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DE1111396B - Process for the polymerization of vinyl acetate and vinyl chloride - Google Patents

Process for the polymerization of vinyl acetate and vinyl chloride

Info

Publication number
DE1111396B
DE1111396B DES67668A DES0067668A DE1111396B DE 1111396 B DE1111396 B DE 1111396B DE S67668 A DES67668 A DE S67668A DE S0067668 A DES0067668 A DE S0067668A DE 1111396 B DE1111396 B DE 1111396B
Authority
DE
Germany
Prior art keywords
polymerization
methanol
vinyl acetate
water
vinyl
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
DES67668A
Other languages
German (de)
Inventor
Rene Jean Marcel Chambard
Gilbert Paul Christen
Andre Fournet
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.)
Rhone Poulenc SA
Original Assignee
Rhone Poulenc SA
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 Rhone Poulenc SA filed Critical Rhone Poulenc SA
Publication of DE1111396B publication Critical patent/DE1111396B/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
    • C08F4/00Polymerisation catalysts
    • C08F4/06Metallic compounds other than hydrides and other than metallo-organic compounds; Boron halide or aluminium halide complexes with organic compounds containing oxygen
    • C08F4/12Metallic compounds other than hydrides and other than metallo-organic compounds; Boron halide or aluminium halide complexes with organic compounds containing oxygen of boron, aluminium, gallium, indium, thallium or rare earths
    • C08F4/14Boron halides or aluminium halides; Complexes thereof with organic compounds containing oxygen

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Transition And Organic Metals Composition Catalysts For Addition Polymerization (AREA)
  • Addition Polymer Or Copolymer, Post-Treatments, Or Chemical Modifications (AREA)

Description

BUNDESREPUBLIK DEUTSCHLAND
DEUTSCHES Mt^Ik PATENTAMT
FEDERAL REPUBLIC OF GERMANY
GERMAN Mt ^ Ik PATENT OFFICE

kl. 39 c 25/01 kl. 39 c 25/01

ESTERNAT.KL. C 08 fESTERNAT.KL. C 08 f

AUSLEGESCHRIFT 1111396EDITORIAL 1111396

S67668IVb/39cS67668IVb / 39c

ANMELDETAG: 21. MÄRZ 1960REGISTRATION DATE: MARCH 21, 1960

"BEKANNTMACHUNG DER ANMELDUNG UNDAUSGABEDER AUSLEGESCHRIFT: 20. JULI 1961"NOTICE THE REGISTRATION ANDOUTPUTE EDITORIAL: JULY 20, 1961

Die vorliegende Erfindung betrifft eine Verbesserung der Verfahren zur Polymerisation von Vinylacetat und -chlorid in Gegenwart von Boralkylkatalysatoren. The present invention relates to an improvement in the methods of polymerizing vinyl acetate and chloride in the presence of boroalkyl catalysts.

Es ist bekannt, organische ungesättigte Verbindüngen in Gegenwart von Bortrialkylen als Katalysatoren zu polymerisieren und zu copolymerisieren. Als verwendbare Lösungsmittel wurden entweder nicht polare organische Lösungsmittel, wie aliphatische, alicyclische und aromatische Kohlen-Wasserstoffe, oder polare organische Lösungsmittel, wie Ketone oder Alkohole, oder Wasser vorgeschlagen. It is known to use organic unsaturated compounds to polymerize and copolymerize in the presence of boron trialkyls as catalysts. Either non-polar organic solvents such as aliphatic, alicyclic and aromatic hydrocarbons, or polar organic solvents, such as ketones or alcohols, or water are suggested.

In nicht polarem organischem Medium verläuft die Polymerisation langsam und unvollständig und führt zu Produkten mit niedriger Viskosität. Wenn man polare organische Lösungsmittel, wie beispielsweise Aceton oder Methanol, verwendet, so sind die Umwandlungsgrade höher, doch bleiben die Viskositäten gering; Methanol weist außerdem, insbesondere im Falle von Vinylacetat, den Nachteil auf, das Polymere zu lösen. Arbeitet man in wäßrigem Medium, so ist man gezwungen, Emulgiermittel zu verwenden, deren vollständige Entfernung von den erhaltenen Polymeren schwierig, wenn nicht unmöglich ist und die die Eigenschaften, insbesondere die elektrischen Eigenschaften der Polymeren nachteilig beeinflussen.In a non-polar organic medium, the polymerization proceeds slowly and incompletely and leads to products with low viscosity. If you have polar organic solvents, such as Acetone or methanol, the degrees of conversion are higher, but the viscosities remain small amount; Methanol also has the disadvantage, especially in the case of vinyl acetate, that the polymer to solve. If you work in an aqueous medium, you are forced to use emulsifiers, their complete removal of the polymers obtained is difficult, if not impossible, and the adversely affect the properties, in particular the electrical properties, of the polymers.

