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CN102040703A - Method for synthesizing cyclic carbonic resin - Google Patents

Method for synthesizing cyclic carbonic resin Download PDF

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Publication number
CN102040703A
CN102040703A CN2009101905607A CN200910190560A CN102040703A CN 102040703 A CN102040703 A CN 102040703A CN 2009101905607 A CN2009101905607 A CN 2009101905607A CN 200910190560 A CN200910190560 A CN 200910190560A CN 102040703 A CN102040703 A CN 102040703A
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methyl
butyl
tert
monomer
synthetic method
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CN2009101905607A
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Chinese (zh)
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任旭
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Individual
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Abstract

The invention discloses a method for synthesizing cyclic carbonic resin, which has the synthesis process of performing solution polymerization for (Meth) acrylic acid glycidyl carbonate and monomers in the presence of an initiator. The obtained cyclic carbonic resin has low cost and is a main material for synthesizing a new generation of environment friendly polyurethane.

Description

A kind of synthetic method of cyclic carbonate ester resin
[technical field]
The present invention relates to a kind of preparation method of cyclic carbonate ester resin.
[background technology]
Environmental issue is subjected to increasing attention all over the world, no matter be product or production process, and nontoxic, free of contamination technology is even more important.Urethane (PU) is meant and contains a plurality of ammonia ester bonds (general name of polymkeric substance NH-COO-) in the molecular chain.Ammonia ester bond is generally obtained by polyisocyanate-based and hydroxyl reaction.Urethane has been used to rapidly make porous plastics, fiber, elastomerics, synthetic leather, coating, sizing agent, pavement material and medical material etc. since being invented by Germanization scholar 0.Bayer the thirties in 20th century, is widely used in fields such as traffic, building, light industry, weaving, electromechanics, aviation, health care.Along with constantly widening of polyurethane chemistry research, product manufacturing and application art development of technology and Application Areas, formed gradually and occupied the 6th big synthetic materials status (PE, PP, PVC, PS, PET, industrial system PU) at present in the world.Over nearly more than 20 years, polyurethane products kind, Application Areas, industry size enlarge rapidly, have become one of high molecular synthetic material industry with fastest developing speed.The China's Mainland becomes urethane market centre with fastest developing speed in the world in recent years.According to the expert's of Britain IAL consulting firm data, China's nineteen eighty-two only 7000 tons of urethane output, and reached 2,900,000 tons by 2005, average growth rate per annum is 25%, estimates will reach 4,300,000 tons in 2010, average growth rate per annum is 8.1%.
But polyisocyanates is to environment and the deleterious high toxic material of HUMAN HEALTH, in polyurethane products, inevitably have residual, and the preparation polyisocyanates raw material phosgene toxicity bigger.For overcoming these shortcomings, developed country pays much attention to the study on the synthesis of non-isocyanate polyurethane since the nineties in 20th century, and obtained many achievements in research, and maintained the leading position, at present, existing non-isocyanate polyurethane product-feed market.The exploitation of China's non-isocyanate polyurethane also is in the starting stage, and the research report is less, does not more see industrialized report.
