Note: Descriptions are shown in the official language in which they were submitted.
20298~2
Case: EI-5984
CES/pk
LUBE OIL ADDITIVE PACKAGE CO~AI ING
VISCOSITY INDEX IMPROVER
Backaround of the Invention
1. Field of the Invention
The present invention relates to concentrates for
formulating lubricating compositions and, more particularly,
relates to concentrates which include a viscosity index
lmprover.
2. Related Art
Lubricant additive concentrates, such as those which are
blended with mineral or synthetic base oils to form motor oils,
normally contain various additives including dispersants,
detergents, corrosion and oxidation inhibitors, and wear
reducing agents along with some process oil. Viscosity index
improvers are also added to the motor oils to reduce viscosity
changes which would normally accompany temperature changes,
i.e., the oil resists thickening at low temperatures and resists
thinning out at high temperatures. Certain viscosity index
improvers also function as dispersants, for example, those
described in U.S. Patent 4,519,929.
, .
In practice, viscosity index improvers, including those
which also function as dispersants, cause irreversible gelling
of the concentrate when added thereto. For this reason,
viscosity index improvers are generally packaged separately and
added to the base oil separately from the lubricant additive
concentrates.
.
--1--
Brief summarY of the Invention
It has now been discovered that viscosity index improvers
can be included with other lubricant additives in a lubricant
additive concentrate without causing gelling. In particular,
viscosity index improvers can be added to a concentrate which
includes an ashless dispersant, diluent oil and, optionally,
other additives, in amounts to effect a ratio of diluent oil to
active ingredients of at least about 0.6:1, preferably to effect
a ratio ranging from about 0.7:1 to about 3.3:1. Accordingly,
this invention provides a storage stable crankcase lubricant
additive concentrate which comprises an ashless dispersant and
diluent oil along with an effective amount of a viscosity index
improver.
Detailed Descri~tion
The present invention resides in the discovery that within a
certain ratio of diluent oil to active additive ingredients,
viscosity index improvers can be included in a concentrate
containing diluent oil, ashless dispersant and, optionally,
other additives such as detergents, antioxidants, antiwear
.~
compositions, anticorrosion compositions and the like. The
resulting concentrate is a storage stable liquid that does not
gel or show significant amounts of precipitation on standing.
It is added to mineral or synthetic base oils to provide an
effective crankcase lubricating composition.
i,!
The term viscosity index improver as used herein denotes
elastomeric polymer compositions which impart improved fluidity
characteristics to the oil so that the tendency of the oil to
change viscosity in response to a change in temperature is
reduced. Viscosity index improvers, or viscosity modifiers,
i impart high and low temperature operability to the lubricating
oil and permit it to remain relatively viscous at elevated
: .
:, 20298~
temperatures and relatively fluid at low temperatures.
viscosity modifiers are generally high molecular weight
hydrocarbon polymers and polyesters. The viscosity modifiers
may also be derivatized to include other properties or
functions, such as the addition of dispersancy properties.
These oil soluble viscosity modifying polymers will generally
have number average molecular weights of from 103 to 107,
preferably 104 to 1o6, e.g., 20,000 to 250,000, as
. ':
determined by gel permeation chromatography or osmometry.
.. ,
Examples of hydrocarbon polymers suitable for preparing
viscosity index improvers include homopolymers and copolymers of
; two or more monomers of C2 to C30, e.g. C2 to C8
olefins, including both alpha olefins and internal olefins,
....
which may be straight or branched, aliphatic, aromatic,
alkyl-aromatic, cycloaliphatic, etc. Frequently they will be of
ethylene with C3 to C30 olefins. Particularly preferred are
the copolymers of ethylene and propylene. Other polymers can be
used such as polyisobutylenes, homopolymers and copolymers of
C6 and higher alpha olefins, acactic polypropylene,
hydrogenated polymers and copolymers and terpolymers of styrene,
e.g., with isoprene and/or butadiene and hydrogenated
derivatives thereof. The polymer may be degraded in molecular
weight, for example by mastication, extrusion, oxidation or
thermal degradation, or it may be oxidized and as such contain
oxygen. Also included are derivatized polymers such as
post-grafted interpolymers of ethylene-propylene with an active
monomer such as maleic anhydride which may be further reacted
with an alcohol, or an amine, e.g., an alkylene polyamine or an
alkylene hydroxy amine, e.g. see U.S. Pat. No.s 4,089,794;
4,160,739; 4,137,185. Other derivatized polymers useful in the
compositions of the present invention include copolymers of
" .
ethylene and propylene reacted or grafted with nitrogen
compounds, e.g., see U.S. Pat. Nos. 4,068,056; 4,068,058;
4,146,489 and 4,149,984.
