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CN104276978A - Method for synthesizing dichloroglyoxime - Google Patents

Method for synthesizing dichloroglyoxime Download PDF

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Publication number
CN104276978A
CN104276978A CN201310289538.4A CN201310289538A CN104276978A CN 104276978 A CN104276978 A CN 104276978A CN 201310289538 A CN201310289538 A CN 201310289538A CN 104276978 A CN104276978 A CN 104276978A
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CN
China
Prior art keywords
dichloroglyoxime
glyoxime
alcoholic solvent
solution
chlorine
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Pending
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CN201310289538.4A
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Chinese (zh)
Inventor
何金选
叶丹阳
卢艳华
雷晴
郭滢媛
曹一林
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Hubei Institute of Aerospace Chemical Technology
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Hubei Institute of Aerospace Chemical Technology
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Priority to CN201310289538.4A priority Critical patent/CN104276978A/en
Publication of CN104276978A publication Critical patent/CN104276978A/en
Pending legal-status Critical Current

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Abstract

The invention relates to a method for synthesizing dichloroglyoxime. In the method, glyoxime and chlorine are taken as raw materials to have chlorination reaction under the temperature condition of -40 DEG C to 20 DEG C by taking alcohol as a solvent. The method comprises the following steps of: firstly introducing chlorine to an alcohol reaction solvent, and dissolving glyoxime into an alcohol solution; then dropwise adding the glyoxime solution into a reaction system. Compared with the prior art, the method disclosed by the invention has the advantages of moderate and controllable reaction condition, stable yield, low cost and easiness in operation, can be used for producing solid dichloroglyoxime products in a large quantity and is a high-efficiency and reliable synthetic method.

