Patented Aug. 7, 1951 2,563,609

UNITED STATES‘ PATENT OFFICE 2,563,609 LUBRICATIN G OIL ADDITIVES Alfred H. Matusxak, Westlield, N. 1., assignor to Standard Oil Development Company, a corpo ration of Delaware No Drawing. Application January 28, 1949, Serial No. 73,445 3 Claims. (Cl. 252—56) 1 2 This invention relates to rust preventing oil acid chloride or of the desired carboxylic compositions and more particularly to mineral acid may be employed instead of the carboxylic lubricating oil compositions which tend to in acid in well-known esteri?cation processes to hibit rusting and corrosion of metal parts which produce the mixed of this in are exposed to moisture. vention. A primary object of the present invention is Where the polyhydroxy is a diol, the the preparation of compositions which may be resulting mixed carbonate ester is formed by employed as internal combustion engine lubri esteri?cation of the diol either partially or com cants and which will also serve for the protection pletely with a derivative of a mono of exposed surfaces of such engines when the 10 hydroxy alcohol, employing well-known esteri same are not in use. When operating engines in ?cation methods. Where the hydroxyl groups of climates having a high humidity, rusting begins the diol are only partially esteri?ed in preparing within a vary short period of time alter the the mixed carbonate ester, the residual or free engine is shut down. The compositions of the hydroxyl group may be converted to an ester present invention are particularly valuable in 15 linkage by esteri?cation with a desired car preventing such rusting, and they are valuable boxylic acid or a derivative thereof. not only in the lubrication of internal combustion Where the polyhydroxy alcohol contains more engines but with oil bases of suitable viscosity than two hydroxyl groups, the polyhydroxy alco they may be employed as turbine oils or as hol may be partially or completely esteri?ed with lubricants for ?re arms, ordnance equipment, 20 a carbonic acid derivative of a monohydroxy industrial machinery, etc., and with more vola alcohol. The resulting mixed carbonate ester tile oil bases and in combination with fatty sub must contain at least one carbonic acid radical stances they may be applied to form protective and may contain one or more carboxylic acid coatings for metal surfaces which are exposed radicals. Where an ester-carbonate is desired, it to humid air. 25 is generally preferable to ?rst partially esteriiy The corrosion-preventing compositions of the the polyhydroxy alcohol with the desired car present invention are formed by adding to a boxylic acid, as this will generally produce a suitable oil base a mixed carbonate ester of a liquid product which can be conveniently handled monohydroxy alcohol and a polyhydric alcohol in the subsequent esteri?cation with the carbonic wherein the monohydroxy alcohol portion of the 30 acid derivative of a monohydroxy alcohol. It mixed carbonate ester consists of a saturated will be understood that in the preparation of the or unsaturated alkyl or cycloalkyl radical and mixed carbonate esters of this invention the car the polyhydroxy alcohol portion of the carbonate bonic acid derivative employed may consist 01' a consists of a radical selected from the class of mixture such as that which may be obtained containing at least two hydroxyl groups 35 by physically combining several pure carbonic and where the functional groups in the poly- ’ acid derivatives or that which may be obtained hydrlc alcohol portion may be partially or com by employing a mixture of monohydroxy alco pletely converted to other polar linkages such hols in the preparation of the carbonic acid as ester, , or amide linkages when the pres derivative reactant. It will be further under ence of such linkages might impart certain de 40 stood that where an ester-carbonate is desired, sired properties to the mixed carbonate ester. one or more than one carboxylic acids or deriva Where the mixed carbonate ester of this inven~ tives thereof- may be employed. In the prepara tion contains one or more free hydroxyl groups tion of these esters it is preferred to employ in the polyhydroxy alcohol portion of the car monocarboxylic acids. However, dicarboxylic bonate, it is preferred in this invention to have 45 acids may be ‘employed instead of, or along with, at least one of these free hydroxyl groups esteri the monocarboxylic acids. In the latter case, ?ed with a carboxylic acid. Such a mixed car dicarboxylic acids containing 0 to 8 carbon atoms bonate ester wherein at least one free hydroxyl in the chain between the two carboxyl groups are group has been converted to an ester group may preferred. Where dicarboxylic acids are em be called an ester-carbonate and such an ester 60 ployed, normal esteri?cation, linear esteri?ca carbonate