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DE1166191B - Process for the preparation of metal complexes of dialkyldithiophosphines - Google Patents

Process for the preparation of metal complexes of dialkyldithiophosphines

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DE1166191B
DE1166191B DEC21151A DEC0021151A DE1166191B DE 1166191 B DE1166191 B DE 1166191B DE C21151 A DEC21151 A DE C21151A DE C0021151 A DEC0021151 A DE C0021151A DE 1166191 B DE1166191 B DE 1166191B
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metal complexes
sulfur
dialkyldithiophosphines
complex
zinc
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Dr Wilhelm Kuchen
Dipl-Chem Josef Metten
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Chemische Fabrik Kalk GmbH
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Chemische Fabrik Kalk GmbH
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    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10LFUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
    • C10L1/00Liquid carbonaceous fuels
    • C10L1/10Liquid carbonaceous fuels containing additives
    • C10L1/14Organic compounds
    • C10L1/30Organic compounds compounds not mentioned before (complexes)
    • C10L1/301Organic compounds compounds not mentioned before (complexes) derived from metals
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J31/00Catalysts comprising hydrides, coordination complexes or organic compounds
    • B01J31/16Catalysts comprising hydrides, coordination complexes or organic compounds containing coordination complexes
    • B01J31/22Organic complexes
    • B01J31/2204Organic complexes the ligands containing oxygen or sulfur as complexing atoms
    • B01J31/226Sulfur, e.g. thiocarbamates
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    • 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
    • C07F9/50Organo-phosphines
    • C07F9/53Organo-phosphine oxides; Organo-phosphine thioxides
    • C07F9/5345Complexes or chelates of phosphine-oxides or thioxides with metallic compounds or metals
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    • 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
    • C07F9/66Arsenic compounds
    • C07F9/68Arsenic compounds without As—C bonds
    • 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
    • C07F9/90Antimony compounds
    • C07F9/902Compounds without antimony-carbon linkages
    • 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
    • C07F9/94Bismuth compounds
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K5/00Use of organic ingredients
    • C08K5/49Phosphorus-containing compounds
    • C08K5/5398Phosphorus bound to sulfur
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10LFUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
    • C10L1/00Liquid carbonaceous fuels
    • C10L1/10Liquid carbonaceous fuels containing additives
    • C10L1/14Organic compounds
    • C10L1/26Organic compounds containing phosphorus
    • C10L1/2608Organic compounds containing phosphorus containing a phosphorus-carbon bond
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10LFUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
    • C10L1/00Liquid carbonaceous fuels
    • C10L1/10Liquid carbonaceous fuels containing additives
    • C10L1/14Organic compounds
    • C10L1/26Organic compounds containing phosphorus
    • C10L1/2608Organic compounds containing phosphorus containing a phosphorus-carbon bond
    • C10L1/2616Organic compounds containing phosphorus containing a phosphorus-carbon bond sulfur containing
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2531/00Additional information regarding catalytic systems classified in B01J31/00
    • B01J2531/20Complexes comprising metals of Group II (IIA or IIB) as the central metal
    • B01J2531/26Zinc
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2531/00Additional information regarding catalytic systems classified in B01J31/00
    • B01J2531/20Complexes comprising metals of Group II (IIA or IIB) as the central metal
    • B01J2531/27Cadmium
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J2531/00Additional information regarding catalytic systems classified in B01J31/00
    • B01J2531/20Complexes comprising metals of Group II (IIA or IIB) as the central metal
    • B01J2531/28Mercury
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2531/00Additional information regarding catalytic systems classified in B01J31/00
    • B01J2531/50Complexes comprising metals of Group V (VA or VB) as the central metal
    • B01J2531/52Antimony
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2531/00Additional information regarding catalytic systems classified in B01J31/00
    • B01J2531/50Complexes comprising metals of Group V (VA or VB) as the central metal
    • B01J2531/54Bismuth

