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CN109020789B - Method for preparing 2-methoxypropene - Google Patents

Method for preparing 2-methoxypropene Download PDF

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Publication number
CN109020789B
CN109020789B CN201710438118.6A CN201710438118A CN109020789B CN 109020789 B CN109020789 B CN 109020789B CN 201710438118 A CN201710438118 A CN 201710438118A CN 109020789 B CN109020789 B CN 109020789B
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methoxypropene
reaction
dimethoxypropane
temperature
cocatalyst
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CN109020789A (en
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翟德伟
霍鸿飞
刘冬
周益辉
邵斌
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Zhejiang Fangyuanxin Biopharmaceutical Co ltd
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Zhejiang Medicine Co Ltd Xinchang Pharmaceutical Factory
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C41/00Preparation of ethers; Preparation of compounds having groups, groups or groups
    • C07C41/01Preparation of ethers
    • C07C41/18Preparation of ethers by reactions not forming ether-oxygen bonds
    • C07C41/28Preparation of ethers by reactions not forming ether-oxygen bonds from acetals, e.g. by dealcoholysis

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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)

Abstract

The invention relates to a method for preparing 2-methoxypropene. In the existing synthesis systems, a solvent is used in some systems; some systems do not use solvents, but the use amount of acid is particularly large, so that the industrial production is difficult. The invention adopts p-toluenesulfonic acid as a catalyst, pyridine, quinoline or hydroquinone and the like as a cocatalyst, and 2, 2-dimethoxypropane is catalytically cracked to prepare 2-methoxypropene; the reaction time is 5-15h, the reaction temperature is 60-150 ℃, the reaction pressure is normal pressure, the product yield can reach 93.0%, and the purity of the product obtained by rectification is 99.5%. The method of the invention does not use solvent or introduce anhydride, has mild reaction conditions and can realize continuous industrial production.

