IP Library Granted Patent US 11,655,202
Granted Patent B2
US 11,655,202 · App. 17/268,991 · Granted May 23, 2023

Process for preparing a cycloaliphatic diester

Inventors: Alexander Meyer (Düsseldorf, DE); Thomas Pfingst (Tönisvorst, DE); Dirk Hinzmann (Pulheim, DE)
Assignee: Covestro Intellectual Property GmbH & Co. KG
C07C67/10C07C69/75C08G63/64C08G64/20
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Quick Facts
Patent No.
US 11,655,202
App. No.
17/268,991
Granted
May 23, 2023
Kind
B2
Abstract

The present invention relates to a method for producing a cycloaliphatic diester, to a method for producing a polyestercarbonate using the one cycloaliphatic diester, to the use of a cycloaliphatic diester for producing polyestercarbonates and also to a polyestercarbonate. The method according to the invention is here in particular characterized in that the cycloaliphatic diester is separated by means of distillation from the reaction mixture.

Claims (43)

1. A method for producing a cycloaliphatic diester of formula (Ia) or (Ib),

in which

A each independently is an aliphatic or aromatic radical and

n is a number between 0 and 3,

comprising the steps of

(i) reacting a mixture comprising at least one cycloaliphatic dicarboxylic acid and at least one aliphatic and/or aromatic carbonate, in the presence of a basic catalyst, to give a cycloaliphatic diester of formula (Ia) or (Ib) and

(ii) separating the cycloaliphatic diester of formula (Ia) or (Ib) from the mixture of method step (i) by means of distillation at a temperature of 180° C. to 280° C.

2. The method according to claim 1 , wherein the distillation in method step (ii) is conducted at pressures of 10 mbar or lower.

3. The method according to claim 1 , wherein, in method step (i), an aromatic carbonate of formula (2) is used

where R, R′ and R″ each independently can be the same or different and are hydrogen, optionally branched C1-C34-alkyl, C7-C34-alkylaryl or C6-C34-aryl, R can additionally also denote —COO—R′″, where R′″ is optionally branched C1-C34-alkyl, C7-C34-alkylaryl or C6-C34-aryl.

4. The method according to claim 3 , wherein, in method step (i), diphenyl carbonate is used as aromatic carbonate.

5. The method according to claim 1 , wherein method steps (i) and (ii) are conducted in the absence of an additional organic solvent.

6. The method according to claim 1 , wherein, in method step (i), at least one stabilizer selected from the group consisting of P-containing stabilizers and/or phenolic free-radical scavengers is added.

7. The method according to claim 1 , wherein the reaction of method step (i) is conducted at temperatures of 180 to 280° C.

8. The method according to claim 1 , wherein, during the reaction in method step (i), the volatile constituents which have a boiling point below the cycloaliphatic diester of formula (Ia) or (Ib) and below the aliphatic and/or aromatic carbonate are removed, optionally in steps, by means of distillation.

9. A method for producing a polyestercarbonate by means of melt transesterification, comprising the steps of:

(a) producing a cycloaliphatic diester of formula (Ia) or (Ib),

in which

A each independently is an aliphatic or aromatic radical and

n is a number between 0 and 3,

by:

(i) reacting a mixture comprising at least one cycloaliphatic dicarboxylic acid and at least one aliphatic and/or aromatic carbonate, in the presence of a basic catalyst, to give the cycloaliphatic diester of formula (Ia) or (Ib); and

(ii) separating the cycloaliphatic diester of formula (Ia) or (Ib) from the mixture of method step (i) by means of distillation at a temperature of 180° C. to 280° C.; and

(b) reacting the cycloaliphatic diester of formula (Ia) or (Ib) from method step (a), at least one dihydroxy compound and at least one diaryl carbonate in a melt transesterification process.

10. The method according to claim 9 , wherein method step (b) is performed immediately after method step (a).

11. The method according to claim 9 , wherein the dihydroxy compound in method step (b) is selected from the group consisting of cyclohexane-1,2-diol, cyclohexane-1,3-diol, cyclohexane-1,4-diol, cyclohexane-1,2-dimethanol, cyclohexane-1,3-dimethanol, cyclohexane-1,4-dimethanol, tricyclodecanedimethanol, 3,9-bis(1,1-dimethyl-2-hydroxyethyl)-2,4,8,10-tetraoxaspiro [5.5] undecane, 2,2-bis(4-hydroxycyclohexyl)propane, tetrahydro-2,5-furandimethanol, bisphenol A, 1,1-bis(4-hydroxyphenyl)-3,3,5-trimethylcyclohexane, 4,4′-dihydroxybiphenyl (DOD), 4,4′-dihydroxybiphenyl ether (DOD ether), bisphenol B, bisphenol M, the bisphenols (I) to (III)

wherein the formula (I) to (III) R′ in each case is C1-C4-alkyl, aralkyl or aryl, butanediol, succinic acid, adipic acid, ethylene glycol, lactic acid, hexanediol and 1,4:3,6-dianhydrohexitols.

12. A method according to claim 9 , wherein as diaryl carbonate in method step (b) a compound of formula (2) is used

where R, R′ and R″ each independently can be the same or different and are hydrogen, optionally branched C1-C34-alkyl, C7-C34-alkylaryl or C6-C34-aryl, R can additionally also denote —COO—R′″, where R′″ is optionally branched C1-C34-alkyl, C7-C34-alkylaryl or C6-C34-aryl.

13. A method of producing a polyestercarbonate by means of melt transesterification comprising:

(a) producing a cycloaliphatic diester of formula (Ia) or (Ib),

in which

A each independently is an aliphatic or aromatic radical and

n is a number between 0 and 3,

by:

(i) reacting a mixture comprising at least one cycloaliphatic dicarboxylic acid and at least one aliphatic and/or aromatic carbonate, in the presence of a basic catalyst, to give the cycloaliphatic diester of formula (Ia) or (Ib); and

(ii) separating the cycloaliphatic diester of formula (Ia) or (Ib) from the mixture of method step (i) by means of distillation at a temperature of 180° C. to 280° C.; and

(b) reacting the cycloaliphatic diester of formula (Ia) or (Ib) with a bio-based dihydroxy compound and a diaryl carbonate.

14. The method according to claim 11 , wherein R′ in each case is methyl or phenyl.

15. The method according to claim 11 , wherein R′ in each case is methyl.

16. The method according to claim 11 , wherein the 1,4:3,6-dianhydrohexitol is selected from the group consisting of isomannide, isoidide and isosorbide.

17. The method according to claim 13 , wherein the bio-based dihydroxy compound comprises a 1,4:3,6-dianhydrohexitol.

18. The method according to claim 17 , wherein the 1,4:3,6-dianhydrohexitol is selected from the group consisting of isomannide, isoidide or isosorbide.

Assignments (2)
MERGER Recorded Oct 29, 2024
From: COVESTRO INTELLECTUAL PROPERTY GMBH & CO. KG
To: COVESTRO DEUTSCHLAND AG
Reel/Frame 069272/0414 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Feb 17, 2021
From: MEYER, ALEXANDER; PFINGST, THOMAS; HINZMANN, DIRK
To: COVESTRO INTELLECTUAL PROPERTY GMBH & CO. KG
Reel/Frame 055283/0213 →
Priority Claims (1)
EP 18189636 · Aug 17, 2018 · regional
Continuity (1)
Related Publication 20220119334A1 · Apr 21, 2022