Rubber composition comprising phyllosilicate minerals, silanes, and quaternary ammonium salts

Claim 2

A rubber composition formed according to an improved rubber compounding process comprising mixing and substantially uniformly dispersing in natural or synthetic rubber the following: A. 1. particulate Agent G at a level of from about 5 to about 200 phr, 2. Agent H at a level of from about 0.005 to about 15 phr, and 3. Agent I at a level of from about 0.005 to about 15 phr; or B. 1. a particulate adduct of Agents G and H having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 5 to about 200 phr and the portion thereof contributed from Agent H is at a level of from about 0.005 to about 15 phr, and 2. Agent I at a level of from about 0.005 to about 15 phr; or C. 1. a particulate adduct of Agents G and I having a median particle size in the range of from about 0.01 to about 20 microns and present at a lever such that the portion thereof contributed from Agent G is at a level of from about 5 to about 200 phr and the portion thereof contributed from Agent I is at a level of from about 0.005 to about 15 phr, and 2. Agent H at a level of from about 0.005 to about 15 phr; or D. a particulate adduct of Agents G, H, and I having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 5 to about 200 phr, the portion thereof contributed from Agent H is at a level of from about 0.005 to about 15 phr and the portion thereof contributed from Agent I is at a level of from about 0.005 to about 15 phr; or E.

Claim 3

a particulate adduct of Agents G and H having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 2.5 to about 100 phr and the portion thereof contributed from Agent H is at a level of from about 0.005 to about 15 phr, and 2. a particulate adduct of Agents G and I having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 2.5 to about 100 phr and the portion thereof contributed from Agent I is at a level of from about 0.005 to about 15 phr; wherein Agent G comprises phyllosilicate mineral particles having a median particle size in the range of from about 0.01 to about 20 microns; wherein Agent H comprises an organosilane of formula I or II ##STR3## wherein X is a group which is, or which upon hydrolysis forms a group which is, capable of reacting with a reactive site on the phyllosilicate mineral particles so as to form a bond between the organosilane of formula I or II and the phyllosilicate mineral particles, wherein Y is an alkyl, aryl or alkyl-substituted aryl group containing from 1 to 40 carbon atoms and bears a functional group capable of reacting with a reactive site on the rubber so as to form a bond between the organosilane of formula I or II and the rubber, wherein R 1 and R 2 are the same of different and are each selected from the group consisting of the groups described by X and Y, an alkyl group containing from 1 to 20 carbon atoms, an aryl group, and an alkyl-substituted aryl group wherein the alkyl substituents contain a total of from 1 to 20 carbon atoms, and wherein K is an alkylenyl group containing from 1 to 20 carbon atoms or an alkyl sulfide or polysulfide group containing from 1 to 6 sulfur atoms and from 2 to 20 carbon atoms; and wherein Agent I comprises a quaternary ammonium salt.

Claim 4

a particulate adduct of Agents G and H having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 2.5 to about 100 phr and the portion thereof contributed from Agent H is at a level of from about 0.005 to about 15 phr, and 2. a particulate adduct of Agents G and I having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 2.5 to about 100 phr and the portion thereof contributed from Agent I is at a level of from about 0.005 to about 15 phr; wherein Agent G comprises phyllosilicate mineral particles having a median particle size in the range of from about 0.01 to about 20 microns; wherein Agent H comprises an organosilane of formula I or II ##STR3## wherein X is a group which is, or which upon hydrolysis forms a group which is, capable of reacting with a reactive site on the phyllosilicate mineral particles so as to form a bond between the organosilane of formula I or II and the phyllosilicate mineral particles, wherein Y is an alkyl, aryl or alkyl-substituted aryl group containing from 1 to 40 carbon atoms and bears a functional group capable of reacting with a reactive site on the rubber so as to form a bond between the organosilane of formula I or II and the rubber, wherein R 1 and R 2 are the same of different and are each selected from the group consisting of the groups described by X and Y, an alkyl group containing from 1 to 20 carbon atoms, an aryl group, and an alkyl-substituted aryl group wherein the alkyl substituents contain a total of from 1 to 20 carbon atoms, and wherein K is an alkylenyl group containing from 1 to 20 carbon atoms or an alkyl sulfide or polysulfide group containing from 1 to 6 sulfur atoms and from 2 to 20 carbon atoms; and wherein Agent I comprises a quaternary ammonium salt.

Claim 5

The rubber composition of claim 1 wherein the rubber comprises natural or synthetic rubber.

Claim 6

The rubber composition of claim 2 wherein the rubber is natural or synthetic rubber.

