CA1072561A - Preparation of n,n-dimethylpiperidinium chloride and n,n-dimethylmorpholinium chloride - Google Patents

Preparation of n,n-dimethylpiperidinium chloride and n,n-dimethylmorpholinium chloride

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Publication number
CA1072561A
CA1072561A CA288,706A CA288706A CA1072561A CA 1072561 A CA1072561 A CA 1072561A CA 288706 A CA288706 A CA 288706A CA 1072561 A CA1072561 A CA 1072561A
Authority
CA
Canada
Prior art keywords
chloride
reaction
dimethylpiperidinium
dimethylmorpholinium
methyl
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.)
Expired
Application number
CA288,706A
Other languages
French (fr)
Inventor
Hans Urbach
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.)
BASF SE
Original Assignee
BASF SE
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 BASF SE filed Critical BASF SE
Application granted granted Critical
Publication of CA1072561A publication Critical patent/CA1072561A/en
Expired legal-status Critical Current

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Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D295/00Heterocyclic compounds containing polymethylene-imine rings with at least five ring members, 3-azabicyclo [3.2.2] nonane, piperazine, morpholine or thiomorpholine rings, having only hydrogen atoms directly attached to the ring carbon atoms
    • C07D295/02Heterocyclic compounds containing polymethylene-imine rings with at least five ring members, 3-azabicyclo [3.2.2] nonane, piperazine, morpholine or thiomorpholine rings, having only hydrogen atoms directly attached to the ring carbon atoms containing only hydrogen and carbon atoms in addition to the ring hetero elements
    • C07D295/023Preparation; Separation; Stabilisation; Use of additives

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Hydrogenated Pyridines (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Pyridine Compounds (AREA)
  • Agricultural Chemicals And Associated Chemicals (AREA)

Abstract

O.Z. 32,292 ABSTRACT OF THE DISCLOSURE: The preparation of N,N-dimethylpiperi-dinium chloride and N,N-dimethylmorpholinium chloride from the corresponding monomethyl compounds with methyl chloride in the presence of water.

Description

:~O~Z~l o, zo 32, 292 PREPARATION OF N,N-DIMETHYLPIPERIDINIUM CHLORIDE
AND N,N DIMETH~LMORPHOLINIUM CHLORIDE
The present invention relates to a process for the preparation o~ N,N-dimethylpiperidinium chloride and N,N-dimethylmorpholinium chloride from the corresponding monomethyl compounds with methyl chloride in the presence of waterO
It is known (German 1,642,215 and German Laid-Open ~pplication DOS 2,207,57~) to use N,N-dimethylpiperidinium chloride and N3N-dimethylmorpholinium chloride as agents for influencing plant growth. They are applied as an aqueous solution. They are prepared - -in conventional manner by conversion o~ N,N-dimethylpiperidinium iodide and N,N-dimethylmorpholinium iodide into the corresponding chlorides (Helv. Chim. Acta, 39, 399, 1956; Chem. Ber., 22, 2091, 1889).
We have now found that N,N-dimethylpiperidinium chloride and NgN-dimethylmorpholinium chloride are easily obtained from N-methyl piperidine and N-methylmorpholine respectively, in excellent yields, when the monomethyl compounds are reacted with methyl chloride in the presence of water as diluent at a temperature of ~rom 0 to 100C and a pressure of ~rom 1 to 7 bars This is surprisin~ and could not have been foreseen, because methylation with methyl chloride hitherto has been carried out in non-aqueous solvents, or, when water has been used as diluent, temperatures far in excess (120C) o~ room temperature and high pressures (20 to 60 bars) have been employedO
The process according to the invention has two essential advan-tages: a) the process is very simple and thus extremely econo~ical as a result of the use of water as diluent, because the aqueous .~

~ S~ OOZo 32,~92 solution of the end products can be employed direct for biolo~ical purposes; b) as the reaction takes place at atmospheric or sli~htly superatmospheric pressure, inexpensive standard stirred vessels may be used, as they are usually~ even when intended for pressureless reactions, designed for safety reasons to withstand a pressure of from 4 to 7 barsO
When N-methylpiperidine is used, the reaction may be represented as follows:

C 3 3 ~ CH3 Compared with prior art processes, the process of the invention provides, in a simpler and more economic manner, the desired quaternary ammonium chlorides in good yield and high purityO Whereas prior art processes were cumbersome because they had to be carried out in two stages, the reaction in the process according to the invention is carried out in one step.
Starting materials for the process are N-methylpiperidine3 N-methylrnorpholine and methyl chloride. They are used for instance in approximately equivalent amounts, optionally with a slight excess of methyl chloride.
The reaction may be carried out for instance as follows~ Water and the monomethylarnine are placed in the reaction vessel, and the mixture is heated to the desired reaction temperature and ~hen treated with methyl chloride. Advantageously, the reaction components are mixed with each other, for example by stirringO A~ter the reaction is over, the reaction solution is cooled to room tempera-ture and then diluted with water to the desired active ingredient concentration.

