US2593496A - Addition agent and mineral oil lubricant compositions containing the same - Google Patents

Description

employed as thelubricant.

' tion of so-calledvarnishes and sludges-on engine surfaces is a result of oxidation effects on the bustion chamber.

" These problems becomev particularly acute when ating conditions are encountered, mineral lubri ticularly' acute becauseof the presence of water in themineral oil lubricant and in addition to tered.

the oxidation, and corrosion difficulties encountered in the use of mineraloil lubricants.

which; are stable instorageand, use and in which oxidation, and corrosion. efiects'gare n ate i 1 hibited, a

Patented Apr. 22, 1952 UNITED" STATES? PATENT OFFICE ADDITION AGENTAND MINERAL OIL LUBRI- CANT COMPOSITIONSCONTAINING THE -SAME Herschel G.. Smith, Wallingford, and Troy L. Cantrell, Lansdowne,,Pag 'assignors. to Gulf Oil Corporation, Pittsburgh;

Pennsylvania No Drawing;

ra, a corporation of Application February 4,- 1948, Serial No. 6,344

25 Claims. "(CL 25246.6')

This. invention. relates to addition agents and mineral oil lubricantcompositions containing.- the same and, more, particularly, it is concerned with improvement agents which, confer improved anti-f oxidant, corrosion-inhibitingand pressure-carry-E 5 ing properties on mineraloil lubricants.

. It is recognized in the art. that mineral oil lubricants are readily. oxidized under service conditionsvthereby reducing the service life of internal combustion engines. and steam turbines. A conl0 comitant effect is corrosion of bearing surfaces.

a highly refined paraflinic base, mineralv oil. is

In. the lubrication of internal combustionengines of all types, particularly whensevere opercating oils frequently prove unsatisfactory because they tend to deposit varnish, gum and sludge on the engine surfaces, such as the cylinder walls, pistons and rings, andial'soto induce corrosionof bearing materials thereby causing failure of the engine. These'problemshave become increasingly serious because ofthe trend toward higher efficiency or higher power output per unit weight of engine, which results in. conditions tending to accelerate the deteriorating in- I 3 fluences on the mineral oil lubricant. The formalubricating oils. The presence of gums, varnishes andsludges is detrimental for" many 'reasons. These substances tendto increase ring sticking and ac'celerate the formation of further deposits on piston surfaces and in fixed parts of the com- The' sludges formed in the crankcase of the engine increase the rate of cor- "rosion of bearing surfaces,- especially of bearing alloys of the types now in use.

. In steam turbines, the corrosion'problem isparhearing corrosion, rustingmay also be encoun- I It is "an-:object'of'this invention, there-fore, to

prepare an improvement agent which willobvlate It is a. further object of this invention to provide improved mineral oil lubricantv compositions It is also an object of this invention to provide mineral oil lubricant compositions which have excellent pressure-carrying. properties.

In our 'copending application Serial No. 718,902, -'-filed' December 27', 1946, there is disclosed and ,claimed an addition agent for mineral oil lubric'ants. which confers excellent antioxidant, corrosion inhibiting' and pressure-carrying properties on mineral oil lubricants. Such improvement agent is prepared by heatingan essentially 1.; parafiinic base lubricating oil with aluminum pchloride, removing aluminum chloride from the r'eaction product and reacting said product with phosphorus pentasulfide at an elevated temperatime to incorporate phosphorus and sulfur therein.

is prepared by heating an essentially parafilnic chloride treatment of the lubricating oil as disclosed in our application Serial No. 718,902 may beomitted. It is also shown in our latter filed plication that when the prior aluminum chlo- V ride treatment of the parafiinic base lubricating oil is combined with reaction of the aluminum chloride treated product with phosphorus. penta- Fv sulfide in the presence of a surface active silicafcontaining catalyst, lighter colored products are obtained.

The objects of thepresent invention are accomplished. by providing improvement agents for mineraloil lubricants by reacting an essentiallypar- "a'flinic base lubricating oil or the aluminum chloride treated product thereof with phosphorus pentasu'lfide through the use of any of the meths disclosed, in our copending applications Serial s. 71.8,902and 736,618 and then reacting-the r sulting product with an ester having the formula:

vhereinla and R1 represent aliphatic hydrocari radicals, atleast onegof'said radicals con- 1 taming olefinicunsaturation, and thesui n, ofthe 3 carbon atoms of both R and R1 being not less than 16. Such improvement agents, as well as the mineral oil lubricant compositions containing them, are believed to be novel and are considered parts of our invention.