Claim 7

The rubber composition of claim 3 wherein natural rubber, polybutadiene rubber, polyisoprene rubber or styrene-butadiene rubber is employed.

Claim 8

The rubber composition of claim 1 wherein a sulfur or sulfur-donating curing agent is employed.

Claim 9

The rubber composition of claim 1 wherein the phyllosilicate mineral is selected from the group consisting of a member of the kaolin group, a member of the mica group, a member of the group characterized by a primitive three-layer structure, a member of the group characterized by an expandable three-layer structure and a member of the group characterized by a four-layer structure.

Claim 10

The rubber composition of claim 6 wherein the phyllosilicate mineral is selected from the group consisting of kaolinite, muscovite, pyrophyllite, talc, vermiculite and chlorite.

Claim 11

The rubber composition of claim 7 wherein the phyllosilicate mineral is talc.

Claim 12

The rubber composition of claim 1 wherein X is a group which upon hydrolysis forms a hydroxyl group.

Claim 13

The rubber composition of claim 1 wherein X is selected from the group consisting of a halogen radical and --OR 13 and wherein R 13 is an alkyl group containing from 1 to 20 carbon atoms.

Claim 14

The rubber composition of claim 10 wherein X is --OR 13 , and R 13 contains from 1 to 7 carbon atoms.

Claim 15

The rubber composition of claim 1 wherein the functional group on Y which is capable of reacting with a reactive site on the rubber is selected from the group consisting of a mercapto group, allyl group, vinyl group, epoxy group, methacryloxy group, acryloxy group, and an amino group having an active hydrogen atom.

Claim 16

The rubber composition of claim 12 wherein the functional group on Y which is capable of reacting with a reactive site on the rubber is selected from the group consisting of a mercapto group, a vinyl group and an amino group having an active hydrogen atom.

Claim 17

The rubber composition of claim 1 wherein Y contains from 1 to 6 carbon atoms.

Claim 18

The rubber composition of claim 1 wherein R 1 and R 2 are the same or different and are each selected from the group consisting of the group described by X.

Claim 19

The rubber composition of claim 15 wherein R 1 and R 2 are the same or different and are each selected from the group consisting of a halogen radical and --OR 13 and wherein R 13 is an alkyl group containing from 1 to 20 carbon atoms.

Claim 20

The rubber composition of claim 16 wherein X, R 1 and R 2 are the same.

Claim 21

The rubber composition of claim 1 wherein the organosilane of formula I or II is selected from the group consisting of 3-aminopropyl-triethoxysilane, 3-mercaptopropyl-trimethoxysilane and vinyl-tri-(2-methoxyethoxy) silane.

Claim 22

The rubber composition of claim 1 wherein the quaternary ammonium salt has a structure of formula III, IV, V, VI or VII: ##STR4## wherein Z is zero or a positive integer from 1 to 100, J is an anionic radical, n is the absolute value of the oxidation state of J, and R 6 is an alkylenyl radical containing from 2 to 20 carbon atoms or an aryl radical containing from 6 to 14 carbon atoms, wherein in formulas III and IV, R 3 , R 4 , R 5 , R 7 , R 8 and R 9 are the same or different and are each selected from the group consisting of: aliphatic radicals containing a total of from 1 to 3 carbon atoms which are saturated or unsaturated and unsubstituted or substituted with at least one hydroxy or alkoxy group; aliphatic radicals containing a total of from 8 to 40 carbon atoms which are saturated or unsaturated and unsubstituted or substituted with at least one hydroxy, alkoxy or polyalkoxy group; aryl radicals containing from 6 to 18 carbon atoms; and saturated or unsaturated araliphatic radicals containing a total of from 7 to 48 carbon atoms, wherein in formulas III and IV, when Z is zero, R 10 is selected from the group consisting of the groups described by R 3 , R 4 , R 5 , R 7 , R 8 and R 9 , and when Z is a positive integer, R 10 is selected from the group consisting of the groups described by R 3 , R 4 , R 5 , R 7 , R 8 and R 9 and a hydrogen atom, wherein in formulas III and IV, (1) at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 and R 10 is an aliphatic radical containing a total of from 1 to 3 carbon atoms and (2) either (a) at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 and R 10 is an aliphatic radical containing at least 12 carbon atoms or (b) at least two of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 and R 10 are aliphatic radicals containing at least 8 carbon atoms, wherein in formulas V, VI and VII, each of T and U is a radical which, in conjunction with each nitrogen atom to which it is shown attached in formula V, VI or VII, forms a heterocyclic radical containing at least one nitrogen atom in the ring system and containing only nitrogen and carbon atoms in the ring system, and the T and U portions of the ring system are unsubstituted or substituted by at least one alkyl group with the total number of ring substituents on each of T and U being from 1 to 32 carbon atoms, wherein in formulas V and VI, R 11 is selected from the group consisting of the groups described by R 3 , R 4 , R 5 , R 7 , R 8 and R 9 and alkylamidoalkyl or alkylesteralkyl groups containing a total of at least 14 carbon atoms, and wherein in formulas V, VI and VII, when Z is zero, R 12 is selected from the group consisting of the groups described by R 11 , and when Z is a positive integer, R 12 is selected from the group consisting of the groups described by R 11 and a hydrogen atom.

