[go: up one dir, main page]

DE1086689B - Process for the transesterification of dialkyl benzene dicarboxylates with glycols - Google Patents

Process for the transesterification of dialkyl benzene dicarboxylates with glycols

Info

Publication number
DE1086689B
DE1086689B DED30702A DED0030702A DE1086689B DE 1086689 B DE1086689 B DE 1086689B DE D30702 A DED30702 A DE D30702A DE D0030702 A DED0030702 A DE D0030702A DE 1086689 B DE1086689 B DE 1086689B
Authority
DE
Germany
Prior art keywords
transesterification
salts
acid
glycols
dialkyl benzene
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
DED30702A
Other languages
German (de)
Inventor
Dipl-Ing Dr Ilse-Ursula Nebel
Dr Rer Nat Siegwart S Dipl-Ing
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.)
Dynamit Nobel AG
Original Assignee
Dynamit Nobel AG
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
Priority to NL251667D priority Critical patent/NL251667A/xx
Application filed by Dynamit Nobel AG filed Critical Dynamit Nobel AG
Priority to DED30702A priority patent/DE1086689B/en
Priority to CH476960A priority patent/CH378303A/en
Priority claimed from FR826880A external-priority patent/FR1256829A/en
Priority to GB17004/60A priority patent/GB922467A/en
Priority to BE590976A priority patent/BE590976A/en
Publication of DE1086689B publication Critical patent/DE1086689B/en
Pending legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G63/00Macromolecular compounds obtained by reactions forming a carboxylic ester link in the main chain of the macromolecule
    • C08G63/78Preparation processes
    • C08G63/82Preparation processes characterised by the catalyst used
    • C08G63/83Alkali metals, alkaline earth metals, beryllium, magnesium, copper, silver, gold, zinc, cadmium, mercury, manganese, or compounds thereof
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J31/00Catalysts comprising hydrides, coordination complexes or organic compounds
    • B01J31/02Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides
    • B01J31/04Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides containing carboxylic acids or their salts
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2231/00Catalytic reactions performed with catalysts classified in B01J31/00
    • B01J2231/40Substitution reactions at carbon centres, e.g. C-C or C-X, i.e. carbon-hetero atom, cross-coupling, C-H activation or ring-opening reactions
    • B01J2231/49Esterification or transesterification

Landscapes

  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Low-Molecular Organic Synthesis Reactions Using Catalysts (AREA)
  • Catalysts (AREA)

Description

Verfahren zur Umesterung - . von Benzoldicarbonsäuredialkylestern mit Glykolen Ein bekanntes und vielfach angewandtes Verfahren zur Gewinnung von neutralen Glykolestern aromatischer Dicarbonsäuren ist die Umesterung der entsprechenden Dialkylester, besonders des Dimethylesters, mit Glykolen in Gegenwart bestimmter Katalysatoren, die die Umesterung zum Teil erheblich beschleunigen. Diese Umesterungsreaktion hat besondere Bedeutung erlangt für die Herstellung der Ausgangsprodukte zur Gewinnung von hochmolekularen Polyestern. Als wirksame Katalysatoren ist unter anderem eine Anzahl von Metallen, Metalloxyden, für sich oder in Kombination, und vor allem eine Vielzahl von Metallsalzen bekanntgeworden. Unter den Metallsalzen werden vornehmlich solche mit organischem Anion empfohlen und unter anderem auch als besondere Gruppe Salze von solchen Säuren, deren Dissoziationskonstante unterhalb eines bestimmten Wertes liegt.Process for transesterification -. of dialkyl benzene dicarboxylates with glycols A well-known and widely used process for the production of neutral glycol esters of aromatic dicarboxylic acids is the transesterification of the corresponding Dialkyl esters, especially the dimethyl ester, with glycols in the presence of certain Catalysts, which in some cases considerably accelerate the transesterification. This transesterification reaction has acquired particular importance for the manufacture of the raw materials for extraction of high molecular weight polyesters. Effective catalysts include one Number of metals, metal oxides, alone or in combination, and above all one A large number of metal salts have become known. Among the metal salts are mainly those with organic anions are recommended and, among other things, as a special group Salts of such acids whose dissociation constant is below a certain Worth.