The present invention may be regarded as an improvement over the inventions disclosed in our above-identified copending applications. While the addition agents disclosed therein confer excellent antioxidant, corrosion-inhibiting and pressure-carrying properties on mineral oil lubricants, they sometimes fail topass the well known Copper Strip Test (Method 530.31, Federal Specification VV-L-79lc, May 12, 1945, page 259) thus indicating the presence of elementary sulfur or the so-called corrosive sulfur. While we do not wish to be bound by any theory as to the exact nature of our phosphorus pentasulfide reaction products, it is our present belief that either elementary sulfur r incompletely bound sulfur or both are formed in the reaction. In accordance with the present invention, such elementary or incompletely bound sulfur is neutralized by combination with the unsaturated ester added to the phosphorus pentasulfide reaction product. In addition, the resulting products have enhanced pressure-carrying properties.

It is still necessary for the purposes of the present invention to employ an essentially parafiinic base lubricating oil as the initial material, be-

. cause other hydrocarbon materials produce a black, sludge-like, difiicultly soluble product regardless of whether the prior aluminum chloride treatment or reaction in the presence of a surface active silica-containing solid catalyst are employed. The reasons for the advantageous effects of the prior aluminum chloride treatment or of the surface active silica-containing solid catalyst on the reaction when an essentially parafiinic base lubricating oil is employed are not fully understood." However, the use of at least one of these methods is essential for the practice of our invention since, if the prior aluminum chloride treatment or the use of a surface active silicacontaining catalyst is omitted, the advantageous results of our invention are not obtained. In order to obtain the results of our invention, therefore, it'is necessary (1) to employ an essentially paraflinic base lubricating oil, and (2) to conduct the reaction of the oil with phosphorus pentasulfide only afteraluminum chloride has been reacted with the oil and/or the reaction with'phosphorus pentasulfide is conducted in the presence of a surface active silica-containing solid catalyst. The essentially paraflinio base lubricating oil used as a starting material in accordance with our invention may be derived from any paraffinic crude, such as Pennsylvania, Mid-Continent, or other paraffinic base crudes. The lubricating oil is manufactured from such crudes in accordance with conventional methods and may be refined in accordance with methods known in the art. If it is desired to treat the essentially paraflinic base lubricating oil with aluminum chloride, such treatment is accomplished as described in our copending application, Serial No. 718,902. Brief- 1y, such treatment comprises heating the essentially parafiinic base lubricating oil with from 1' to per cent by weight of anhydrous aluminum chloride at a temperature of from 150 to 300 F. while the mixture is vigorously agitated. The time of treatment may vary in accordance with 4 temperatures. In general, the treatment will be completed after four or five hours. After the treatment is completed, agitation is stopped and the sludge containingmost of the aluminum chloride settles out from the main body of the oil and is drawn off. The supernatant body of the treated oil may contain further quantities of aluminum chloride finely dispersed therethrough, and in order to insure the removal of all aluminum chloride from the treated oil, agitating with an adsorbent clay followed by filtration may be employed. At the higher temperatures of treatment with aluminum chloride some conversion of the parafiinic base oil to lower boiling products may take place. Although such conversion is slight, the product may be topped if desired, that is, distilled to remove the lower boiling products overhead and to recover as a residue the bulk of the aluminum chloride treated oil having a minimum initial boiling point in the range 490 to 530 F. The essentially parafiinic base lubricating oil treated with aluminum chloride as disclosed hereinabove may then be reacted with phosphorus pentasulfide. This may be accomplished either by reacting with phosphorus pentasulfide per se, as disclosed in our CODBIldlllg application Serial No. 718,902, or in the presence of a surface active silica-containing solid catalyst as disclosed in .our copending application, Serial No. 736,618.

If it is desired to react the aluminum chloride treated oil with phosphorus pentasulfide per se, this reaction is accomplished by adding from 2 to 20 per cent by weight of P285, preferably 5 to 10 percent, and heating with agitation at a minimum reaction temperature of 450 F. and a maximum reaction temperature below the temperature where cracking of the oil begins. Hydrogen sulfide is evolved and when the evolution of hydrogen sulfide has nearly ceased, the temperature of the reaction mixture may be increased within the maximum temperature disclosed above, say to about 500 F. for the completion of the reaction.