may be formed by esterifying at least tion or cross linkage esteri?cation may occur. one hydroxyl group of the polyhydroxy alcohol In the preparation of the mixed carbonate with a carbonic acid derivative of a monohy esters of the present invention any carbonic acid droxy alcohol and esteriiying at least one hy derivative of a monohydroxy alcohol or mixture droxyl group of the polyhydroxy alcohol with a 55 of monohydroxy alcohols and any polyhydroxy carboxylic acid. In many cases, the anhydride, alcohol may be employed. The carbonic acid 2,563,009‘ 3 a 4 derivatives of monohydroxy alcohols which are stearic, oleic, linoleic, ricinoleic, eleomargic, to be employed in the preparation of the mixed eruclc, behenic, arachidic, lignoceric and similar carbonate esters of this invention include any‘ fatty acids, also the naphthenic acids, as well as carbonic acid derivative of a monohydroxy alco carboxylic acids derived by the oxidation of hol containing a saturated or'unsaturated ali petroleum products or by the oxidation of alde phatic or cycloaliphatic hydrocarbon chain of. 1 hydes such as those produced in the 0x0 process. to 30 carbon atoms per molecule. The preferred Naturally occurring products containing any of number of carbon atoms in the monohydroxy the above or similar acids, such as talloil, castor ' alcohol portion of the carbonic acid derivative oil, soybean oil, linseed oil, olive oil, tung oil, generally will be 8 to 20 carbon atoms; however, 10 rapeseed oil, menhaden oil and the like, or acids where the mixed carbonate ester contains other derived therefrom may be conveniently employed. long hydrocarbon chains such as may be ob Dicarboxylic acids such as succinic acid, maleic tained when a long chain fatty acid is employed acid, fumeric acid, azelaic acid, andsebacic‘acid to produce an ester-carbonate, the number of car may likewise be employed. bon atoms in the monohydroxy alcohol portion of 15 Some speci?c examples of ester- the carbonic acid derivative generally will be less wherein a mixed carbonate ester is further esteri than 8 carbon atoms. The carbonic acid deriva ?ed with a carboxylic acid as described above tives of monohydroxy alcohols may be conven are: pentaerythritol mono-oleate mono-allyl iently prepared by the reaction of in carbonate, pentaerythritol di-oleate mono-petro the presence of pyridine with monohydroxy alco leumcarbonate mono-ethylcarbonate, pentaery hols to give alkylchlorocarbonates or dialkyl thritol mono - laurate mono - hexyl - carbonate, carbonates. The monohydroxy alcohols which tetramethylolcyclohexanol mono-oleate mono may be utilized in the preparation of these car allylcarbonate, sorbitan mono-oleate mono-allyl bonic acid derivativas-may be saturated or un carbonate, glycerol mono-stearate mono-allyl saturated and may be individual alcohols or mix carbonate, and dipentaerythritol mono-oleate tures of alcohols such as may be obtained by dl-Co “Oxo" carbonate, pentaglycerol mono-tall physicallymixing several alcohols or by the‘ re oil ester mono-allylcarbonate, triethanol amine duction of naturally occurring fatty esters, or by mono-stearate mono-allylcarbonate and tris(hy the fermentation process, or by the reduction of droxy methyl) ‘amino methane mono-stearate an ole?n with and hydrogen as 80 mono-allylcarbonate. . .I in the "Oxo” process. Among the more preferred The additives of the present invention may be ‘examples of monohydroxy alcohols may be men advantageously employed with petroleum frac tioned ethyl, propyl, allyl. amyl, 2-ethylhexyl, tions of .a wide variety, although their preferred 2-ethylbutyl “Cellosolve',” Ca Oxo, C9 Oxo, Ci: use is in lubricating oil bases to form lubricant 0x0, cetyl, oleyl, octadecyl, myristyl, linoleyl, compositions which also act as corrosion pre erucyl and lauryl alcohols, also furfuryl, tetra ventives. The base stocks may be derived from hydrofurfuryl, and cyclohexanol alcohols- The . various types of crude petroleum and may consist polyhydroxy alcohols which are to be used in the of distillates or blends of various kinds which preparation of the mixed carbonate esters of this have been refined by any of the conventional invention are selected from the. class of poly methods. Synthetic oils may also be used such hydroxy alcohols containing at least two hydroxyl as those obtained by the polymerization of ole?ns groups. Such polyhydroxy alcohols may contain or by the hydrogenation of coal or its products. ‘besides the hydroxyl groups additional groups In the case of lubricants, the base stock chosen such as nitro, carboxylic, ‘ester, amide, ether, will normally be that oil which without the new pyridyl, quinolyl, phenyl, sulfonate and primary, 45 additives gives the optimum performance in the _ secondary, and tertiary amino groups in the service contemplated. These base oils may