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SE504282C2 - Process for the preparation of a selectively substituted triol - Google Patents

Process for the preparation of a selectively substituted triol

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Publication number
SE504282C2
SE504282C2 SE9500206A SE9500206A SE504282C2 SE 504282 C2 SE504282 C2 SE 504282C2 SE 9500206 A SE9500206 A SE 9500206A SE 9500206 A SE9500206 A SE 9500206A SE 504282 C2 SE504282 C2 SE 504282C2
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SE
Sweden
Prior art keywords
triol
formal
cyclic
process according
ethoxylated
Prior art date
Application number
SE9500206A
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Swedish (sv)
Other versions
SE9500206D0 (en
SE9500206L (en
Inventor
Carl-Axel Edvard Sjoegreen
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Perstorp Ab
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.)
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Publication date
Application filed by Perstorp Ab filed Critical Perstorp Ab
Priority to SE9500206A priority Critical patent/SE504282C2/en
Publication of SE9500206D0 publication Critical patent/SE9500206D0/en
Priority to PCT/SE1996/000056 priority patent/WO1996022956A1/en
Priority to AU45931/96A priority patent/AU4593196A/en
Priority to TW85100749A priority patent/TW318835B/zh
Publication of SE9500206L publication Critical patent/SE9500206L/en
Publication of SE504282C2 publication Critical patent/SE504282C2/en

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    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G65/00Macromolecular compounds obtained by reactions forming an ether link in the main chain of the macromolecule
    • C08G65/02Macromolecular compounds obtained by reactions forming an ether link in the main chain of the macromolecule from cyclic ethers by opening of the heterocyclic ring
    • C08G65/26Macromolecular compounds obtained by reactions forming an ether link in the main chain of the macromolecule from cyclic ethers by opening of the heterocyclic ring from cyclic ethers and other compounds
    • C08G65/2603Macromolecular compounds obtained by reactions forming an ether link in the main chain of the macromolecule from cyclic ethers by opening of the heterocyclic ring from cyclic ethers and other compounds the other compounds containing oxygen
    • C08G65/2606Macromolecular compounds obtained by reactions forming an ether link in the main chain of the macromolecule from cyclic ethers by opening of the heterocyclic ring from cyclic ethers and other compounds the other compounds containing oxygen containing hydroxyl groups
    • 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
    • C07C41/26Preparation of ethers by reactions not forming ether-oxygen bonds by introduction of hydroxy or O-metal groups
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D319/00Heterocyclic compounds containing six-membered rings having two oxygen atoms as the only ring hetero atoms
    • C07D319/041,3-Dioxanes; Hydrogenated 1,3-dioxanes
    • C07D319/061,3-Dioxanes; Hydrogenated 1,3-dioxanes not condensed with other rings

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Health & Medical Sciences (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Low-Molecular Organic Synthesis Reactions Using Catalysts (AREA)
  • Preparation Of Compounds By Using Micro-Organisms (AREA)

Abstract

A process for production of a selectively alkoxylated triol, which process comprises two or more Steps including the Steps of a) reacting a cyclic triol formal having one reactive hydroxyl group with an alkylene oxide or correponding glycol, which reaction yields a corresponding alkoxylated cyclic triol formal; and b) acidic hydrolysis of the alkoxylated cyclic triol in the presence of a triol, which hydrolysis yields a selectively alkoxylated triol having one alkoxysubstituted and two unsubstituted hydroxyl groups and formaldehyde, which formaldehyde reacts with the triol yielding a cyclic triol formal, whereby in Step b) yielded cyclic triol formal can be used for alkoxylation in Step a). A further aspect of the invention relates to an acidic hydrolysis of a hydroxysubstituted cyclic triol formal. The hydrolysis is performed in the presence of a triol and the hydrolysis yields a selectively hydroxysubstituted triol having one substituted and two unsubstituted hydroxyl groups and formaldehyde, which formaldehyde reacts with the triol yielding a cyclic triol formal.