Es wurde nun überraschenderweise gefunden, daü unter den Metallsalzen organischer Säuren eine Gruppe bezüglich ihrer Fähigkeit, die genannte Umesterung zu beschleunigen, besonders hervortritt. Es handelt sich hierbei um die Salze der Metalle der II. Gruppe des Periodensystems der Elemente, besonders des Zinks und Cadmiums, mit solchen organischen Säuren, deren Molekül ungesättigten Charakter in Form einer Doppelbindung hat. Es ist hierbei gleichgültig, ob es sich um ein- oder mehrbasische Säuren handelt.It has now surprisingly been found that among the metal salts Organic acids a group with regard to their ability, the so-called transesterification to accelerate, especially emerges. These are the salts of Metals of group II of the periodic table of the elements, especially zinc and Cadmium, with such organic acids, whose molecule is unsaturated in character in the form of a double bond. It does not matter whether it is a or polybasic acids.

Die Anwendung des Katalysators geschieht in bekannter Weise so, daB man 0,02 bis 0,2°/o, vornehmlich 0,0,5 bis 0,1'°/o, berechnet auf die Menge des oder der eingesetzten Benzoldicarbonsäureester, zu dem Alkylester-Glykol-Gemisch gibt und dann die Umesterung in bekannter Weise unter Rühren bei Temperaturen zwischen 170 und 200' C durchführt, wobei der ursprünglich in Estergruppierung vorhanden gewesene Alkylalkohod, in den meisten Fällen der Methylalkohol, abdestilliert.The catalyst is used in a known manner in such a way that 0.02 to 0.2%, especially 0.0.5 to 0.1%, calculated on the amount of the benzenedicarboxylic acid ester (s) used, is added to the There are alkyl ester-glycol mixture and then the transesterification is carried out in a known manner with stirring at temperatures between 170 and 200 ° C, the alkyl alcohol originally present in ester grouping, in most cases the methyl alcohol, being distilled off.

Die besonders gute katalytische Wirksamkeit der angeführten Verbindungsklasse zeigt sich in einer sehr schnell verlaufenden vollständigen Umesterung im Vergleich zu anderen als Katalysatoren brauchbaren Salzen. Die im folgenden beschriebenen Versuche wurden unter mengenmäßig und apparativ völlig gleichartigen Bedingungen durchgeführt, so daB die angeführten Zeitwerte vergleichbar sind.The particularly good catalytic effectiveness of the listed class of compounds is shown in a very rapid complete transesterification in comparison to other salts which can be used as catalysts. The ones described below Experiments were carried out under conditions of the same type in terms of quantity and equipment carried out so that the quoted fair values are comparable.

Beispiel 100 g Terephthalsäuredimethylester werden mit 110 g Äthylenglykol gemischt und :das Gemisch unter Zusatz von 0,05 bis 0,2g Katalysator in einem 500 cm3 fassenden Dreihalskolben, der mit einem mechanischen Rührer, einem absteigenden Kühler und einer Kapillare zum Durchleiten von trockenem Stickstoff versehen ist, im Ölbad erwärmt. Die Badtemperatur wird so geregelt, daß nach Einsetzen der Umesterung, was zwischen 170 und 1851 C geschieht, das Abdestidlleren des frei werdenden Methanols möglichst mit konstanter Geschwindigkeit vor sich geht. Die Temperatur übersteigt lin keinem Falle 200'C (im Bad gemessen). Als Umesterungszeit wird,die Dauer des Abdestilllierens von Methanol gemessen, beginnend Menge in % Lfd. des eingesetzten Temperatur Zeit tlbdeshlliertes Nr. Katalysator Tere hthalsäure- Methanol di ethylesters o C Minuten °/° der Theorie 1 Zn-maleinat . . . . . . . . . . . . . .. . . ..... 0,1 185 bis 190 40 99,5 2 Cd-maleinat . .. . . . . .. . .. . . . . . . . . . . 0,1 185 bis 190 90 99,3 3 Zn-methacrylat . . . . . . . . . . . . . . . . . . . . 0,05 185 bis 190 90 99,4 4 Zimtsaures Zn . . . . . . . . . . . . . . . . . . . . 0,1 185 bis 200 65 99,7 5 Aconitsaures Zn . . . . . . . . . . . . . . . . . . 0,1 185 bis 200 85 99,6 6 Zn-malonat . . . . . . . . . . . . . . . . . . . . . . . 0,1 185 bis 195 135 99,2 7 Zn-citrat . . . . . . . . . . . . . . . . . . . . . . . . 0,2 185 bis 200 300 99,5 mit dem übergang des -,ersten Tropfens bis zu dem Zeitpunkt, bei dem mindestens 99% des theoretisch zu erwartenden Methanols überdesüi,lliert sind.Example 100 g of dimethyl terephthalate are mixed with 110 g of ethylene glycol and: the mixture with the addition of 0.05 to 0.2 g of catalyst in a 500 cm3 three-necked flask equipped with a mechanical stirrer, a descending condenser and a capillary for the passage of dry nitrogen is heated in an oil bath. The bath temperature is regulated in such a way that after the onset of transesterification, which takes place between 170 and 1851 C, the removal of the methanol liberated by distillation takes place at a constant rate as far as possible. The temperature never exceeds 200 ° C (measured in the bath). The duration of the distilling off of methanol is measured as the transesterification time, beginning Quantity in% running. the used temperature time tlbdeshllierter No. Catalyst terephthalic acid-methanol di ethyl ester o C minutes ° / ° of theory 1 Zn maleat. . . . . . . . . . . . . ... . . .... 0.1 185 to 190 40 99.5 2 cd maleat. ... . . . ... ... . . . . . . . . . 0.1 185 to 190 90 99.3 3 Zn methacrylate. . . . . . . . . . . . . . . . . . . . 0.05 185 to 190 90 99.4 4 cinnamic acid Zn. . . . . . . . . . . . . . . . . . . . 0.1 185 to 200 65 99.7 5 aconitic acid Zn. . . . . . . . . . . . . . . . . . 0.1 185 to 200 85 99.6 6 Zn malonate. . . . . . . . . . . . . . . . . . . . . . . 0.1 185 to 195 135 99.2 7 Zn citrate. . . . . . . . . . . . . . . . . . . . . . . . 0.2 185 to 200 300 99.5 with the transition of the -, first drop to the point in time at which at least 99% of the theoretically expected methanol has overdesüi, lliert.

