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EP0000778A1 - Procédé pour la préparation de polyamines de la série des diphénylméthanes - Google Patents

Procédé pour la préparation de polyamines de la série des diphénylméthanes Download PDF

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Publication number
EP0000778A1
EP0000778A1 EP7878100591A EP78100591A EP0000778A1 EP 0000778 A1 EP0000778 A1 EP 0000778A1 EP 7878100591 A EP7878100591 A EP 7878100591A EP 78100591 A EP78100591 A EP 78100591A EP 0000778 A1 EP0000778 A1 EP 0000778A1
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EP
European Patent Office
Prior art keywords
water
weight
ion exchangers
styrene
divinyl 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.)
Granted
Application number
EP7878100591A
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German (de)
English (en)
Other versions
EP0000778B1 (fr
Inventor
Rainer Dr. Neumann
Hans-Helmut Dr. Schwarz
Jürgen Dr. Heuser
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.)
Bayer AG
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Bayer AG
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Publication of EP0000778B1 publication Critical patent/EP0000778B1/fr
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Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C209/00Preparation of compounds containing amino groups bound to a carbon skeleton
    • C07C209/68Preparation of compounds containing amino groups bound to a carbon skeleton from amines, by reactions not involving amino groups, e.g. reduction of unsaturated amines, aromatisation, or substitution of the carbon skeleton
    • C07C209/78Preparation of compounds containing amino groups bound to a carbon skeleton from amines, by reactions not involving amino groups, e.g. reduction of unsaturated amines, aromatisation, or substitution of the carbon skeleton from carbonyl compounds, e.g. from formaldehyde, and amines having amino groups bound to carbon atoms of six-membered aromatic rings, with formation of methylene-diarylamines