Description

A kind of method of synthesizing dichloroglyoxime
Technical field
The present invention relates to the novel preparation method of a kind of industrial bactericide and energy-containing compound synthetic intermediate-dichloroglyoxime (DCG)
Background technology
Dichloroglyoxime, English name Dichloroglyoxim, is called for short DCG.Molecular formula C 2h 2cl 2n 2o 2, molecular weight 156.95.DCG outward appearance is white crystalline, and fusing point 204 DEG C, is soluble in polar organic solvent.α-halogen oximido compound has anti-microbial activity, and on market, common fungicide mostly is this type of material, and actual sterilizing power, restraint are very not strong.But two this active groups combine the dichloroglyoxime formed, and its sterilizing ability then strongly.Nearest research finds that DCG is used in mthod of white water from paper making and sizes mixing agent aspect, and its sterilizing ability is about stronger 10 times than sterilant DBNPA (2,2-bis-bromo-3-cyano group propionic acid amide).Therefore, dichloroglyoxime has become a kind of novel, efficient industrial bactericide.In 0.5 ~ 3pg/L concentration range, can disturb and even interrupt the flowing of endochylema, finally cause the disintegration of cellular plasm film and play the effect of sterilization.Dichloroglyoxime can be used for mthod of white water from paper making and generates to control rotten slurry, also can be used for the sanitas of industrial detergent, water coolant, lubricating oil, metal working fluid, textile finish oil, coating, latex, tackiness agent, this material leather etc.Dichloroglyoxime is not only a kind of efficient industrial bactericide, is also the important intermediate of heterocyclic nitrogen compound study on the synthesis, is the important raw and processed materials building tetrazole ring, two tetrazolium, the contour nitrogen heterocyclic of furazan.High Nitrogen Heterocyclic Energetic Compounds is widely used in energetic material field, particularly for the current low signature greatly developed low sensitivity propelling agent, novel desensitized explosive, Novel non-toxic high efficient cryogenic gas-evolution agent, low cigarette or smokeless pyrotechnic and the application of nonflame fire-fighting medium etc., high Nitrogen Heterocyclic Energetic Compounds is one of important research object.
But dichloroglyoxime product commercially available at present, substantially be all the high-boiling point alcohol solution of dichloroglyoxime 10%, be difficult to obtain large batch of highly purified dichloroglyoxime solid phase prod, and pure dichloroglyoxime product is its basis as the widespread use of nitrogen heterocyclic important as precursors.
The method of synthesis dichloroglyoxime is mainly following three kinds both at home and abroad at present:
(1) English Patent GB1307223 describes a kind of synthetic method of dichloroglyoxime.Be specially: 18g glyoxime being added 70ml mass fraction is in the hydrochloric acid of 10%, passes into chlorine 8 hours, finally obtains 12g product, and productive rate is 37.5%.
Energetic material volume the 4th phase December the 11st in 2003 reports the method that the people such as Wang Jianlong synthesize dichloroglyoxime, is specially: added by 50g glyoxime in 1000ml water, add 250ml concentrated hydrochloric acid while stirring.Under violent stirring, dissolved by glyoxime, be then cooled with an ice bath, slowly logical chlorine reaction 2h, filters, and dry, obtain dichloroglyoxime product 47g, productive rate is (53%).
(2) US Patent No. 4539405 reports a kind of method of synthesizing dichloroglyoxime.Be specially: under-20 DEG C of conditions, in 95% ethanolic soln, add 17.6g glyoxime solid, pass into chlorine 30 minutes, obtain 24.2-30.2g solid, productive rate is 77%-97%.
Energetic material volume the 5th phase October the 17th in 2009 reports the people such as Bi Fuqiang and adopts US4539405 report method to synthesize the method for dichloroglyoxime, and productive rate is 90.8%.
(3) method of US Patent No. 5476967 pairs of US4539405 reports of nineteen ninety-five is studied, think this method Shortcomings, research finds that this synthetic method must be carried out below-20 DEG C, and the reaction times is sufficiently short, after reaction times extends, productive rate reduces a lot, only may have 10%.US5476967 it is also proposed oneself synthetic method simultaneously, be specially: 172.4g glyoxime is dissolved in 1980g ethylene glycol solvent, pass into 350g chlorine again, temperature of reaction is 15 DEG C, reaction times is 4.5 hours, finally obtain product solution 2114g, calculate by the dichloroglyoxime dissolved in the solution, productive rate is 10.4%.This method can produce the solution product of dichloroglyoxime in a large number, but can not get pure solid phase prod.
Northwest University's journal volume the 1st phase February the 33rd in 2003 reports the method that the people such as Hou Dangshe synthesize dichloroglyoxime solution, be specially: the ethylene glycol solution adding glyoxime in 250mL three-necked bottle, start stirring, under-5 DEG C of conditions, slowly pass into 0.1mol chlorine, 30min has led to.Slowly rise to room temperature after completion of the reaction, underpressure distillation, removing HCl and a small amount of water, obtain glassy yellow settled solution, productive rate is 87.5%.
As can be seen from several method preparing dichloroglyoxime above, the shortcoming of these methods is: method one productivity ratio is lower.Method two thermal discharge is very large, and temperature rise rate is wayward, is only applicable to short run and prepares dichloroglyoxime sample, amplifying (or even hectogram level is amplified) with this technique may cause interior temperature to rise rapidly, test is dangerous to increase, and productive rate reduces rapidly, even cannot obtain product.Method three is only applicable to the ethylene glycol solution preparing dichloroglyoxime.
Summary of the invention
The object of the present invention is to provide a kind of method improving the synthesis dichloroglyoxime of reaction efficiency and product yield, the method is applicable to preparing dichloroglyoxime pure substance product on a large scale.
Solution of the present invention is: with glyoxime and chlorine for raw material, adopts alcoholic solvent, as follows by chlorination synthesis dichloroglyoxime reaction formula:
The present invention adds alcoholic solvent in a reservoir, alcoholic solvent is cooled to-40 ~-20 DEG C, passes into chlorine to saturated while stirring in alcoholic solvent; Glyoxime is dissolved in alcoholic solvent and forms solution, then drip in container, temperature of reaction condition-40 ~-20 DEG C, after dropwising, system rises to room temperature naturally, obtains the alcohol solution of dichloroglyoxime, evaporate to dryness solution obtains solid, with trichloromethane washing, obtains dichloroglyoxime white crystal; The feed molar proportioning of described chlorine and glyoxime is 1:1-10:1, and the feed molar proportioning of alcoholic solvent and glyoxime is 1:1-1:10.
Alcoholic solvent of the present invention is boiling point lower than the straight chain of 100 DEG C and branched alkyl alcohol.
Alcoholic solvent of the present invention is methyl alcohol, ethanol, propyl alcohol, Virahol, the trimethyl carbinol etc.
Be dissolved in alcoholic solvent by glyoxime in the present invention and form solution, then drip in container, wherein time for adding is 0.5 hour ~ 10 hours, and after dripping, the reaction times is 1 hour ~ 48 hours.
Chlorination of the present invention first in alcohols reaction solvent, passes into chlorine.Described chlorination is first dissolved in alcoholic solution by glyoxime, then dripped in reaction system by glyoxime solution.
The present invention's advantage is compared with prior art:
(1) compared with domestic and international existing bibliographical information, this synthetic method mild condition is controlled, and yield stable is reliable.
(2) compared with domestic and international existing bibliographical information, this synthetic method is applicable to amplifying produces, and can synthesize dichloroglyoxime solid phase prod in a large number.
The dichloroglyoxime synthetic method that the present invention introduces is that a kind of efficiency is high, low, the easy-operating synthetic method of stable yield, cost.Adopting the method synthesis dichloroglyoxime, when not reducing product yield, dichloroglyoxime product can be synthesized in a large number.
Specific embodiments
Embodiment 1:
In 1000ml beaker, add 500ml methanol solvate and 10g glyoxime, dissolve stand-by.500ml methanol solvate is added in 3000ml there-necked flask.After methanol solution is cooled to-40 DEG C, start to pass into chlorine in solution, after 30 minutes, in there-necked flask, drip glyoxime solution, control rate of addition, within 0.5 hour, drip off, start stirring.After dropwising, react 1 hour, slowly go up to room temperature.Except desolventizing, with trichloromethane cleaning, obtain product 16.41g, productive rate is 92%.
Embodiment 2:
In 1000ml beaker, add 500ml alcohol solvent and 100g glyoxime, dissolve stand-by.1000ml alcohol solvent is added in 3000ml there-necked flask.After ethanolic soln is cooled to-10 DEG C, start to pass into chlorine in solution, after 1 hour, in there-necked flask, drip glyoxime solution, control rate of addition, within 5 hours, drip off, start stirring.After dropwising, react 20 hours, slowly go up to room temperature.Except desolventizing, with trichloromethane cleaning, obtain product 169.48g, productive rate is 95%.
Embodiment 3:
In 1000ml beaker, add 600ml isopropanol solvent and 50g glyoxime, dissolve stand-by.500ml isopropanol solvent is added in 3000ml there-necked flask.After aqueous isopropanol being cooled to 20 DEG C, start to pass into chlorine in solution, after 30 minutes, in there-necked flask, drip glyoxime solution, control rate of addition, within 10 hours, drip off, start stirring.After dropwising, react 48 hours, slowly go up to room temperature.Except desolventizing, with trichloromethane cleaning, obtain product 85.632g, productive rate is 96%.