vary molecule. A preferred group of polyhydroxy al considerably in viscosity and other properties de cohols comprises those alcohols containing four pending upon the particular uses for which they and five hydroxyl groups per molecule, among are desired. For crankcase use they usually range which pentaerythritol, sorbitan and tetramethyl 60 from about 40 to 130 seconds viscosity Saybolt olcyclohexanol are especially suitable examples. at 210 F. The viscosity index may range from As further illustrations of polyhydroxy alcohols less than 0 to 130 or even higher. Turbine oils which may be conveniently employed in accord usually have a viscosity of 40 to 60 seconds Say ance with the present invention may be men bolt at 210° F. Use may also be found in torque tioned ethylene. glycol, propylene glycol, 1,3 55 converter ?uids having a viscosity of 35 to 45 propanediol, pentaglycerol, glycerol, diglycerol, . seconds at 210° F. and a viscosity index of 155 polyglycerol, tetramethylolcyclopentanol, anhy to 1'70. Corrosion-preventing compositions other dro-ennea-heptitol, 2-amino—2-methylol-1,3 Where ester-carbonates are desired, the car base stock according to the present invention, , boxylic acids which are suitable for the prepara other agents may be present in lubricating com , tion of the rust inhibiting-compositions of the positions and other corrosion~preventing com present invention include any aliphatic or cyclo positions, such as heat-thickened fatty oils, sul aliphatic carboxylic acids having 1 to 30 carbon 70 furized oils, organo-metallic compounds, metal atoms per molecule and these include saturated lic or other soaps, sludge dispersers, antioxidants. as well as. unsaturated acids having one or, two thickeners, viscosity index improvers, pour point carboxyl groups. Among the more preferred ex depressors, oiliness agents, resins, ole?n polymers amples of monocarboxylic acids may be men and colloidal solids such as graphite or zinc tioned acetic, butyric, valeric, lauric, palmitic, 75 oxides. and assisting agents such as 2,683,609 . 5 6 esters, ketones, alcohols, aldehydes, halogenated one liter 4 necked ?ask equipped with a stirrer, and nitrated compounds and the like may also be thermometer, separatory funnel, nitrogen inlet employed. tube, and re?ux condenser were added 200 g. of For the purpose of the present invention, the toluene and 80 g. (1 mol) of pyridine. To the esters described herein are added to the base stirred mixture cooled to 10° C. was added 60.3 stock in proportions preferably ranging from g. 0/: mol) of allylchlorcarbonate (ClCOOCsHs). 0.01% to 10% by weight and in some cases larger ‘ Addition was made dropwise over a period of 20 proportions may be employed to advantage. minutes with the temperature being held at 10° The esteriilcation of the polyhydroxy alcohols C. The mixture was stirred for 1 hour with the used in the present invention is carried out in temperature at 3° C. and then was allowed to _ such a manner that atv least one and preferably remain at room temperature for 16 hours. The not more than 1 hydroxyl group per molecule white crystals of pyridine hydrochloride (60 is condensed with the carbonic acid derivative grams, approximately 1/2 mol) were separated of a monohydroxy alcohol. It is understood, by suction ?ltration and washed with 200 g. of however, that because of the high concentration 16 toluene. The toluene solution was washed thor of polar groups in these alcohols, more than one oughly with dilute hydrochloric acid, saturated per molecule may react with sodium carbonate solution, and ?nally with water the carbonic acid derivative of a monohydroxy until it was neutral to litmus paper. The toluene alcohol. For instance, where an amino group is ' was distilled off under a reduced pressure of 30 present, a urethane may be formed concurrently mm. The product was a clear light amber colored with the mixed carbonate ester. However, when liquid weighing 227 g. (94% yield). secondary products arise, they are present in very Analyses of this product for carbon and hydro low concentration and, generally, do not affect gen content and inspection for saponification the inhibiting properties of the primary mixed number and netralization number were per carbonate ester adversely but rather tend to in formed. The following data were obtained: crease the effectiveness and solubility of the de sired mixed carbonate ester in its base oil. Theo Where pronounced oil solubility is desired or Found “meal an increased number of polar linkage is necessary to impart certain desired properties to the addi 80 Saponi?cation Number, mg. KOH/g ______._ M3. 2 231. 6 tive, the manner of treating the functional Neutralization Number, in KOH/ ..- 0.38 0. 0 Carbon, Per Cent ...... - 70. 95 66.8 groups of the polyhydroxy alcohol may be modi Hydrogen, Per Cent ______10.56 9. 