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Description

Verfahren zur Herstellung von Metallkomplexen der Dialkyldithiophosphine Die Zinksalze der Diorganodithiopbosphinsäuren können durch Umsetzung von Phosphorsulfiden mit aromatischen Kohlenwasserstoffen und Zinkhalogeniden in Gegenwart von Aluminiumhalogeniden gewonnen werden. Aluminiumsalze der Diorganoditbiophosphinsäuren sind auch durch Einwirkung von Aluminiumalkoholaten auf Diorganodithiophosphinsäuren darstellbar. Diese Salze, die sich bei Temperaturen um oder über 2000 C, ohne zu schmelzen, zersetzen, sind kaum löslich in organischen Lösungsmitteln, wie beispielsweise Benzol, Alkohol, Chlorofonn usw. Durch eine bessere Löslichkeit in diesen Lösungsmitteln zeichnen sich Aluminiumverbindungen aus, die durch Umsetzung von nur 1 bis 2 Mol Diorganodithiophosphinsäure mit 1 Mol Aluminiumalkoholat entstehen und noch eine Alkoholatgruppe im Molekül enthalten.Process for the preparation of metal complexes of dialkyldithiophosphines The zinc salts of diorganodithiophosphinic acids can be obtained by reacting phosphorus sulfides with aromatic hydrocarbons and zinc halides in the presence of aluminum halides be won. Aluminum salts of diorganoditol biophosphinic acids are also through Effect of aluminum alcoholates on diorganodithiophosphinic acids can be shown. These salts, which decompose at temperatures around or above 2000 C without melting, are hardly soluble in organic solvents such as benzene, alcohol, Chlorofonn, etc. Draw by a better solubility in these solvents aluminum compounds are obtained by reacting only 1 to 2 moles of diorganodithiophosphinic acid with 1 mole of aluminum alcoholate and another alcoholate group in the molecule contain.

Die zu diesen Umsetzungen notwendigen Diorganodithiophosphinsäuren können durch Einwirkung von Schwefel auf Diorganophosphine hergestellt werden. The diorganodithiophosphinic acids necessary for these reactions can be produced by the action of sulfur on diorganophosphines.

Die Umsetzung von Tetraorganodiphosphinen mit metallischem Natrium oder wäßrigen Alkalien führt ebenso zu Diorganophosphinen, wie die Einwirkung von Wasserstoff und zweiwertigen Metallen, die wie beispielsweise Kupfer - Wasserstoff zu aktivieren vermögen auf Tetraorganodiphosphindisulfide oder Tetraorganodiphosphine. The implementation of tetraorganodiphosphines with metallic sodium or aqueous alkalis also leads to diorganophosphines, as does the action of Hydrogen and divalent metals such as copper - hydrogen able to activate on tetraorganodiphosphine disulfide or tetraorganodiphosphine.

In gleicher Weise wird die P-P-Bindung von Tetraalkyldiphosphindisulfiden unter gleichzeitiger Desulfurierung durch die Einwirkung Lithiumalanat gespalten, so daß Dialkylphosphine entstehen. Die Umsetzung von Tetraorganodiphosphind isulfiden mit Wasserstoffperoxyd führt dagegen zu Diorganodiphosphonsäuren. In the same way, the P-P bond of tetraalkyldiphosphine disulfides with simultaneous desulfurization, the action of lithium alanate cleaved, so that dialkylphosphines are formed. The implementation of tetraorganodiphosphine isulfiden with hydrogen peroxide, on the other hand, leads to diorganodiphosphonic acids.

Mit Metallen, wie beispielsweise Kupfer, ließ sich nach den bisherigen Kenntnissen lediglich eine Desulfurierung von Tetraorganodiphosphindisulfiden erreichen, wobei neben Metallsulfiden Tetraorganodiphosphine als Reaktionsprodukte entstehen. Die P-P-Bindung der Tetraorganodiphosphindisulfide wird hierbei nicht gespalten. Metals, such as copper, followed the previous ones Knowledge can only achieve a desulfurization of tetraorganodiphosphine disulfides, whereby, in addition to metal sulfides, tetraorganodiphosphines are formed as reaction products. The P-P bond of the tetraorganodiphosphine disulfide is not split in this case.

