US3849473A - Diesters of 1,3-bis(carboxymethyl)adamantanes and process for preparing same - Google Patents

Diesters of 1,3-bis(carboxymethyl)adamantanes and process for preparing same Download PDF

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Publication number
US3849473A
US3849473A US00156114A US15611471A US3849473A US 3849473 A US3849473 A US 3849473A US 00156114 A US00156114 A US 00156114A US 15611471 A US15611471 A US 15611471A US 3849473 A US3849473 A US 3849473A
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Prior art keywords
adamantane
bis
parts
carboxymethyl
calculated
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US00156114A
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English (en)
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H Takenaka
Y Kimura
Y Inamoto
H Nakayama
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Kao Corp
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Kao Corp
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C69/00Esters of carboxylic acids; Esters of carbonic or haloformic acids
    • C07C69/608Esters of carboxylic acids having a carboxyl group bound to an acyclic carbon atom and having a ring other than a six-membered aromatic ring in the acid moiety
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M105/00Lubricating compositions characterised by the base-material being a non-macromolecular organic compound
    • C10M105/08Lubricating compositions characterised by the base-material being a non-macromolecular organic compound containing oxygen
    • C10M105/32Esters
    • C10M105/36Esters of polycarboxylic acids
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2603/00Systems containing at least three condensed rings
    • C07C2603/02Ortho- or ortho- and peri-condensed systems
    • C07C2603/04Ortho- or ortho- and peri-condensed systems containing three rings
    • C07C2603/22Ortho- or ortho- and peri-condensed systems containing three rings containing only six-membered rings
    • C07C2603/26Phenanthrenes; Hydrogenated phenanthrenes

