# US 2014/0155518 A1 · Rubber mixtures containing silicic acid and sulfur-containing additives

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- Number: US 2014/0155518 A1
- Document ID: US20140155518A1
- Status: Published application
- Kind: A1
- Application number: 14/114,362
- Filed: 2012-04-27
- Published: 2014-06-05
- Earliest claimed: 2011-04-29
- Assignees: LANXESS Deutschland GmbH
- Inventors: Melanie Wiedemeier; Hermann-Josef Weidenhaupt; Ulrich Feldhues; Irene Moll
- Web page: https://patentgrep.com/patent/US20140155518A1

## CPC

- C08K 13/02: Organic and inorganic ingredients
- B29B 7/005: {for mixing in batches}
- B29B 7/286: {measuring properties of the mixture, e.g. temperature, density (B29B7/283 takes precedence)}
- B29B 7/7495: {for mixing rubber}
- B29B 7/90: Fillers or reinforcements {, e.g. fibres}
- B60C 1/00: Tyres characterised by the chemical composition or the physical arrangement or mixture of the composition
- C08K 3/36: Silica
- C08K 5/372: Sulfides {, e.g. R-(S)x-R'}
- C08K 5/378: containing heterocyclic rings
- C08K 5/548: containing sulfur {(C08K5/5477 takes precedence)}
- C08L 9/00: Compositions of homopolymers or copolymers of conjugated diene hydrocarbons
- C08L 9/06: Copolymers with styrene
- B29B 7/183: {having a casing closely surrounding the rotors, e.g. of Banbury type (with single shaft B29B7/125)}
- C08K: Use of inorganic or non-macromolecular organic substances as compounding ingredients (paints, inks, varnishes, dyes, polishes, adhesives C09)
- B29B: PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
- B60C: VEHICLE TYRES; TYRE INFLATION; TYRE CHANGING; CONNECTING VALVES TO INFLATABLE ELASTIC BODIES IN GENERAL; DEVICES OR ARRANGEMENTS RELATED TO TYRES
- C08L: COMPOSITIONS OF MACROMOLECULAR COMPOUNDS (compositions based on polymerisable monomers C08F, C08G; artificial filaments or fibres D01F; textile treating compositions D06)

## Abstract

The present invention relates to silica-containing rubber mixture produced from at least one rubber, from a sulphur-containing alkoxysilane, from a crosslinking agent, from a filler, and optionally from further rubber auxiliaries, where the said mixture comprises from 0.1 to 15 parts by weight, based on 100 parts by weight of rubber used, of a silicon-free polysulphide additive of the formula (I) A-S—(S)x—S—B (I) in which x is 0, 1, 2, 3 or 4, A is a moiety and B is a moiety in which R1 to R4 are identical or different and are hydrogen, C1-C6-alkyl, C5-C6-cycloalkyl, C6-C10-aryl or a group —CH2—OR5, —CH2—CH2—OR5, —NHR5, —COR5, —COOR5, —CH2COOR5, where R5=hydrogen, C1-C6-alkyl, C5-C6-cycloalkyl, C6-C10-aryl or C1-C6-acyl, and R6 to R7 are identical or different and are hydrogen C1-C6-alkyl, C5-C6-cycloalkyl, C6-C10-aryl or a group —CH2—OR5, —CH2—CH2—OR5, —NHR5, —COR5, —COOR5, —CH2COOR5, with R5=hydrogen, C1-C6-alkyl, C5-C6-cycloalkyl, C6-C10-aryl or C1-C6-acyl and y, z are mutually independently 0, 1 or 2, or A and B are mutually independently one of the moieties in which R1 and R2 are identical or different and are hydrogen, C1-C6-alkyl, C5-C6-cycloalkyl, C6-C10-aryl or a group —CH2—OR5, —CH2—CH2—OR5, —NHR5, —COR5, —COOR5, —CH2COOR5, where R5=hydrogen, C1-C6-alkyl, C5-C6-cycloalkyl, C6-C10-aryl or C1-C6-acyl.

## Claims

### Claim 1

Silica-containing rubber mixture produced from at least one rubber, from a sulphur-containing alkoxysilane, from a crosslinking agent, from a filler, and optionally from further rubber auxiliaries, characterized in that the said mixture comprises from 0.1 to 15 parts by weight, based on 100 parts by weight of rubber used, of a silicon-free polysulphide additive of the formula (I)
A-S—(S)x—S—B (I)
in which x is 0, 1, 2, 3 or 4,
A is a moiety
and
B is a moiety
in which
R1 to R4 are identical or different and are hydrogen, C1-C6-alkyl, C5-C6-cycloalkyl, C6-C10-aryl or a group —CH2—OR5, —CH2—CH2—OR5, —NHR5, —COR5, —COOR5, —CH2COOR5, where R5=hydrogen, C1-C6-alkyl, C5-C6-cycloalkyl, C6-C10-aryl or C1-C6-acyl, and
R6 to R7 are identical or different and are hydrogen C1-C6-alkyl, C5-C6-cycloalkyl, C6-C10-aryl or a group —CH2—OR5, —CH2—CH2—OR5, —NHR5, —COR5, —COOR5, —CH2COOR5, with R5=hydrogen, C1-C6-alkyl, C5-C6-cycloalkyl, C6-C10-aryl or C1-C6-acyl and
y, z are mutually independently 0, 1 or 2, or
A and B are mutually independently one of the moieties
in which R1 and R2 are identical or different and are hydrogen, C1-C6-alkyl, C5-C6-cycloalkyl, C6-C10-aryl or a group —CH2—OR5, —CH2—CH2—OR5, —NHR5, —COR5, —COOR5, —CH2COOR5, where R5=hydrogen, C1-C6-alkyl, C5-C6-cycloalkyl, C6-C10-aryl or C1-C6-acyl.

