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Vulcanized Rubber Composition, Pneumatic Tire

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Vulcanized Rubber Composition, Pneumatic Tire (19) & (11) EP 2 072 574 B1 (12) EUROPEAN PATENT SPECIFICATION (45) Date of publication and mention (51) Int Cl.: of the grant of the patent: C08L 7/00 (2006.01) B60C 1/00 (2006.01) 25.04.2012 Bulletin 2012/17 C08L 1/10 (2006.01) C08L 9/00 (2006.01) B60C 15/04 (2006.01) (21) Application number: 08830800.2 (86) International application number: (22) Date of filing: 04.09.2008 PCT/JP2008/065931 (87) International publication number: WO 2009/034902 (19.03.2009 Gazette 2009/12) (54) VULCANIZED RUBBER COMPOSITION, PNEUMATIC TIRE, AND THEIR PRODUCTION METHODS VULKANISIERTE KAUTSCHUKZUSAMMENSETZUNG, LUFTREIFEN UND HERSTELLUNGSVERFAHREN DAFÜR COMPOSITION DE CAOUTCHOUC VULCANISÉ, PNEU ET LEURS PROCÉDÉS DE FABRICATION (84) Designated Contracting States: • ICHIKAWA, Naoya DE Kobe-shi Hyogo 651-0072 (JP) (30) Priority: 10.09.2007 JP 2007234080 • HATTORI, Takayuki 02.09.2008 JP 2008224908 Kobe-shi Hyogo 651-0072 (JP) (43) Date of publication of application: 24.06.2009 Bulletin 2009/26 (74) Representative: Manitz, Finsterwald & Partner GbR (73) Proprietor: Sumitomo Rubber Industries, Ltd. Martin-Greif-Strasse 1 Kobe-shi, Hyogo 651-0072 (JP) 80336 München (DE) (72) Inventors: (56) References cited: • YANO, Hiroyuki EP-A1- 1 650 253 WO-A1-2005/092971 Uji-shi CS-B1- 237 729 JP-A- 11 078 437 Kyoto 611-0011 (JP) JP-A- 2002 524 618 JP-A- 2003 064 221 • ISOBE, Yukio JP-A- 2006 206 837 JP-A- 2006 206 864 Kobe-shi US-A- 2 486 720 US-A- 2 650 891 Hyogo 651-0072 (JP) US-A- 4 508 860 Note: Within nine months of the publication of the mention of the grant of the European patent in the European Patent Bulletin, any person may give notice to the European Patent Office of opposition to that patent, in accordance with the Implementing Regulations. Notice of opposition shall not be deemed to have been filed until the opposition fee has been paid. (Art. 99(1) European Patent Convention). EP 2 072 574 B1 Printed by Jouve, 75001 PARIS (FR) EP 2 072 574 B1 Description TECHNICAL FIELD 5 [0001] The present invention relates to an environmentally conscious vulcanized rubber composition and a pneumatic tire produced by using the same. BACKGROUND ART 10 [0002] Heretofore, there have been known technologies of improving the hardness and the modulus of a rubber by reinforcing the rubber with staple fibers such as aramid and cellulose, or with a crystalline polymer such as syndiotactic polybutadiene, thereby increasing the complex modulus (E*) at for example 70°C to improve steering stability (JP 2005 133025 (patent document 1)) [0003] JP 20005 133025 (patent document 1) proposes a rubber composition composed of a diene-based rubber 15 component, starch and cellulose for the purpose of providing a rubber composition excellent in abrasion resistance. It also proposes to use bacterial cellulose as the cellulose. However, the technologies of patent document 1 are problematic in poor rupture characteristics and large energy loss at the interface between a rubber and cellulose because of poor compatibility of the rubber and the cellulose. [0004] JP 2005 075856 (patent document 2) discloses a rubber composition prepared by incorporating a fine powdery 20 cellulose fiber prepared from natural vegetable fiber into a diene-based rubber as a rubber composition that can exert low repellency and rigidity (steering stability) simultaneously. However, the technology of patent document 2 has some room for improvement for obtaining rigidity and reinforcing property suitable for the incorporated amount of cellulose fibers for reasons of being short of fiber length of a cellulose fiber in a production method [0005] Therefore, it is still difficult to obtain a vulcanized rubber composition that is environmentally conscious and 25 excellent in rupture characteristics and that causes less energy loss. Patent document 1: Japanese Patent Laying-Open No. 2005-133025 Patent document 2: Japanese Patent Laying-Open No. 2005-075856 [0006] US 2,650,891 discloses a rubber composition for a tire comprising modified cellulose fibers, which are pretreated with a 2,2’-diaminodialkyl-sulfide (cf. D1, column 2, lines 11 to 14). CS 237,729 relates to a vulcanizable rubber mixture 30 containing chemically treated, short cellulose fibers. DISCLOSURE OF THE INVENTION PROBLEMS TO BE SOLVED BY THE INVENTION 35 [0007] The present invention intends to solve the above problems to provide a vulcanized rubber composition that is environmentally conscious and that has both excellent rupture characteristics and a low energy loss, and a pneumatic tire produced by using the vulcanized rubber composition that is environmentally conscious and that is excellent in rolling resistance property, steering stability and durability. 