Aus diesen bekannten Reaktionen konnte nicht geschlossen werden, daß Tetraalkyldiphosphindisulfide in Metallkomplexe von Dialkyldithiophosphinen übergeführt werden können. From these known reactions it could not be concluded that tetraalkyldiphosphine disulfides in metal complexes of dialkyldithiophosphines can be transferred.

Es wurde ein Verfahren zur Herstellung von Metallkomplexen der Dialkyldithiophosphine gefunden, nach dem Tetraalkyldiphosphindisulfide mit Arsen, Antimon, Wismut, Zink, Cadmium oder Quecksilber in Gegenwart von Schwefel in elementarer Form oder als Sulfid der genannten Metalle, wobei den genannten Metallsulfiden noch Schwefel zugesetzt werden kann, auf etwa 200 bis 250"C erwärmt werden. It became a process for the preparation of metal complexes of the dialkyldithiophosphines found, after the tetraalkyldiphosphine disulfide with arsenic, antimony, bismuth, zinc, Cadmium or mercury in the presence of sulfur in elemental form or as Sulphide of the metals mentioned, sulfur being added to the metal sulphides mentioned can be heated to about 200 to 250 "C.

Die Metallkomplexe der Dialkyldithiophosphine entstehen, wenn Tetraalkyldiphosphindisulfide mit den Metallen und Schwefel oder mit den Metallsulfiden vermischt langsam auf Temperaturen bis zu 250"C erhitzt werden. In manchen Fällen kann es auch vorteilhaft sein, neben dem Metallsulfid noch freien Schwefel in das Reaktionsgemisch einzubringen. Mit dem erfindungsgemäßen Verfahren werden Ausbeuten zwischen 60 und 900/o der Theorie erhalten. The metal complexes of the dialkyldithiophosphines are formed when tetraalkyldiphosphine disulfides slowly mixed with the metals and sulfur or with the metal sulfides Temperatures up to 250 "C can be heated. In some cases it can also be advantageous be to introduce free sulfur into the reaction mixture in addition to the metal sulfide. With the process according to the invention, yields between 60 and 900 / o of theory are achieved obtain.

Die erfindungsgemäß hergestellten Metallkomplexe der Dialkyldithiophosphine zeichnen sich durch Eigenschaften aus, die ihnen technischen Wert verleihen. The metal complexes of the dialkyldithiophosphines prepared according to the invention are characterized by properties that give them technical value.

Die Metallkomplexe sind in Wasser und in verdünnten Säuren unlöslich, dagegen lösen sie sich sehr leicht in fast allen organischen Lösungsmitteln. In Benzol und Tetrahydrofuran sind sie weder in der Kälte noch in der Siedehitze merklich dissoziiert. In einigen organischen Lösungsmitteln, wie beispielsweise Dimethylformamid, läßt sich eine geringe Dissoziation der erfindungsgemäß erzeugten Metallkomplexe durch Leitfähigkeitsmessungen feststellen. Die Leitfähigkeit einer 0,Olmolaren Lösung eines erfindungsgemäß hergestellten Metallkomplexes in Dimethylformamid beträgt etwa 2,6 10-5 Q-1 cm-1. Außerdem haben die Metallkomplexe einen scharfen Schmelzpunkt und können unzersetzt destilliert werden. Diese Eigenschaften zeigen, daß es sich bei den erfindungsgemäß hergestellten Metallkomplexen um innerkomplex gebundene Nichtelektrolyte handelt. Die Metallkomplexe sind teilweise in wäßrigen Alkalien löslich und können aus solchen Lösungen durch Zusatz von Säuren unverändert wieder ausgefällt werden. Sowohl im festen als auch im gelösten Zustand sind die Metallkomplexe, selbst bei Luftzutritt, unbegrenzt haltbar.The metal complexes are insoluble in water and in dilute acids, on the other hand, they dissolve very easily in almost all organic solvents. In Benzene and tetrahydrofuran are not noticeable either in the cold or in the boiling point dissociated. In some organic solvents, such as dimethylformamide, a slight dissociation of the metal complexes produced according to the invention can be observed determine by conductivity measurements. The conductivity of a 0.1 molar solution of a metal complex prepared according to the invention in dimethylformamide about 2.6 10-5 Ω-1 cm-1. In addition, the metal complexes have a sharp melting point and can be distilled without decomposition. These properties show that it is in the case of the metal complexes prepared according to the invention, bound by intrinsic complexes Non-electrolytes. Some of the metal complexes are in aqueous alkalis soluble and can be recovered unchanged from such solutions by adding acids be precipitated. Both in the solid and in the dissolved state are the metal complexes, even when exposed to air, it can be kept indefinitely.