The monomethylamine concentration in the water upon cornmencement of the reaction may be varied within wide limits. It is preferred to use concentrations whlch, upon completion Or the reaction~ give end product concentrations slightly above the concentration of the 7Z~6~
0 ZO 32,292 aqueous solutlons when marketedD However~ it is also possible to start with more dilute aqueous solution and to distil off some~of the water used after che reaction is over without the quality of the end products sufferingO The concentration of the monomethyl~
amines in the water may also be so high that they are not fully -dissolved, either initially or during the reactionc As methyl chloride is a gas, it is advantageous to employ a closed apparatusO The process according to the invention may be operated at atmospheric or superatmospheric pressureO In the latter case the reaction proceeds somewhat more quicklyO I~ the process is operated at atmospheric pressure, it is expedient to free the reaction vessel substantially from air by partial evacuation; the desired pressure can now be set up by introduction of the methyl chlorideO
If the pressure is constant during the reaction, the progress of the reaction can be followed by the amount of methyl chloride suppliedO
The reaction is carried out at from 0 to 100C, preferably ~-at at least 20C, advantageously from 30 to 80C, and especially at from 40 to 60C, and continuously or batchwiseO
The duration of the reaction is without relevance for the quality of the end products~ The reaction period can therefore be chosen in accordance with economic considerations. It may for instance be more favorable to operate at atmospheric pressure because only a vessel designed for atmospheric operation is available, and to accept a longer reaction periodD
Upon conclusion of the reaction no more methyl chloride is taken up; the pH of the reaction solution is 6 to 70 The solution is a clear almost colorless liquidO
In the reaction according to the invention, the desired end products are formed practically exclusively, iOeO, no byproducts are obtained, and consequently the yield is practically quantitative.
The only byproducts which may occur are those from impurities ~3--O~Z 32,292 in the starting materialsO If~ for example~ the N-methylpiperidine still contains small amounts of unsubstituted piperldine, N-methyl-piperidine hydrochloride, which is not further methylated because of the hydrochloride formation3 is formed in the reaction with methyl chlorideO If basic compounds which liberate the amines from amins hydrochlorides, eOg., sodiu~ hydroxide, are added to the starting solution, the formation of the hydrochloride of the tertiary amine described above can be preventedO I~ the metal chloride formed from the amine hydrochloride and the basic additive is no handicap, it is possible to make the process even more econo-mical by starting from impure amihesO If a fairly large amount of metal chloride is no drawback, it is even possible to start from the secondary amines, iOe., from piperidine and morpholine, and ~o react them under the abovementioned reaction conditions with methyl chloride in the presence of an equivalent of a basic additiveO The end product obtained is an aqueous solution of a mixture of 1 mole of quaternary ammonium chloride and an equivalent of metal chlorideO
The process of the invention also represents an advance because it does not harm the environment. There is absolutely no solid or liquid waste, as the reaction solution is the desired end product.
Gaseous emissions can be substantially avoided if the reaction vessel is emptied and charged with the starting materials without being previously vented; this can be done without dif~iculty with the aid of pumps.
As the aqueous solution contains some methyl chloride upon completion of the reaction, this solution might be considered to be a source of impurities. In this case, the solution may~ a~ter completion of the reaction, be passed through an evaporator or a distillation column to free it from methyl chlorideO The aqueous distillate thus obtained can then be added to the next production batch as a diluent.
Both N,N-dimethylpiperidinium chloride and N,N-dimethylmorpho-linium chloride can be produced with the same equipment 9 which can 5~ OOZo 32g292 conceivably be of economic importanceO If desiredg both products may be produced together in admixture; this measure can definit~ely be meaning~ul3 because both products can also be particularly success-fully applied together in some cropsO
If it is desired to isolate both products in the form of solid crystalline substances, this can readily be achieved by evaporating the aqueous solutionsO They are obtained as coarse colorless crystals of hi~h purity which have melting points of more than 300Co EXAMPLE
30 parts by volurne of water and 15 o 6 parts by weight o~
N-methylpiperidine (parts by volume bear the same relationship to parts by weight as liters to kilo~rams) were introduced into a -jacketed s~irred vessel having a volume of 100 parts by volume.
The apparatus was evacuated and heated to 50Co At this temperature, ~.
a maximum of 1,000 parts by volume of methyl chloride was intro-duced per hour through a flowmeter, and the mixture was stirred.
After about 2 hours a pressure of 2 bars had been reached, which was maintained by continuously controlled addition of methyl chlorideO
During the reaction, water at 55C was passed through the jacketing, thus maintaining the internal temperature at 49~50C.
After 7025 hours, the pressure remained constant without methyl chloride being passed inO The mixture was stirred for a further 0075 hour, and the apparatus was then emptied in such a manner that the bottom valve just stayed covered, thus preventing the pressure on the vessel from being releasedO
The solution thus obtained was a yellowish clear li~uid having a pH of 6.9 and containing, in accordance with a test in which the N,N-dimethylpiperidinium chloride was precipitated and determined gravimetricallyg 0 46 part by weight per part by volume.