Definitions

  • a compound of the formula ca cooa wherein R is selected from the group of hydrocarbon radicals having 4 to 20 carbon atoms consisting of (a) linear and branched-chain alkyls and alkenyls, and (b) monocyclic and polycyclic cycloalkyls and cycloalkenyls; and R is H or alkyl having 1 to 4 carbon atoms.
  • the compound is prepared by reacting l,3-bis(carboxymethyl)adamantane, or its 5,7-alkyl derivatives, with a monohydric alcohol (ROH) in the presence of esterification catalyst.
  • ROH monohydric alcohol
  • This invention relates to diesters of l,3-bis(carboxymethyladamantanes and a process for preparing same. More precisely, it relates to a process for preparing diesters of 1,3-bis(carboxymethyl)adamantane with higher alcohols having from 4 to 20 carbon atoms.
  • a compound according to the invention has the formula l CH CQOR wherein R is selected from the group of univalent hydrocarbon radicals having 4 to 20 carbon atoms consisting of (a) linear and branched-chain alkyls and alkenyls, and (b) monocyclic and polycyclic cycloalkyls and cycloalkenyls; and R is H or alkyl having 1 to 4 carbon atoms.
  • the present inventors found that l,3-bis(carboxymethyl)adamantane and its derivatives with alkyl substituents in the adamantane ring can be esterified readily with higher alcohols.
  • the present invention provides a process for manufacturing diesters of 1,3-bis(carboxyrnethyl)adamantane or its ring-substituted alkyl derivatives by esterifying the said adamantane compound with a monohydric alcohol having from 4 to 20 carbon atoms selected from the group consisting of aliphatic alkanols and alkenols with a linear or branched structure and cycloaliphatic alkanols and alkenols with monoor poly-cyclic structure and in the presence of acidic, neutral or alkaline catalyst.
  • the diesters of l,3-bis(carboxymethyl)adamantane compounds thus obtained are novel substances that have not been synthesized before.
  • novel diesters have high heat stabilities and many other unsual properties that are not seen in ordinary aliphatic esters, e.g., low viscosities and high viscosity indiees, which are the result of the presence of the adamantane ring, they are very useful, for instance, as oiling agents for synthetic fibers and synthetic lubricating oil bases, particularly for aviation engines.
  • the products of this invention are obtained by heating and dehydrating a mixture of 1,3-bis(carboxymethyl)ada mantane, or its ring-substituted alkyl derivatives, and one of the above-described alcohols, in the presence of the catalyst.
  • the reactivities of the two carbonyl groups in the l,3-bis(carboxymethyl)adamantane compounds in the said esterification reactions are the same, thus indicating that the two carboxyl groups are separated far enough to be electronically as Well as sterically independent of each other. Therefore, it is unnecessary to provide different reaction conditions between the first and the second esterifications, and diesterification can be carried out smoothly in one and the same reaction.
  • the presence of alkyl substituents in the adamantane ring does not affect the reactivity of the carboxyl groups, and, therefore the reaction conditions do not need to be altered substantially, depending on the presence or absence of alkyl substituents in the adamantane ring.
  • the catalyst which can be used effectively for the esterification reaction of this invention includes all the substances that are known as so-called esterification catalysts, for example, acid catalysts such as sulfuric acid, aliphatic and aromatic sulfonic acids, and boron trifiuoride, and neutral or alkaline catalysts such as oxides or hydroxides of alkali metals, alkali earth metals, zinc, cadmium, tin, lead, antimony and bismuth.
  • esterification catalysts for example, acid catalysts such as sulfuric acid, aliphatic and aromatic sulfonic acids, and boron trifiuoride
  • neutral or alkaline catalysts such as oxides or hydroxides of alkali metals, alkali earth metals, zinc, cadmium, tin, lead, antimony and bismuth.
  • ring-substituted alkyl derivatives of 1,3-bis(carboXymethyDadamantane there are exemplified 5-methyl-, 5,7-dimethyl-, 5- methyl-7-ethyl-, and S-ethyl-substituted adamantanes.
  • linear alkanols such as nbutyl alcohol, n-amyl alcohol, n-hexyl alcohol, n-octyl alcohol, lauryl alcohol, myristyl alcohol, cetyl alcohol, and stearyl alcohol, branched alkanols such as i-butyl alcohol, i-amyl alcohol, Z-ethylhexanol-l, and 2-methyldodecanol-l, linear alkenols such as crotyl alcohol, oleyl alcohol and linoleyl alcohol, branched alkenols such as methallyl alcohol, monocyclic saturated alcohols such as cyclohexanol, methylcyclohexanols, and cyclohexylcarbinol, monocyclic unsaturated alcohols such as 2-cyclohexenol, polycyclic saturated alcohols such as Z
  • the esterification reaction it is generally advantageous to use either said dicarboxylic acid component (1,3-bis(carboxylmethyl)adamantane) or said alcohol component in excess from the viewpoint of obtaining a shorter reaction time, but the reaction can be of course completed smoothly with the use of substantially stoichiometric amounts of each component.
  • the amount of the catalyst used for this esterification reaction is in the range of 0.0002-0.2 mol, preferably 0.001-0.01 .mol for each mol of the dicarboxylic acid component. When the adequate kind and amount of catalyst is selected and used as described above, the esterification reaction of this invention can be completed within 15 hours.
  • the reaction temperature in this reaction is not substantially different from those used in the esterification of aliphatic carboxylic acids generally; that is, the temperature is in the range from 30 to 300 C., preferably from 50 to 260 C.
  • any known means such as distillation under atmospheric or reduced pressure, removal by passing an inert gas through the reaction mixture, and removal by an azeotropic distillation. But it is most convenient to carry out azeotropic distillation using cyclohexane, benzene, toluene, or xylene, considering the highly sublimable property of the adamantane compounds. Indeed the loss of adamantane compounds due to sublimation causes a major problem when an excess of adamantane acids is used to esterify high boiling point alcohols.
  • Mass spectrum (m/e, relative intensity): 364 (10.0) (parent peak), 309 (11.6), 291 (18.7), 262 (18.4), 249 (100.0), 206 (24.3), 192 (81.8), 175 (25.0), 169 (12.2), 162 (11.4), l47(27.9), 133 (46.2).
  • Acetyl value Observed, 0.2; calculated, 0.
  • Acetyl value Found, 0.30; calculated, 0.
  • Mass spectrum (m/e, relative intensity): 416 (1.1) (parent peak), 335 (1.5), 334 (1.8), 317 (2.0), 275 (118), 253 (51.8), 252 (12.9), 235 (34.9), 234 (22.0), 206 (31.9), 193 (100.0), 175 (4.8), 147 (9.0).
  • NMR spectrum (CCl; solution, I MS as internal stand- R is selected from the group consisting of crotyl, oleyl, ard, r): linoleyl and methallyl, and
  • v R is H or alkyl having 1 to 4 carbon atoms. 5.3-5.6 (undissolved resonance, 2H): :2, A compound of the formula p v I a 5 1 cu cooa -Q v 1 5 4 E Y I cs cook wherein g R is selected from the group consisting of cyclohexyl, methylcyclohexyl, hexahydrobenzyl, cyclohexeny], p 111, Peaks at 843, -9 (4&1) decalyl, adamantyl, exo-trimethylene norbornyl and 7.96 (s) 2,3-dihydro-exo-dicyclopentadienyl, and