Claim 23

The rubber composition of claim 19 wherein, in each of formulas III, IV, V, VI and VII, at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 , R 10 , R 11 and R 12 is a methyl radical.

Claim 24

The rubber composition of claim 19 wherein, in each of formulas III, IV, V, VI and VII, at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 , R 10 , R 11 and R 12 is an aliphatic radical containing from 12 to 22 carbon atoms.

Claim 25

The rubber composition of claim 19 wherein, in each of formulas III, IV, V, VI and VII, at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 , R 10 , R 11 and R 12 is an aliphatic radical containing a polyalkoxy radical containing from 2 to 15 repeating ethoxy radical units.

Claim 26

The rubber composition of claim 19 wherein, in each of formulas III, IV, V, VI and VII, at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 , R 10 , R 11 and R 12 is an araliphatic radical containing from 7 to 22 carbon atoms.

Claim 27

The rubber composition of claim 19 wherein R 6 is an alkylenyl radical containing from 2 to 6 carbon atoms.

Claim 28

The rubber composition of claim 19 wherein each of T and U is a radical which in conjunction with each nitrogen atom to which it is shown as attached in formula V, VI or VII forms a quaternary ammonium salt selected from the group consisting of pyrrolidinium, pyrrolium, pyrrolinium, imidazolium, pyrazolium, triazolium, pyridinium, pyrimidinium, pyridazinium, pyrazinium, triazinium, indolium, indazolium, benzimidazolium, quinolinium, isoquinolinium, cinnolinium, phthalazinium, quinazolinium, quinoxalinium, naphthyridinium, quinolizinium, carbazolium, acridinium, phenazinium, phenanthridinium, phenanthrolinium, benzoisoquinolinium, purinium, porphinium, and pteridinium, the heterocyclic rings being unsubstituted or substituted by at least one alkyl group, and the quaternary ammonium salts formed by partial or complete hydrogenation of the heterocyclic rings of any of the aforesaid quaternary ammonium salts.

Claim 29

The rubber composition of claim 19 wherein Z is zero or a positive integer from 1 to 5.

Claim 30

The rubber composition of claim 26 wherein Z is zero or 1.

Claim 31

The rubber composition of claim 19 wherein J is an inorganic radical.

Claim 32

The rubber composition of claim 1 wherein the median particle size of Agent G and of the adducts is in the range of from about 0.1 to about 5 microns.

Claim 33

The rubber composition of claim 1 wherein Agent G and the portions of the adducts contributed from Agent G are each at a level of from about 50 to about 150 phr.

Claim 34

The rubber composition of claim 1 wherein Agent H and the portions of the adducts contributed from Agent H are each at a level of from about 0.02 to about 3 phr.

Claim 35

The rubber composition of claim 1 wherein Agent I and the portions of the adducts contributed from Agent I are each at a level of from about 0.02 to about 3 phr.

Claim 36

A rubber composition comprising a substantially uniform dispersion in natural or synthetic rubber of: A. 1. particulate Agent G at a level of from about 5 to about 200 phr, 2. Agent H at a level of from about 0.005 to about 15 phr, and 3. Agent I at a level of from about 0.005 to about 15 phr; or B. 1. a particulate adduct of Agents G and H having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 5 to about 200 phr and the portion thereof contributed from Agent H is at a level of from about 0.005 to about 15 phr, and 2. Agent I at a level of from about 0.005 to about 15 phr; or C. 1. a particulate adduct of Agents G and I having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 5 to about 200 phr and the portion thereof contributed from Agent I is at a level of from about 0.005 to about 15 phr, and 2. Agent H at a level of from about 0.005 to about 15 phr; or D. a particulate adduct of Agents G, H, and I having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 5 to about 200 phr, the portion thereof contributed from Agent H is at a level of from about 0.005 to about 15 phr and the portion thereof contributed from Agent I is at a level of from about 0.005 to about 15 phr; or E.