Es wurde nun gefunden, daß man ausgezeichnete Umwandlungsgrade und viel höhere Viskositäten erzielt, wenn man die Polymerisation von Vinylacetat und von Vinylchlorid mit Boralkylen in einem wäßrig-alkoholischen Medium durchführt, das aus einem Gemisch von Alkohol (z. B. Methyl- oder Äthylalkohol) und Wasser in einem solchen Mengenverhältnis besteht, daß das Monomere darin löslich ist, das Polymere jedoch ausfällt.It has now been found that there are excellent degrees of conversion and much higher viscosities achieved when the polymerization of vinyl acetate and vinyl chloride with boron alkylene in one Aqueous-alcoholic medium, which consists of a mixture of alcohol (e.g. methyl or Ethyl alcohol) and water in such a proportion that the monomer is soluble therein but the polymer precipitates.

Im Falle von Vinylacetat eignet sich ein Verhältnis von etwa 1 Volumen Methanol je 1 Volumen Wasser gut. Ein solches Gemisch löst etwa ein Drittel seines Volumens an Vinylacetat bei 20° C.In the case of vinyl acetate, a ratio of about 1 volume of methanol per 1 volume of water is suitable Well. Such a mixture dissolves about a third of its volume in vinyl acetate at 20 ° C.

Im Falle von Vinylchlorid kann man gleiche Mengenverhältnisse verwenden. Die Grenzen sind hier jedoch weit, und ein Gemisch von 20 Volumina Wasser und 60 Volumina Methanol ist ebenfalls noch geeignet.In the case of vinyl chloride, the same proportions can be used. The limits are here, however, far, and a mixture of 20 volumes of water and 60 volumes of methanol is also still available suitable.

Als Boralkyle kann man die niedrigen Bortrialkyle, wie beispielsweise Bortrimethyl, Bortriäthyl, Bortrin-propyl oder -triisopropyl, Bortributyle u. dgl., verwenden. The lower boron trialkyls, such as, for example, boron trimethyl, boron triethyl, boron-propyl, can be used as boron alkyls or triisopropyl, boron tributyls, and the like.

In der folgenden Tabelle sind die Versuchsergebnisse von Polymerisationen von Vinylacetat zusammengestellt, die bei 20° C mit 0,6% Bortri-Verfahren zur Polymerisation von Vinylacetat und VinylchloridIn the following table are the experimental results of polymerizations of vinyl acetate compiled that at 20 ° C with 0.6% Bortri process for the polymerization of vinyl acetate and vinyl chloride

Anmelder:Applicant:

Societe des Usines Chimiques Rhöne-Poulenc, ParisSociete des Usines Chimiques Rhone-Poulenc, Paris

Vertreter: Dr. F. Zumstein,Representative: Dr. F. Zumstein,

Dipl.-Chem. Dr. rer. nat. E. AssmannDipl.-Chem. Dr. rer. nat. E. Assmann

und Dipl.-Chem. Dr. R. Koenigsberger,and Dipl.-Chem. Dr. R. Koenigsberger,

Patentanwälte, München 2, Bräuhausstr. 4Patent Attorneys, Munich 2, Bräuhausstr. 4th

Beanspruchte Priorität-Frankreich vom 21. April 1959Claimed priority France from April 21, 1959

Andre Fournet, Gilbert Paul Christen und Rene Jean Marcel Chambard,Andre Fournet, Gilbert Paul Christen and Rene Jean Marcel Chambard,

Lyon (Frankreich), sind als Erfinder genannt wordenLyon (France) have been named as inventors

äthyl, bezogen auf das Monomere, und einer Dauer von 7 Stunden durchgeführt wurden.ethyl, based on the monomer, and a duration of 7 hours were carried out.

Lösungsmittelsolvent Umwand
lungsgrad
°/o
Conversion
degree of efficiency
° / o
Spezifische
Viskosität *
Specific
Viscosity *
Heptan
Tetrahydrofuran
Aceton
Methanol
Methanol—Wasser,
50:50 Volumen
Methanol—Wasser,
55 :45 Volumen
Heptane
Tetrahydrofuran
acetone
Methanol
Methanol - water,
50:50 volume
Methanol - water,
55: 45 volume
39
57,9
57,5
71,5
94,7
100
39
57.9
57.5
71.5
94.7
100
0,155
0,036
0,100
0,130
0,329
0,330
0.155
0.036
0.100
0.130
0.329
0.330

* Berechnet für eine Lösung mit 0,5 °/o in Benzol bei 25° C.* Calculated for a solution with 0.5% in benzene at 25 ° C.

Aus dieser Tabelle ist ersichtlich, daß die Polymerisation in dem Gemisch Methanol—Wasser quantitative Umwandlungen in Polymere mit einer Viskosität ermöglicht, die doppelt so hoch als die in anderen Lösungsmitteln erzielte ist.It can be seen from this table that the polymerization in the methanol-water mixture is quantitative Allows conversions to polymers with a viscosity twice that of other solvents.

109 648/445109 648/445

In der nachfolgenden Tabelle sind die Ergebnisse für die Polymerisation von Vinylchlorid bei — 20° C mit 2 g Katalysator und 500 g Lösungsmittel zusammengestellt. The table below shows the results for the polymerization of vinyl chloride at -20 ° C compiled with 2 g of catalyst and 500 g of solvent.

