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DE1216862B - Process for the preparation of mono- or polyunsaturated aldehydes or their functional derivatives - Google Patents

Process for the preparation of mono- or polyunsaturated aldehydes or their functional derivatives

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Publication number
DE1216862B
DE1216862B DEB79333A DEB0079333A DE1216862B DE 1216862 B DE1216862 B DE 1216862B DE B79333 A DEB79333 A DE B79333A DE B0079333 A DEB0079333 A DE B0079333A DE 1216862 B DE1216862 B DE 1216862B
Authority
DE
Germany
Prior art keywords
parts
mono
functional derivatives
preparation
aldehydes
Prior art date
Legal status (The legal status 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 status listed.)
Pending
Application number
DEB79333A
Other languages
German (de)
Inventor
Dr Herwig Freyschlag
Dr Werner Reif
Dr Axel Nuerrenbach
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
BASF SE
Original Assignee
BASF SE
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.)
Filing date
Publication date
Application filed by BASF SE filed Critical BASF SE
Priority to DEB79333A priority Critical patent/DE1216862B/en
Priority to US413617A priority patent/US3471569A/en
Priority to SE14375/64A priority patent/SE328861B/xx
Publication of DE1216862B publication Critical patent/DE1216862B/en
Pending legal-status Critical Current

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Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07FACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
    • C07F9/00Compounds containing elements of Groups 5 or 15 of the Periodic Table
    • C07F9/02Phosphorus compounds
    • C07F9/28Phosphorus compounds with one or more P—C bonds
    • C07F9/54Quaternary phosphonium compounds
    • C07F9/5428Acyclic unsaturated phosphonium compounds
    • 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
    • C07C45/51Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by pyrolysis, rearrangement or decomposition
    • C07C45/511Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by pyrolysis, rearrangement or decomposition involving transformation of singly bound oxygen functional groups to >C = O groups
    • C07C45/515Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by pyrolysis, rearrangement or decomposition involving transformation of singly bound oxygen functional groups to >C = O groups the singly bound functional group being an acetalised, ketalised hemi-acetalised, or hemi-ketalised hydroxyl group
    • 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
    • C07C45/51Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by pyrolysis, rearrangement or decomposition
    • C07C45/518Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by pyrolysis, rearrangement or decomposition involving transformation of sulfur-containing compounds to >C = O groups
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07FACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
    • C07F9/00Compounds containing elements of Groups 5 or 15 of the Periodic Table
    • C07F9/02Phosphorus compounds
    • C07F9/28Phosphorus compounds with one or more P—C bonds
    • C07F9/54Quaternary phosphonium compounds
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07FACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
    • C07F9/00Compounds containing elements of Groups 5 or 15 of the Periodic Table
    • C07F9/02Phosphorus compounds
    • C07F9/28Phosphorus compounds with one or more P—C bonds
    • C07F9/54Quaternary phosphonium compounds
    • C07F9/5407Acyclic saturated phosphonium compounds
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2601/00Systems containing only non-condensed rings
    • C07C2601/12Systems containing only non-condensed rings with a six-membered ring
    • C07C2601/16Systems containing only non-condensed rings with a six-membered ring the ring being unsaturated

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Biochemistry (AREA)
  • General Health & Medical Sciences (AREA)
  • Molecular Biology (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Description

Verfahren zur Herstellung von ein- oder mehrfach ungesättigten Aldehyden oder ihren funktionellen Derivaten Zusatz zur Anmeldung: B 74477 IV b/12o -Auslegeschrift 1 211 616 Gegenstand der Hauptpatentanmeldung B 74477 IVb/ 120 (deutsche Auslegeschrift 1 211 616) ist ein Verfahren zur Herstellung von ein- oder mehrfach ungesättigten Aldehyden oder ihren Acetalen, Acylalen, Oximen, Hydrazonen, Semicarbazonen oder Schiffschen Basen, das dadurch gekennzeichnet ist, daß man Phosphoniumsalze der allgemeinen Formel in der Ar einen gegebenenfalls durch Alkyl- oder Alkoxygruppen substituierten Arylrest, R1, R2 und Rs Wasserstoff oder Alkyl, X ein einwertiges Anion und n eine ganze Zahl von 0 bis 3 bedeutet, in jeweils an sich bekannter Weise in vorstehend genannten Aldehydderivaten überführt, diese, gewünschtenfalls ohne Isolierung, mittels Protonenakzeptoren zu den entsprechenden Yliden umsetzt, die Ylide mit Aldehyden oder Ketonen zur Umsetzung bringt und die erhaltenen Aldehydderivate gewinnt oder gegebenenfalls zu den freien Aldehyden spaltet.Process for the preparation of mono- or polyunsaturated aldehydes or their functional derivatives mono- or polyunsaturated aldehydes or their acetals, acylals, oximes, hydrazones, semicarbazones or Schiff's bases, which is characterized in that phosphonium salts of the general formula are used in which Ar is an aryl radical optionally substituted by alkyl or alkoxy groups, R1, R2 and Rs are hydrogen or alkyl, X is a monovalent anion and n is an integer from 0 to 3, these are converted in a manner known per se into the aforementioned aldehyde derivatives , if desired without isolation, is converted to the corresponding ylides by means of proton acceptors, the ylides are reacted with aldehydes or ketones and the aldehyde derivatives obtained are obtained or, if appropriate, cleaved to give the free aldehydes.