Claim 37

A rubber composition comprising a substantially uniform dispersion in natural or synthetic rubber of: A. 1. particulate Agent G at a level of from about 5 to about 200 phr, 2. Agent H at a level of from about 0.005 to about 15 phr, and 3. Agent I at a level of from about 0.005 to about 15 phr; or B. 1. a particulate adduct of Agents G and H having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 5 to about 200 phr and the portion thereof contributed from Agent H is at a level of from about 0.005 to about 15 phr, and 2. Agent I at a level of from about 0.005 to about 15 phr; or C. 1. a particulate adduct of Agents G and I having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 5 to about 200 phr and the portion thereof contributed from Agent I is at a level of from about 0.005 to about 15 phr, and 2. Agent H at a level of from about 0.005 to about 15 phr; or D. a particulate adduct of Agents G, H, and I having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 5 to about 200 phr, the portion thereof contributed from Agent H is at a level of from about 0.005 to about 15 phr and the portion thereof contributed from Agent I is at a level of from about 0.005 to about 15 phr; or E.

Claim 38

a particulate adduct of Agents G and H having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 2.5 to about 100 phr and the portion thereof contributed from Agent H is at a level of from about 0.005 to about 15 phr, and 2. a particulate adduct of Agents G and I having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 2.5 to about 100 phr and the portion thereof contributed from Agent I is at a level of from about 0.005 to about 15 phr; or F. B, C, D or E above wherein the particulate adduct in B, C or D or at least one of the particulate adducts in E is also an adduct with the rubber; wherein Agent G comprises phyllosilicate mineral particles having a median particle size in the range of from about 0.01 to about 20 microns; wherein Agent H comprises an organosilane of formula I or II ##STR5## wherein X is a group which is, or which upon hydrolysis forms a group which is, capable of reacting with a reactive site on the phyllosilicate mineral particles so as to form a bond between the organosilane of formula I or II and the phyllosilicate mineral particles, wherein Y is an alkyl, aryl or alkyl-substituted aryl group containing from 1 to 40 carbon atoms and bears a functional group capable of reacting with a reactive site on the rubber so as to form a bond between the organosilane of formula I or II and the rubber, wherein R 1 and R 2 are the same or different and are each selected from the group consisting of the groups described by X and Y, an alkyl group containing from 1 to 20 carbon atoms, an aryl group, and an alkyl-substituted aryl group wherein the alkyl substituents contain a total of from 1 to 20 carbon atoms, and wherein K is an alkylenyl group containing from 1 to 20 carbon atoms or an alkyl sulfide or polysulfide group containing from 1 to 6 sulfur atoms and from 2 to 20 carbon atoms; and wherein Agent I comprises a quaternary ammonium salt.

Claim 39

a particulate adduct of Agents G and H having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 2.5 to about 100 phr and the portion thereof contributed from Agent H is at a level of from about 0.005 to about 15 phr, and 2. a particulate adduct of Agents G and I having a median particle size in the range of from about 0.01 to about 20 microns and present at a level such that the portion thereof contributed from Agent G is at a level of from about 2.5 to about 100 phr and the portion thereof contributed from Agent I is at a level of from about 0.005 to about 15 phr; or F. B, C, D or E above wherein the particulate adduct in B, C or D or at least one of the particulate adducts in E is also an adduct with the rubber; wherein Agent G comprises phyllosilicate mineral particles having a median particle size in the range of from about 0.01 to about 20 microns; wherein Agent H comprises an organosilane of formula I or II ##STR5## wherein X is a group which is, or which upon hydrolysis forms a group which is, capable of reacting with a reactive site on the phyllosilicate mineral particles so as to form a bond between the organosilane of formula I or II and the phyllosilicate mineral particles, wherein Y is an alkyl, aryl or alkyl-substituted aryl group containing from 1 to 40 carbon atoms and bears a functional group capable of reacting with a reactive site on the rubber so as to form a bond between the organosilane of formula I or II and the rubber, wherein R 1 and R 2 are the same or different and are each selected from the group consisting of the groups described by X and Y, an alkyl group containing from 1 to 20 carbon atoms, an aryl group, and an alkyl-substituted aryl group wherein the alkyl substituents contain a total of from 1 to 20 carbon atoms, and wherein K is an alkylenyl group containing from 1 to 20 carbon atoms or an alkyl sulfide or polysulfide group containing from 1 to 6 sulfur atoms and from 2 to 20 carbon atoms; and wherein Agent I comprises a quaternary ammonium salt.

Claim 40

The rubber composition of claim 33 wherein the rubber comprises natural or synthetic rubber.

Claim 41

The rubber composition of claim 34 wherein the rubber is natural or synthetic rubber.

Claim 42

The rubber composition of claim 35 wherein the rubber is natural rubber, polybutadiene rubber, polyisoprene rubber or styrene-butadiene rubber.