Claims (5)

1. synthesize a method for dichloroglyoxime, it is characterized in that: with glyoxime and chlorine for raw material, adopt alcoholic solvent, synthesize dichloroglyoxime by chlorination.
2. the method for synthesis dichloroglyoxime according to claim 1, is characterized in that: add alcoholic solvent in a reservoir, alcoholic solvent is cooled to-40 ~-20 DEG C, passes into chlorine to saturated while stirring in alcoholic solvent; Glyoxime is dissolved in alcoholic solvent and forms solution, then drip in container, temperature of reaction condition-40 ~-20 DEG C, after dropwising, system rises to room temperature naturally, obtains the alcohol solution of dichloroglyoxime, evaporate to dryness solution obtains solid, with trichloromethane washing, obtains dichloroglyoxime white crystal; The feed molar proportioning of described chlorine and glyoxime is 1:1-10:1, and the feed molar proportioning of alcoholic solvent and glyoxime is 1:1-1:10.
3. the method for synthesis dichloroglyoxime according to claim 2, is characterized in that: described being dissolved in alcoholic solvent by glyoxime forms solution and drip in container, and time for adding is 0.5 hour ~ 10 hours, and after dripping, the reaction times is 1 hour ~ 48 hours.
4. the method for synthesis dichloroglyoxime according to claim 1 and 2, is characterized in that: alcoholic solvent is boiling point lower than the straight chain of 100 DEG C and branched alkyl alcohol.
5. the method for synthesis dichloroglyoxime according to claim 1 and 2, is characterized in that: described alcoholic solvent is methyl alcohol, ethanol, propyl alcohol, Virahol or the trimethyl carbinol.
CN201310289538.4A 2013-07-10 2013-07-10 Method for synthesizing dichloroglyoxime Pending CN104276978A (en)

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4539405A (en) * 1984-04-16 1985-09-03 The United States Of America As Represented By The Secretary Of The Navy Synthesis of 1,4-dinitrofurazano(3,4-b)piperazine
EP0636605A1 (en) * 1993-07-27 1995-02-01 Junsei Chemical Co., Ltd. Production method of organic solvent solution of dichloroglyoxime
DE102011081254A1 (en) * 2011-08-19 2013-02-21 Ludwig-Maximilians-Universität München Energetic active mass, useful as an explosive, comprises a dihydroxylammonium salt or diammonium salt of 5,5'-bistetrazol-1,1'-diol, 5,5'-bistetrazol-1,2'-diol, or 5,5'-bistetrazol-2,2'-diol or a mixture of at least two of these salts

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4539405A (en) * 1984-04-16 1985-09-03 The United States Of America As Represented By The Secretary Of The Navy Synthesis of 1,4-dinitrofurazano(3,4-b)piperazine
EP0636605A1 (en) * 1993-07-27 1995-02-01 Junsei Chemical Co., Ltd. Production method of organic solvent solution of dichloroglyoxime
DE102011081254A1 (en) * 2011-08-19 2013-02-21 Ludwig-Maximilians-Universität München Energetic active mass, useful as an explosive, comprises a dihydroxylammonium salt or diammonium salt of 5,5'-bistetrazol-1,1'-diol, 5,5'-bistetrazol-1,2'-diol, or 5,5'-bistetrazol-2,2'-diol or a mixture of at least two of these salts

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
毕福强等: "1 , 4-二硝基呋咱并[ 3 , 4-b]哌嗪(DNFP)的合成", 《含能材料》 *

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