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • Emergency Medicine (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Low-Molecular Organic Synthesis Reactions Using Catalysts (AREA)
  • Lubricants (AREA)
US00156114A 1970-06-24 1971-06-23 Diesters of 1,3-bis(carboxymethyl)adamantanes and process for preparing same Expired - Lifetime US3849473A (en)

Applications Claiming Priority (1)

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JP45054979A JPS4911226B1 (enrdf_load_stackoverflow) 1970-06-24 1970-06-24

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Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3962105A (en) * 1975-03-25 1976-06-08 The Lubrizol Corporation Lubricating compositions
US4707301A (en) * 1986-07-11 1987-11-17 The Lubrizol Corporation Norbornyl dimer ester and polyester additives for lubricants and fuels
US4729840A (en) * 1986-07-11 1988-03-08 The Lubrizol Corporation Lubricant and fuel additives derived from O,O-dialkyldithiophosphoric acid and a norbornyl reactant
US5318711A (en) * 1993-01-21 1994-06-07 Quaker Chemical Corporation Method for lubricating metal-metal contact systems in metalworking operations with cyclohexyl esters
US5334228A (en) * 1993-10-18 1994-08-02 Mobil Oil Corporation Deposit control additives and fuel compositions containing the same
US5397488A (en) * 1993-12-09 1995-03-14 Mobil Oil Corporation Oxidatively stable esters derived from diamondoids totally hydroxylated at the bridgeheads

Cited By (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3962105A (en) * 1975-03-25 1976-06-08 The Lubrizol Corporation Lubricating compositions
US4707301A (en) * 1986-07-11 1987-11-17 The Lubrizol Corporation Norbornyl dimer ester and polyester additives for lubricants and fuels
US4729840A (en) * 1986-07-11 1988-03-08 The Lubrizol Corporation Lubricant and fuel additives derived from O,O-dialkyldithiophosphoric acid and a norbornyl reactant
US4753662A (en) * 1986-07-11 1988-06-28 The Lubrizol Corporation Norbornyl dimer ester and polyester additives for lubricants and fuels
US5318711A (en) * 1993-01-21 1994-06-07 Quaker Chemical Corporation Method for lubricating metal-metal contact systems in metalworking operations with cyclohexyl esters
US5334228A (en) * 1993-10-18 1994-08-02 Mobil Oil Corporation Deposit control additives and fuel compositions containing the same
WO1995011286A1 (en) * 1993-10-18 1995-04-27 Mobil Oil Corporation Deposit control additives and fuel compositions containing the same
US5397488A (en) * 1993-12-09 1995-03-14 Mobil Oil Corporation Oxidatively stable esters derived from diamondoids totally hydroxylated at the bridgeheads

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Publication number Publication date
JPS4911226B1 (enrdf_load_stackoverflow) 1974-03-15

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