If desired, the aluminum chloride treated parafiinic base lubricating oil may be reacted with phosphorus pentasulfide in the presence of a surface active silica-containing catalyst; or, the prior aluminum chloride treatment may be omitted and the essentially paraffinic base lubricating oil may be reacted with phosphorus'pentasulfide in the presence of a surface active silicacontaining solid catalyst. The reaction of the essentially paraifinic'base lubricating oil, whether or not pretreated with aluminum chloride, with phosphorus pentasulfide in the presence of a surface active silica-containing solid catalyst is accomplished by adding'2 to 20 per cent by weight of PzSs, preferably from 5 to 10 per cent, to the essentially parafiinic base lubricating oil and heating with agitation at a temperature in the range from 300 F. to a maximum temperature below the temperature where cracking of the oil, that is, 'pyrolytic decomposition of the oil, begins.

Generally the minimum cracking temperature of the oil varies between 490 to 530 F., depending upon the particular oil used. The surface active silica-containing solid catalyst is employed in the amount of aluminum chloride used and the};

temperature of treatment, longer times being rc quired with less aluminum chloride and lower amounts of from 2 to 25 per cent by Weight of the oil charged and preferably in an amount of 10 per cent by weight. Larger amounts than 10 per cent are ordinarily not necessary, but larger amounts will produce a product having a lighter color. During the course of the reaction hydrogen sulfide is evolved and the phosphorus and sulfur become incorporated in the oil. When cracking catalyst and the like. Thus, activated clays, that is, natural clays such as bentonite, smectite, floridin, fullers earth and the like which have been treated with acid, such as are.

described in U. S. Patent No. 1,898,165, for example, may be advantageously employed. Synthetic silica-alumina catalysts of the type used for the cracking of hydrocarbon oils, examples of which are described in U. S. Patent No. 2,078,945 and U. S. Patent No. 2,283,173, may also be employed. Activated silica gel is also suitable. Asmay be seen, the term surface active silica-containing solid catalyst comprises a wide variety of materials, the predominant characteristic of which is the presence of silica in a surface active, that is, activated form.

After reaction of the essentially paraffinic base lubricating oil with the phosphorus pentasulfide as disclosed hereinabove, the resulting reaction products are reacted, in accordance with the present invention, with an ester having the formula:

wherein R and R1. represent aliphatic hydrocarbon radicals, at least one of said radicals containing olefinic unsaturation, and the sum of the carbon atoms of both R and R1 being not less than 16. The reaction with the ester takes place at a temperature in the range 300 to 400 F., preferably about 350 F. The ester is ordinarily added in proportions ranging from 1.0 to per cent byweight of the reaction mixture, sufiicient to combine with free or corrosive sulfur in the -'phosphorus pentasulfide reaction product. When reacted under these conditions, we believe that theester is linked te the phosphorus pentasulfide reaction product through a sulfur atom, and any free sulfur will also react with the ester.

Among the esters encompassed by the present invention and having the formula:

as defined hereinabove, there are included the following types:

(1)i Those esters in Which both R and R1 have v olefinic unsaturation. These include such esters as allyl oleate, decylene oleate, dodecylene' oleate,

pentadecylene oleate, oleyl oleate, and particularly sperm oil which provides an excellent source of this type of ester.

(2) These esters in which R has olefinic unsaturation, but R1 is saturated. These include methyl' oleate, isopropyl oleate, hexyl' oleate,

lauryl'oleate, cetyl oleate and the like. In lieu of esters of oleic acid, esters of other olcfinic mono-carboxylic fatty acids may be employed,

such as esters of decenoic, undecenoic, linoleic and linolenic acids.

(3 These esters in which R is saturated,,but Rrhas olefinic unsaturation. These include allyl ,nalmitate', ,decylene, laurate, dodecylene caprylate and oleyl butyrate.

In. selecting any ester of the above: types, it should be borne in mind that the; sum. of the carbon. atoms of. R and Rrmust benot: lessthan 16'.

The. following examples illustrate the, preparation ofour new improvement agents.