The yield was thus quantitativeO
Methyl chloride consumption corresponded to a molar ratio of N-methylpiperidine to methyl chloride of 1 : 1~02 o~
o~Zo 3~,292 Completely analogously, N,N dimethylmorpholiniuM chloride is obtained ~rom N~methylmorpholine and methyl chloride~ In this ~case the reaction period is 14 hoursO

Claims

O.Z. 32,292 The embodiments of the invention in which an exclusive property or privilege is claimed are defined as follows:-A process for the manufacture of N,N-dimethylpiperidinium chloride by reacting N-methylpiperidine, or of N,N-dimethylmorpho-linium chloride by reacting N-methylmorpholine, with a methylating agent, wherein the monomethyl compounds are reacted with methyl chloride in the presence of water as diluent, at a temperature of from 0° to 100°C and a pressure of from 1 to 7 bars.
CA288,706A 1976-11-15 1977-10-13 Preparation of n,n-dimethylpiperidinium chloride and n,n-dimethylmorpholinium chloride Expired CA1072561A (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DE2651984A DE2651984C2 (en) 1976-11-15 1976-11-15 Process for the preparation of N, N-dimethylpiperidinium chloride or N, N-dimethylmorpholinium chloride

Publications (1)

Publication Number Publication Date
CA1072561A true CA1072561A (en) 1980-02-26

Family

ID=5993174

Family Applications (1)

Application Number Title Priority Date Filing Date
CA288,706A Expired CA1072561A (en) 1976-11-15 1977-10-13 Preparation of n,n-dimethylpiperidinium chloride and n,n-dimethylmorpholinium chloride

Country Status (14)

Country Link
JP (1) JPS5363384A (en)
BE (1) BE860788A (en)
CA (1) CA1072561A (en)
CH (1) CH630913A5 (en)
DD (1) DD132342A5 (en)
DE (1) DE2651984C2 (en)
DK (1) DK159682C (en)
FR (1) FR2370740A1 (en)
GB (1) GB1587925A (en)
IL (1) IL53112A (en)
IT (1) IT1091782B (en)
NL (1) NL189131C (en)
SE (1) SE7712787L (en)
SU (1) SU671730A3 (en)

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
AU670783B2 (en) * 1992-06-04 1996-08-01 Micro Flo Company Mepiquat chloride
US9321723B2 (en) * 2013-08-28 2016-04-26 Johnson Matthey Plc Method of making a templating agent
CN113024413B (en) * 2019-12-25 2022-12-06 北京颖泰嘉和生物科技股份有限公司 Synthesis method of salicylonitrile co-produced plant growth regulator
CN117756748A (en) * 2023-12-26 2024-03-26 中棉小康生物科技有限公司 Synthesis method of mepiquat chloride

Family Cites Families (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE756185C (en) * 1939-08-27 1952-05-19 Onderzoekings Inst Res Process for the preparation of quaternary aliphatic ammonium chlorides
US3928423A (en) * 1972-07-17 1975-12-23 Kendall & Co Monomeric emulsion stabilizers
DE2247501A1 (en) * 1971-10-02 1973-04-05 Inst Przemyslu Organiczego Quaternary ammonium halides prepn - from sec amines
BE795534A (en) * 1972-02-18 1973-08-16 Basf Ag AGENTS FOR REGULATING PLANT GROWTH, CONTAINING NITROGEN SALT AS ACTIVE INGREDIENT

Also Published As

Publication number Publication date
FR2370740B1 (en) 1981-06-19
SE7712787L (en) 1978-05-16
NL7712395A (en) 1978-05-17
DK159682C (en) 1991-04-15
IT1091782B (en) 1985-07-06
DD132342A5 (en) 1978-09-20
DK159682B (en) 1990-11-19
JPS6225144B2 (en) 1987-06-01
IL53112A0 (en) 1977-12-30
DE2651984A1 (en) 1978-05-18
FR2370740A1 (en) 1978-06-09
GB1587925A (en) 1981-04-15
SU671730A3 (en) 1979-06-30
DE2651984C2 (en) 1983-01-27
BE860788A (en) 1978-05-16
DK503177A (en) 1978-05-16
NL189131C (en) 1993-01-18
JPS5363384A (en) 1978-06-06
CH630913A5 (en) 1982-07-15
IL53112A (en) 1981-03-31

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