Description

' 504 282 varvid den under (ii) bildade cykliska triolformalen kan reageras med etenoxid el- ler propenoxid till motsvarande etoxylerade eller propoxylerade cykliska triolfor- mal enligt (i). '504 282 wherein the cyclic triol formula formed under (ii) can be reacted with ethylene oxide or propylene oxide to the corresponding ethoxylated or propoxylated cyclic triol form according to (i).

Triolen i den cykliska triolformalen utgörs företrädesvis av trimetylolpropan, tri- metyloletan eller glycerol. Den cykliska triolformalen kan framställas genom reak- tion av triolen med formaldehyd. Reaktionen utföres företrädesvis i närvaro av en sur katalysator såsom svavelsyra, saltsyra, metansulfonsyra eller paratoluensulfon- syra samt vid en temperatur av 20-l50°C, vanligtvis 20-100°C.The triol in the cyclic triol formal is preferably trimethylolpropane, trimethylolethane or glycerol. The cyclic triol formal can be prepared by reacting the triol with formaldehyde. The reaction is preferably carried out in the presence of an acid catalyst such as sulfuric acid, hydrochloric acid, methanesulfonic acid or paratoluenesulfonic acid and at a temperature of 20-150 ° C, usually 20-100 ° C.

Det är ofta lämpligt att reaktionen utföres i närvaro av ett lågkokande lösningsme- del såsom bensen.It is often convenient for the reaction to be carried out in the presence of a low boiling solvent such as benzene.

Normalt anlagras i steg (i) i genomsnitt 2-30 mol etenoxid eller propenoxid till formalens fria hydroxylgrupp.Normally, in step (i), an average of 2-30 moles of ethylene oxide or propylene oxide are deposited to the free hydroxyl group of the form.

Reaktionen i stg (i) går lämpligen till så att etenoxid eller propenoxid leds in i for- malen vilken föreligger i flytande form. Temperaturen under reaktionen är vanligen 100-l80°C, trycket 100-1000 kPa (1-10 bar) och reaktionen utföres företrädesvis i alkalisk miljö, varvid bla. natriumhydroxid eller kaliumhydroxid kan användas som katalysator.The reaction in step (i) is conveniently carried out so that ethylene oxide or propylene oxide is introduced into the form which is in liquid form. The temperature during the reaction is usually 100-180 ° C, the pressure 100-1000 kPa (1-10 bar) and the reaction is preferably carried out in an alkaline environment, whereby i.a. sodium hydroxide or potassium hydroxide can be used as catalyst.

Spaltningen i steg (ii) utföres i sur miljö samt lämpligen under vakuum. Företrä- desvis höjs temperaturen tills bildad formal avgår varpå överskott av polyol avdri- ves och den etoxylerade eller propoxylerade triolen kvarstår. Vakuumet är O-l3,3 kPa (0-100 torr), företrädesvis 0-665 Pa (0-5 torr) och allra helst 0-399 (O-3 torr) Genom att enligt uppfinningen utföra spaltningen i steg (ii) i närvaro av den triol som ingår i den cykliska triolformalen som används i steg (i) når man flera förde- lar. Den allra viktigaste är naturligtvis att en tillfredsställande spaltningsreaktion över huvud taget möjliggörs Eventuellt överskott av triol som avdrivs i steg (ii) kan användas för framställning av den cykliska formalen. Samma cykliska formal bildas i steg (ii) och kan överföras till steg (i). Processen i sin helhet blir därför synnerligen ekonomiskt fördelaktig. De ekonomiska fördelarna förstärks givetvis också av att användningen av en lägre envärd alkohol samt avskiljning och uppar- betning av denna undviks.The cleavage in step (ii) is carried out in an acidic environment and preferably under vacuum. Preferably, the temperature is raised until the formal formed leaves, after which excess polyol is evaporated off and the ethoxylated or propoxylated triol remains. The vacuum is 0-13.3 kPa (0-100 torr), preferably 0-665 Pa (0-5 torr) and most preferably 0-399 (0-3 torr). According to the invention, by carrying out the decomposition in step (ii) of the presence of the triol included in the cyclic triol formula used in step (i) achieves several benefits. The most important is, of course, that a satisfactory cleavage reaction is possible at all. Any excess triol stripped in step (ii) can be used to prepare the cyclic formula. The same cyclic form is formed in step (ii) and can be transferred to step (i). The process as a whole will therefore be extremely economically advantageous. Of course, the economic benefits are also enhanced by avoiding the use of a lower monovalent alcohol and its separation and processing.