Es wurde nun gefunden, daß man in Abwandlung des Verfahrens gemäß Hauptpatentanmeldung B 74477 IVb/120 die Phosphoniumsalze an Stelle der Umwandlung in die Acetale, Acylale, Oxime, Hydrazone, Semicarbazone oder Schiffschen Basen in die Halbacetale, Mercaptale oder Aminale in jeweils an sich bekannter Weise überführt. Die nach dem erfindungsgemäßen Verfahren aus den Phosphoniumsalzen in der ersten Verfahrensstufe herstellbaren Aldehydderivate haben demnach die allgemeine Formel in der Ar, R1, R2, Rs, n und X die vorstehend angegebene Bedeutung haben: A Alkoxy B Hydroxy A Alkylmercapto B Alkylmercapto A N(R')2 B N(R')2 R' = Alkyl Die Beispiele erläutern das erfindungsgemäße Verfahren. Im übrigen gelten die Angaben der Hauptpatentanmeldung.It has now been found that, in a modification of the process according to main patent application B 74477 IVb / 120, the phosphonium salts, instead of converting them into the acetals, acylals, oximes, hydrazones, semicarbazones or Schiff's bases, into the hemiacetals, mercaptals or aminals in each case known per se Way convicted. The aldehyde derivatives which can be prepared by the process according to the invention from the phosphonium salts in the first process stage accordingly have the general formula in which Ar, R1, R2, Rs, n and X have the meaning given above: A alkoxy B hydroxy A alkyl mercapto B alkyl mercapto AN (R ') 2 BN (R') 2 R '= alkyl The examples illustrate the process according to the invention. Otherwise, the information in the main patent application applies.

Beispiel 1 10 Teile Triphenyl - 3 - formyl - buten - (2) - yl - (1)-phosphoniumchlorid werden mit 20 Teilen Isopropanol und einem Kriställchen p-Toluolsulfonsäure zum Sieden erhitzt. Das Lösungsmittel wird langsam über 4 Stunden hinweg abdestilliert. Es bleiben als durchkristallisierendes Dl 11,6 Teile Triphenyl-3-(hydroxy-isopropoxy-methyl)-buten-(2)-yl-(1)-phospho niumchlorid zurück. Nach Umfällen aus einer Methylenchloridlösung mit Tetrahydrofuran schmilzt das Halbacetal bei 87 bis 90°C. Das NMR-, das UR-Spektrum und die Analyse sichern die Konstitution. Example 1 10 parts of triphenyl - 3 - formyl - buten - (2) - yl - (1) - phosphonium chloride are p-toluenesulfonic acid with 20 parts of isopropanol and a crystal Boiling heated. The solvent is slowly distilled off over 4 hours. 11.6 parts of triphenyl-3- (hydroxy-isopropoxy-methyl) -butene- (2) -yl- (1) -phospho remain as fully crystallizing Dl nium chloride back. After reprecipitation from a methylene chloride solution with tetrahydrofuran the hemiacetal melts at 87 to 90 ° C. The NMR, the UR spectrum and the analysis secure the constitution.

Analysenwerte: Gefunden ... C 70,3, P 6,9°/o; berechnet . . . C 70,7, P 7,00/0.Analysis values: Found ... C 70.3, P 6.9%; calculated . . . C 70.7, P 7.00 / 0.

4,4 Teile des Triphenyl-3-(hydroxy-isopropoxy-methyl)-buten-(2)-yl-(1)-phosphoniumchlorids werden in 20 Teilen Methanol gelöst und mit 0,23 Teilen Natrium in 10 Teilen Methanol sowie mit 2,84 Teilen Vitamin A-Aldehyd versetzt. In einer Stickstoffatmosphäre wird 1 Stunde unter Rückfluß gekocht. 4.4 parts of triphenyl-3- (hydroxy-isopropoxy-methyl) -butene- (2) -yl- (1) -phosphonium chloride are dissolved in 20 parts of methanol and 0.23 part of sodium in 10 parts of methanol and 2.84 parts of vitamin A aldehyde are added. In a nitrogen atmosphere is refluxed for 1 hour.