, . ~
-3-
2029842
The preferred hydrocarbon polymers are ethylene copolymers
containing from 15 to 90 wt. % ethylene copolymerized with 10 to
85 wt. % of at least one C3 to C28 alpha-olefin. Most
preferably, the hydrocarbon copolymers are 30 to 80 wt. %
ethylene copolymerized with 20 to 70 wt. % of a C3 to C18
alpha-olefin. Particularly preferred hydrocarbon polymers are
those of ethylene and the C3 to C8 alpha-olefins. of the
particularly preferred hydrocarbon polymers, those of ethylene
and propylene are most preferred. While not essential, such
copolymers preferably have a degree of cystallinity of less than
25 wt. %, as determined by X-ray and differential scanning
calorimetry.
Other alpha-olefins suitable for use in place of propylene
to form the above copolymers, or to be used in combination with
... .
~! ethylene and propylene to form a terpolymer, tetrapolymer, and
. 1
so forth, include l-butene, l-pentene, l-hexene, l-heptene,
l-octene, l-nonene, l-decene, and the like; also useful are
~)
branched chain alpha-olefins, such as 4-methyl-1-pentene,
4-methyl-1-hexene, 5-methylheptene-1, and the like, and mixtures
l thereof.
: !
Terpolymer, tetrapolymers, and the like, of ethylene, the
C3_28 alpha-olefin, and a non-conjugated diolefin or mixtures
of such diolefins may also be used. The amount of the
non-conjugated diolefin generally ranges from about 0.5 to 20
mole percent, preferably from about 1 to about 7 mole percent,
most preferrably 1.5 to 5.5 mole percent based on the total
amount of ethylene and alpha-olefin present.
1 .
The polyester viscosity index (V.I.) improvers are generally
polymers of esters of ethylenically unsaturated C3 to C8
mono- and/or dicarboxylic aclds such as methacrylic and acrylic
--4--
.
2029842
acids, maleic acid, maleic anhydride, fumaric acid, and the
like. Examples of unsaturated esters that may be used in this
embodiment of the present invention include aliphatic saturated
mono alcohols of at least 1 carbon atom up to about 25 carbon
atoms and preferably of from 12 to 20 carbon atoms, such as
decyl acrylate, lauryl acrylate, stearyl acrylate, eicosanyl
acrylate, docosanyl acrylate, decyl methacrylate, diamyl
fumarate, lauryl methacrylate, cetyl methacrylate, stearyl
methacrylate, and the like and mixtures thereof. Other esters
include the vinyl alcohol esters of C2 to C22 fatty or mono
carboxylic acids, preferably the saturated fatty or mono
carboxylic acids, such as vinyl acetate, vinyl laurate, vinyl
palmitate, vinyl stearate, vinyl oleate, and the like and
mixtureæ thereof. Copolymers of vinyl alcohol esters with
unsaturated acid esters such as the copolymer of vinyl acetate
with dialkyl fumarates, can also be used.
The esters may be copolymerized with still other unsaturated
monomers such as olefins e.g. 0.2 to 5 moles of C2-C20
aliphatic or aromatic olefin per mole of unsaturated ester, or
per mole of unsaturated acid or anhydridè followed by
esterification, e.g., copolymers of styrene with maléic
anhydride esterified with alcohols and amines. See U.S. Pat.
No. 3,702,300. In such copoIymerized enters, 0.2 to 5 moles of
C2-C20 aliphatic or aromatic olefin per mole of unsaturated
ester is used. Instead of the unsaturated ester, the
corr sponding unsaturated acid or anhydride may be first treated
with the olefin and the resulting copolymer esterified with
alcohols or reacted with amines.
