JP2005133025A - Rubber composition - Google Patents

Rubber composition Download PDF

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JP2005133025A
JP2005133025A JP2003372908A JP2003372908A JP2005133025A JP 2005133025 A JP2005133025 A JP 2005133025A JP 2003372908 A JP2003372908 A JP 2003372908A JP 2003372908 A JP2003372908 A JP 2003372908A JP 2005133025 A JP2005133025 A JP 2005133025A
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cellulose
weight
starch
parts
rubber composition
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Katsumi Terakawa
克美 寺川
Tetsuro Mizoguchi
哲朗 溝口
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Sumitomo Rubber Industries Ltd
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Sumitomo Rubber Industries Ltd
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Abstract

<P>PROBLEM TO BE SOLVED: To provide a rubber composition, particularly a rubber composition which is for use in tires and is excellent in the wear resistance. <P>SOLUTION: The composition comprises a blend of a diene-based rubber component with a starch and a cellulose. The cellulose has a fiber diameter of preferably 1 μm or less. It is preferable that the composition has a content of the starch of 5-75 parts by weight and a content of the cellulose of 0.1-40 parts by weight relative to 100 parts by weight of the diene-based rubber component. The cellulose is preferably a bacteria cellulose. <P>COPYRIGHT: (C)2005,JPO&NCIPI

Description

本発明はゴム組成物に関し、とりわけタイヤ用ゴム組成物に関する。   The present invention relates to a rubber composition, and more particularly to a rubber composition for a tire.

従来より、タイヤ用ゴム組成物に多糖類を配合することが提案されている。たとえば、特許文献1には、シリカの一部を澱粉/可塑剤・複合材で置換することにより、転がり抵抗を低減させる技術が開示されている。また、特許文献2および3には、ジエン系ゴムに米殻のもみ殻などのセルロース粉体を配合することによって、氷雪上性能を改善する技術が開示されている。   Conventionally, it has been proposed to blend a polysaccharide into a tire rubber composition. For example, Patent Document 1 discloses a technique for reducing rolling resistance by replacing part of silica with starch / plasticizer / composite. Patent Documents 2 and 3 disclose techniques for improving performance on ice and snow by blending cellulose powder such as rice hulls with diene rubber.

しかしながら、澱粉単独では、シリカやカーボンブラックなどの補強剤と比べて補強性に劣るため、耐摩耗性に問題があった。また、セルロース単独では、粘度が高くなり過ぎる等、加工性に問題があった。   However, starch alone has a problem in wear resistance because it is inferior in reinforcing properties as compared with reinforcing agents such as silica and carbon black. In addition, cellulose alone has a problem in processability, such as excessively high viscosity.

特開2003−192832号公報JP 2003-192832 A 特開2000−351304号公報JP 2000-351304 A 特開2000−129038号公報JP 2000-129038 A

本発明は、耐摩耗性に優れるゴム組成物を提供することを目的とする。   An object of this invention is to provide the rubber composition excellent in abrasion resistance.

すなわち、本発明は、ジエン系ゴム成分、澱粉およびセルロースからなるゴム組成物に関する。   That is, the present invention relates to a rubber composition comprising a diene rubber component, starch and cellulose.

前記ゴム組成物において、セルロースの繊維直径は、1μm以下であることが好ましい。ジエン系ゴム成分100重量部に対して、澱粉の含有量が5〜75重量部であり、セルロースの含有量が0.1〜40重量部であることが好ましい。また、セルロースがバクテリアセルロースであることが好ましい。   In the rubber composition, the fiber diameter of cellulose is preferably 1 μm or less. The starch content is preferably 5 to 75 parts by weight and the cellulose content is preferably 0.1 to 40 parts by weight with respect to 100 parts by weight of the diene rubber component. In addition, the cellulose is preferably bacterial cellulose.

本発明によれば、ジエン系ゴム成分に、澱粉およびセルロースを配合することにより、耐摩耗性が改善されたゴム組成物を得ることができる。   According to the present invention, a rubber composition with improved wear resistance can be obtained by blending starch and cellulose with a diene rubber component.

本発明のゴム組成物は、ジエン系ゴム成分に澱粉およびセルロースを配合することによって得られる。   The rubber composition of the present invention can be obtained by blending starch and cellulose with a diene rubber component.

本発明に用いられるジエン系ゴム成分としては、天然ゴム、エポキシ化天然ゴム、イソプレンゴム、スチレン−ブタジエンゴム、ブタジエンゴム、アクリロニトリル−ブタジエンゴム、ブチルゴム、エチレン−プロピレン−ジエンゴムなどをあげることができる。   Examples of the diene rubber component used in the present invention include natural rubber, epoxidized natural rubber, isoprene rubber, styrene-butadiene rubber, butadiene rubber, acrylonitrile-butadiene rubber, butyl rubber, and ethylene-propylene-diene rubber.