9 ?ed so that, in addition to the formation of the mixed carbonate ester, other polar groups, This product was then evaluated for its rust especially hydroxyl and/or amino groups, are inhibiting properties by employing it in a' 1 wt. condensed with, for instance, a saturated or un percent concentration in a phenol treated Mid saturated monocarboxylic acid anhydride, ester Continent oil which was then used as a crankcase or an acid chloride to form an ester-carbonate oil in a single cylinder Wisconsin engine. After which is a preferred compound in this invention running the engine for 8 hours with this test oil, as stated previously, and/or an amide, or with the cylinder was removed from the engine and an alkyl halide to form an ether and/or an stored in a Tenney humidity cabinet kept at amine, or with an alkyl chlorocarbonate to form conditions of temperature and humidity which a di- and/or tricarbonate and/or a urethane, or are known to favor rusting and which simulate with a sulfonic acid or a sulfonyl chloride to form a typical summer day in Cuba. After each of a partial sulfonate and/or a sulfonamide, or with the first five 24-hourcycles, the amount of rusted an aldehyde to form an acetal and/or a Schiif’s area developed was determined and recorded as base, or with carbon disulilde and an alkali to the per cent of the total cylinder barrel area give a xanthate and/or a thiocar'bamate which rusted. Three evaluations were made on this may be followed by reaction with an alkyl halide, product. For comparative purposes, the base oil acid chloride, chloromethyl ether, chloracetic 50 alone and with 1% pentaerythritol mono-oleate acid ester, chlorethyl ester or an alkyl chlorocar were also evaluated in the same manner. bonate to give the corresponding xanthate After five days’ storage in the humidity cab and/ or thlocarbamate derivative. In addition to inet, the average rust observed with the blends the above reactions,'increased chain lengthening containing 1 % pentaerythritol mono-oleate mono may be accomplished in the presence of a suitable 55 catalyst by condensing a long chain mercaptan allylcarbonate was only 4% of the total cylinder with the mixed carbonate ester providing it has barrel area. This was substantially better than an ethylenic bond on one side of the carbonate the 10% obtained with a blend containing 1% linkage. Because of the many different linkages pentaerythritol mono-oleate and considerably that may be introduced into the mixed carbonate better than the 30% rusting obtained with the ester molecule, it will be recognized as a further base oil. The complete data are tabulated below. disclosure of this invention that any combination of the above-cited linkages may be utilized in the Per Cent of Total Cylinder mixed carbonate ester by properly selecting the Barrel Area Rusted initial reactants in order to obtain the ultimate 05 Test Additive in Base Oil, Wt. in additive effectiveness. Per Cent Days Storage The following example illustrates the applica tion of the present invention as an additive ma 1 2 3 4 5 terial suitable for inhibiting rust formation in A ..... _. 1% Pentaerytlu'itol Mono- l5 2 3 3 3.5 internal combustion engines. 70 Oleate Mono-Allylcar bonatc. s Example I B ______-.do ______._ 0.5 0.5 0.5 l 1.5 C ...... _do ______._ 3 4 6 7 7 D ______1% Pentaerythritol Mono- 1 3 5 8 10 To 200.3 g. 0/; mol) of pentaerythritol mono Oleate. oleate (prepared by esterifying equal molecular E _____ ._ None ______5 10 15 22 30 quantities of penterythritol and oleic acid) in a aosaeoo 7 8 These data clearly demonstrate that the addi taerythritol with a su?lcient amount 01’ oleic acid tion of the allylcarbonate linkage enhances the to esterity at least one hydroxyl group of said rust inhibiting effectiveness of the pentaerythritol pentaerythritol and subsequently reacting the mono-oleate molecule in such a manner that product thus formed with a sutllcient amount of blends containing pentaerythritol mono-oleate chloroallylcarbonate to esterify at least an addi mono-allylcarbonate a?ord greater rust inhi tional hydroxyl group of said pentaerythritol. bition in this test than the base oil or blends con ALFRED H. MATUSZAK. taining the same weight per cent of pentaerythri tol mono-oleate. REFERENCES CITED What is claimed is: ' The following references are of record in the 1. A mineral lubricating 011 containing dis ?le of this patent: . solved therein 0.1% to 10% 01' pentaerythritol _ mono-oleate mono-allylcarbonate. UNITED STATES A'I'ENTS' 2. A mineral lubricating 011 containing dis .Number Name ' Date solved therein about 1% by weight of pentaery 2,153,137 Dickey ______.._ Apr. 4, 1939 ’ thritol mono-oleate mono-allylcarbonate. 2,371,333 Johnston ______Mar. 13, 1945 3. The process which comprises reacting pen 2,414,400 Strain ______Jan. 14, 1947