Description

Method for preparing 2-methoxypropene
Technical Field
The invention relates to a method for preparing 2-methoxy propylene, in particular to a method for preparing 2-methoxy propylene by catalytically cracking 2, 2-dimethoxypropane at normal pressure and high temperature by adopting a catalyst and a cocatalyst.
Background
2-methoxy propylene is an important organic compound, is a key raw material in the synthesis of a plurality of medicaments, and is widely applied to the industrial fields of materials, medicines, dyes, feeds and the like. Currently, the main routes for the synthesis of 2-methoxypropene are: 1. carrying out addition reaction on methanol and unsaturated hydrocarbon to generate 2-methoxypropene; 2. 2, 2-dimethoxypropane is synthesized by an indirect or direct method, and then the 2, 2-dimethoxypropane is catalytically cracked by a gas phase or liquid phase method to prepare the 2-methoxypropene. Route 1 has simple steps, high reaction yield and good selectivity, but the route has the following disadvantages: (1) the related reaction catalyst has strong corrosion to equipment at high temperature; (2) unsaturated hydrocarbons have high chemical activity, violent reaction, difficult control and poor operation safety; (3) the unsaturated hydrocarbon propyne or allene is difficult to be sourced, and only large petrochemical enterprises of the raw material consider the synthetic route. Route 2 methanol and acetone which are used as raw materials for synthesizing 2, 2-dimethoxypropane by a direct method are cheap and easy to obtain, and the industrial production of 2-methoxypropene is easy to realize. However, the conversion rate of the condensation reaction is low, and methanol and acetone, 2-dimethoxypropane generate azeotrope, so that the preparation of 2, 2-dimethoxypropane becomes one of the difficulties of the route. The gas phase cracking method in the route 2 is to obtain 2-methoxypropene by vaporizing 2, 2-dimethoxypropane, passing through a heated catalyst bed, and carrying out catalytic cracking at high temperature. The gas phase cracking process consumes a large amount of energy because the raw material is vaporized first and then cracked at a high temperature. The liquid phase cracking method can catalytically crack the 2, 2-dimethoxypropane under mild conditions.
Much work has been done by scholars both at home and abroad on the study of the preparation of 2-methoxypropene by liquid phase cracking of 2, 2-dimethoxypropane.
In the research of fine chemical intermediates, the xi' an modern chemical research institute, popsensitivity et al, published in 2002, benzoic acid and pyridine are used as catalysts, diglyme is used as a solvent, and a certain amount of succinic anhydride is added to absorb methanol generated by cracking so as to promote the reaction to proceed towards 2-methoxypropene. The rectification yield is 80.06%, and the product purity is more than 98%. This system adds significant cost due to the use of solvents and the introduction of succinic anhydride.
In 2009, Li Xiao et al, Wuhan theory university, used benzoic acid and pyridine as catalysts, toluene as a solvent, and succinic anhydride to absorb methanol. The product yield can reach 81.1 percent, and the purity is more than 97 percent. In this system, although the cost is reduced by using toluene as a solvent instead of diglyme. However, the use of a solvent and the introduction of succinic anhydride make the reaction system complicated and cause inconvenience in the post-reaction treatment.
Manfred Kaufhold in US 5,576,465 adopts pelargonic acid to catalyze and crack 2, 2-dimethoxypropane at 130 ℃ to prepare 2-methoxypropene, the conversion rate can reach 78%, and the cracking solution is washed by water and then rectified to obtain 2-methoxypropene with the purity of 99.3%. Although no solvent is used in the system, the use amount of the nonanoic acid is particularly large, and the industrial production is not easy.
Disclosure of Invention
The invention aims to provide a method for preparing 2-methoxypropene by high-efficiency liquid phase cracking of 2, 2-dimethoxypropane without using a solvent or introducing anhydride, and provides a more reasonable industrial production method for 2-methoxypropene.
Therefore, the technical scheme adopted by the invention is as follows: a process for preparing 2-methoxypropene comprising the steps of:
step a), mixing 2, 2-dimethoxypropane, a catalyst and a cocatalyst;
step b), carrying out cracking reaction at the temperature of 60-150 ℃ for 5-15 hours to obtain a 2-methoxypropene product;
wherein the molar ratio of 2, 2-dimethoxypropane, catalyst and cocatalyst = 1: 0.01% -5.0%: 0.05% -8.0%;
the catalyst is selected from one or more of toluene sulfonic acid compounds, and the cocatalyst is selected from one or more of pyridine compounds, quinoline compounds or benzenediol.
Preferably, the 2-methoxypropene product of step b) is further subjected to water washing and rectification steps.
Preferably, the heating of step b) is carried out at atmospheric pressure.
Preferably, the reaction temperature in step b) is from 80 to 120 ℃.
Preferably, the molar ratio of the 2, 2-dimethoxypropane, the catalyst and the cocatalyst = 1: 0.01% -2.0%: 1.0 to 8.0 percent.
Preferably, the catalyst is p-toluenesulfonic acid.
Preferably, the cocatalyst is pyridine.
Preferably, the cocatalyst is quinoline.
Preferably, the cocatalyst is hydroquinone.
Under the premise of not introducing a solvent and anhydride, the method adopts a small amount of p-toluenesulfonic acid and a cocatalyst to efficiently crack 2, 2-dimethoxypropane at the temperature of 60-150 ℃, and after the reaction is carried out for 5-15 hours, the cracking solution is washed by water and rectified to obtain the high-purity 2-methoxypropene. The invention provides a new idea and a new mode for synthesizing 2-methoxypropene through a pipeline continuous reaction.
Detailed Description
In order to better illustrate the patent of the invention, the following examples are given for the purpose of illustration, but the invention is not limited in any way by these examples, the content and purity of the product being determined by gas chromatography.
Example 1
200g of 2, 2-dimethoxypropane, 0.3g of p-toluenesulfonic acid and 0.5g of pyridine are added into a 250ml three-necked bottle, stirring is started, heating and raising the temperature are carried out, the reaction temperature is controlled at 100 ℃, the temperature is kept for reaction for 8 hours, and then cooling and temperature reduction treatment are carried out. The cracked product is washed by water and then rectified to obtain the 2-methoxy propylene with the purity of 99.3 percent, and the product yield is 90.3 percent.
Example 2
200g of 2, 2-dimethoxypropane, 0.5g of p-toluenesulfonic acid and 0.8g of pyridine are added into a 250ml three-necked bottle, stirring is started, heating and raising the temperature are carried out, the reaction temperature is controlled to be 90 ℃, the temperature is kept for reaction for 6.8h, and then cooling and cooling treatment are carried out. The cracked product is washed by water and then rectified to obtain 2-methoxy propylene with the purity of 99.1 percent, and the product yield is 91.8 percent.
Example 3
200g of 2, 2-dimethoxypropane, 0.3g of p-toluenesulfonic acid and 0.5g of quinoline are added into a 250ml three-necked bottle, stirring is started, heating and raising the temperature are carried out, the reaction temperature is controlled at 100 ℃, the temperature is kept for reaction for 10h, and then cooling and temperature reduction treatment are carried out. The cracking product is washed by water and then rectified to obtain the 2-methoxypropene with the purity of 99.2 percent, and the product yield is 92.5 percent.
Example 4
200g of 2, 2-dimethoxypropane, 0.5g of p-toluenesulfonic acid and 0.8g of quinoline are added into a 250ml three-necked bottle, stirring is started, heating and raising the temperature are carried out, the reaction temperature is controlled to be 90 ℃, the temperature is kept for reaction for 9 hours, and then cooling and temperature reduction treatment are carried out. The cracking product is washed by water and then rectified to obtain the 2-methoxypropene with the purity of 99.1 percent, and the product yield is 92.8 percent.
Example 5
200g of 2, 2-dimethoxypropane, 0.3g of p-toluenesulfonic acid and 0.5g of hydroquinone are added into a 250ml three-necked bottle, stirring is started, heating and reaction are carried out, the temperature is controlled at 100 ℃, the reaction is carried out for 13h under heat preservation, and then cooling is carried out. The cracked product is washed by water and then rectified to obtain 2-methoxypropene with the purity of 99.4 percent, and the product yield is 89.7 percent.
Example 6
200g of 2, 2-dimethoxypropane, 0.5g of p-toluenesulfonic acid and 0.8g of hydroquinone are added into a 250ml three-necked bottle, stirred, heated and reacted, the temperature is controlled to be 90 ℃, the reaction is kept for 12 hours, and then cooled. The cracking product is washed by water and then rectified to obtain the 2-methoxypropene with the purity of 99.2 percent, and the product yield is 90.5 percent.
Comparative example 1
200g of 2, 2-dimethoxypropane and 0.5g of p-toluenesulfonic acid are added into a 250ml three-necked bottle, stirring is started, heating and reaction are carried out, the temperature is controlled at 100 ℃, the reaction is carried out for 18h, and then cooling is carried out. The cracking product is washed by water and then rectified to obtain the 2-methoxypropene with the purity of 98.4 percent, and the product yield is 70.5 percent.
Comparative example 2
200g of 2, 2-dimethoxypropane and 0.5g of phosphoric acid are added into a 250ml three-necked bottle, stirring is started, heating and temperature rising reaction are carried out, the temperature is controlled to be 110 ℃, heat preservation reaction is carried out for 20 hours, and then cooling is carried out. The cracked product is washed by water and then rectified to obtain the 2-methoxy propylene with the purity of 96.7 percent, and the product yield is 50.3 percent.
Comparative example 3
200g of 2, 2-dimethoxypropane, 0.5g of phosphoric acid and 0.5g of quinoline are added into a 250ml three-necked bottle, stirring is started, heating and reaction are carried out, the temperature is controlled to be 110 ℃, the reaction is carried out for 17 hours under heat preservation, and then cooling is carried out. The cracking product is washed by water and then rectified to obtain the 2-methoxypropene with the purity of 97.2 percent, and the product yield is 56.6 percent.