Uppfmningen förklaras närmare i anslutning till nedanstående utföringsexempel samt bifogade figur som schematiskt formelmässigt illustrerar de olika stegen i förfarandet enligt uppfinningen utgående från en reaktion mellan TMP och formaldehyd. 504 282 Exempel 1 illustrerar därvid en utföringsform enligt uppfinningen medan exempel 2 avser jämförelseförsök där steg (ii) utförs utanför uppfinningens ram.The invention is explained in more detail in connection with the following exemplary embodiments and the accompanying figure which schematically illustrates in formula form the various steps in the process according to the invention based on a reaction between TMP and formaldehyde. Example 1 illustrates an embodiment according to the invention, while Example 2 relates to comparative experiments where step (ii) is performed outside the scope of the invention.

Exempel I I en reaktor utrustad med omrörare, återloppskondensor och termometer satsades 400 g trimetyolpropan (TMP), 243,2 g 37-procentig formalin, 18 g paratoluensul- fonsyra och 3 lbensen.Example I 400 g of trimethiol propane (TMP), 243.2 g of 37% formalin, 18 g of paratoluenesulphonic acid and 3 l of benzene were charged to a reactor equipped with a stirrer, reflux condenser and thermometer.

Blandningen återloppskokades vid ca lO0°C tills ungeför 209 g vatten hade av- lägsnats. Reaktionsblandningen kyldes sedan och extraherades med 3 x 100 ml 30-procentig vattenlösning av natriumformiat för att avlägsna katalysatorn.The mixture was refluxed at about 100 ° C until about 209 g of water had been removed. The reaction mixture was then cooled and extracted with 3 x 100 ml of 30% aqueous sodium formate solution to remove the catalyst.

Det erhållna organiska skiktet torkades varpå bensenet avlägsnades genom indunstning, Den kvarstående produkten destillerades under vakuum, 381 g av den cykliska for- malen 5-etyl-5-hydroximetyl-1,3-dioxan erhölls, kokpunkt 110-'120°C vid 399 Pa (3 torr), 292 g (2,0 mol) S-etyl-S-hydroximetyl-l,3-dioxan i flytande form satsades i en re- aktor. 14,0 mol etenoxid leddes in i det flytande dioxanderivatet i reaktorn. Tem- peraturen i reaktorn var 150°C och trycket 500 kPa (5 bar). I reaktorn fanns 0,61 g KOH. Den erhållna reaktionsblandningen neutraliserades genom tillsatsav 0,66 g ättiksyra.The resulting organic layer was dried and the benzene was removed by evaporation. The residual product was distilled under vacuum, 381 g of the cyclic formula 5-ethyl-5-hydroxymethyl-1,3-dioxane were obtained, b.p. 110 DEG-120 DEG C. at 399 DEG. Pa (3 torr), 292 g (2.0 mol) of S-ethyl-S-hydroxymethyl-1,3-dioxane in liquid form were charged to a reactor. 14.0 moles of ethylene oxide were introduced into the liquid dioxane derivative in the reactor. The temperature in the reactor was 150 ° C and the pressure was 500 kPa (5 bar). The reactor contained 0.61 g of KOH. The resulting reaction mixture was neutralized by the addition of 0.66 g of acetic acid.

S92 g etoxylat av S-etyl-S-hydroximetyl-l,3-dioxan erhölls, där i genomsnitt 6,9 mol etenoxid anlagrats till den fria hydroxylgruppen.S92 g of ethoxylate of S-ethyl-S-hydroxymethyl-1,3-dioxane was obtained, where an average of 6.9 mol of ethylene oxide was deposited to the free hydroxyl group.