Lösungsmittelsolvent

Gewicht
des eingesetzten
weight
of the used
Dauerduration Gewicht
des erhaltenen
weight
of the received
Umwand
lungsgrad
Conversion
degree of efficiency
SpezifischeSpecific
VinylchloridsVinyl chloride Stundenhours PolymerenPolymers °/o° / o Viskosität *Viscosity * gG gG 27,527.5 221221 2424 6161 2020th 0,2460.246 152152 6 V2 6 V 2 30,430.4 14,514.5 0,0680.068 225225 2424 32,532.5 6565 0,1970.197 116116 2424 142142 6262 0,4840.484 227227 2424 141,5141.5 41,641.6 0,5880.588 149149 63/46 3/4 6262 61,561.5 0,5720.572 206206 2424 126,5126.5 1,0211.021

Heptan Heptane

Tetrahydrofuran Tetrahydrofuran

Diäthyläther Diethyl ether

Methanol Methanol

Methanol—Wasser, 80:20 Volumen ... Methanol—Wasser, 50:50 Volumen ... Methanol—Wasser, 50: 50 Volumen ...Methanol — water, 80:20 volume ... Methanol — water, 50:50 volume ... Methanol — water, 50:50 volume ...

* Berechnet für eine Lösung mit 0,5 °/o in Cyclohexanon bei 25° C.* Calculated for a solution with 0.5% in cyclohexanone at 25 ° C.

Aus dieser Tabelle ist ersichtlich, daß man bei Ersatz des Tetrahydrofurans und des Diäthyläthers durch Methanol zwar viel höhere Umwandlungsgrade erzielt, jedoch bei Verwendung von Gemischen Wasser—Methanol — bei Umwandlungsgraden, die ebenso hoch sind wie mit Methanol allein—Polymere mit sehr viel höherer spezifischer Viskosität erhält und diese um so größer ist, je mehr Wasser das Medium enthält.From this table it can be seen that when replacing tetrahydrofuran and diethyl ether Much higher degrees of conversion are achieved with methanol, but when mixtures are used Water — methanol - at degrees of conversion that are as high as with methanol alone — polymers with a much higher specific viscosity and this is the greater, the more water is in the medium contains.

Claims (1)

PATENTANSPRUCH: Verfahren zur Polymerisation von Vinylacetat und Vinylchlorid mit Hilfe von Boralkylkatalysatoren, dadurch gekennzeichnet, daß man diePATENT CLAIM: Process for the polymerization of vinyl acetate and vinyl chloride with the aid of boron alkyl catalysts, characterized in that the Polymerisation in wäßrig-alkoholischem Medium durchführt, das ein solches Mengenverhältnis von Wasser und Alkohol aufweist, daß das Monomere löslich ist, das Polymere jedoch ausfällt.Carries out polymerization in an aqueous-alcoholic medium that has such a quantitative ratio of Water and alcohol indicate that the monomer is soluble but the polymer precipitates. In Betracht gezogene Druckschriften:Considered publications: Deutsche Auslegeschrift Nr. 1 056 372; bekanntgemachte Unterlagen der belgischen tente Nr. 569 632, 560 624, 562 433, 570 024.German Auslegeschrift No. 1,056,372; published documents of the Belgian tente nos. 569 632, 560 624, 562 433, 570 024. 648/445 7. 61648/445 7. 61
DES67668A 1959-04-21 1960-03-21 Process for the polymerization of vinyl acetate and vinyl chloride Pending DE1111396B (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
FR792696A FR1232428A (en) 1959-04-21 1959-04-21 Improvement in the polymerization processes of chloride and vinyl acetate

Publications (1)

Publication Number Publication Date
DE1111396B true DE1111396B (en) 1961-07-20

Family

ID=8713915

Family Applications (1)

Application Number Title Priority Date Filing Date
DES67668A Pending DE1111396B (en) 1959-04-21 1960-03-21 Process for the polymerization of vinyl acetate and vinyl chloride

Country Status (3)

Country Link
DE (1) DE1111396B (en)
FR (1) FR1232428A (en)
GB (1) GB887398A (en)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3138577A (en) * 1961-10-12 1964-06-23 Borden Co Suspension polymerization of vinyl chloride and vinyl acetate

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
BE570024A (en) *
BE560624A (en) * 1957-09-06
BE569632A (en) * 1958-07-22
DE1056372B (en) * 1956-07-14 1959-04-30 Bayer Ag Process for the polymerization of unsaturated compounds

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
BE570024A (en) *
DE1056372B (en) * 1956-07-14 1959-04-30 Bayer Ag Process for the polymerization of unsaturated compounds
BE560624A (en) * 1957-09-06
BE562433A (en) * 1957-09-06
BE569632A (en) * 1958-07-22

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3138577A (en) * 1961-10-12 1964-06-23 Borden Co Suspension polymerization of vinyl chloride and vinyl acetate

Also Published As

Publication number Publication date
FR1232428A (en) 1960-10-07
GB887398A (en) 1962-01-17

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