Claims (4)

1. A process for preparing 2-methoxypropene comprising the steps of:
step a), mixing 2, 2-dimethoxypropane, a catalyst and a cocatalyst;
step b), carrying out cracking reaction at the temperature of 90-100 ℃ for 5-15 hours to obtain a 2-methoxypropene product;
wherein the molar ratio of 2, 2-dimethoxypropane, catalyst and cocatalyst = 1: 0.01% -5.0%: 0.05% -8.0%;
the catalyst is p-toluenesulfonic acid, and the cocatalyst is pyridine, quinoline or hydroquinone.
2. The process of claim 1, wherein the 2-methoxypropene product of step b) is further subjected to water washing and rectification steps.
3. The method of claim 1, wherein the heating of step b) is performed at atmospheric pressure.
4. The process of claim 1, wherein the molar ratio of 2, 2-dimethoxypropane, catalyst and cocatalyst = 1: 0.01% -2.0%: 1.0 to 8.0 percent.
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CN110724038A (en) * 2019-11-06 2020-01-24 安徽华甬新材料股份有限公司 Preparation method of methyl isopropenyl ether
CN111187149B (en) * 2020-02-18 2022-11-08 万华化学集团股份有限公司 Method for preparing 2-alkoxy propylene
CN114149310B (en) * 2021-11-23 2024-08-16 万华化学(四川)有限公司 Preparation method of unsaturated ketone
CN116444352B (en) * 2022-01-06 2024-06-25 万华化学集团股份有限公司 Novel method for liquid phase synthesis of 2-methoxypropene
CN115490575A (en) * 2022-10-13 2022-12-20 辽宁惠风生物医药科技有限公司 A kind of preparation method of 2-ethoxypropene
CN117623878A (en) * 2023-10-25 2024-03-01 宁夏天新药业有限公司 Synthesis method of 2-methoxypropene

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