Example I Fifty-one parts by" weight of an essentially paraflinic base lubricating oil (S.A.E. 30) which had been treated with aluminum chloride in accordance with our copending application Serial No. 718,902 were placed in a reaction vessel together with 5.6 partsby weight of phosphorus pentasuliide. The mixture was then agitated and heated to 450 F. for a period of 2 hours. The temperature was then gradually raised to 525 F. over a period of 4 hours and maintained at that point for 2 hours. The mixture was then cooled to 350 F. and 5.1- parts by weight of sperm oil were added. The mixture was held at this temperature for 4 hours and then cooled and diluted with anequal weight of a light lubricating oil, thereby forming a concentrate of the improvementagent. The product had the following properties:

Gravity, API 24.0

Viscosity, SUV, F 520 Sulfur, per cent 1.94

Phosphorus, per cent 1.68

Example II An essentially parafiinic base lubricating oil (S.A.E. 50) was pretreated with aluminum chloride as herein disclosed and reacted with 10 per cent by Weight of phosphorus pentasulfide at 500 After completion of the reaction, 10 per cent by weight on the reaction mixture of sperm oil was added and the mixture agitated for 6 hours at 400 F. The product had the following properties Gravity, API 23.4 Viscosity, SUV, 100 F 1692 Sulfur, per cent 4.5 Phosphorus, per cent 1.6 Neutralization No 0.04

Example I II Five thousand four hundred parts byweight of an SAE 30 grade essentially paraffinic base lubricating oil were reacted with 600 parts by weight of phosphorus pentasulfide in the presence of 600 parts by weight of an activated clay catalyst at a temperature in the range 480 to 500 F. The reaction was completed after 6 hours. The mixture was then cooled to 350 F. and 600 parts by weight of sperm oil were added.

The mixture was held at 350 F. for 2 hours and then filtered. The product had the following f properties:

Gravity, API 22.6 Viscosity, SUV,210 F 78.7 Color, NPA 6.5 "Sulfur, per cent 3.12 Phosphorus, per cent 2.33 Neutralization No 13.9

The reaction products obtained in accordance with the precedingv examplesare excellent imprcvernent agents for mineral oil lubricant compositions. "They are light-colored and readily soluble in all types of mineral oils, that is paraffinic, naphthenic or mixed base mineral oils and,

as a matter of fact, can be blended with mineral oils in proportions as high as 50 per cent by weight or higher. This excellent solubility of our new improvement agents enables the preparation of concentrated solutions, which may then be diluted down to the proportion desired in the final mineral oil lubricant composition. As stated, our new improvement agents confer excellent pressure-carrying, anti-oxidant and corrosion-inhibiting properties on the mineral lubricating oils with which they are incorporated. For these purposes, our new improvement agents are generally added to mineral oils in minor amounts, say from 0.1 to 20 per cent by weight of mineral oil, sufficient to confer im proved pressure-carrying, anti-oxidant and corrosion-inhibiting properties on the mineral lubricating oils with which they are incorporated. When our new improvement agents are to be used for their anti-oxidant and corrosion-inhibiting effects, small proportions as low as 0.1 per cent by weight are suflicient to effect the improvement. When extreme pressure properties are to be conferred on a lubricating oil, higher proportions, as high as 20 per cent may conveniently be used. Lubricating oils containing our new improvement agents successfully pass the Copper Strip Test.

The following examples illustrate the use of our new improvement agents to obtain improved mineral oil lubricant compositions.

properties of the improved lubricant and the base lubricant follows:

Base Improved Lubricant Lubricant Gravity: API- 28.2 28. 3 Viscosity, SUV:

210 F 67. 5 67.8 Viscosity Index. 101 102 Color, NPA 4. 5 4. 5 Sulfur: Per Cent 0.18 0.19 Phosphorus: Per Cent 0.03 Neutralization No nil 0.00 Oxidation and Bearing Corrosion Test, Method 257, Gulf:

Duration of Test: Hrs 48 48 Oil Bath Temperature: I! 347 347 Air Rate: cc./Hr 2, 000 2, 000

Quantity of Oil' 0 300 300 Bearing Type. Gd-Ag Ou-Pb Dd-Ag Cu-Pb Wt. Change: Grains. 0. 0989 0. 1488 -0.0003 +0. 0035 Wt. Change: Per Cent -0. 51 0. 74 0.0l 0 02 Copper Strip Test Passes Passes Example VI In order to determine the improvement in pressure carrying properties obtained by using the addition agent of the present invention, additives prepared in accordance with the disclosures of Serial No. 718,902, Serial No. 736,618 and in accordance with the present invention were blended in a motor oil, and the lubricants were subjected to the Well known Falex Wear Test. In each instance, 15 parts by Weight of the addition agent were added to 85 parts by weight of a highly refined motor oil. The uncompounded oil is included for purposes of comparison.