Die entsprechend der vorstehenden Versuchsbeschreibung erhaltenen Ergebnisse sind in der vorstehenden Tabelle zusammengefaßt.Those obtained according to the above description of the experiment Results are summarized in the table above.

Die unter Nr.6 und 7 aufgeführten Beispiele der Verwendung von Zinksalzen mit Anionen, die keine Doppelbindung enthalten, sind zum Vergleich aufgeführt.The examples of the use of zinc salts listed under Nos. 6 and 7 with anions that do not contain a double bond are listed for comparison.

Claims (4)

PATENTANSPRÜCHE-1. Verfahren zur Umesterung von aromatischen Dicarbonsäuredialkylestern mit Hilfe von Salzen der Metalle der II. Gruppe des Periodensystems, dadurch gekennzeichnet, .daß man solche Salze, die als Anion den Rest einer organischen, eine Doppel-(bindung besitzenden ein- oder mehrbasischen Säure enthalten, bei 170 bis 200° C verwendet. PATENT CLAIMS-1. Process for the transesterification of aromatic dicarboxylic acid dialkyl esters with the help of salts of metals of group II of the periodic table, characterized in that .that such salts, which as the anion are the remainder of an organic, double (bond containing mono- or polybasic acid, used at 170 to 200 ° C. 2. Verfahren nach Anspruch 1, dadurch gekennzeichnet, daß man --die Zink- und Cadmiuansalze der Maleinsäure, Methacrylsäure, Zimtsäure und Aconitsäure verwendet. 2. The method according to claim 1, characterized in that - the zinc and cadmium salts the maleic acid, methacrylic acid, cinnamic acid and aconitic acid are used. 3. Verfahren nach Anspruch 1 und 2, dadurch gekennzeichnet, daß man 0,02 bis 0,2 Gewichtsprozent der Salze, bezogen auf das Gewicht der eingesetzten aromatischen Dicarbonsäuredialkylester, verwendet. 3. Procedure according to claim 1 and 2, characterized in that 0.02 to 0.2 percent by weight the salts, based on the weight of the aromatic dialkyl dicarboxylate used, used. 4. Verfahren nach Anspruch 1 bis 3, dadurch gekennzeichnet, daß man die Umesterung mit einem Glykalüberschuß durchführt.4. The method according to claim 1 to 3, characterized in that the Carries out transesterification with an excess of glycal.
DED30702A 1959-05-20 1959-05-20 Process for the transesterification of dialkyl benzene dicarboxylates with glycols Pending DE1086689B (en)

Priority Applications (5)

Application Number Priority Date Filing Date Title
NL251667D NL251667A (en) 1959-05-20
DED30702A DE1086689B (en) 1959-05-20 1959-05-20 Process for the transesterification of dialkyl benzene dicarboxylates with glycols
CH476960A CH378303A (en) 1959-05-20 1960-04-26 Process for the catalytic transesterification of benzene dicarboxylic acid alkyl esters with glycols
GB17004/60A GB922467A (en) 1959-05-20 1960-05-13 Improvements in or relating to the catalytic transesterification of aromatic dicarboxylic acid dialkyl esters with glycols
BE590976A BE590976A (en) 1959-05-20 1960-05-18 Process for the catalytic transesterification of alkyl esters of benzene dicarboxylic acids.

