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GB971170A - Process for producing dimers and polymers of acetylenic compounds - Google Patents

Process for producing dimers and polymers of acetylenic compounds

Info

Publication number
GB971170A
GB971170A GB11739/61A GB1173961A GB971170A GB 971170 A GB971170 A GB 971170A GB 11739/61 A GB11739/61 A GB 11739/61A GB 1173961 A GB1173961 A GB 1173961A GB 971170 A GB971170 A GB 971170A
Authority
GB
United Kingdom
Prior art keywords
acetylenic
cuprous salt
amines
butyne
oxygen
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.)
Expired
Application number
GB11739/61A
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.)
General Electric Co
Original Assignee
General Electric Co
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 General Electric Co filed Critical General Electric Co
Publication of GB971170A publication Critical patent/GB971170A/en
Expired legal-status Critical Current

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Classifications

    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08FMACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F38/00Homopolymers and copolymers of compounds having one or more carbon-to-carbon triple bonds
    • 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
    • B01J31/18Catalysts comprising hydrides, coordination complexes or organic compounds containing coordination complexes containing nitrogen, phosphorus, arsenic or antimony as complexing atoms, e.g. in pyridine ligands, or in resonance therewith, e.g. in isocyanide ligands C=N-R or as complexed central atoms
    • B01J31/1805Catalysts comprising hydrides, coordination complexes or organic compounds containing coordination complexes containing nitrogen, phosphorus, arsenic or antimony as complexing atoms, e.g. in pyridine ligands, or in resonance therewith, e.g. in isocyanide ligands C=N-R or as complexed central atoms the ligands containing nitrogen
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2/00Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms
    • C07C2/02Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by addition between unsaturated hydrocarbons
    • C07C2/04Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by addition between unsaturated hydrocarbons by oligomerisation of well-defined unsaturated hydrocarbons without ring formation
    • C07C2/38Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by addition between unsaturated hydrocarbons by oligomerisation of well-defined unsaturated hydrocarbons without ring formation of dienes or alkynes
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2/00Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms
    • C07C2/76Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen
    • C07C2/82Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen oxidative coupling
    • C07C2/84Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen oxidative coupling catalytic
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C403/00Derivatives of cyclohexane or of a cyclohexene or of cyclohexadiene, having a side-chain containing an acyclic unsaturated part of at least four carbon atoms, this part being directly attached to the cyclohexane or cyclohexene or cyclohexadiene rings, e.g. vitamin A, beta-carotene, beta-ionone
    • C07C403/24Derivatives of cyclohexane or of a cyclohexene or of cyclohexadiene, having a side-chain containing an acyclic unsaturated part of at least four carbon atoms, this part being directly attached to the cyclohexane or cyclohexene or cyclohexadiene rings, e.g. vitamin A, beta-carotene, beta-ionone having side-chains substituted by six-membered non-aromatic rings, e.g. beta-carotene
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08FMACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F4/00Polymerisation catalysts
    • C08F4/06Metallic compounds other than hydrides and other than metallo-organic compounds; Boron halide or aluminium halide complexes with organic compounds containing oxygen
    • C08F4/10Metallic compounds other than hydrides and other than metallo-organic compounds; Boron halide or aluminium halide complexes with organic compounds containing oxygen of alkaline earth metals, zinc, cadmium, mercury, copper or silver
    • 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
    • B01J2531/10Complexes comprising metals of Group I (IA or IB) as the central metal
    • B01J2531/16Copper
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2527/00Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
    • C07C2527/06Halogens; Compounds thereof
    • C07C2527/122Compounds comprising a halogen and copper
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2531/00Catalysts comprising hydrides, coordination complexes or organic compounds
    • C07C2531/02Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Health & Medical Sciences (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Inorganic Chemistry (AREA)
  • Addition Polymer Or Copolymer, Post-Treatments, Or Chemical Modifications (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Catalysts (AREA)