I en reaktionskolv nedsänkt i ett oljebad och försedd med omrörare och termome- ter samt kopplad till kylare, förlag, kylfälla och vakuumpump satsades 599,3 g (1,34 mol) av det etoxylerade dioxanderivatet, 273 g (2,03 mol) TMP och 4,4 g 96 procentig H2SO4, Blandningen sattes under ett vakuum av 133 Pa (1 torr) varpå temperaturen höjdes tills S-etyl-S-hydroximetyl-l,3-dioxan började drivas av.599.3 g (1.34 mol) of the ethoxylated dioxane derivative, 273 g (2.03 mol) of TMP were charged to a reaction flask immersed in an oil bath and equipped with stirrers and thermometers and connected to coolers, feeders, cooling traps and vacuum pumps. and 4.4 g of 96% H 2 SO 4. The mixture was placed under a vacuum of 133 Pa (1 torr) and the temperature was raised until S-ethyl-S-hydroxymethyl-1,3-dioxane began to evaporate.

Trycket bibehölls vid ca 133 Pa och temperaturen i kolven fick stiga till ca 145°C.The pressure was maintained at about 133 Pa and the temperature in the flask was allowed to rise to about 145 ° C.

Reaktionen fick fortgå i 2,4 timmar. Därvid erhålls ca 1,2 mol S-etyl-S-hydroximetyl-l,3-dioxan som destillat. Detta kunde användas vid förnyad etoxylering enligt ovan.The reaction was allowed to proceed for 2.4 hours. About 1.2 mol of S-ethyl-S-hydroxymethyl-1,3-dioxane are obtained as distillate. This could be used in renewed ethoxylation as above.

Därefter neutraliserades reaktionsblandningen. Temperaturen höjdes till 165°C, varvid trycket hölls vid ca 133 Pa, Temperaturen höjdes sedan successivt till ca 504 282 180°C, varvid kvarvarande överskott av TMP destillerade över tillsammans med den mindre del av dioxanderivatet som inte avdestillerades vid det första destilla- tionssteget. Denna TMP kunde användas vid förnyad reaktion med den etoxylerade dioxanen till 5-etyl-5-hydroximetyl-1,3-dioxan.Then the reaction mixture was neutralized. The temperature was raised to 165 ° C, keeping the pressure at about 133 Pa. The temperature was then gradually raised to about 504 282 180 ° C, with the remaining excess of TMP distilled over together with the smaller part of the dioxane derivative which was not distilled off in the first distillation step. . This TMP could be used in the reaction with the ethoxylated dioxane to give 5-ethyl-5-hydroxymethyl-1,3-dioxane.

I reaktionskolven kvarstod 580 g TMP-trietoxylat där etoxylatsubstitutionen ute- slutande fanns på en av OH-grupperna. Produkten innehöll ca 2 % ej avdestillerad TMP.580 g of TMP triethoxylate remained in the reaction flask, where the ethoxylate substitution was exclusively on one of the OH groups. The product contained about 2% non-distilled TMP.

Exempel 2 5 g av det etoxylerade S-etyl-S-hydroximetyl-1,3-dioxanet från exempel 1 löstes i etanol och l-n HCl. Viktförhållandet mellan de tre ingredienserna var 2:1:1.Example 2 5 g of the ethoxylated S-ethyl-S-hydroxymethyl-1,3-dioxane from Example 1 were dissolved in ethanol and 1-n HCl. The weight ratio of the three ingredients was 2: 1: 1.