Auf Grund dieser Eigenschaften und der verhältnismäßig beständigen Kombination der Elemente Phosphor und Schwefel- mit einem Metall in einer Verbindung lassen sich die erfindungsgemäß hergestellten Metallkomplexe für katalytische Zwecke, als Heizöladditiv, das eine rauchlose Verbrennung des Heizöls bewirkt, als Treibstoffzusatz, als Vulkanisationsbeschleuniger verwenden. Because of these properties and the relatively stable ones Combination of the elements phosphorus and sulfur with a metal in one compound permit the metal complexes prepared according to the invention for catalytic purposes, as Heating oil additive, which causes a smokeless combustion of the heating oil, as a fuel additive, Use as a vulcanization accelerator.

Beispiel 1 Antimonkomplex des Dipropyldith iophosphins [(C3H7)pPS2]3Sb Tetrapropyldiphosphindisulfid (1,5 Mol), Antimonpulver (1,0 Mol) und Schwefel (3,0 Mol) werden 2 Stunden auf etwa 200°C erwärmt. Das Reaktionsprodukt gibt nach Umkristallisation aus wenig Isobutanol obigen Komplex in Form orangegelber Kristalle, F. 148,5°C. Ausbeute 900/, der Theorie, bezogen auf Antimon. Example 1 Antimony complex of dipropyldithiophosphine [(C3H7) pPS2] 3Sb Tetrapropyl diphosphine disulfide (1.5 moles), antimony powder (1.0 moles) and sulfur (3.0 Mol) are heated to about 200 ° C for 2 hours. The reaction product gives after recrystallization from a little isobutanol the above complex in the form of orange-yellow crystals, mp 148.5 ° C. Yield 900 /, of theory, based on antimony.

Beispiel 2 Wismutkomplex des Dipropyldithiophosphins [(C3H7)2PS2]3Bi kann entsprechend Beispiel 1 hergestellt werden. Tiefgelbe Kristalle, F. 179"C, Ausbeute 900/0. Example 2 Bismuth complex of dipropyldithiophosphine [(C3H7) 2PS2] 3Bi can be produced according to example 1. Deep yellow crystals, F. 179 "C, Yield 900/0.

Beispiel 3 Arsenkomplex des Dipropyldithiophosphins [(C3H,)2PSj3As kann entsprechend Beispiel 1 hergestellt werden. Hellgelbe Kristalle, F. 128,5°C, Ausbeute etwa 750/o. Example 3 Arsenic complex of dipropyldithiophosphine [(C3H,) 2PSj3As can be produced according to example 1. Light yellow crystals, m.p. 128.5 ° C, Yield about 750 / o.