Abstract

Carbon is obtained by igniting a film of a polymeric, polyacetylenic compound obtained by oxidizing a compound containing at least two terminal acetylenic groups (-CC­H) (see Division C3). In a preferred embodiment the polymer is derived from meta-diethynyl benzene; the polymer is dissolved in chlorobenzene, nitrobenzene or tetrachlorethane and cast on a glass plate and the solvent evaporated. The film decomposes above 180 DEG C. to leave a coherent carbon film.ALSO:Compounds containing two conjugated acetylenic linkages are obtained by reacting a compound containing a terminal acetylenic group (-C­CH) with oxygen in the presence of a solution of a cuprous salt-tertiary amine complex, said cuprous salt being one for which a corresponding cupric salt exists. The acetylenic group may be attached to an aliphatic or aromatic radical which may contain as substituents, halogen, -OH, -OR, -OCOR, -COOR, -COR, -CONH2, -CONHR, -CONR2, -CH, -SH, -SR, -SSH, -SSR, -SOR, -NO2, -SO2R, -NH2, -NHR or -NR2 e.g. 5-fluoro-1-pentyne, 3-chloro-3-phenylpropyne, 3-bromopropyne, 3-chloro-1-butyne, ethynylpyridines, 3-butyne-1-ol, 2-propyne-1-ol, N-propynyl-aniline, propiolic acetate, propiolic amide, propiolophenone, 2-propynylamine, N,N-dimethylpropynylamine 2-propynyl sulphide, methyl-3-butynoate, 3-butyne-2-ol, 3-butyne-2-one, parabromophenylacetylene, nitrophenyl-acetylene and 1-ethynyl-cyclohexanol. The cuprous salt is preferably the chloride but others are specified and many tertiary amines are specified including heterocyclic amines and di-tertiary amines; preferably N-aryl amines are not used. Excess amine may be used to dissolve the complex and other solvents may be present, e.g. alcohols, ketones, hydrocarbons, chlorohydrocarbons, nitrohydrocarbons, ethers, esters, amides, ether esters or sulphoxides. Oxygen is bubbled into the mixture as such or diluted with nitrogen, helium or argon or as air. The reaction mixture is cooled if necessary to prevent the temperature rising above 100 DEG C. and the reaction is terminated by addition of an acid by pouring into a non-solvent for the product or by adding a copper chelating agent.ALSO:Polymeric polyacetylenic compounds are obtained by reacting acetylene or a compound containing two or more terminal acetylenic groups (-C==CH) with oxygen in the presence of a cuprous salt-tertiary amine complex, the cuprous salt being one for which a corresponding cupric salt exists. The products are linear polymers formed for example according to the equation: [-C==C-R-C==C-]n <FORM:0971170/C3/1> where n is usually at least 10 and probably at least 50. Compounds containing two terminal acetylenic groups are preferred, compounds with one such group being added as a chain stopper if required; compounds with three or more acetylenic groups yield three-dimensional, cross-linked, insoluble, infusible polymers. The radical to which the acetylenic groups are attached may be aliphatic or aromatic, hydrocarbon or substituted hydrocarbon, e.g. 1,4-pentadiyne, 1,5-hexadiyne, 1,6-heptadiyne, 1,7-octadiyne, 1,8-nonadiyne 1,11-dodecadiyne, o-, m-, or p-diethynyl benzene, or diethynyl naphthalenes, anthracenes, pyridines or pyrimidines. The polymers and copolymers obtained from m-diethynyl benzene are soluble in chlorobenzene, nitrobenzene, or tetrachloroethane above 100 DEG C. and can be cast, e.g. on glass, to produce tough transparent films stable up to 180 DEG C. The cuprous salt is preferably the chloride but others are specified and many tertiary amines are specified including heterocyclic amines and di-tertiary amines; preferably N-aryl amines are not used. Excess amine may be used to dissolve the complex and other solvents may be present, e.g. alcohols, ketones, hydrocarbons, chlorohydrocarbons, nitrohydrocarbons, ethers, esters, amides, ether esters or sulphoxides. Oxygen is bubbled through the mixture as such or diluted with nitrogen, helium or argon or as air. The reaction mixture is cooled to prevent the temperature rising above 100 DEG C. and the reaction is terminated by adding an acid, by pouring into a non-solvent for the product or by adding a copper chelating agent.ALSO:Compounds containing two conjugated acetylenic linkages are obtained by reacting a compound containing a terminal acetylenic group (-C ­ CH) with oxygen in the presence of a solution of a cuprous salt-tertiary amine complex, said cuprous salt being one for which a corresponding cupric salt exists. The acetylenic group may be attached to an aliphatic or aromatic radical e.g. acetylene, propyne, 1-butyne, 3-methyl-1-butyne, 3-phenylpropyne, 1 - pentyne, 3 - ethyl - 3 - methyl - 1 - pentyne, 1 - dodecyne, 1 - octadecyne, phenylacetylene, ethynylnaphthalenes, ethynylanthracenes. The cuprous salt is preferably the chloride but others are specified and many tertiary amines are specified including heterocyclic amines and di-tertiary amines; preferably N-aryl amines are not used. Excess amine may be used to dissolve the complex and other solvents may be present, e.g. alcohols, ketones, hydrocarbons, chlorohydrocarbons, nitrohydrocarbons, ethers, esters, amides, ether esters or sulphoxides. Oxygen is bubbled into the mixture as such or diluted with nitrogen, helium or argon or as air. The reaction mixture is cooled if necessary to prevent the temperature rising above 100 DEG C. and the reaction is terminated by addition of an acid by pouring into a non-solvent for the product or by adding a copper chelating agent.ALSO:Clear, tough coatings on glass are obtained by casting a solution of a polyacetylenic compound containing meta-diethynyl benzene groups with or without para-diethynyl benzene or diethynyl alkane groups, i.e. containing the recurring structure [-C­C-R-C­C-]n, and evaporating the solvent. On heating above 180 DEG C. the film is converted to a coherent coating of carbon.
GB11739/61A 1960-04-01 1961-03-30 Process for producing dimers and polymers of acetylenic compounds Expired GB971170A (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
US1918660A 1960-04-01 1960-04-01