Claim 43

The rubber composition of claim 33 formed by a vulcanization process employing a sulfur or sulfur-donating curing agent.

Claim 44

The rubber composition of claim 33 wherein the phyllosilicate mineral is selected from the group consisting of a member of the kaolin group, a member of the mica group, a member of the group characterized by a primitive three-layer structure, a member of the group characterized by an expandable three-layer structure and a member of the group characterized by a four-layer structure.

Claim 45

The rubber composition of claim 38 wherein the phyllosilicate mineral is selected from the group consisting of kaolinite, muscovite, pyrophyllite, talc, vermiculite and chlorite.

Claim 46

The rubber composition of claim 39 wherein the phyllosilicate mineral is talc.

Claim 47

The rubber composition of claim 33 wherein X is a group which upon hydrolysis forms a hydroxyl group.

Claim 48

The rubber composition of claim 33 wherein X is selected from the group consisting of a halogen radical and --OR 13 and wherein R 13 is an alkyl group containing from 1 to 20 carbon atoms.

Claim 49

The rubber composition of claim 42 wherein X is --OR 13 and R 13 contains from 1 to 7 carbon atoms.

Claim 50

The rubber composition of claim 33 wherein the functional group on Y which is capable of reacting with a reactive site on the rubber is selected from the group consisting of a mercapto group, allyl group, vinyl group, epoxy group, methacryloxy group, acryloxy group and an amino group having an active hydrogen atom.

Claim 51

The rubber composition of claim 44 wherein the functional group on Y which is capable of reacting with a reactive site on the rubber is selected from the group consisting of mercapto, vinyl and an amino group having an active hydrogen atom.

Claim 52

The rubber composition of claim 33 wherein Y contains from 1 to 6 carbon atoms.

Claim 53

The rubber composition of claim 33 wherein R 1 and R 2 are the same or different and are each selected from the group consisting of the group described by X.

Claim 54

The rubber composition of claim 47 wherein R 1 and R 2 are the same or different and are each selected from the group consisting of a halogen radical and --OR 13 and wherein R 13 is an alkyl group containing from 1 to 20 carbon atoms.

Claim 55

The rubber composition of claim 48 wherein X, R 1 and R 2 are the same.

Claim 56

The rubber composition of claim 33 wherein the organosilane of formula I or II is selected from the group consisting of 3-aminopropyl-triethoxysilane, 3-mercaptopropyl-trimethoxysilane, and vinyl-tri-(2-methoxyethoxy) silane.

Claim 57

The rubber composition of claim 33 wherein the quaternary ammonium salt has a structure of formula III, IV, V, VI or VII: ##STR6## wherein Z is zero or a positive integer from 1 to 100, J is an anionic radical, n is the absolute value of the oxidation state of J, and R 6 is an alkylenyl radical containing from 2 to 20 carbon atoms or an aryl radical containing from 6 to 14 carbon atoms, wherein in formulas III and IV, R 3 , R 4 , R 5 , R 7 , R 8 and R 9 are the same or different and are each selected from the group consisting of: aliphatic radicals containing a total of from 1 to 3 carbon atoms which are saturated or unsaturated and unsubstituted or substituted with at least one hydroxy or alkoxy group; aliphatic radicals containing a total of from 8 to 40 carbon atoms which are saturated or unsaturated and unsubstituted or substituted with at least one hydroxy, alkoxy or polyalkoxy group; aryl radicals containing from 6 to 18 carbon atoms; and saturated or unsaturated araliphatic radicals containing a total of from 7 to 48 carbon atoms, wherein in formulas III and IV, when Z is zero, R 10 is selected from the group consisting of the groups described by R 3 , R 4 , R 5 , R 7 , R 8 and R 9 , and when Z is a positive integer, R 10 is selected from the group consisting of the groups described by R 3 , R 4 , R 5 , R 7 , R 8 and R 9 and a hydrogen atom, wherein in formulas III and IV, (1) at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 and R 10 is an aliphatic radical containing a total of from 1 to 3 carbon atoms and (2) either (a) at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 and R 10 is an aliphatic radical containing at least 12 carbon atoms or (b) at least two of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 and R 10 are aliphatic radicals containing at least 8 carbon atoms, wherein in formulas V, VI and VII, each of T and U is a radical which, in conjunction with each nitrogen atom to which it is shown attached in formula V, VI or VII, forms a heterocyclic radical containing at least one nitrogen atom in the ring system and containing only nitrogen and carbon atoms in the ring system, and the T and U portions of the ring system are unsubstituted or substituted by at least one alkyl group with the total number of ring substituents on each of T and U being from 1 to 32 carbon atoms, wherein in formulas V and VI, R 11 is selected from the group consisting of the groups described by R 3 , R 4 , R 5 , R 7 , R 8 and R 9 alkylamidoalkyl or alkylesteralkyl groups containing a total of at least 14 carbon atoms, and wherein in formulas V, VI and VII, when Z is zero, R 12 is selected from the group consisting of the groups described by R 11 and when Z is a positive integer, R 12 is selected from the group consisting of the groups described by R 11 and a hydrogen atom.