Blandningen värmdes till 80°C i 4 timmar. Alla flyktiga beståndsdelar avdestillera- des. OH-talet för den erhållna produkten blev 128, dvs praktiskt taget samma som för S-etyl-S-hydroximetyl-LB-dioxanet som har ett OH-tal av 1251 En fullständig spaltning till TMP-trietoxylat hade gett ett OH-tal av ca 3801 Försöket visar att etoxylatet av S-etyl-S-hydroximetyl-l,3-dioxan spaltas i mycket 'liten utsträckning under dessa betingelser.The mixture was heated to 80 ° C for 4 hours. All volatile constituents were distilled off. The OH number of the product obtained was 128, i.e. practically the same as for the S-ethyl-S-hydroxymethyl-LB-dioxane which has an OH number of 1251 A complete cleavage to TMP triethoxylate had given an OH number of approx. The experiment shows that the ethoxylate of S-ethyl-S-hydroxymethyl-1,3-dioxane is decomposed to a very small extent under these conditions.

Uppñnningen är inte begränsad till de visade utföringsformerna, då dessa kan mo- difieras på olika sätt inom uppfinningens ramaThe invention is not limited to the embodiments shown, as these can be modified in different ways within the scope of the invention.

Claims (10)

504 282504 282 1. Patentkrav l _Claim 1 _ 2. Förfarande för tillverkning av en selektivt alkoxylerad triol kännetecknat av, att (i) en cyklisk triolformal med en hydroxylgrupp reageras med etenoxid eller propenoxid till motsvarande etoxylerad eller propoxylerad cyklisk triolformal, och (ii) den etoxylerade eller propoxylerade cykliska triolformalen i närvaro av i denna ingående triol undergår sur spaltning, varvid etoxylerad eller propoxylerad triol och formaldehyd bildas och varvid bildad formaldehyd reagerar med triolen till cyklisk triolformal med en reaktiv hydroxylgrupp. varvid den under (ii) bildade triolformalen kan reageras med etenoxid eller pro- penoxid till motsvarande etoxylerade eller propoxylerade cykliska triolformal enligt (i).Process for the preparation of a selectively alkoxylated triol, characterized in that (i) a cyclic triol formal with a hydroxyl group is reacted with ethylene oxide or propylene oxide to the corresponding ethoxylated or propoxylated cyclic triol formal, and (ii) the ethoxylated or propoxylated cyclic triol formal in the presence of this constituent triol undergoes acidic cleavage, whereby ethoxylated or propoxylated triol and formaldehyde are formed and wherein formed formaldehyde reacts with the triol to form a cyclic triol formal with a reactive hydroxyl group. wherein the triol formal formed under (ii) can be reacted with ethylene oxide or propylene oxide to the corresponding ethoxylated or propoxylated cyclic triol formal according to (i). 3. . Förfarande enligt krav l k 'a n n e t e c k n a t a v, att den cykliska triolformalen och den etoxylerade eller propoxylerade cykliska triolformalen är en formal av trimetylolpropan, tri- metyloletan eller glycerol.3.. A process according to claim 1, wherein the cyclic triol formal and the ethoxylated or propoxylated cyclic triol formal are a form of trimethylolpropane, trimethylolethane or glycerol. 4. , Förfarande enligt krav 2 k ä n n e t e c k n a t a v, att triolen är trimetylolpropan, trimetyloletan eller glycerol. _ Förfarande enligt något av kraven 1-3 k á n n e t e c k n at a v, att den cykliska triolformalen i närvaro av en alka- lisk katalysator reageras med etenoxid eller propenoxid vid en temperatur av l0O-l80°C och ett tryck av 100-1000 kPa4. A process according to claim 2, characterized in that the triol is trimethylolpropane, trimethylolethane or glycerol. Process according to any one of claims 1-3, characterized in that the cyclic triol formal in the presence of an alkaline catalyst is reacted with ethylene oxide or propylene oxide at a temperature of 10-180 ° C and a pressure of 100-1000 kPa 5. Förfarande enligt kravet 4 k a n n e t e c k n at a v, att den alkaliska katalysatorn är natriumhydroxid el- ler kaliumhydroxid5. A process according to claim 4, wherein the alkaline catalyst is sodium hydroxide or potassium hydroxide. 6. Förfarande enligt något av kraven l-S k ä n n e t e c k n at a v, att 2-30 mol etenoxid eller propenoxid anlagras till den cykliska triolformalens hydroxylgrupp.A process according to any one of claims 1 to 5, wherein 2-30 moles of ethylene oxide or propylene oxide are deposited to the hydroxyl group of the cyclic triol formal. 7. Förfarande enligt något av kraven 1-6 k ä n n e t e c k n a t a v, att den sura spaltningen utförs i närvaro av en sur katalysator och under ett vakuum av O-l3,3 kPa, företrädesvis 0-655 Pa och helst 0-3 99 Pa. 504 282Process according to any one of claims 1-6, characterized in that the acidic cleavage is carried out in the presence of an acid catalyst and under a vacuum of 0-1,3 kPa, preferably 0-655 Pa and most preferably 0-3 99 Pa. 504 282 8. Förfarande enligt krav 7 k ä n n e t e c k n at a v, att den sura katalysatorn är svavelsyra.Process according to Claim 7, characterized in that the acid catalyst is sulfuric acid. 9. Förfarande enligt krav 7 eller 8 k ä n n e t e c k n a t a v, att cyklisk triolformal bildad under den sura spalt- ningen genom en temperaturhöjning avgår, varefter eventuellt överskott av triol avdrivs och den etoxylerade eller propoxylerade triolen kvarstår.Process according to Claim 7 or 8, characterized in that cyclic triol formal formed during the acidic cleavage is carried out by an increase in temperature, after which any excess triol is evaporated off and the ethoxylated or propoxylated triol remains. 10.Förfarande enligt något av kraven 1-9 k ä n n e t e c k n a t a v, att den cykliska triolformalen är S-etyl-S-hydroximetyl-lß-dioxan och att triolen är trimetylolpropan.10. A process according to any one of claims 1-9 characterized in that the cyclic triol formula is S-ethyl-S-hydroxymethyl-1β-dioxane and that the triol is trimethylolpropane.
SE9500206A 1995-01-23 1995-01-23 Process for the preparation of a selectively substituted triol SE504282C2 (en)

