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CN107973703B - Synthetic method of aryl olefin - Google Patents

Synthetic method of aryl olefin Download PDF

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CN107973703B
CN107973703B CN201711252869.5A CN201711252869A CN107973703B CN 107973703 B CN107973703 B CN 107973703B CN 201711252869 A CN201711252869 A CN 201711252869A CN 107973703 B CN107973703 B CN 107973703B
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reaction
aryl
acetal
molecular sieve
anethole
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CN107973703A (en
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黄战鏖
侯峰
钱正刚
裴继红
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Shanghai Wanxiang Flavors And Fragrances Co ltd
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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
    • C07C41/30Preparation of ethers by reactions not forming ether-oxygen bonds by increasing the number of carbon atoms, e.g. by oligomerisation
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C45/00Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Abstract

The invention discloses a synthesis method of aryl-containing substituted olefin, which is characterized in that aliphatic acetal is used as an alkylating agent to react with an aromatic compound, and the aryl-containing substituted olefin such as anise camphor and the like is directly obtained through a one-pot reaction at the normal pressure or the low pressure of 0.1-1.0MPa and the reaction temperature of 90-160 ℃ under the catalysis of a solid acid catalyst. The invention has the following characteristics: 1) is a new synthetic route, and the reaction is finished in one pot. 2) The aromatic compound serves as both a reactant and a solvent, and no other organic solvent is used. 3) The catalyst is solid acid such as H-Beta molecular sieve and metal ion modified molecular sieve thereof, and is catalytic amount. 4) The produced alcohol can be recycled for use in the synthesis of acetal after recovery. 5) The reaction may be carried out batchwise or in a tubular reactor or a fixed bed reactor. 6) The post-treatment is simple, no waste is generated in the reaction process, and the method is a green and environment-friendly synthetic route.