2~2~84~
The term dispersant viscosity index improver as used herein
denotes polymer compositions ~hich not only enhance the
viscosity characteristics of the oil but also contain functional
groups to impart improved dispersancy to crankcase lubricants
used in spark ignition and compression ignition engines so as to
assist in dispersing the sludge formed in the lubricant oil
during operation of the engines. Thus, the above described
hydrocarbon polymers or polyesters may be grafted with, or
c op ol y m e r iæ ed w it h, polymerizable unsaturated
nitrogen-containing monomers to impart dispersant
characteristics to the V.I. improvers. Examples of suitable
unsaturated nitrogen-containing monomers include those
containing 4 to 20 carbon atoms such as amine substituted
olefins, e.g., p-(beta-diethylaminoethyl)styrene; basic
nitrogen-containing heterocycles carrying a polymerizable
ethylenically unsaturated substituent, e.g. the vinyl pyridines
and the vinyl alkyl pyridines such as 2-vinyl-pyridine,
4-vinyl-pyridine , 3-vinyl-pyridine 3-methyl-5-vinyl-pyridine,
4-methyl-2-vinyl-pyridine, 4-ethyl-2-vinyl-pyridine and
2-butyl-1-vinyl-pyridine and the like. N-vinyl lactams are also
suitable as functionalizing groups to produce dispersant
viscosity index improvers, e.g. N-vinyl pyrrolidones or N-vinyl
piperidones.
' ~
Examples of the dispersant viscosity index improving (DVII)
compositions include alkyl methacrylate based copolymers, e.g.,
methyl methacrylate based copolymers, such as those containing
N-vinylpyrrolidone and functionalized high molecular weight
olefin polymers, especially ethylene-propylene based copolymers,
which are reacted, i.e., are grafted, with vinyl monomers such
as maleic anhydride, 2-vinyl pyridine, acrylonitrile,
N-vinylpyrrolidone or an N-allyl amide to form graft
copolymers. Other examples of DVII compositions include
copolymers of olefins and the above described vinyl monomers.
(- ¢202~842
Additional examples include high molecular weight olefin
polymers (to produce functionalized polyolefin elastomers) and
high molecular weight olefin polyers which are oxidized and then
reacted with a functionalizing component such as an amine or an
amine and formaldehyde combination to thereby form a Mannich
condensation product. Several of such dispersant viscosity
index improvers and their methods of preparation are described,
for example, in U.S. 4,411,804 and 4,51g,929 whose teachings are
incorporated herein by reference.
. . ,
Ashless dispersants suitable for use in lubricating oils are
well known in the art. Examples of such dispersants include
polyolefin-substituted succinimides and/or succinimides of
polyethylene polyamines such as diethylene triamine and
tetraethylenepentamine. Additional examples include
polyolefin-substituted succinimid-s of amido-amines. The
polyolefin succinic substituent is preferably a polyisobutene
group having a number average molecular weight of from about 800
to about 5000. Such ashless dispersants are more fully
described in U.S. Patents 3,172,892; 3,219,666; 4,234,435; and
4,857,217, which are incorporated herein by referènce.
" .
; Another useful class of ashless dispersants are the
polyolefin succinic esters of mono- and polyhydroxy alcohols
containing from 1 to about 40 carbon atoms. Such dispersants
are described in U.S. Patent 3,381,022 and U.S. Patent
3,522,179, both of which are incorporated herein by reference.
Mixed ester-amides of polyolefin substituted succinic acid made
using alkanols, amines and/or aminoalkanols also represent a
useful class of ashless dispersants.
202~2
The succinic amide, imide and/or ester type ashless
dispersants may be post-treated, e.g., boronated by reaction
with a boron compound such as boric acid or maleated by reaction
with maleic anhydride. In addition, the succinic amide, imide,
and/or ester may be hydroxyalkylated by reaction with an
alkylene oxide such as ethylene oxide or propylene oxide.
Other useful ashless dispersants include the neutralized
reaction products of phosphorus sulfides and polyalkenes as well
as elastomeric copolymers functionalized with an N-allyl amide,
e.g., EPDM functionalized with diallylformamide. See, for
example, U.S. 4,519,929.
Still other useful ashless dispersants are Mannich
condensation products of polyolefin-substituted phenols,
formaldehyde and polyethylene polyamine. Preferably, the
polyolefin phenol is a polyisobutylene-substituted phenol in
which the polyisobutylene group has a molecular weight of from
about 800 to about 5000. The preferred polyethylene polyamine
is tetraethylene pentamine. Such Mannich ashless dispersants
are more fully described in U.S. Patents 3,368,972; 3,413,347;
3,442,808; 3,448,047; 3,539,633; 3,591,598; 3,600,372;
3,634,515; 3,697,574; 3,703,536; 3,704,308; 3,725,480;
3,726,882; 3,736,357; 3,751,365; 3,756,953; 3,792,202;
3,798,165; 3,798,247 and 3,803,039 incorporated herein by
reference.