Example IV An improved motor oil was prepared by blending 0.3 per cent by weight of the additive of Example II-with 99.7 per cent by Weight of a highly refined motor oil. A comparison of the properties of the improved lubricant and the base lubricant follows:

Unimproved Improved Lubricant Lubricant Gravity: API 29.2 29. 2 Viscosity, SUV 100 F. 524 526 Color, NPA 1. 75 1. 75 Oxidation and Bearing Corrosion Test, Method 257, Gulf:

Duration of Test: Hrs. 48 48 Oil Bath Temperature: F 347 347 Air Rate: coJHr 2,000 2, 000 Quantity of Oil: cc 300 300 Bearing Type CdAg Cu-Pb Cd-Ag Cu-Pb Wt. Change: Grams 0. 500 0. 250 0.06 0.157 Wt. Change: ler CeuL... -O. 25 0.06 0. 01 0.04 Copper Strip Test Passes Passes Example V para fiinic base motor oil; A comparison of the V The Oxidation and Bearing Corrosion Test, Method 257 Gulf referred to in the foregoing examples is conducted as follows: An alloy bearing shell of certain commonly used standard dimensions is submerged in 300 cc. of the oil or oil composition to be tested in a 400 cc. Pyrex beaker and heated in a thermostatic oil bath to 370 F. Air is then bubbled through the oil in contact with the bearing shell at a rate of 2000 cc. per hour. At the end of 48 hours the loss of weight and condition of the bearing shell are determined, the bearing shell being Washed free of oil and dried before weighing. When determining the effectiveness of various improvement agents, the usual procedure is to run a blank test simultaneously with the oil composition being tested, employing for that purpose a sample of the untreated oil. In this test it is advantageous to employ commercial bearing shells. These shells comprise a suitable metal backing faced with the alloy bearing metal. In this way the actual bearlng face is subjected to severe deterioration conditions. By comparison of the results of such tests with actual service tests, We have found them to be in substantial agreement as to suitability of particular lubricants.

As shown in the above examples, the addition of our new improvement agents to mineral oil lubricant compositions confers excellent pressure-carrying, anti-oxidant and corrosion-inhibiting properties. At the same time the compositions so obtained are stable in storage and use and have a color which is substantially unaffected by the addition of the improvement agent. The lubricants obtained pass the Copper Strip Test and show enhanced pressure-carrying properties over the lubricants of our copending applications.

While we have shown in the examples the preparation of compounded, lubricating oils, our invention is not limited theretobut comprises all mineral oil lubricant compositions containing our new improvementagentsfs'uch as greases and the like. Furthermore, conventional addition agents such as viscosity index improvers, pour pointgdepressants and the like may be added withoutdeparting from the spirit of the invention.

We claim:

1. The process of preparing an improvement agent for mineral oil lubricants which comprises heating an essentially paraffinic base lubricating oil with anhydrous aluminum chloride at a temperature of from 150 to 300 F., removing aluminum chloride from the reaction product, reacting said product with phosphorus pentasulfide at a temperature of from 450 F. to a maximum temperature below the minimum cracking temperature of said product to incorporate phosphorus and sulfur therein, and then further reacting the resulting product at a temperature of from 300 to 400 F. with an ester having the formula:

wherein R and R1 represent aliphatic hydrocarbon radicals, at least one of said radicals containing olefinic unsaturation, and the sum of the carbon atoms of both R and R1, being not less than 16.

2. The process of claim 1, wherein the aluminum chloride is employed in an amount of from 1 to 20 per cent by Weight, the phosphorus pentasulfide is employed in an amount of from 2 to 20 per cent by weight, and the ester is employed in an amount of from 1 to per cent by weight, suificient to combine with free or corrosive sulfur in the phosphorus pentasulfide reaction prodnot.