Claim 58

The rubber composition of claim 51 wherein, in each of formulas III, IV, V, VI, and VII, at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 , R 10 , R 11 and R 12 is a methyl radical.

Claim 59

The rubber composition of claim 51 wherein, in each of formulas III, IV, V, VI and VII, at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 , R 10 , R 11 and R 12 is an aliphatic radical containing from 12 to 22 carbon atoms.

Claim 60

The rubber composition of claim 51 wherein, in each of formulas III, IV, V, VI and VII, at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 , R 10 , R 11 and R 12 is an aliphatic radical containing a polyalkoxy radical containing from 2 to 15 repeating ethoxy radical units.

Claim 61

The rubber composition of claim 51 wherein, in each of formulas III, IV, V, VI and VII at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 , R 10 , R 11 and R 12 is an araliphatic radical containing from 7 to 22 carbon atoms.

Claim 62

The rubber composition of claim 51 wherein R 6 is an alkenyl radical containing from 2 to 6 carbon atoms.

Claim 63

The rubber composition of claim 51 wherein each of T and U is a radical which in conjunction with each nitrogen atom to which it is shown as attached in formula V, VI or VII forms a quaternary ammonium salt selected from the group consisting of pyrrolidinium, pyrrolium, pyrrolinium, imidazolium, pyrazolium, triazolium, pyridinium, pyrimidinium, pyridazinium, pyrazininium, triazinium, indolium, indazolium, benzimidazolium, quinolinium, isoquinolinium, cinnolinium, phthalazinium, quinazolinium, quinoxalinium, naphthyridinium, quinolizinium, carbazolium, acridinium, phenazinium, phenanthridinium, phenanthrolinium, benzo[H]isoquinolinium, purinium, porphinium, and pteridinium, the heterocyclic rings being unsubstituted or substituted by at least one alkyl group, and the quaternary ammonium salts formed by partial or complete hydrogenation of the heterocyclic rings of any of the aforesaid quaternary ammonium salts.

Claim 64

The rubber composition of claim 51 wherein Z is zero or a positive integer from 1 to 5.

Claim 65

The rubber composition of claim 58 wherein Z is zero or 1.

Claim 66

The rubber composition of claim 51 wherein J is an inorganic radical.

Claim 67

The rubber composition of claim 33 wherein the median particle size of Agent G and the adducts is in the range of from about 0.1 to about 5 microns.

Claim 68

The rubber composition of claim 33 wherein Agent G and the portions of the adducts contributed from Agent G are each at a level of from about 50 to about 150 phr.

Claim 69

The rubber composition of claim 33 wherein Agent H and the portions of the adducts contributed from Agent H are each at a level of from about 0.02 to about 3 phr.

Claim 70

The rubber composition of claim 33 wherein Agent I and the portions of the adducts contributed from Agent I are each at a level of from about 0.02 to about 3 phr.

Claim 71

A particulate adduct of Agents G, H, and I having a median particle size in the range of from about 0.01 to about 20 microns, wherein the concentration levels of Agents H and I are each in the range of from about 0.1 to about 7.5 weight percent, based on the weight of Agent G; wherein Agent G comprises phyllosilicate mineral particles having a median particle size in the range of from about 0.01 to about 20 microns; wherein Agent H comprises an organosilane of formula I or II ##STR7## wherein X is a group which is, or which upon hydrolysis forms a group which is, capable of reacting with a reactive site on the phyllosilicate mineral particles so as to form a bond between the organosilane of formula I or II and the phyllosilicate mineral particles, wherein Y is an alkyl, aryl or alkyl-substituted aryl group containing from 1 to 40 carbon atoms and bears a functional group capable of reacting with a reactive site on the rubber so as to form a bond between the organosilane of formula I or II and the rubber, wherein R 1 and R 2 are the same or different and are each selected from the group consisting of the groups described by X and Y, an alkyl group containing from 1 to 20 carbon atoms, an aryl group, and an alkyl-substituted aryl group wherein the alkyl substituents contain a total of from 1 to 20 carbon atoms, and wherein K is an alkylenyl group containing from 1 to 20 carbon atoms or an alkyl sulfide or polysulfide group containing from 1 to 6 sulfur atoms and from 2 to 20 carbon atoms; and wherein Agent I comprises a quaternary ammonium salt.