.1
Mixtures of any of the above useful ashless dispersants,
such as a mixture of a Mannich ashless dispersant with a
succinimide dispersant or a mixture of a succinimide and a
succinic ester, are also suitable for use in the present
invention. Such mixtures may also be post-treated such as by
boronation or maleation.
--8--
2~2~842
The concentrates of this invention can contain optional
additives. See, for example, U.S. Pat. No. 4,857,217. For
example, detergent additives are one such optional additive. As
used in the compositions of the present invention, such
additives include alkali and alkaline earth metal petroleum
sulfonates, alkali and alkaline earth metal alkyl or alkaryl
sulfonates, alkyl phenates and metal carboxylates. Examples of
these are calcium petroleum sulfonates, magnesium petroleum
sulfonates, barium alkaryl sulfonates, calcium alkaryl
sulfonates, magnesium alkaryl sulfonates and calcium, and
magnesium alkylsulfonates. Both neutral and overbased
sulfonates or phenates, which have base numbers up to about 600
to provide acid neutralizing properties, can be beneficially
used and are commercially available. These detergent additives
are generally used in an amount to provide about 0.05-1.5 weight
..
percent alkaline earth metal and more preferably about 0.1-1.0
weight percent. The lubricating oil compositions of the
present invention preferably contain a calcium petroleum
sulfonate or an alkaryl (e.g. alkylbenzene) sulfonate as a
detergent additive.
,, .
Additional optional additives for the compositions of the
present invention include ashless antioxidants such as hindered
I alkyl phenols, alkyl diphenyl amines, and sulfur-bridged alkyl
.,
phenols; antiwear/corrosion inhibitors such as dialkyl
selenides, metal dithiocarbamates, sulfurized terpenes and zinc
dihydrocarbyldithiophosphates (ZDDP); friction reducers and EP
additives such as N-alkylglycine-amides, chlorinated para`ffins,
sulfurized olefins, sulfurized fatty oils, sulfurized hydroxy
substituted fatty amides, and co-sulfurized fatty acid amides
and esters; antifoam agents such as acrylate copolymers and
silicones; and surfactants such as ethoxylated alkyl phenols and
poly(alkyleneoxides).
.
_ g _
20298~2
The compone~ts of the present invention are combined in a
diluent oil such as mineral oil, synthetic oil or mixtures
thereof in proportions by weight which are effective in
providing a liquid concentrate which is a storage stable liquid
composition in that it does not form a gel, or significant
amounts of precipitate, on standing for at least 30 days at
70C. Useful diluent oils for forming the concentrates include
neutral mineral oils which can be process oils, which are
solvent refined oils, and hydro-treated (hydrogen treated)
oils. Examples include process oil #5 and 80 neutral oil.
Normally, the diluent oil is added to the lubricant additive
concentrates either during their preparation and/or after
preparation for ease of handling purposes, and this oil, in
addition to all other oil, is included in calculating the total
amount of oil required in providing the stable compositions of
the invention. Accordingly, the proportions of all of the
active components given herein are on the basis of "active
ingredient" i.e. not including added oil.
To provide a concentrate, the ratio of the amount of oil
based on the total weight of concentrate to the amount of active
ingredients is typically from about 0.4:1 to about 0.56:1 for
conventional dispersant-inhibitor (DI) packages without a
viscosity index improver.
To provide a concentrate of the present invention which
includes a viscosity index improver, the ratios of total oil
(the sum of all oil utilized in the concentrate) to total active
or additive ingredients (active ingredients not including any
oil) are at least about 0.6:1, preferably at least about 0.7:1,
most preferably from about 0.7:1 to about 3.3:1.