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DED30702A DE1086689B (en) 1959-05-20 1959-05-20 Process for the transesterification of dialkyl benzene dicarboxylates with glycols
FR826880A FR1256829A (en) 1960-05-11 1960-05-11 Catalytic trans-esterification process, using glycols, of alkyl esters of benzenedicarboxylic acid

Publications (1)

Publication Number Publication Date
DE1086689B true DE1086689B (en) 1960-08-11

Family

ID=25970950

Family Applications (1)

Application Number Title Priority Date Filing Date
DED30702A Pending DE1086689B (en) 1959-05-20 1959-05-20 Process for the transesterification of dialkyl benzene dicarboxylates with glycols

Country Status (4)

Country Link
CH (1) CH378303A (en)
DE (1) DE1086689B (en)
GB (1) GB922467A (en)
NL (1) NL251667A (en)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1244797B (en) 1962-07-06 1967-07-20 Witten Gmbh Chem Werke Process for the preparation of phenyl esters of carbocyclic, aromatic, optionally ring-substituted mono- and polycarboxylic acids

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1244797B (en) 1962-07-06 1967-07-20 Witten Gmbh Chem Werke Process for the preparation of phenyl esters of carbocyclic, aromatic, optionally ring-substituted mono- and polycarboxylic acids

Also Published As

Publication number Publication date
NL251667A (en) 1900-01-01
GB922467A (en) 1963-04-03
CH378303A (en) 1964-06-15

Similar Documents

Publication Publication Date Title
DE1156788B (en) Process for the conversion of fatty acid esters of monohydric alcohols with isolated double bonds (íÀIsolenfettsaeureesterníÂ) into fatty acid esters with conjugated double bonds (íÀkonjuenfettsaeureesteríÂ)
DE1039748B (en) Process for the production of polyesters
DE2003579B2 (en)
DE1468932B2 (en) PROCESS FOR THE CONTINUOUS PRODUCTION OF LOW MOLECULAR ALIPHATIC ACRYLIC ACID ESTERS
DE870107C (en) Process for the catalytic hydrogenation of organic compounds
DE1086689B (en) Process for the transesterification of dialkyl benzene dicarboxylates with glycols
DE1520079B2 (en) PROCESS FOR MANUFACTURING HIGH POLYMERIC POLYMETHYLENE TEREPHTHALATE
DE1570627C3 (en) Process for making linear fiber-forming polyesters
DE2111669A1 (en) Manufacture of alcohols
DE1173473B (en) Process for the preparation of aliphatic or aromatic carboxylic acid esters
DE1283228B (en) Process for the preparation of vinyl esters
DE755279C (en) Process for the production of higher unsaturated aliphatic alcohols
AT281006B (en) PROCESS FOR THE MANUFACTURING OF DIALKYLTEREPHTHALATES BY DEGRADING WASTE FROM LINEAR POLYESTERS OR MIXED POLYESTERS
DE1002751B (en) Process for the preparation of monomeric and polymeric polycarboxylic acid glycol esters
DE1052394B (en) Process for the production of terephthalic acid-bis-ethylene glycol ester by degradation vo
DE863938C (en) Process for the production of aldol condensation products
DE626290C (en) Process for the production of higher molecular alcohols
DE2156133C3 (en) Process for the preparation of butyl glycolate
AT142785B (en) Process for the preparation of higher aliphatic alcohols.
DE1144710B (en) Process for the preparation of tere- or isophthalic acid dialkyl esters
DE592053C (en) Process for the preparation of esters
DE1003734B (en) Process for the production of oxygen-containing compounds, preferably consisting of alcohols and ketones, by the oxidation of aliphatic hydrocarbons
DE949652C (en) Process for the rearrangement of naphthalic acid into naphthalene-2,6-dicarboxylic acid
DE2203813A1 (en) Process for the preparation of carboxylic acid esters
DE895899C (en) Process for the production of dichlorocarbonic acid esters