Priority Applications (4)

Application Number Priority Date Filing Date Title
SE9500206A SE504282C2 (en) 1995-01-23 1995-01-23 Process for the preparation of a selectively substituted triol
PCT/SE1996/000056 WO1996022956A1 (en) 1995-01-23 1996-01-22 Selectively hydroxysubstituted triol
AU45931/96A AU4593196A (en) 1995-01-23 1996-01-22 Selectively hydroxysubstituted triol
TW85100749A TW318835B (en) 1995-01-23 1996-01-23

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
SE9500206A SE504282C2 (en) 1995-01-23 1995-01-23 Process for the preparation of a selectively substituted triol

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SE9500206D0 SE9500206D0 (en) 1995-01-23
SE9500206L SE9500206L (en) 1996-07-24
SE504282C2 true SE504282C2 (en) 1996-12-23

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WO (1) WO1996022956A1 (en)

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Publication number Priority date Publication date Assignee Title
SE509144C2 (en) * 1997-04-09 1998-12-07 Perstorp Ab Shrink reducing agents for cement compositions
WO2022082285A1 (en) * 2020-10-19 2022-04-28 Oxiteno S.A. Indústria E Comércio Composition, agrochemical formulation, methods for increasing water and nutrient availability and for improving pest control in plants and seeds, and uses of the composition and the agrochemical formulation

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DE3163056D1 (en) * 1980-06-20 1984-05-17 Goldschmidt Ag Th Process for the production of polymers with at least one terminal primary hydroxyl group
US5135683A (en) * 1991-03-28 1992-08-04 Arco Chemical Technology, L.P. Process for producing a deprotected alkoxylated polyol

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WO1996022956A1 (en) 1996-08-01
SE9500206D0 (en) 1995-01-23
AU4593196A (en) 1996-08-14
TW318835B (en) 1997-11-01
SE9500206L (en) 1996-07-24

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