-10-
2~298~2
The composition can also comprise one or more of the other
additives described above in effective amounts. For example, to
the compositions of the present invention can be added up to
about 10 weight percent ashless antioxidants (preferably about
0.05 to 5 weight percent), up to about 15 weight percent
detergent (preferably about 5 to lO weight percent), up to about
lO weight percent antiwear/corrosion inhibitor (preferably about
0.05 to 5 weight percent), up to about 10 weight percent
friction reducer (preferably about 0.05 to 5 weight percent), up
to about 2 percent surfactant (preferably about 0.1 to 1
percent) and up to about 2 percent surfactant (preferably o.l to
l percent) and up to about 1 weight percent antifoam (preferably
about 0.01 to 0.1 weight percent). It is well known in the art
that the presence of some of these other additives as well as
other factors can cause a change in the above concentration
parameters, i.e., the amount of components useful in the
,,~,
compositions of the present invention for dispersant, dispersant
viscosity index improver and oil which are necessary to provide
a stable concentrate. The type and molecular weight of the
viscosity index improver will also shift the parameters. It is
well within the ability of one skilled in the art to modify the
weight percentages of each of the additives and the diluent oil
to achieve a stable concentrate containing a selected dispersant
viscosity index improver according to the teachings of the
present invention.
'
The concentrates of the present invention can be formed
using conventional blending equipment and techniques. They are
blended with base oils in amounts to provide the required
additive levels in the finished crankcase lubricating oils, e.g.
. . ~
treat rates of from about lO to about 20 percent. Suitable base
oils, as known in the art, include both mineral and synthetic
oils and blends thereof.
. -11-
20~842
Mineral oils include those of suitable viscosity refined
from crude oil from all sources including Gulf coast,
mid-continent, Pennsylvania, California, Mideast, North Sea,
Alaska, the Far Eagt and the like. Various standard refinery
operations are useful in processing the mineral oil.
Synthetic oils include both hydrocarbon synthetic oils and
synthetic esters. Useful synthetic hydrocarbon oils include
liquid polymers of alpha-olefins having the proper viscosity.
Especially useful are the hydrogenated liquid oligomers of
C6-C12 alpha-olefins such as alpha-decene trimer. Likewise,
alkyl-benzenes of proper viscosity can be used as a synthetic
oil, such as didodecylbenzene.
Useful synthetic esters include the esters of both
monocarboxylic acids and polycarboxylic acids as T.~ell as
monohydroxy alkanols and polyols. Typical examples are
didodecyl adipate, trimethylol propane tripelargonate,
pentaerythritol tetracaproate, di(2-ethylhexyl)adipate, dilauryl
sebacate and the like. Complex esters prepared from mixtures of
mono- and dicarboxylic acids and mono- and polyhydroxyl alkanols
can also be used.
The invention is further illustrated by, but is not intended
to be limited to, the following examples wherein parts and
percentages are by weight unleas otherwise indicated.
~. . ..
20~9842
Examples 1-9
These examples illustrate storage stable concentrates having
a selected viscosity index improver included therewith according
to the teachings of the present invention. The liquid crankcase
concentrate formulations identified in Table 1 are prepared by
blending all additive ingredients in an amount of diluent oil
followed by blending therein an oil solution of a viscosity
index improver. The concentrates thus prepared are held at 70C
to determine storage stability (days at 70C without gel
formation). For the purpose of determining gelation for these
examples, visual determinations are made. If the concentrate
contains a thick, sometimes tacky mass (usually on the top of
the fluid) or contains a web-like structure dispersed throughout
the fluid (usually appearing as a stringy mass when poured),
such concentrates are identified as "gelled".
'
-13-
TA3LE 1 2029842
DAYS
RATIO AT 70C
DILUENT OTHER C WITHOUT
EXAMPLE DISPERSANT(A? VIltB~ OILfC) ADDITIVES r~) A+B+D GEL
1 14.11 1.92 66.29 17.682:1 65
2 14.11 1.92 66.29 17.682:1 65
3 13.56 1.02 65.84 19.581.9:1 73
4 13.56 1.02 65.84 19.581.9:1 65
12.53 1.71 66.79 18.972:1 73
6 12.53 1.71 66.79 18.972:1 65
7 12.03 2.26 68.34 17.372.2:1 65
8 12:03 2.26 68.34 17.372.2:1 74
9 11:86 1.75 64.52 21.871.8:1 60
;
A - WEIGHT % ACTIVE ALKENYL (Mn ABOUT 1300) SUCCINIMIDE ASHLESS
DISPERSANT
. B - WEIGHT ~ ACTIVE EPDM OLEFIN COPOLYMER COMPRISING ETHYLENE,
PROPYLENE AND A DIENE MONOMER (ORTHOLEUM 2052), 40,000 Mn,
GRAFTED WITH ABOUT 5% N,N-DIALLYL FORMAMIDE
C - WEIGHT % ACTIVE PROCESS OIL
D - WEIGHT % ACTIVE ADDITIVES SUCH AS DETERGENTS, WEAR REDUCING
AGRNTS, OXIDATION ~ CORROSION INHIBITORS AND TRE LIKE.