Beispiel 4 Zinkkomplex des Diamyldithiophosphins kC5H11)2PS22Zn Tetraamyldiphosphondisulfid (1 Mol), Zinkstaub (1 Mol) und Schwefel (2 Mol) werden 2 Stunden auf 2000 C erwärmt. Umkristallisation des Reaktionsprodukts aus Äthanol, Isobutanol oder Ligroin gibt den Komplex in etwa 750/o Ausbeute. Weiße Kristalle, F. 112,5°C. Example 4 Zinc complex of diamyldithiophosphine kC5H11) 2PS22Zn tetraamyldiphosphone disulfide (1 mol), zinc dust (1 mol) and sulfur (2 mol) are heated to 2000 C for 2 hours. Recrystallization of the reaction product from ethanol, isobutanol or ligroin gives the complex in about 750 / o yield. White crystals, m.p. 112.5 ° C.

Beispiel 5 Zinkkomplex des Dibutyldithiophosphins [(C4H9)2PS2]2Zn analog mit Tetrabutyldiphosphindisulfid. Farblose Kristalle, F. 110°C. Example 5 Zinc complex of dibutyldithiophosphine [(C4H9) 2PS2] 2Zn analogously with tetrabutyldiphosphine disulfide. Colorless crystals, m.p. 110 ° C.

Beispiel 6 Zinkkomplex des Diäthyldithiophosphins [(C2H5)2PS2]2Zn analog mit Tetraäthyldiphosphindisulfid. Farblose Kristalle, F. 164,5°C. Example 6 Zinc complex of diethyldithiophosphine [(C2H5) 2PS2] 2Zn analogously with tetraethyldiphosphine disulfide. Colorless crystals, mp 164.5 ° C.

Beispiel 7 Cadmiumkomplex des Diäthyldithiophosphins [(C4Hg)2PS2]2Cd analog mit Cadmiumpulver. Farblose Kristalle, F. Example 7 Cadmium complex of diethyldithiophosphine [(C4Hg) 2PS2] 2Cd analogous with cadmium powder. Colorless crystals, F.

167,5°C, Ausbeute etwa 700/o.167.5 ° C, yield about 700 / o.

Beispiel 8 Quecksilberk omplex des Dipropyldithiophosphins [(C3H7)2PSe]2Hg analog mit Quecksilbermetall. Farblose Kristalle, F. Example 8 Mercury complex of dipropyldithiophosphine [(C3H7) 2PSe] 2Hg analogous with mercury metal. Colorless crystals, F.

167,5°C, Ausbeute 70%.167.5 ° C, yield 70%.

Beispiel 9 Cadmiumkomplex des Dipropyldithiophosphins [(C3H7)2PS2]2Cd Tetrapropyldiphosphindisulfud (1 Mol) wird mit Cadmiumsulfid (1 Mol) und Schwefel (1Mol) während 4 Stunden in Ligroin unter Stickstoff auf 200°C erwärmt. Die heiße Reaktionslösung wurde filtriert. Example 9 Cadmium complex of dipropyldithiophosphine [(C3H7) 2PS2] 2Cd Tetrapropyldiphosphine disulfide (1 mole) is made with cadmium sulfide (1 mole) and sulfur (1 mol) heated in ligroin under nitrogen to 200 ° C for 4 hours. The hot one Reaction solution was filtered.

Aus dem Filtrat wurde der Komplex in etwa 400/o Ausbeute in Form weißer Kristalle, F. 184° C, erhalten.From the filtrate, the complex became whiter in a yield of about 400% Crystals, mp 184 ° C, obtained.

Beispiel 10 Zinkkomplex des Dipropyldithiophosphins [(C3H7)2PS2j2Zn Tetrapropyldiphosphindisulfid (1 Mol) wird mit Zinkstaub (2 Mol) unter Stickstoff auf etwa 250°C erwärmt. Bei der Destillation des Reaktionsprodukts im Wasserstrahlvakuum wurde bei 245 bis 250°C der Komplex als farbloses, viskoses Destillat erhalten, das beim Abkühlen zu einer kristallinen Masse erstarrte. Example 10 Zinc complex of dipropyldithiophosphine [(C3H7) 2PS2j2Zn Tetrapropyl diphosphine disulfide (1 mole) is made with zinc dust (2 moles) under nitrogen heated to about 250 ° C. During the distillation of the reaction product in a water jet vacuum the complex was obtained as a colorless, viscous distillate at 245 to 250 ° C, which solidified to a crystalline mass on cooling.