Non-isocyanate polyurethane is meant and does not use isocyanic ester to be raw material synthetic urethane, be called for short NIPU, mainly be to react by cyclic carbonate ester resin and aliphatics or alicyclic primary amine to prepare at present, NIPU has structure different with conventional urethane and performance, contain hydroxyl on the β position carbon atom of its structural unit carbamate, can form intramolecular hydrogen bond with the carbonyl in the amino-formate bond, therefore, NIPU has remedied the weak bond structure the conventional urethane from molecular structure, chemical resistant properties, hydrolytic resistance and permeability resistance are all than more excellent, and do not use high toxicity and moisture-sensitive material polyisocyanates in its preparation process, can not make material form textural defect, bring convenience for the construction and the storage of raw material because of producing bubble.
NIPU almost is safe from harm to environment, causes people's attention in recent years.Along with people to NIPU research deeply and the updating and improve of performance, NIPU will be used in more field, becomes a new highlight of urethane industry.
[summary of the invention]
A technical problem to be solved by this invention provides a kind of preparation method of cyclic carbonate ester resin, can be under relatively mild condition, and efficient, environmental protection, economy, technology realize simply.
Synthetic method of the present invention is as follows:
(1), solvent is added in the reactor, be warming up to 50-200 ℃;
(2), under temperature of reaction, drip initiator, monomer and (methyl) vinylformic acid Racemic glycidol carbonic ether;
(3), transferring pH value with the PH conditioning agent after reaction finishes is 7-9.
The time of dropwise reaction thing is 0.5-6 hour in the step (2) as mentioned above.
Solvent in the step (1) is acetone, methylethylketone, pimelinketone, methyl butyl ketone, methyl iso-butyl ketone (MIBK), methyl isoamyl ketone, isophorone, normal hexane, normal heptane, toluene, dimethylbenzene, methylene dichloride, trichloromethane, ethylene dichloride, vinyl acetic monomer, N-BUTYL ACETATE, octyl acetate, C as mentioned above nH 2n+1OH (n=1-10), tetrahydrofuran (THF), dimethyl formamide, dimethyl sulfoxide (DMSO), gylcol ether, propylene glycol ethers etc.
Aforesaid initiator is benzoyl peroxide, peroxidation-2 ethyl hexanoic acid tert-pentyl ester, peroxide-2-ethyl hexanoic acid tert-butyl, peroxidation tert-butyl acetate, peroxidized t-butyl perbenzoate, 1,1-di-tert-butyl peroxide-3,3,5,-trimethyl-cyclohexane, Diisopropyl azodicarboxylate, tert-butyl hydroperoxide octanoate, di-t-butyl peroxide, peroxidation two tert-pentyls, dicumyl peroxide, 2,2-two (tert-butyl hydroperoxide) butane.
Aforesaid monomer is (methyl) vinylformic acid, (methyl) methyl acrylate, (methyl) ethyl propenoate, (methyl) butyl acrylate, (methyl) Isooctyl acrylate monomer, (methyl) Hydroxyethyl acrylate, (methyl) Propylene glycol monoacrylate, vinylbenzene, vinyl acetate, (methyl) acrylamide, the combination of one or more in methylene-succinic acid, toxilic acid, Vinylstyrene, ethylene glycol diacrylate, the diallyl maleate.
The aforesaid reaction times is 0.5-10 hour.
Aforesaid (methyl) vinylformic acid Racemic glycidol carbonic ether and monomeric weight ratio are 5-95%.
Aforesaid initiator is the 0.01-10% of monomer weight.
The weight ratio of aforesaid monomer and solvent is 15-80%.
Aforesaid PH conditioning agent is ammoniacal liquor, sodium hydroxide, potassium hydroxide, yellow soda ash, sodium bicarbonate, triethylamine, trolamine or dimethylethanolamine.
The invention has the beneficial effects as follows:
1, reaction conditions gentleness, technological process are simple, are convenient to operation;
2, raw material is cheap and easy to get, and cost is low.
[embodiment]
Embodiment 1:
In the reactor that whipping appts, thermometer, prolong, feeding device are housed, add butanone, be heated to 80 ℃, be incubated 20 minutes, drip initiator, monomer, (methyl) vinylformic acid Racemic glycidol carbonic ether, dropwised insulation reaction 6 hours, naturally cooling then in 2 hours, treating to add when temperature is reduced to 45 ℃ ammoniacal liquor adjusting pH value is 7-9, last cooling discharge.
In above-mentioned synthesizing, described initiator is 6 parts of Diisopropyl azodicarboxylates, and described monomer is 55 parts of vinylbenzene, 50 parts of butyl acrylates, 4 parts of vinylformic acid, 50 parts of methyl propenoic acid glycidyl carbonic ethers.
Make the cyclic carbonate ester resin with aforesaid method and contain 55% admittedly, monomer conversion is more than 98%, and PH is 8.5.
Embodiment 2:
In the reactor that whipping appts, thermometer, prolong, feeding device are housed, add dimethylbenzene, be heated to 140 ℃, be incubated 20 minutes, drip the mixed solution of initiator, monomer, (methyl) vinylformic acid Racemic glycidol carbonic ether, dropwised insulation reaction 7 hours, naturally cooling then in 3 hours, treating to add when temperature is reduced to 45 ℃ ammoniacal liquor adjusting pH value is 7-9, last cooling discharge.
In above-mentioned synthesizing, described initiator is 15 parts of tert-butyl hydroperoxide octanoates, and described monomer is 260 parts of vinylbenzene, 90 parts of butyl acrylates, 4 parts of vinylformic acid, 80 parts of methyl propenoic acid glycidyl carbonic ethers.
Make the cyclic carbonate ester resin with aforesaid method and contain 50% admittedly, monomer conversion is more than 98%, and PH is 8.5.
Embodiment 3:
In the reactor that whipping appts, thermometer, prolong, feeding device are housed, add methyl isoamyl ketone, be heated to 145 ℃, be incubated 20 minutes, drip the mixed solution of initiator, monomer, (methyl) vinylformic acid Racemic glycidol carbonic ether, dropwised insulation reaction 8 hours, naturally cooling then in 4 hours, treating to add when temperature is reduced to 45 ℃ sodium hydroxide adjusting pH value is 7-9, last cooling discharge.
In above-mentioned synthesizing, described initiator is 15 parts of peroxidized t-butyl perbenzoates, and described monomer is 200 parts of vinylbenzene, 270 parts of butyl acrylates, 3 parts of vinylformic acid, 100 parts of methyl propenoic acid glycidyl carbonic ethers.
Make the cyclic carbonate ester resin with aforesaid method and contain 45% admittedly, monomer conversion is more than 98%, and PH is 8.0.
Embodiment 4:
In the reactor that whipping appts, thermometer, prolong, feeding device are housed, add dimethylbenzene, be heated to 141 ℃, be incubated 20 minutes, drip the mixed solution of initiator, monomer, (methyl) vinylformic acid Racemic glycidol carbonic ether, dropwised insulation reaction 10 hours, naturally cooling then in 2 hours, treating to add when temperature is reduced to 45 ℃ sodium hydroxide adjusting pH value is 7-9, last cooling discharge.
Above-mentioned synthetic in, described initiator is 11 parts of peroxidation two tert-pentyls, described monomer is 40 parts of vinylbenzene, 30 parts of butyl acrylates, 1.5 parts of vinylformic acid, 27 Rocryl 410s, 18 parts of methyl propenoic acid glycidyl carbonic ethers.
Make the cyclic carbonate ester resin with aforesaid method and contain 60% admittedly, monomer conversion is more than 98%, and PH is 8.6.
Above content be in conjunction with concrete preferred implementation to further describing that the present invention did, can not assert that concrete enforcement of the present invention is confined to these explanations.For the general technical staff of the technical field of the invention, without departing from the inventive concept of the premise, can also make some simple deduction or replace, all should be considered as belonging to protection scope of the present invention.