3. The process of claim 2, wherein the ester is sperm oil.

4. The process of claim 2, wherein the product is dissolved in a mineral lubricating oil.

5. The process of preparing an improvement agent for mineral oil lubricants which comprises heating an essentially parafiinic base lubricating oil with phosphorus pentasulfide in the presence of a surface active silica-containing solid catalyst at a temperature of from 300 F. to a maximum temperature below the minimum cracking temperature of said lubricating oil to incorporate phosphorus and sulfur therein, and then further reacting the resulting product at a temperature of from 300 to 400 F. with an ester having .the formula: 1

R- OR1 wherein R and R1 represent aliphatic hydrocarbon radicals, at least one of said radicals containing olefinic unsaturation, the sum of the carbon atoms of both R and R1 being not less than 16, and recovering the reaction product.

6. The process of claim 5, wherein the phoscombine with free or corrosive sulfur in the phosphorus pentasulfide reaction product.

7. The process of claim 6, wherein the ester is sperm'oil.

8. The process of preparing an improvement agent for mineral oil lubricants which comprises heating-an essentially paraflinic base lubricating oil with from'l to per cent by weight of anhydrous aluminum chloride at a temperature of from 150 to 300 F., removing aluminum chloridefrom the reaction product, heating said product with from 2 to 20 per cent by weight of phosphorus pentasulfide in the presence of from 2 to 25 per cent by weight of a surface active silica-containing solid catalyst at a temperature of from 300 F. to a maximum temperature below the minimum crackin temperature of the aluminum chloride treated oil to incorporate phosphorus and sulfur therein, and then further reacting the resulting product at a temperature of from 300 to 400 F. with an ester having the formula:

wherein R and R1 represent aliphatic hydrocarbon radicals, at least one of said radicals containing olefinic unsaturation, the sum of the carbon atoms of both R and R1 being not less than 16, and recovering the reaction product.

9. The process of claim 8, wherein the ester is sperm oil and is employed in an amount of from 1 to 10 per cent by weight, suflicient to combine with free or corrosive sulfur in the phosphorus pentasulfide reaction product.

10. The product obtained by the process claim 1.

11. The claim 2.

12. The claim 4.

13. The product obtained by the claim 5.

14. The claim 8.

15. A lubricant composition comprising a major amount of a mineral lubricating oil and a minor amount, sufiicient to confer improved bearing corrosion-inhibiting properties on the composition of the product obtained by the process of claim 1.

16. A lubricant composition comprising a major amount of a mineral lubricating oil and a minor amount, from 0.1 to 20 per cent by weight, of the product obtained by the process of claim 2.

17. A lubricant composition comprising a major amount of a mineral lubricating oil and a minor amount, sufficient to confer improved bearing corrosion-inhibiting properties on the composition, of the product obtained by the process of claim 5.

18. A lubricant composition comprising a major amount of a mineral lubricating oil and a minor amount, from 0.1 to 20 per cent by weight, of the product obtained by the process of claim 6.

19. A lubricant composition comprising a major amount of a mineral lubricating oil and a minor amount, suflicient to confer improved product obtained by the process of product obtained by the process of process of product obtained by the process of bearing corrosion-inhibiting properties on the composition, of the product obtained by the process of claim 8.

20. The product obtained by. the process of claim 3.

21. The product obtained by the process of claim 7.

22. The product obtained by the process of claim 9.

23. A lubricant composition comprising a major amount of a mineral lubricating oil and a minor amount, from 0.1 to 20 per cent by weight, of the product obtained by the process of claim 3.

24. A lubricant composition comprising a major amount of a mineral lubricating oil and a minor amount, from 0.1 to 20 per cent by weight, of the product obtained by the process of claim 'I.

a 25. A lubricant composition comprising a ma jor amount of a mineral lubricating oil and a minor amount, from 0.1 to 20 per cent by weight, of the product obtained by the process of claim 9.

HERSCHEL G. SMITH. TROY L. CANTRELL.

REFERENCES CITED The following references are of record in the file of this patent:

, UNITED STATES PATENTS Number

Claims (1)

16. A LUBRICANT COMPOSITION COMPRISING A MAJOR AMOUNT OF A MINERAL LUBRICATING OIL AND A MINOR AMOUNT, FROM 0.1 TO 20 PER CENT BY WEIGHT, OF THE PRODUCT OBTAINED BY THE PROCESS OF CLAIM 2.