Umkristallisation aus Ligroin gab die Verbindung in Form farbloser, glänzender Kristalle, F. 159°C. Ausbeute etwa 35°lo.Recrystallization from ligroin gave the compound in the form of colorless, shiny crystals, m.p. 159 ° C. Yield about 35 ° lo.

Um die Eignung der erfindungsgemäß herstellbaren Verbindungen als Vulkanisationsbeschleuniger zu demonstrieren, werden 5 Gewichtsteile Zinkoxyd und 2,5 Gewichtsteile Schwefel in 100 Gewichtsteilen Naturkautschuk (sheets) verteilt. In order to determine the suitability of the compounds which can be prepared according to the invention as To demonstrate vulcanization accelerators, 5 parts by weight of zinc oxide and 2.5 parts by weight of sulfur distributed in 100 parts by weight of natural rubber (sheets).

Der Hälfte der so erhaltenen Mischung wurden noch 1,0 Gewichtsteil des Zinksalzes der Diäthyldithiocarbaminsäure und 0,2 Gewichtsteile Dibenzothiazyldisulfid zugesetzt und das Gemisch vulkanisiert (Produkt I). Half of the mixture thus obtained was still 1.0 part by weight of the zinc salt of diethyldithiocarbamic acid and 0.2 part by weight of dibenzothiazyl disulfide added and the mixture vulcanized (product I).

In die andere Hälfte der Ausgangsmischung wurden 1,0 Gewichtsteil des erfindungsgemäß hergestellten Zinkkomplexes des Diäthyldithiophosphins und 0,2 Gewichtsteile Dibenzothiazyldisulfid eingearbeitet und das Gemisch vulkanisiert (Produkt II). 1.0 part by weight was added to the other half of the starting mixture of the zinc complex of diethyldithiophosphine prepared according to the invention and 0.2 Parts by weight of dibenzothiazyl disulfide incorporated and the mixture vulcanized (Product II).

Die Prüfung beider Produkte auf ihre mechanischen Eigenschaften hatte folgende Ergebnisse: Geprüfte Eigenschaften Produkt I Produkt II Zerreißfestigkeit, kg/cm2.. 91 124 Dehnung, °/0 .......... 765 975 Modul 3000/0, kg/cm2 . . . 10 9 Shore Härte ............. 32 30 Elastizität, %........... 70 68 Diese Ergebnisse zeigen, daß der erfindungsgemäß hergestellte Zinkkomplex als Vulkanisationsbeschleuniger genauso gut geeignet ist wie das für diesen Zweck bekannte Zinksalz der Diäthyldithiocarbaminsäure.The test of both products for their mechanical properties had the following results: Tested properties Product I Product II Tensile strength, kg / cm2 .. 91 124 Elongation, ° / 0 .......... 765 975 Module 3000/0, kg / cm2. . . 10 9 Shore hardness ............. 32 30 Elasticity,% ........... 70 68 These results show that the zinc complex prepared according to the invention is just as suitable as a vulcanization accelerator as the zinc salt of diethyldithiocarbamic acid known for this purpose.