Definitions

  • Polyamines of the diphenylmethane series are formed as condensation products from aniline and formaldehyde on acidic catalysts.
  • aniline and formaldehyde react without catalysts to form N-alkyl compounds, which are referred to as precondensates.
  • this precondensate rearranges into polyamines of the diphenylmethane series. This creates a mixture of 2,2'-, 2,4'-, 4,4'-diaminodiphenyl-methane and higher condensation products (trinuclear to hexahedral).
  • the corresponding polyisocyanates of the diphenylmethane series are obtained, which are valuable starting materials in the production of polyurethane plastics, in particular polyurethane foams.
  • polyurethane plastics in particular polyurethane foams.
  • the proportion of ortho-standing isocyanate groups present in them in particular the proportion of 2,2'- and 2,4'-diisocyanatodiphenylmethane, is as low as possible. Accordingly, strives already in the aniline / formaldehyde condensation polyamine mixtures of the diphenylmethane series which meet these requirements with regard to the isomer distribution.
  • hydrochloric acid When using hydrochloric acid as a catalyst, it is possible to keep the o-isomer content in the condensation mixture low, but the use of hydrochloric acid (or aniline hydrochloride) has the disadvantages of corrosiveness and the need for neutralization or elaborate removal of the catalyst connected by the reaction product. In principle, these disadvantages can be avoided by using heterogeneous acidic catalysts, such as ion exchangers, but it has so far not been possible to use these catalysts to produce polyamines of the diphenylmethane series which, for example, contain less than 12% of 2,4 ' -Diaminodiphenylmethane and have a content of less than 2% of 2,2'-diaminodiphenylmethane.
  • heterogeneous acidic catalysts such as ion exchangers
  • a polyamine mixture of the diphenylmethane series is obtained on organic acidic ion exchangers which contains 24-26% by weight of 2,4'- and approx. 2.8% by weight of 2,2'-diaminodiphenylmethane.
  • polyamines of the diphenylmethane series are to be understood both as polyamine mixtures as they arise in the condensation of aniline itself with formaldehyde in the presence of acid catalysts, and as polyamine mixtures as they are through acid-catalyzed condensation on nitrogen or on the nucleus substituted anilines can be obtained with formaldehyde.
  • the preferred polyamines of the diphenylmethane series according to the invention are the classic aniline / formaldehyde condensates.
  • any primary or secondary arylamines to be regarded as substituted anilines can be used as starting materials in the process according to the invention.
  • the only prerequisite for the suitability of the amines as starting material in the process according to the invention is that the substituents which may be present are inert under the reaction conditions of the process according to the invention and that the para-position which is unsubstituted to an aromatically bound amino group is present.
  • Arylamines suitable as starting materials are accordingly N-methylaniline, N-ethylaniline, o-toluidine, o-chloroaniline, m-chloroaniline, o-anisidine, 2,3-xylidine, 3,5-xylidine, o-cyclohexylaniline, o-benzylaniline, ⁇ -naphthylaniline, methylmercaptoaniline or the aniline particularly preferred in the context of the present invention.
  • the formaldehyde to be used as a reactant for the arylamine in the process according to the invention is preferably used as an aqueous formalin solution, although. in principle also gaseous formaldehyde or substances which release formaldehyde under the reaction conditions, e.g. Paraformaldehyde or trioxymethylene are suitable.
  • the catalysts can be used in various external forms, e.g. in lumpy form, in the form of commercially available pearl granules or in a finely ground state. Activation of the catalyst can optionally be achieved in a manner known per se by acid treatment.
  • the molar ratio of arylamine: formaldehyde is generally kept in the range from 3: 1 to 15: 1, preferably 5: 1 to 10: 1.
  • the process according to the invention is carried out in such a way that the aqueous formaldehyde solution or the formaldehyde-releasing substance is added to the aromatic amine, care being taken to ensure thorough mixing and removal of the heat of reaction.
  • the aromatic amine is expediently used immediately in the excess desired for the further conduct of the reaction and at the same time serves as a solvent for the N-substituted precondensate which forms, under certain circumstances. in any case, the reaction mixture must be saturated with water by the additional addition of water.
  • the water-saturated reaction mixture is now using the above. Catalysts further reacted at elevated temperature, the process product according to the invention being formed from the precondensate and part of the amine present in excess.
  • the process product according to the invention being formed from the precondensate and part of the amine present in excess.
  • the process according to the invention is used in particular during the catalyzed rearrangement of the N-substi according to the invention tuated intermediates in the process products according to the invention at elevated temperatures generally carried out in the temperature range from 50 to 150 ° C.
  • care must be taken to ensure that pressure and temperature ratios are chosen so that the water and condensation water introduced into the reaction mixture are not distilled off to any appreciable extent, so that it is always ensured that the catalyst is present in the water-saturated state. It is essential, therefore, that when working at temperatures above 100 ° C., a pressure preventing the water from distilling off is maintained.
  • the formation of the N-substituted precondensates generally in the temperature range from 20 to 50 ° C. and the catalytic rearrangement of these precondensation products in the process products according to the invention in the temperature range from 50 to 120 ° C is done.
  • the process according to the invention can be carried out continuously in a contact bed, a stirred tank or a stirred tank cascade, or batchwise in the stirred tank. Since it is not necessary to separate and recycle the catalyst in the contact bed, this type of procedure is recommended.
  • reaction management in particular to remove the heat of reaction, it can also be expedient to have the reaction run in a plurality of stages connected in series, the heat of reaction formed in each case being able to be removed after the individual stages.
  • the reaction mixture is preferably worked up by distillation, although in principle any other suitable separation process can be used.
  • the lower boiling excess amine is distilled off overhead and returned to the process, while the polyamine mixture present as a distillation residue is immediately, e.g. can be further processed in known manner to a polyisocyanate mixture by phosgenation.
  • reaction solution was separated off and the ion exchanger was reacted again with a new starting solution.
  • the reaction solution was saturated with water in each case, which could be recognized by clouding the reaction solution or by forming a separate water phase.
  • the reaction solution after dist. Separation of the aniline examined by high pressure liquid chromatography.
  • the polyamine mixture contained 0.6% by weight of 2,2'-, 10.8% by weight of 2,4'- and 75.3% by weight of 4,4'-diaminodiphenylmethane, the rest consisted of 3- or 4-core connections.
  • Example 1 is repeated with the only difference that an appropriate amount of a water-moist, macroporous ion exchanger which is crosslinked with 18% by weight of divinylbenzene based on divinylbenzene-styrene copolymer was used.
  • the polyamine mixture obtained consisted of 0.6 wt .-% 2,2'-, 8.0 wt .-% 2.4 1 and 73.2 wt .-% of 4,4'-diaminodiphenylmethane and polynuclear compounds together .
  • the tests were carried out as in Example 1 for 3000 h without any change in conversion or selectivity.
  • Example 1 is repeated, with the only difference that a gel-shaped, water-moist ion exchanger crosslinked with 4% by weight of divinylbenzene based on divinylbenzene-styrene copolymer was used.
  • the polyamine mixture obtained was composed of 1.1% by weight of 2,2'-, 14.6% by weight of 2,4'- and 57.2% by weight of 4,4'-diaminodiphenylmethane. Almost 20% by weight consisted of 3- and higher-core compounds.
  • Example 1 is repeated with the only difference that. that a gel-shaped, water-moist, with 8 wt .-% divinylbenzene based on divinylbenzene-styrene copolymer ver networked ion exchanger was used.
  • the polyamine mixture formed contained 3.4% by weight of 2,2'-, 16.5% by weight of 2,4'- and 54% by weight of 4,4'-diaminodiphenylmethane. The rest consisted of higher core connections. The experiments were carried out up to a total of 3000 h without a product corresponding to Examples 1 and 2 being obtained by changing reaction parameters, such as aniline / formaldehyde molar ratio, temperature or residence time.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Low-Molecular Organic Synthesis Reactions Using Catalysts (AREA)
EP78100591A 1977-08-16 1978-08-04 Procédé pour la préparation de polyamines de la série des diphénylméthanes Expired EP0000778B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE19772736862 DE2736862A1 (de) 1977-08-16 1977-08-16 Verfahren zur hestellung von polyaminen der diphenylmethanreihe
DE2736862 1977-08-16

