of os-methylstyrene and 2.9 g of N-vinylsuccinic acid imide is placed in a test tube at 85 ° C. in the presence of 20 mg of dilauroyl peroxide and 10 mg of tert-butyl hydroperoxide, ie 20 mg of tert .-Dodecyl mercaptan polymerized for 5 days.

Claims (1)

Patentanspruch: Verfahren zur Herstellung von Mischpolymerisaten durch Block- oder Perlpolymerisation von überwiegenden Mengen an Methacrylsäuremethyl- ester und 5. bis 30 Gewichtsprozent o;-Methylstyrol zusammen mit än4eren polymerisierbaren Monomeren in Gegenwart von Beschleunigern, gegebenenfalls von Reglern, bei Temperaturen von 50 bis 130°C, d a d u r c h g e k e n n z e i c h n e t, daß als anderes polymerisierbares Monomeres 2 bis 20 Gewichtsprozent N-Vinylbernsteinsäureimid oder N-Vinylphthalsäureimid eingesetzt werden. Claim: Process for the production of copolymers by block or bead polymerization of predominant amounts of methacrylic acid methyl ester and 5. to 30 percent by weight of o; -methylstyrene together with other polymerizable Monomers in the presence of accelerators, optionally regulators, at temperatures from 50 to 130 ° C, d u r c h e k e n n n e i c h n e t that as other polymerisable Monomeric 2 to 20 weight percent N-vinyl succinic acid imide or N-vinyl phthalic acid imide can be used. In Betracht gezogene Druckschriften: Britische Patentschrift Nr. 836 837; USA.-Patentschriften Nr. 2 862 906, 2 862907. Documents considered: British Patent No. 836 837; U.S. Patent Nos. 2,862,906, 2,862907.
DE1960R0029241 1960-12-08 1960-12-08 Process for the production of mixed polymers of methacrylic acid methyl ester Pending DE1210189B (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
DE1960R0029241 DE1210189B (en) 1960-12-08 1960-12-08 Process for the production of mixed polymers of methacrylic acid methyl ester

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DE1960R0029241 DE1210189B (en) 1960-12-08 1960-12-08 Process for the production of mixed polymers of methacrylic acid methyl ester

Publications (1)

Publication Number Publication Date
DE1210189B true DE1210189B (en) 1966-02-03

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4636458A (en) * 1982-12-30 1987-01-13 Rohm Gmbh Storage disk made of para-methyl styrene
US4754008A (en) * 1986-04-16 1988-06-28 Rohm Gmbh Heat resistant molding compounds

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2862907A (en) * 1957-04-01 1958-12-02 Monsanto Chemicals Suspension process for the polymerization of vinylidene aromatic hydrocar-bons having rubbery conjugated 1, 3-diene polymers dissolved therein
US2862906A (en) * 1957-04-01 1958-12-02 Monsanto Chemcial Company Suspension process for the polymerization of vinylidene aromatic hydrocarbons
GB836837A (en) * 1956-01-23 1960-06-09 Baker Chem Co J T Improvements to polymerization products

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB836837A (en) * 1956-01-23 1960-06-09 Baker Chem Co J T Improvements to polymerization products
US2862907A (en) * 1957-04-01 1958-12-02 Monsanto Chemicals Suspension process for the polymerization of vinylidene aromatic hydrocar-bons having rubbery conjugated 1, 3-diene polymers dissolved therein
US2862906A (en) * 1957-04-01 1958-12-02 Monsanto Chemcial Company Suspension process for the polymerization of vinylidene aromatic hydrocarbons

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4636458A (en) * 1982-12-30 1987-01-13 Rohm Gmbh Storage disk made of para-methyl styrene
US4754008A (en) * 1986-04-16 1988-06-28 Rohm Gmbh Heat resistant molding compounds

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