Das erhaltene Gemisch wird mit Wasser versetzt und mit Äther extrahiert. Zur Spaltung des Halbacetals wird die ätherische Lösung 1/2 Stunde mit 2n-Schwefelsäure gerührt. Nach Trocknen der Atherphase und Abdestillieren des Lösungsmittels bleiben 3,3 Teile eines orangeroten Ols zurück.The mixture obtained is mixed with water and extracted with ether. To split the hemiacetal, the ethereal solution is treated with 2N sulfuric acid for 1/2 hour touched. After drying the ether phase and distilling off the solvent stay 3.3 parts of an orange-red oil.

Nach Kristallisation aus tiefsiedendem Petroläther kann das ,B-Apo-12'-carotinal kristallin erhalten werden. Gelborange Kristalle, F. 88 bis 92°C; Amax 414 mp; E:S, = 2130 (gemessen in Cyclohexan).After crystallization from low-boiling petroleum ether, the 'B-apo-12'-carotenal can can be obtained in crystalline form. Yellow-orange crystals, m.p. 88 to 92 ° C; Amax 414 mp; IT, = 2130 (measured in cyclohexane).

Beispiel 2 7,6 Teile Triphenyl 3 - formyl - buten - (2) - yl - (1)-phosphoniumchlorid werden in 50 Teilen Methanol mit 2,1 Teilen o-Ameisensäuremethylester und einem Kriställchen p-Toluolsulfonsäure 2 Stunden erhitzt. Example 2 7.6 parts of triphenyl 3-formyl-buten- (2) -yl- (1) -phosphonium chloride are in 50 parts of methanol with 2.1 parts of methyl o-formate and one Crystals of p-toluenesulfonic acid heated for 2 hours.

Nach dem Abkühlen versetzt man mit 0,36 Teilen Wasser und engt die Mischung zur Trocknung ein.After cooling, it is mixed with 0.36 parts of water and concentrated Mixture to dry.

Es bleiben 8,2 Teile einer kristallinen Substanz zurück, bei der es sich nach UR- und NMR-Spektrum um das Halbacetal handelt. F. 113 bis 115"C.8.2 parts of a crystalline substance remain in which it is the hemiacetal according to the UR and NMR spectrum. F. 113 to 115 "C.

Analysenwerte: Gefunden ... C 69,6, P 6,4°/o; berechnet . . C 69,8, P 6,30/0.Analysis values: Found ... C 69.6, P 6.4%; calculated . . C 69.8, P 6.30 / 0.

4,3 Teile des so erhaltenen Methyl-halbacetals des Triphenyl-3-formylbuten-(2)-yl-(1)-phosphoniumchlorids werden mit 30 Teilen Methanol und 0,23 Teilen Na in 10 Teilen Methanol versetzt. Nach Zugabe von 3,5 Teilen ß - Apo - 12' - carotinal erhitzt man 2 Stunden in einer Stickstoffatmosphäre unter Rückfluß. Das erkaltete Reaktionsgemisch wird mit Wasser und verdünnter Schwefelsäure versetzt und mit Octan extrahiert. Nach dem Trocknen der Octanphase über Natriumsulfat und Abdestillieren des Lösungsmittels bleiben 4,2 Teile eines tiefroten Kristallbreis zurück. Nach Umkristallisieren aus Benzol-Methanol erhält man das ß-Apo-8'-carotinal in kristalliner Form. F. 137"C; Ämaz 458 my; % = 2600 (gemessen in Cyclohexan). 4.3 parts of the methyl hemiacetal of triphenyl-3-formylbutene- (2) -yl- (1) -phosphonium chloride thus obtained 30 parts of methanol and 0.23 part of Na in 10 parts of methanol are added. After adding 3.5 parts of ß-apo-12 '-carotinal, the mixture is heated for 2 hours in a Nitrogen atmosphere under reflux. The cooled reaction mixture is washed with water and dilute sulfuric acid are added and the mixture is extracted with octane. After drying the octane phase over sodium sulfate and distilling off the solvent remain 4.2 parts of a deep red crystal pulp. After recrystallization from benzene-methanol the ß-apo-8'-carotenal is obtained in crystalline form. F. 137 "C; Ämaz 458 my;% = 2600 (measured in cyclohexane).