Publications (2)

Publication Number Publication Date
EP0000778A1 true EP0000778A1 (fr) 1979-02-21
EP0000778B1 EP0000778B1 (fr) 1980-07-23

Family

ID=6016494

Family Applications (1)

Application Number Title Priority Date Filing Date
EP78100591A Expired EP0000778B1 (fr) 1977-08-16 1978-08-04 Procédé pour la préparation de polyamines de la série des diphénylméthanes

Country Status (6)

Country Link
EP (1) EP0000778B1 (fr)
JP (1) JPS5432461A (fr)
BR (1) BR7805250A (fr)
DE (2) DE2736862A1 (fr)
ES (1) ES472514A1 (fr)
IT (1) IT1106878B (fr)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0043933A1 (fr) * 1980-07-12 1982-01-20 BASF Aktiengesellschaft Procédé pour la préparation de mélanges de polyamines ayant un taux élevé de 4,4'-diaminodiphénylméthane
EP0078414A1 (fr) * 1981-10-27 1983-05-11 Chemie Linz Aktiengesellschaft Procédé pour la préparation de diamines de la série de diphényl méthane
WO2009144148A1 (fr) * 2008-05-27 2009-12-03 Evonik Degussa Gmbh Procédé pauvre en chlore en plusieurs étapes, pour la préparation de diisocyanates cycloaliphatiques

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2009129286A1 (fr) * 2008-04-16 2009-10-22 Dow Global Technologies Inc. Procédé pour la production de méthane à base de polyaminopolyphényle utilisant un système catalyseur d’acide solide mixte
DE102008001469A1 (de) * 2008-04-30 2009-11-05 Evonik Degussa Gmbh Verfahren zur Herstellung von Diaminodiphenylalkanen
DE102008001492A1 (de) * 2008-04-30 2009-11-05 Evonik Degussa Gmbh Verfahren zur Herstellung von Diaminodiphenylalkanen

Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1179945B (de) * 1962-12-11 1964-10-22 Basf Ag Verfahren zur Herstellung von 4, 4'-Diaminodiphenylmethanen
US3367969A (en) * 1965-03-08 1968-02-06 Du Pont Process for the preparation of 4, 4'-methylenedianiline
DE2037550A1 (de) * 1969-07-31 1971-02-11 Kaiser Aluminum & Chemical Corp., Oakland. Calif (VStA) Verfahren zur Herstellung aromatischer Polyamine
DD109615A1 (fr) * 1972-08-14 1974-11-12
US3971829A (en) * 1974-11-18 1976-07-27 Jefferson Chemical Company, Inc. Preparation of methylene-bridged polyphenylpolyamine mixtures
FR2370032A1 (fr) * 1976-11-06 1978-06-02 Elprochine Ag Procede pour l'obtention de polyarylamines possedant des ponts methylenes

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1179945B (de) * 1962-12-11 1964-10-22 Basf Ag Verfahren zur Herstellung von 4, 4'-Diaminodiphenylmethanen
US3367969A (en) * 1965-03-08 1968-02-06 Du Pont Process for the preparation of 4, 4'-methylenedianiline
DE2037550A1 (de) * 1969-07-31 1971-02-11 Kaiser Aluminum & Chemical Corp., Oakland. Calif (VStA) Verfahren zur Herstellung aromatischer Polyamine
DD109615A1 (fr) * 1972-08-14 1974-11-12
US3971829A (en) * 1974-11-18 1976-07-27 Jefferson Chemical Company, Inc. Preparation of methylene-bridged polyphenylpolyamine mixtures
FR2370032A1 (fr) * 1976-11-06 1978-06-02 Elprochine Ag Procede pour l'obtention de polyarylamines possedant des ponts methylenes

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0043933A1 (fr) * 1980-07-12 1982-01-20 BASF Aktiengesellschaft Procédé pour la préparation de mélanges de polyamines ayant un taux élevé de 4,4'-diaminodiphénylméthane
EP0078414A1 (fr) * 1981-10-27 1983-05-11 Chemie Linz Aktiengesellschaft Procédé pour la préparation de diamines de la série de diphényl méthane
WO2009144148A1 (fr) * 2008-05-27 2009-12-03 Evonik Degussa Gmbh Procédé pauvre en chlore en plusieurs étapes, pour la préparation de diisocyanates cycloaliphatiques
US8536370B2 (en) 2008-05-27 2013-09-17 Evonik Degussa Gmbh Low chlorine, multi-staged method for producing cycloaliphatic disocyanates

Also Published As

Publication number Publication date
ES472514A1 (es) 1979-02-16
EP0000778B1 (fr) 1980-07-23
DE2736862A1 (de) 1979-03-01
BR7805250A (pt) 1979-04-24
IT7850728A0 (it) 1978-08-11
JPS5432461A (en) 1979-03-09
IT1106878B (it) 1985-11-18
DE2860072D1 (en) 1980-11-13

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