Description

Synthetic method of aryl olefin
Technical Field
The invention belongs to the field of organic synthesis, and particularly relates to a synthesis method of aryl olefin, in particular to synthesis of anethole.
Background
The anethole (also called anethole or anethole) with the chemical name of 1-methoxy-4- (1-propenyl) benzene naturally exists in essential oil such as anise oil and fennel oil, and trans-isomer accounts for most of the essential oil. Has characteristic sweet fennel fragrance, and is mainly used for blending edible essence and toothpaste essence.
The traditional preparation method of the anise camphor is to obtain a crude product of the anise camphor from natural essential oil rich in the anise camphor through freezing crystallization and centrifugation, and then extract the crude product by a rectification method. For example, it is extracted from oleum Anisi Stellati and oleum Foeniculi (CN 102491884 and essence and perfume cosmetic, 2013, stage 02).
Due to the limited sources and amounts of natural essential oils, naturally produced anise camphor cannot meet the increasing demand. Therefore, the synthesized finished product has great market demand and commercial value. Its synthesis has been receiving wide attention.
CN103058835 describes a synthesis method of anethole, which comprises obtaining p-methoxypropiophenone by friedel-Crafts reaction of propionyl chloride and anisole, then obtaining corresponding alcohol by reduction with sodium borohydride, and then obtaining anethole by dehydration under acidic conditions of p-toluenesulfonic acid and the like. Because excessive aluminum trichloride is needed to be used for catalyzing the propionylation of anisole, the obtained p-methoxypropiophenone is reduced by using sodium borohydride, and the final dehydration reaction generates a large amount of waste to be discharged, so that the environmental protection problem is not small.
DE19742418974 discloses a two-step synthesis of anethole using anisole and propionaldehyde as starting materials. Firstly, anisole and propionaldehyde generate a mixture of bis (methoxyphenyl) propane under the action of an acid catalyst, and secondly, the condensation product generates elimination reaction at 200-300 ℃ and a certain vacuum degree in the presence of a catalytic amount of acid catalysts such as phosphoric acid and the like, and a crude product is distilled out. The conversion rate of the condensation compound is 67.3 percent, the selectivity of the anethole is about 41 percent, and the crude product contains part of unreacted condensation compound, trans-anethole, cis-anethole, ortho-trans-anethole and the like; it is stated that cleavage of the condensation mixture obtained by the renewed reaction of ortho-anethole with anisole gives about 8% of anethole. The disadvantages are that the reaction needs to take place at higher temperatures, the cracking of the condensation intermediates is incomplete; also obtain a considerable amount of o-anethole and other by-products; due to the long heating time of the cleavage process and the complexity of the process of recycling the ortho-anethole, considerable amounts of by-products, undesired isomers and other polymers are produced.
CN103755533 describes a method for synthesizing anethole from artemisia scoparia naphtha, which comprises isomerizing artemisia scoparia naphtha at 140-215 deg.C for 0.5-3h under the action of alkaline catalyst, isomerizing the estragole into anethole, and then obtaining the anethole by freezing crystallization, filtration and rectification.
CN106103398 discloses a process for the preparation of arylpropenes, especially 1-methoxy-4- (1-propenyl) benzene (anethole) involving thermal decomposition of the corresponding 1, 1-diarylpropane. Removing one aromatic hydrocarbon molecule by performing gas-phase thermal decomposition on 1, 1-diaryl propane under reduced pressure and at the temperature of 300-400 ℃ under the action of a boron-containing molecular sieve catalyst to obtain the anethole.
The materials used in the relevant processes are expensive or not easily available, or the three wastes in the process are seriously discharged, or the reaction conditions are harsh, and the like, so the exploration of the synthetic route of the anethole still arouses people's interest.
Disclosure of Invention
The invention aims to: provides a synthetic method of aryl-containing substituted olefin, in particular to a novel synthetic method of anethole.
The technical solution of the invention is as follows:
a synthetic method of aryl-containing substituted olefin is characterized in that aliphatic acetal is used as an alkylating agent to react with an aromatic compound, and the aryl-containing substituted olefin such as anise camphor and the like is directly obtained through one-pot reaction at the reaction temperature of 90-160 ℃ under the catalysis of a solid acid catalyst and under the normal pressure or the low pressure of 0.1-1.0MPa, wherein the specific reaction formula is as follows:
Figure BDA0001492113470000021
in a preferred embodiment of the invention, the aliphatic acetal is a C1-C12 aliphatic acetal.
In a preferred embodiment of the invention, the solid acid catalyst is molecular sieve H-Beta.
In a preferred embodiment of the invention, the reaction temperature is in the range of 110 to 140 ℃.
Due to the adoption of the technical scheme, the invention has the following characteristics:
1) is a new synthetic route, and the reaction is finished in one pot.
2) The aromatic compound serves as both a reactant and a solvent, and no other organic solvent is used.
3) The catalyst is solid acid such as H-Beta molecular sieve and metal ion modified molecular sieve thereof, and is catalytic amount.
4) The produced alcohol can be recycled for use in the synthesis of acetal after recovery.
5) The reaction may be carried out batchwise or in a tubular reactor or a fixed bed reactor.
6) The post-treatment is simple, no waste is generated in the reaction process, and the method is a green and environment-friendly synthetic route.
Detailed Description
The technical solution of the invention is further illustrated below with reference to specific examples, which are not to be construed as limiting the technical solution.
Example 1:
100ml autoclave, oil bath, electromagnetic stirring. Adding 18g of anisole into a kettle, and adding 3.9g of propionaldehyde dimethanol acetal; then 0.78g H-Beta molecular sieve powder is added. Carrying out oil bath at 120 ℃, and stirring for reaction for 3 hours; cooling to room temperature, filtering the material out of the catalyst, and detecting by gas chromatography. Acetal conversion 74%; the selectivity of the anise camphor is 52.4 percent, and the 2-methyl-2-pentenal content is 25.3 percent.
Example 2:
100ml autoclave, oil bath, electromagnetic stirring. Adding 30g of anisole into a kettle, and adding 4.5g of propionaldehyde dimethanol acetal; then 1.1g of Ce-Beta molecular sieve powder is added. Stirring and reacting for 4 hours at 130 ℃ in an oil bath; cooling to room temperature, filtering the reaction mass out of the catalyst, and detecting by gas chromatography. Acetal conversion 63.5%; the selectivity of the anise camphor is 61.2 percent, and the 2-methyl-2-pentenal is 15.1 percent.
Example 3:
100ml autoclave, oil bath, electromagnetic stirring. Adding 50g of anisole into a kettle, and adding 7.5g of propionaldehyde dimethanol acetal; then 3g of Ni-Y molecular sieve powder is added. Stirring and reacting for 5 hours at 135 ℃ in an oil bath; cooling to room temperature, filtering the reaction mass out of the catalyst, and detecting by gas chromatography. Acetal conversion 33.5%; the selectivity of the anise camphor is 24.6 percent, and the 2-methyl-2-pentenal content is 35.1 percent.
Example 4:
250ml three-mouth bottle, oil bath, electromagnetic stirring, installation of thermometer, condenser tube. 74g of anisole is added into a bottle, and 9.5g of propionaldehyde di-n-propanol acetal is added; then adding 2.8g H-Beta molecular sieve powder. Stirring and reacting for 4.5 hours at 132 ℃; cooling to room temperature, filtering the material out of the catalyst, and detecting by gas chromatography. Acetal conversion 39.3%; the selectivity of the anise camphor is 36.6 percent, and the 2-methyl-2-pentenal content is 27.4 percent.

Claims (1)

1. A synthetic method of aryl-containing substituted olefin is characterized in that aliphatic acetal is used as an alkylating agent to react with an aromatic compound, and aryl-containing substituted olefin is directly obtained through one-pot reaction under the catalysis of a solid acid catalyst and under the pressure of 0.1-1.0MPa and at the reaction temperature of 110-140 ℃, and the specific reaction formula is as follows:
Figure FDA0002777046140000011
wherein, R is1Methoxy, ethoxy, C1-C4 alkyl; r2A ═ C1-C10 alkyl group; r ═ n-propyl;
the solid acid catalyst is molecular sieve H-Beta.
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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4026951A (en) * 1974-04-19 1977-05-31 Haarmann & Reimer Gmbh Process for the production of anethole
JP2014172834A (en) * 2013-03-07 2014-09-22 National Institute Of Advanced Industrial & Technology Method for producing aromatic olefins
CN106103398A (en) * 2014-01-17 2016-11-09 巴斯夫欧洲公司 Process for the production of arylpropylene

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4026951A (en) * 1974-04-19 1977-05-31 Haarmann & Reimer Gmbh Process for the production of anethole
JP2014172834A (en) * 2013-03-07 2014-09-22 National Institute Of Advanced Industrial & Technology Method for producing aromatic olefins
CN106103398A (en) * 2014-01-17 2016-11-09 巴斯夫欧洲公司 Process for the production of arylpropylene

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
缩醛与吲哚或苯并呋喃的烷基化反应;刘宁宁等;《有机化学》;20141231(第34期);2523-2528 *

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