Claim 72

A particulate adduct of Agents G, H, and I having a median particle size in the range of from about 0.01 to about 20 microns, wherein the concentration levels of Agents H and I are each in the range of from about 0.1 to about 7.5 weight percent, based on the weight of Agent G; wherein Agent G comprises phyllosilicate mineral particles having a median particle size in the range of from about 0.01 to about 20 microns; wherein Agent H comprises an organosilane of formula I or II ##STR7## wherein X is a group which is, or which upon hydrolysis forms a group which is, capable of reacting with a reactive site on the phyllosilicate mineral particles so as to form a bond between the organosilane of formula I or II and the phyllosilicate mineral particles, wherein Y is an alkyl, aryl or alkyl-substituted aryl group containing from 1 to 40 carbon atoms and bears a functional group capable of reacting with a reactive site on the rubber so as to form a bond between the organosilane of formula I or II and the rubber, wherein R 1 and R 2 are the same or different and are each selected from the group consisting of the groups described by X and Y, an alkyl group containing from 1 to 20 carbon atoms, an aryl group, and an alkyl-substituted aryl group wherein the alkyl substituents contain a total of from 1 to 20 carbon atoms, and wherein K is an alkylenyl group containing from 1 to 20 carbon atoms or an alkyl sulfide or polysulfide group containing from 1 to 6 sulfur atoms and from 2 to 20 carbon atoms; and wherein Agent I comprises a quaternary ammonium salt.

Claim 73

The adduct of claim 65 wherein the phyllosilicate mineral is selected from the group consisting of a member of the kaolin group, a member of the mica group, a member of the group characterized by a primitive three-layer structure, a member of the group characterized by an expandable three-layer structure and a member of the group characterized by a four-layer structure.

Claim 74

The adduct of claim 66 wherein the phyllosilicate mineral is selected from the group consisting of kaolinite, muscovite, pyrophyllite, talc, vermiculite and chlorite.

Claim 75

The adduct of claim 67 wherein the phyllosilicate mineral is talc.

Claim 76

The adduct of claim 65 wherein X is a group which upon hydrolysis forms a hydroxyl group.

Claim 77

The adduct of claim 65 wherein X is selected from the group consisting of a halogen radical and --OR 13 and wherein R 13 is an alkyl group containing from 1 to 20 carbon atoms.

Claim 78

The adduct of claim 70 wherein X is --OR 13 , and R 13 contains from 1 to 7 carbon atoms.

Claim 79

The adduct of claim 65 wherein the functional group on Y which is capable of reacting with a reactive site on the rubber is selected from the group consisting of a mercapto group, allyl group, vinyl group, epoxy group, methacryloxy group, acryloxy group, and an amino group having an active hydrogen atom.

Claim 80

The adduct of claim 72 wherein the functional group on Y which is capable of reacting with a reactive site on the rubber is selected from the group consisting of a mercapto group, a vinyl group and an amino group having an active hydrogen atom.

Claim 81

The adduct of claim 65 wherein Y contains from 1 to 6 carbon atoms.

Claim 82

The adduct of claim 65 wherein R 1 and R 2 are the same or different and are each selected from the group consisting of the group described by X.

Claim 83

The adduct of claim 75 wherein R 1 and R 2 are the same or different and are each selected from the group consisting of a halogen radical and --OR 13 and wherein R 13 is an alkyl group containing from 1 to 20 carbon atoms.

Claim 84

The adduct of claim 76 wherein X, R 1 and R 2 are the same.

Claim 85

The adduct of claim 65 wherein the organosilane of formula I or II is selected from the group consisting of 3-aminopropyl-triethoxysilane, 3-mercaptopropyl-trimethoxysilane and vinyl-tri-(2-methoxyethoxy)silane.