### Claim 2 (depends on 1)

Silica-containing rubber mixture according to claim 1, characterized in that at least one compound of the formula (II) is used as the polysulphide additive,
in which x is 0, 1, 2, 3 or 4, particularly preferably 2.

### Claim 3 (depends on 1)

Silica-containing rubber mixture according to claim 1, characterized in that at least one compound of the formula (IIa) is used as the polysulphide additive,
in which x is 0, 1, 2, 3 or 4, particularly preferably 2.

### Claim 4 (depends on 1)

Silica-containing rubber mixture according to claim 1, characterized in that at least one compound of the formulae (III), (IIIa), (IIIb) is used as the polysulphide additive,
in which x is 0, 1, 2, 3 or 4, particularly preferably 2 and 0.

### Claim 5

Silica-containing rubber mixture according to any of the preceding claims, characterized in that the amount of sulphur-containing alkoxysilanes is greater than or equal to the amount of silicon-free polysulphide additives.

### Claim 6

Silica-containing rubber mixture according to any of the preceding claims, characterized in that it comprises at least one SBR rubber and at least one BR rubber.

### Claim 7 (depends on 6)

Silica-containing rubber mixture according to claim 6, characterized in that it comprises at least one SBR rubber and at least one BR rubber in an SBR:BR ratio by weight of from 60:40 to 90:10.

### Claim 8 (depends on 7)

Silica-containing rubber mixture according to claim 7, characterized in that it also comprises at least one NR rubber.

### Claim 9 (depends on 8)

Silica-containing rubber mixture according to claim 8, characterized in that it comprises at least one SBR rubber and at least one BR rubber and at least one NR rubber in a ratio of at least 60 and at most 85 percent by weight of SBR, based on rubber, and at least 10 and at most 35 percent by weight of BR, based on rubber, and at least 5 and at most 20 percent by weight of NR, based on rubber.

### Claim 10

Silica-containing rubber mixture according to any of the preceding claims, characterized in that it comprises from 1 to 15 parts by weight of one or more sulphur-containing alkoxysilanes, based on 100 parts by weight of rubber used.

### Claim 11

Silica-containing rubber mixture according to any of the preceding claims, characterized in that it comprises from 0.3 to 7 parts by weight of one or more silicon-free polysulphide additives, based on 100 parts by weight of rubber used.

### Claim 12

Silica-containing rubber mixture according to any of the preceding claims, characterized in that the sulphur-containing alkoxysilane is used in a ratio by weight of from 1.5:1 to 20:1, preferably from 5:1 to 15:1, in relation to the silicon-free polysulphide additive.

### Claim 13

Silica-containing rubber mixture according to any of the preceding claims, characterized in that the said mixture comprises from 0.5 to 5 parts by weight, based on 100 parts by weight of rubber used, of a silicon-free polysulphide additive.

### Claim 14

Silica-containing rubber mixture according to any of the preceding claims, characterized in that it comprises one or more inorganic and/or organic fillers, where the amounts used of the fillers are in the range from 50 to 200 parts by weight, preferably from 60 to 120 parts by weight, based on 100 parts by weight of rubbers used.

### Claim 15 (depends on 14)

Silica-containing rubber mixture according to claim 14, characterized in that the fillers are selected from the group of oxidic and silicatic fillers and carbon blacks or a mixture of these.

### Claim 16 (depends on 15)

Silica-containing rubber mixture according to claim 15, characterized in that at least one filler is selected from the group of precipitated silicas and/or silicates with a specific surface area of from 20 to 400 m2/g, preferably with a specific surface area of from 100 to 200 m2/g.

### Claim 17

Silica-containing rubber mixture according to any of the preceding claims, characterized in that the loss factor tan delta of a vulcanizate produced therefrom by heating at 170° C./t95 is <0.2 at 60° C. and the Shore A hardness thereof is simultaneously >67 at 23° C. and the 300 modulus value thereof is >12 MPa, preferably >15 MPa.

### Claim 18

Silica-containing rubber mixture according to any of the preceding claims, characterized in that the loss factor tan delta of a vulcanizate produced therefrom by heating at 170° C./t95 is <0.17 at 60° C. and the Shore A hardness thereof is simultaneously >70 at 23° C.

### Claim 19

Silica-containing rubber mixture according to any of the preceding claims, characterized in that the loss factor tan delta of a vulcanizate produced therefrom by heating at 170° C./t95 is less than 0.17 at 60° C. and its scorch time is simultaneously greater than 1000 seconds.

### Claim 20

Silica-containing rubber mixture according to any of the preceding claims, characterized in that the loss factor tan delta of a vulcanizate produced therefrom by heating at 170° C./t95 is less than 0.17 at 60° C. and its full vulcanization time is simultaneously less than 2000 seconds.

### Claim 21

Silica-containing rubber mixture according to any of the preceding claims, characterized in that the scorch time of a vulcanizate produced therefrom by heating at 170° C./t95 is greater than 1000 seconds and its full vulcanization time is simultaneously less than 2000 seconds.

### Claim 22 (depends on 1, 2, 3, 4)

Silica-containing mixture according to claims 1 to 4, characterized in that the ML 1+4 viscosity of the mixture at 100° C. is less than 150, preferably less than 100, particularly preferably less than 95.

### Claim 23

Use of the rubber mixture according to any of the preceding claims for producing vulcanizates and rubber mouldings of any type, in particular for producing tyres and tyre components.

### Claim 24

Vulcanizates and rubber mouldings of any type, in particular tyres and tyre components, based on rubber mixtures according to any of the preceding claims.

### Claim 25

Polysulphide additives of the formula