IP Library › Granted Patent US 12,612,356
Granted Patent B2
US 12,612,356 · App. 17/919,932 · Granted Apr 28, 2026

Process for nitrate ester formation of an α,ω-alkanediol monoacylate

Inventors: Peter Hans Riebel (Kaiseraugst, CH); Angela Wildermann (Kaiseraugst, CH)
Assignee: DSM IP Assets B.V.
C07C201/02C07C67/08C07C203/02
View Patent ↗
Loading inventors, assignments & file history…
Monitor This Case
Get email alerts when status or documents change.
Order Certified Copies
Most orders are placed with the USPTO same day — all within 24 business hours.
Order via The Patent Place →
Pre-filled with this patent's details
Quick Facts
Patent No.
US 12,612,356
App. No.
17/919,932
Granted
Apr 28, 2026
Kind
B2
Abstract

The invention relates to a safe and efficient process for the nitrate ester formation of an α,ω-C 3-10 alkanediol monoacylate. The process is safer to operators and allows to obtain advantageous yields on industrial scale.

Claims (31)

1 . A continuous process for nitrate ester formation of an α,ω-C 3-10 alkanediol monoacylate, wherein the process comprises a step of:

reacting a nitrating agent with a solution comprising an α,ω-C 3-10 alkanediol monoacylate and an inert solvent in a group of pieces of equipment comprising at least two reactors in series, wherein

the reacting step comprises:

(i) simultaneously feeding the solution into a first reactor and a second reactor of the at least two reactors in series, and

(ii) allowing the nitrating agent to react with the solution in the first and second reactors for a mean residence time of about 5 seconds to about 30 seconds.

2 . The process for the continuous nitrate ester formation according to claim 1 , wherein step (i) comprises feeding 40 to 60% of the total mass flow of the solution into the first reactor, while simultaneously feeding a remaining portion of the total mass flow of the solution into the second reactor.

3 . The process for the continuous nitrate ester formation according to claim 1 , wherein the α,ω-C 3-10 alkanediol monoacylate in the inert solvent in a concentration of from 10 to 60 wt.-%.

4 . The process for the continuous nitrate ester formation according to claim 1 , wherein the nitrating agent is a mixture of H 2 SO 4 and HNO 3 , wherein

a) the mol ratio of HNO 3 to the α,ω-C 3-10 alkanediol monoacylate is selected in the range from 1 to 1.5, and

b) the mole ratio of the H 2 SO 4 to the HNO 3 is selected in the range from 1.5 to 2.5.

5 . The process for the continuous nitrate ester formation according to claim 1 , wherein the reaction volume ratio of the first reactor to the second reactor is selected in the range from 4:1 to 1:4.

6 . The process for the continuous nitrate ester formation according to claim 1 , wherein the mean residence time of the solution in the first and second reactors is about 10 to about 20 seconds.

7 . The process for the continuous nitrate ester formation according to claim 1 , wherein

a) the first reactor has an outlet reaction temperature which is equal to or below 40° C., and

b) the second reactor has an outlet reaction temperature which is equal to or below 25° C.

8 . The process for the continuous nitrate ester formation according to claim 1 , wherein the process forms an α,ω-C 3-10 alkanediol mononitrate, and wherein the process further comprises a step (A) preceding the reacting step which consists of:

(A) an acylation reaction step by conducting an acylation reaction of an α,ω-C 3-10 alkanediol with an acylation agent, wherein α,ω-C 3-10 alkanediol monoacylate and α,ω-C 3-10 alkanediol diacylate back into the acylation reaction such that the acylation reaction comprises adding water in an amount of 0.5 to 1.5 mole per mole of recycled acylate groups, and a molar ratio of a molar sum of the acylating agent, α,ω-C 3-10 alkanediol monoacylate and 2 times of α,ω-C 3-10 alkanediol diacylate to the sum of the α,ω-C 3-10 alkanediol, α,ω-C3-10alkanediol monoacylate and α,ω-C 3-10 alkanediol diacylate is in a range from 0.5 to 1.1 mol per mol of α,ω-C3-10alkanediol, and wherein

the process comprises a step (C) and optionally a step (D) subsequent to the reacting step which consist of:

(C) conducting a two-phase hydrolysis of the α,ω-C3-10alkanediol mononitrate monoacylate by continuously feeding a base and a solution comprising the α,ω-C3-10alkanediol mononitrate monoacylate and an inert solvent into a cascade reactor to obtain a solution comprising the inert solvent and α,ω-C3-10alkanediol mononitrate, and optionally

(D) removing and recovering the inert solvent from the solution by distillation, the process comprising partial condensation and continuous back-feeding of liquid fractions comprising mixtures of the inert solvent and α,ω-C3-10alkanediol mononitrate into the distillation.

9 . The process according to claim 8 , wherein the acylation reaction step

(A) is a continuous process carried out in a vessel cascade set-up.

10 . The process according to claim 8 , wherein the acylation reaction step

(A) comprises a separation step comprising separating the α,ω-C 3-10 alkanediol monoacylate such that:

a) an amount of α,ω-C 3-10 alkanediol in the α,ω-C 3-10 alkanediol monoacylate is less than 0.5 wt.-%, and/or

b) an amount of the α,ω-C 3-10 alkanediol diacylate in the α,ω-C 3-10 alkanediol monoacylate is less than 5 wt. %.

11 . The process according to claim 8 , wherein the acylation agent in the acylation reaction step (A) is a carboxylic acid.

12 . The process according to claim 8 , wherein the two-phase hydrolysis step (C) comprises continuously feeding the base and the solution comprising an α,ω-C 3-10 alkanediol mononitrate monoacylate and an inert solvent a stirred cascade reactor.

13 . The process according to claim 8 , wherein the base in the two-phase hydrolysis step (C) is selected from the group consisting of NaOH, KOH, Ca(OH) 2 , ammonia, and aqueous solutions thereof.

14 . The process according to claim 8 , wherein the two-phase hydrolysis step (C) comprises continuously feeding an aqueous solution of the base in a concentration of from 1 to 50 wt.-%.

15 . The process according to claim 8 , wherein the two-phase hydrolysis step (C) is conducted at a reaction temperature of 20 to 70° C.

Assignments (1)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Oct 19, 2022
From: RIEBEL, PETER HANS; WILDERMANN, ANGELA
To: DSM IP ASSETS B.V.
Reel/Frame 061472/0773 →
Priority Claims (1)
EP 20170758 · Apr 22, 2020 · regional
Continuity (1)
Related Publication 20230150916A1 · May 18, 2023
References Cited (14)
US 7632960B2 · Pöhlmann et al. · 2009 [cited by applicant]
US 10450590B2 · Haas et al. · 2019 [cited by applicant]
US 20100137599A1 · Hack et al. · 2010 [cited by applicant]
CN 1978423 · 2007 [cited by applicant]
CN 101730676 · 2010 [cited by applicant]
EP 2048129 · 2009 [cited by examiner]
EP 2759598 · 2014 [cited by applicant]
GB 432488 · 1935 [cited by examiner]
WO WO2009000723 · 2008 [cited by examiner]
WO 2012084629 · 2012 [cited by applicant]
WO WO2019115503 · 2019 [cited by applicant]
International Search Report for PCT/EP2021/060406, mailed Jun. 29, 2021, 3 pages. [cited by applicant]
Written Opinion of the ISA for PCT/EP2021/060406, mailed Jun. 29, 2021, 5 pages. [cited by applicant]
Second Examination Opinion Notice, CN Application No. 202180029958.1, Dec. 9, 2024. [cited by applicant]