Claim 86

The adduct of claim 65 wherein the quaternary ammonium salt has a structure of formula III, IV, V, VI or VII: ##STR8## wherein Z is zero or a positive integer from 1 to 100, J is an anionic radical, n is the absolute value of the oxidation state of J, and R 6 is an alkylenyl radical containing from 2 to 20 carbon atoms or an aryl radical containing from 6 to 14 carbon atoms, wherein in formulas III and IV, R 3 , R 4 , R 5 , R 7 , R 8 and R 9 are the same or different and are each selected from the group consisting of: aliphatic radicals containing a total of from 1 to 3 carbon atoms which are saturated or unsaturated and unsubstituted or substituted with at least one hydroxy or alkoxy group; aliphatic radicals containing a total of from 8 to 40 carbon atoms which are saturated or unsaturated and unsubstituted or substituted with at least one hydroxy, alkoxy or polyalkoxy group; aryl radicals containing from 6 to 18 carbon atoms; and saturated or unsaturated araliphatic radicals containing a total of from 7 to 48 carbon atoms, wherein in formulas III and IV, when Z is zero, R 10 is selected from the group consisting of the groups described by R 3 , R 4 , R 5 , R 7 , R 8 and R 9 , and when Z is a positive integer, R 10 is selected from the group consisting of the groups described by R 3 , R 4 , R 5 , R 7 , R 8 and R 9 and a hydrogen atom, wherein in formulas III and IV, (1) at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 and R 10 is an aliphatic radical containing a total of from 1 to 3 carbon atoms and (2) either (a) at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 and R 10 is an aliphatic radical containing at least 12 carbon atoms or (b) at least two of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 and R 10 are aliphatic radicals containing at least 8 carbon atoms, wherein in formulas V, VI, and VII, each of T and U is a radical which, in conjunction with each nitrogen atom to which it is shown attached in formula V, VI or VII, forms a heterocyclic radical containing at least one nitrogen atom in the ring system and containing only nitrogen and carbon atoms in the ring system, and the T and U portions of the ring system are unsubstituted or substituted by at least one alkyl group with the total number of ring substituents on each of T and U being from 1 to 32 carbon atoms, wherein in formulas V and VI, R 11 is selected from the group consisting of the groups described by R 3 , R 4 , R 5 , R 7 , R 8 and R 9 and alkylamidoalkyl or alkylesteralkyl groups containing a total of at least 14 carbon atoms, and wherein in formulas V, VI and VII, when Z is zero, R 12 is selected from the group consisting of the groups described by R 11 , and when Z is a positive integer, R 12 is selected from the group consisting of the groups described by R 11 and a hydrogen atom.

Claim 87

The adduct of claim 79 wherein, in each of formulas III, IV, V, VI and VII, at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 , R 10 , R 11 and R 12 is a methyl radical.

Claim 88

The adduct of claim 79 wherein, in each of formulas III, IV, V, VI and VII, at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 , R 10 , R 11 and R 12 is an aliphatic radical containing from 12 to 22 carbon atoms.

Claim 89

The adduct of claim 79 wherein, in each of formulas III, IV, V, VI and VII, at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 , R 10 , R 11 and R 12 is an aliphatic radical containing a polyalkoxy radical containing from 2 to 15 repeating ethoxy radical units.

Claim 90

The adduct of claim 79 wherein, in each of formulas III, IV, V, VI and VII, at least one of R 3 , R 4 , R 5 , R 7 , R 8 , R 9 , R 10 , R 11 and R 12 is an araliphatic radical containing from 7 to 22 carbon atoms.

Claim 91

The adduct of claim 79 wherein R 6 is an alkylenyl radical containing from 2 to 6 carbon atoms.

Claim 92

The adduct of claim 79 wherein each of T and U is a radical which in conjunction with each nitrogen atom to which it is shown as attached in formula V, VI or VII forms a quaternary ammonium salt selected from the group consisting of pyrrolidinium, pyrrolium, pyrrolinium, imidazolium, pyrazolium, triazolium, pyridinium, pyrimidinium, pyridazinium, pyrazinium, triazinium, indolium, indazolium, benzimidazolium, quinolinium, isoquinolinium, cinnolinium, phthalazinium, quinazolinium, quinoxalinium, naphthyridinium, quinolizinium, carbazolium, acridinium, phenazinium, phenanthridinium, phenanthrolinium, benzo[H]isoquinolinium, purinium, porphinium, and pteridinium, the heterocyclic rings being unsubstituted or substituted by at least one alkyl group, and the quaternary ammonium salts formed by partial or complete hydrogenation of the heterocyclic rings of any of the aforesaid quaternary ammonium salts.

Claim 93

The adduct of claim 79 wherein Z is zero or a positive integer from 1 to 5.

Claim 94

The adduct of claim 86 wherein Z is zero or 1.

Claim 95

The adduct of claim 79 wherein J is an inorganic radical.

Claim 96

The adduct of claim 65 having the median particle size in the range of from about 0.1 to about 5 microns.

Claim 97

The adduct of claim 65 wherein Agent H is at a level of from about 0.5 to about 1.5 weight percent, based on the weight of Agent G.

Claim 98

The adduct of claim 65 wherein Agent I is at a level of from about 0.5 to about 1.5 weight percent, based on the weight of Agent G.