Claims (10)

1. the synthetic method of a cyclic carbonate ester resin.It is characterized in that:
A: in reactor, add solvent, be warming up to 50-200 ℃;
B: in 0.5-6 hour, drip initiator, (methyl) vinylformic acid Racemic glycidol carbonic ether and monomer, insulation reaction 0.5-10 hour continuously;
C: transfer pH value to 7-10 with the PH conditioning agent.
2. synthetic method according to claim 1 is characterized in that: used solvent is: acetone, methylethylketone, pimelinketone, methyl butyl ketone, methyl iso-butyl ketone (MIBK), methyl isoamyl ketone, isophorone, normal hexane, normal heptane, toluene, dimethylbenzene, methylene dichloride, trichloromethane, ethylene dichloride, vinyl acetic monomer, N-BUTYL ACETATE, octyl acetate, C nH 2n+1OH (n=1-10), tetrahydrofuran (THF), dimethyl formamide, dimethyl sulfoxide (DMSO), gylcol ether, propylene glycol ethers etc.
3. synthetic method according to claim 1 is characterized in that: the temperature of reaction of synthesizing cyclic carbonate ester resin is 50-200 ℃, and the reaction times is 0.5-10 hour.
4. synthetic method according to claim 1 is characterized in that: dripping initiator, (methyl) vinylformic acid Racemic glycidol carbonic ether and monomeric time is 0.5-6 hour.
5. synthetic method according to claim 1, it is characterized in that: described monomer is that content is 5-95% (methyl) vinylformic acid, (methyl) methyl acrylate, (methyl) ethyl propenoate, (methyl) butyl acrylate, (methyl) Isooctyl acrylate monomer, (methyl) Hydroxyethyl acrylate, (methyl) Propylene glycol monoacrylate, vinylbenzene, vinyl acetate, (methyl) acrylamide, the combination of one or more in methylene-succinic acid, toxilic acid, Vinylstyrene, ethylene glycol diacrylate, the diallyl maleate.
6. synthetic method according to claim 1, it is characterized in that: described initiator is benzoyl peroxide, peroxidation-2 ethyl hexanoic acid tert-pentyl ester, peroxide-2-ethyl hexanoic acid tert-butyl, peroxidation tert-butyl acetate, peroxidized t-butyl perbenzoate, 1,1-di-tert-butyl peroxide-3,3,5,-trimethyl-cyclohexane, Diisopropyl azodicarboxylate, tert-butyl hydroperoxide octanoate, di-t-butyl peroxide, peroxidation two tert-pentyls, dicumyl peroxide, 2,2-two (tert-butyl hydroperoxide) butane.
7. according to claim 1 and 5 described synthetic methods, it is characterized in that: described (methyl) vinylformic acid Racemic glycidol carbonic ether and monomeric weight ratio are 5-95%.
8. according to claim 1,5,6 and 7 described synthetic methods, it is characterized in that: used initiator is the 0.01-10% of monomer weight.
9. according to claim 1,5,6 and 7 described synthetic methods, it is characterized in that: the used monomer and the weight ratio of solvent are 15-80%.
10. synthetic method according to claim 1 is characterized in that: used PH conditioning agent is ammoniacal liquor, sodium hydroxide, potassium hydroxide, yellow soda ash, sodium bicarbonate, triethylamine, trolamine or dimethylethanolamine.
CN2009101905607A 2009-10-13 2009-10-13 Method for synthesizing cyclic carbonic resin Pending CN102040703A (en)

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104231191A (en) * 2014-09-16 2014-12-24 上海金力泰化工股份有限公司 Preparation method of waterborne non-isocyanate polyurethane modified polyester
CN104995270A (en) * 2012-12-19 2015-10-21 阿科玛法国公司 Organic resin bearing cyclic carbonate groups and aqueous dispersion for crosslinked polyurethanes
CN105542044A (en) * 2016-01-22 2016-05-04 浙江大学 Method for preparing transparent polyacrylate for selectively absorbing ultraviolet light
CN111448265A (en) * 2017-12-11 2020-07-24 宣伟公司 Process for making water-dispersible polymers and water-dispersed polymers

Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104995270A (en) * 2012-12-19 2015-10-21 阿科玛法国公司 Organic resin bearing cyclic carbonate groups and aqueous dispersion for crosslinked polyurethanes
CN104995270B (en) * 2012-12-19 2017-12-08 阿科玛法国公司 The organic resin and aqueous dispersion with cyclic carbonate groups for the polyurethane of crosslinking
CN104231191A (en) * 2014-09-16 2014-12-24 上海金力泰化工股份有限公司 Preparation method of waterborne non-isocyanate polyurethane modified polyester
CN104231191B (en) * 2014-09-16 2018-04-24 上海金力泰化工股份有限公司 The preparation method for the polyester that water-based non-isocyanate polyurethane is modified
CN105542044A (en) * 2016-01-22 2016-05-04 浙江大学 Method for preparing transparent polyacrylate for selectively absorbing ultraviolet light
CN105542044B (en) * 2016-01-22 2017-09-12 浙江大学 A kind of preparation method of polyacrylate that is transparent and absorbing ultraviolet light
CN111448265A (en) * 2017-12-11 2020-07-24 宣伟公司 Process for making water-dispersible polymers and water-dispersed polymers
CN111448265B (en) * 2017-12-11 2022-04-15 宣伟公司 Process for making water-dispersible polymers and water-dispersed polymers
US12168703B2 (en) 2017-12-11 2024-12-17 Swimc Llc Method for making water-dispersible and water-dispersed polymers

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Application publication date: 20110504