40 MEANS FOR SOLVING THE PROBLEMS [0008] The present invention provides a vulcanized rubber composition including a rubber component composed of at least any one of a natural rubber, a modified natural rubber an acrylonitrile- butadiene rubber and a butadiene rubber 45 and chemically modified microfibril cellulose, wherein the chemical modification in the chemically modified microfibril cellulose is at least one selected from the group consisting of acetylation, alkyl esterification, complex esterification, β- ketoesterification, alkyl carbamatation and aryl carbamatation, and wherein the chemically modified microfibril cellulose has an average fiber diameter within the range of 4 nm to 1 Pm. [0009] In the vulcanized rubber composition of the present invention, it is preferable that the chemically modified 50 microfibril cellulose have been chemically modified to have a substitution degree within the range of 0.2 to 2.5, wherein the substitution degree is the average number of the hydroxyl groups of the cellulose substituted with other functional groups through chemical modification among the hydroxyl groups of cellulose per glucose ring unit. [0010] In the vulcanized rubber composition of the present invention, it is preferable that the content of the chemically modified microfibril cellulose be within the range of 1 to 50 parts by mass relative to 100 parts by mass of the rubber 55 component. [0011] In the vulcanized rubber composition of the present invention, it is preferable that the rubber component be composed of at least either a natural rubber or a modified natural rubber. [0012] The present invention also provides a pneumatic tire comprising the aforementioned vulcanized rubber com- 2 EP 2 072 574 B1 position. [0013] Moreover, the present invention provides a method of producing the aforementioned vulcanized rubber com- position including mixing, to a rubber latex containing at least one rubber component of a natural rubber, a modified natural rubber an acrylonitrile-butadiene rubber and a butadiene rubber, 1 to 50 parts by mass, relative to 100 parts by 5 mass of the rubber component, of chemically modified microfibril cellulose, followed by drying to prepare a masterbatch, wherein the chemical modification in the chemically modified microfibril cellulose is at least one selected from the group consisting of acetylation, alkyl esterification, complex esterification,β -ketoesterification, alkyl carbamatation and aryl carbamatation, and wherein the chemically modified microfibril cellulose has an average fiber diameter within the range of 4 nm to 1 Pm. 10 [0014] In the method of producing the vulcanized rubber composition of the present invention, it is preferable that the mixing be a mixing method using a high-speed disperser. [0015] In the method of producing the vulcanized rubber composition of the present invention, it is preferable that the drying be a drying method of any one of drying in a heating oven, air-drying and pulse drying. [0016] In the method of producing the vulcanized rubber composition of the present invention, it is preferable that the 15 chemically modified microfibril cellulose have been chemically modified so as to have a substitution degree within the range of 0.2 to 2.5. [0017] The present invention also provides a method of producing a pneumatic tire including the steps of: kneading a compounding agent to a masterbatch prepared in the method of producing the vulcanized rubber composition, adding a vulcanizing agent and a vulcanization accelerator and kneading, and vulcanizing the mixture under an application of 20 pressure and heating in a tire mold. EFFECTS OF THE INVENTION [0018] According to the present invention, it becomes possible to provide a vulcanized rubber composition that is 25 environmentally conscious and at the same time, has both excellent rupture characteristics and a low energy loss, and a pneumatic tire produced by using the vulcanized rubber composition that is environmentally conscious and that is excellent in rolling resistance property, steering stability and durability. BRIEF DESCRIPTION OF THE DRAWINGS 30 [0019] Fig. 1 is a schematic sectional view showing an example of the pneumatic tire of the present invention. DESCRIPTION OF THE REFERENCE SIGNS 35 [0020] 1 pneumatic tire, 2 tread portion, 3 sidewall portion, 4 bead portion, 5 bead core, 6 carcass, 7 belt layer, 8 bead apex rubber, 9 inner liner rubber, 2a cap tread, 2b base tread, 3G sidewall rubber, 4G clinch rubber. BEST MODES FOR CARRYING OUT THE INVENTION 40 [0021] The vulcanized rubber composition according to the present invention contains a rubber component composed of at least one of a natural rubber, a modified natural rubber an acrylonitrile-butadiene rubber and a butadiene rubber and chemically modified microfibril cellulose, wherein the chemical modification in
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