Beispiel 3 Man versetzt 10 Teile Triphenyl-3-formyl-buten-(2)-yl-(1)-phosphoniumchlorid mit 30 Teilen Chloroform und 2,5 Teilen Dithioglykol. Nach Einleiten einer Spur Chlorwasserstoff wird bei Zimmertemperatur 5 Stunden gerührt. Nach Einengen erhält man 12,1Teile des Mercaptals als Dl, das in 50 Teilen Methanol gelöst und mit 0,61 Teilen Natrium in 10 Teilen Methanol sowie mit 7,5 Teilen Vitamin A-Aldehyd versetzt wird. In einer Stickstoffatmosphäre wird 3 Stunden unter Rückfluß gekocht. Zur Spaltung des Mercaptals wird die erkaltete Lösung mit Quecksilber(II)-chlorid in Aceton versetzt und unter Erwärmen auf 40"C weitere 2 Stunden gerührt. Example 3 10 parts of triphenyl-3-formyl-buten- (2) -yl- (1) -phosphonium chloride are added with 30 parts of chloroform and 2.5 parts of dithioglycol. After initiating a track Hydrogen chloride is stirred at room temperature for 5 hours. Receives after narrowing one 12.1 parts of the mercaptal as Dl, dissolved in 50 parts of methanol and with 0.61 Parts of sodium in 10 parts of methanol and 7.5 parts of vitamin A aldehyde are added will. The mixture is refluxed for 3 hours in a nitrogen atmosphere. To split of the mercaptal, the cooled solution is mixed with mercury (II) chloride in acetone and stirred for a further 2 hours while warming to 40 ° C.

Nach Extrahieren der Mischung mit Octan, Trocknen und Abdestillieren des Lösungsmittels bleiben 8,2 Teile eines roten uns zurück (Ämaz 414 m). Nach Kristallisation aus tiefsiedendem Petroläther kann das BApo-12'-carotinal in kristalliner Form erhalten werden; gelborange Kristalle, F. 91 bis 94"C; Ämax 414mm; E:C, = 2160 (gemessen in Cyclohexan).After extracting the mixture with octane, drying and distilling off of the solvent, 8.2 parts of a red us remain (Ämaz 414 m). After crystallization The BApo-12'-carotenal can be obtained in crystalline form from low-boiling petroleum ether will; yellow-orange crystals, m.p. 91 to 94 "C; Ämax 414mm; E: C, = 2160 (measured in cyclohexane).

Claims (1)

Patentanspruch: Abwandlung des Verfahrens gemäß Hauptpatentanmeldung B 74477 IVb/12O zur Herstellung von ein- oder mehrfach ungesättigten Aldehyden oder ihren funktionellen Derivaten, dadurch gekennzeichnet, daß man die Phosphoniumsalze an Stelle der Umwandlung in die Acetale, Acylale, Oxime, Hydrazone, Semicarbazone oder Schiffschen Basen in die Halbacetale, Mercaptale oder Aminale in jeweils an sich bekannter Weise überführt. Claim: Modification of the process according to the main patent application B 74477 IVb / 12O for the production of mono- or polyunsaturated aldehydes or their functional derivatives, characterized in that the phosphonium salts instead of the conversion into the acetals, acylals, oximes, hydrazones, semicarbazones or Schiff's bases into the hemiacetals, mercaptals or aminals in each case convicted in a known manner.
DEB79333A 1963-11-30 1964-11-14 Process for the preparation of mono- or polyunsaturated aldehydes or their functional derivatives Pending DE1216862B (en)

Priority Applications (3)

Application Number Priority Date Filing Date Title
DEB79333A DE1216862B (en) 1964-11-14 1964-11-14 Process for the preparation of mono- or polyunsaturated aldehydes or their functional derivatives
US413617A US3471569A (en) 1963-11-30 1964-11-24 Process for producing acetals and hemiacetals of phosphonium salt compounds
SE14375/64A SE328861B (en) 1963-11-30 1964-11-27

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DEB79333A DE1216862B (en) 1964-11-14 1964-11-14 Process for the preparation of mono- or polyunsaturated aldehydes or their functional derivatives

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DE1216862B true DE1216862B (en) 1966-05-18

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8222458B2 (en) 2008-06-13 2012-07-17 University Of Maryland, College Park Process or synthesis of (3S)- and (3R)-3-hydroxy-beta-ionone, and their transformation to zeaxanthin and beta-cryptoxanthin

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8222458B2 (en) 2008-06-13 2012-07-17 University Of Maryland, College Park Process or synthesis of (3S)- and (3R)-3-hydroxy-beta-ionone, and their transformation to zeaxanthin and beta-cryptoxanthin

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