- ..
.
~, ,
.! 14
202~8~
Example lQ
A formulation was prepared according to the procedure of
Example 1-9 which included 2.07 wt. percent of a commercial
pyrrolidone containing acrylate type dispersant viscosity index
improver ~DVI improver or DVII) (Acryloid 956 DVII Rohm & Haas)
68.S3 wt. percent total oil and 12.03 wt. percent alkenyl (Mn
about 1300) succinimide ashless dispersant (ratio of total oil
to total active ingredient is 2.2). No gel formed after 57 days
at 70C. A formulation which contained 1.73 wt. % of the
Acryloid 956 DVII, 15.09 wt. % succinimide dispersant and 62.98
wt. % diluent oil (ratio of total oil to total active ingredient
is 1.7) was also stable for 57 days.
Example 11
A formulation according to Example 10 was prepared except
that the DVI improver was replaced by 2.07 wt. percent of an
oxidized, functionalized (Schiff's base) olefin polymer type
dispersant viscosity index (DVI) improver (Amoco 6906 DVII) and
the total oil was adjusted to 68.53 wt. percent. The
concentrate was stable after 57 days at 70C.
Example 12
' A formulation according to Example 10 was prepared except
that the DVI improver was replaced by 2.07 wt. percent of a
succinimide grafted olefin polymer type DVI improver (Paratone
856 DVII, Exxon Corporation) and the total oil was adjusted to
'' 68.53 wt. percent. The concentrate was stable after 57 days at
70C.
3 ,
.~
.'
2~8~2
Example 13
A formulation according to Example 10 was prepared except
that the DVI improver was replaced by 2.07 wt. percent of a
Mannich reaction product type DVI improver (Amoco 6565, Amoco
Corporation) and the total oil was adjusted to 68.53 wt.
percent. The concentrate was stable after 57 days at 70C.
Examples 14-21
Table 2 contains examples which illustrate additional
additive concentrates of the present invention wherein a
viscosity index improver (VII) is added to a concentrate and
held at 70C for at least about 30 days without causing a gel to
form in the concentrate. These concentrates were prepared
according to the procedures utilized in Examples 1-13 except
that the ratio of total oil (the sum of all oil utilized in the
concentrate) to total additives (active ingredients not
including any oil) was varied. In the table, the letters a-i
represent dispersants and VI improvers according to the
following scheme:
:, .
a. Alkenyl (Mn about 1300) succinimide ashless dispersant
b. Alkenyl (Mn about 900) succinimide ashless dispersant
c. Alkenyl (Mn about 2100) succinimide ashless dispersant
d. EPDM (Ortholeum 2052), 40,000 Mn, grafted with about 5%
N,N-diallyl formamide
e. Mixture of (d) and (f)
f. Olefin copolymer type VII which is a non-dispersant type
(Ortholeum 2052)
g. Amoco 6565 identified, in Ex. 13
h. Acryloid 702 DVII, from Rohm & Haas, which is an acrylate
type non-dispersant VI improver
i. Olefin copolymer type VII (Paratone 715, from Exxon Corp.)
-16-
2~2~42
TABLE 2
_
Ratio of
Total Oil to
Ex. No.Dis~ersant VIITotal Active Ing.
14 a d 1.3
a e 1.4
16 a f 2.4
17 a g 2.5
18 a h 0.7
l9 b d 1.6
c d 2.6
21 a i 2.5
Examples 22-25
Summarized in Table 3, these examples illustrate the
effect of varying the ratio of total oil to total active
inqredients to achieve a concentrate which does not gel. The
letters a, d and g represent dispersants and VI improvers
according to the scheme set forth for Table 2, the concentrates
being prepared as in Example 1.
TABLE 3
Ratio of
Total Oil to
Ex. No.Dispersant VIITotal Active Ina.
22 a d 1.2 Gel
23 a d 1.4 Clear
24 a g 1.2 Gel
a g 1.4 Clear~