Publications (1)

Publication Number Publication Date
GB971170A true GB971170A (en) 1964-09-30

Family

ID=21791877

Family Applications (1)

Application Number Title Priority Date Filing Date
GB11739/61A Expired GB971170A (en) 1960-04-01 1961-03-30 Process for producing dimers and polymers of acetylenic compounds

Country Status (2)

Country Link
DE (1) DE1158272B (en)
GB (1) GB971170A (en)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3993711A (en) * 1975-03-19 1976-11-23 Hercules Incorporated Carboxylated poly(arylacetylenes)
US4255535A (en) 1974-12-30 1981-03-10 Allied Chemical Corporation Organic polymers with near-zero uniaxial thermal expansion coefficients

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3617365A (en) * 1969-03-25 1971-11-02 American Can Co Composite coated with acetylene-oxygen polymers

Family Cites Families (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR733663A (en) * 1931-06-19 1932-10-10 Du Pont Improvements to acetylene reactions
FR829617A (en) * 1936-11-21 1938-07-01 Ig Farbenindustrie Ag Process for the preparation of acyclic polymers of acetylene and catalysts suitable for carrying out this process

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4255535A (en) 1974-12-30 1981-03-10 Allied Chemical Corporation Organic polymers with near-zero uniaxial thermal expansion coefficients
US3993711A (en) * 1975-03-19 1976-11-23 Hercules Incorporated Carboxylated poly(arylacetylenes)

Also Published As

Publication number Publication date
DE1158272B (en) 1963-11-28

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