Claims (1)

Patentanspruch: Verfahren zur Herstellung von Metallkomplexen der Dialkyldithiophosphine, d a d u r c h g e -k e n n z e i c h n e t, daß Tetraalkyldiphosphindisulfide mit Arsen, Antimon, Wismut, Zink, Cadmium oder Quecksilber in Gegenwart von Schwefel in elementarer Form oder als Sulfid der genannten Metalle, wobei den genannten Metallsulfiden noch Schwefel zugesetzt werden kann, auf etwa 200 bis 250"C erwärmt werden. Claim: Process for the production of metal complexes of the Dialkyldithiophosphines, d a d u r c h e -k e n n n z e i c h n e t, that tetraalkyldiphosphine disulphides with Arsenic, antimony, bismuth, zinc, cadmium or mercury in the presence of sulfur in elemental form or as a sulfide of the metals mentioned, the metal sulfides mentioned nor sulfur can be added, can be heated to about 200 to 250.degree. In Betracht gezogene Druckschriften: Deutsche Auslegeschriften Nr. 1 054453, 1 014 989; britische Patentschrift Nr. 859 373; USA.-Patentschriften Nr. 2 727 067, 2 809 979, 2929828; Angewandte Chemie, 69, 1957, S. 307, 308; 71, 1959, S. 162, und 72, 1960, S. 210; Chemische Berichte, 90, 1957, S. 1656 bis 1660; 92, 1959, S. 227 bis 231 und 704 und 93, 1960, S. 861; Journal of the Chemical Society, 1953, S. 1565 bis 1571. Publications considered: German Auslegeschriften No. 1,054,453, 1,014,989; British Patent No. 859,373; U.S. Patent No. 2,727,067, 2,809,979, 2929828; Angewandte Chemie, 69, 1957, pp. 307, 308; 71, 1959, P. 162, and 72, 1960, p. 210; Chemical Reports, 90, 1957, pp. 1656 to 1660; 92, 1959, pp. 227 to 231 and 704 and 93, 1960, p. 861; Journal of the Chemical Society, 1953, pp. 1565 to 1571. In Betracht gezogenes älteres Patent: Deutsches Patent Nr. 1149 355. Earlier patent considered: German Patent No. 1149 355.
DEC21151A 1960-04-07 1960-04-07 Process for the preparation of metal complexes of dialkyldithiophosphines Pending DE1166191B (en)

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Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2727067A (en) * 1954-01-26 1955-12-13 Lubrizol Corp Preparation of phosphinodithioic acid anhydrides by heating the corresponding acids
DE1014989B (en) * 1954-01-26 1957-09-05 Lubrizol Corp Process for the production of aromatic dithiophosphinic acids or their salts
US2809979A (en) * 1954-01-26 1957-10-15 Lubrizol Corp Organic phosphinodithioic compounds and methods for preparing same
DE1054453B (en) * 1958-02-12 1959-04-09 Bayer Ag Process for the production of dialkyl thionophosphinic acid halides
US2929828A (en) * 1955-09-28 1960-03-22 Exxon Research Engineering Co Lubricant additives
GB859373A (en) * 1957-12-21 1961-01-18 Koppers Co Inc Process for the preparation of organophosphines
DE1149355B (en) 1958-04-17 1963-05-30 Koppers Co Inc Process for the production of organic diphosphines, phosphines or their metal compounds

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2727067A (en) * 1954-01-26 1955-12-13 Lubrizol Corp Preparation of phosphinodithioic acid anhydrides by heating the corresponding acids
DE1014989B (en) * 1954-01-26 1957-09-05 Lubrizol Corp Process for the production of aromatic dithiophosphinic acids or their salts
US2809979A (en) * 1954-01-26 1957-10-15 Lubrizol Corp Organic phosphinodithioic compounds and methods for preparing same
US2929828A (en) * 1955-09-28 1960-03-22 Exxon Research Engineering Co Lubricant additives
GB859373A (en) * 1957-12-21 1961-01-18 Koppers Co Inc Process for the preparation of organophosphines
DE1054453B (en) * 1958-02-12 1959-04-09 Bayer Ag Process for the production of dialkyl thionophosphinic acid halides
DE1149355B (en) 1958-04-17 1963-05-30 Koppers Co Inc Process for the production of organic diphosphines, phosphines or their metal compounds

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