澱粉は、通常、アミロースの繰り返し単位(グルコシド結合により結合されたアンヒドログルコピラノース単位)と分枝鎖構造を構成するアミロペクチンの繰り返し単位とからなる糖鎖である。   Starch is usually a sugar chain composed of amylose repeating units (anhydroglucopyranose units linked by glucoside bonds) and amylopectin repeating units constituting a branched chain structure.

本発明に用いられる澱粉としては、とくに限定はなく、とうもろこし、タピオカ、じゃがいも、小麦、米、サゴヤシ、さつまいもなどを原料として得られる。また、アセチル化澱粉、エーテル化澱粉、リン酸化澱粉、スルフォン化澱粉、アミノ化澱粉、デキストリン、アルファー化澱粉、酸処理澱粉などの各種化工澱粉を用いることもできる。   The starch used in the present invention is not particularly limited, and can be obtained using corn, tapioca, potato, wheat, rice, sago palm, sweet potato and the like as raw materials. Various modified starches such as acetylated starch, etherified starch, phosphorylated starch, sulfonated starch, aminated starch, dextrin, pregelatinized starch, and acid-treated starch can also be used.

前記澱粉の含有量は、前記ジエン系ゴム成分100重量部に対して、5〜75重量部であることが好ましい。前記澱粉の含有量の下限については15重量部であることがより好ましく、上限については60重量部であることがより好ましい。澱粉の含有量が5重量部未満では、補強効果が得られない傾向があり、75重量部をこえると、硬くなりすぎる傾向がある。   The starch content is preferably 5 to 75 parts by weight with respect to 100 parts by weight of the diene rubber component. The lower limit of the starch content is more preferably 15 parts by weight, and the upper limit is more preferably 60 parts by weight. If the starch content is less than 5 parts by weight, there is a tendency that the reinforcing effect cannot be obtained, and if it exceeds 75 parts by weight, it tends to be too hard.

セルロースは、D−グルコピラノースがβ−1,4グルコシド結合で連なった繊維状高分子である。   Cellulose is a fibrous polymer in which D-glucopyranose is linked by β-1,4 glucoside bonds.

本発明に用いられるセルロースとしては、バクテリアセルロースが好ましい。バクテリアセルロースは菌細胞から分泌されたセルロースであり、植物セルロースに比べて純度が高く、繊維が細かいという特徴を有しており、繊維状に処理されたものが好ましく用いられる。バクテリアセルロースの製法としては、特開昭61−221201号公報、特開昭61−152296号公報、特開昭62−265990号公報、特開平7−274987号公報に記載の方法などが挙げられる。また、植物セルロースに強力な機械的せん断力を加えてミクロフィブリル化したものも好ましく用いられる。   Bacterial cellulose is preferred as the cellulose used in the present invention. Bacterial cellulose is cellulose secreted from fungal cells and has characteristics of higher purity and finer fibers than plant cellulose, and those processed into a fibrous form are preferably used. Examples of the method for producing bacterial cellulose include the methods described in JP-A Nos. 61-221201, 61-152296, 62-265990, and 7-274987. Moreover, the thing made into microfibrils by applying a strong mechanical shear force to plant cellulose is also preferably used.

前記セルロースの繊維直径は1μm以下であることが好ましい。セルロースの繊維直径の下限については0.01μmであることがより好ましい。また、セルロースの繊維直径の上限については0.6μmであることがより好ましく、0.3μmであることがさらに好ましい。セルロースの繊維直径が0.01μm未満では、ゴム中に微分散させることが難しくなる傾向があり、1μmをこえると、耐摩耗性の改善効果が小さくなる傾向がある。   The fiber diameter of the cellulose is preferably 1 μm or less. The lower limit of the fiber diameter of cellulose is more preferably 0.01 μm. Further, the upper limit of the fiber diameter of cellulose is more preferably 0.6 μm, and further preferably 0.3 μm. If the fiber diameter of cellulose is less than 0.01 μm, it tends to be difficult to finely disperse in the rubber, and if it exceeds 1 μm, the effect of improving wear resistance tends to be small.

前記セルロースの含有量は、前記ジエン系ゴム成分100重量部に対して、0.1〜40重量部であることが好ましい。セルロース含有量の下限については1重量部であることがより好ましく、上限については30重量部であることがより好ましい。0.1重量部未満では、耐摩耗性が低い傾向があり、40重量部をこえると、硬くなりすぎる傾向がある。   The cellulose content is preferably 0.1 to 40 parts by weight with respect to 100 parts by weight of the diene rubber component. The lower limit of the cellulose content is more preferably 1 part by weight, and the upper limit is more preferably 30 parts by weight. If it is less than 0.1 part by weight, the wear resistance tends to be low, and if it exceeds 40 parts by weight, it tends to be too hard.

さらに、本発明のゴム組成物には、カーボンブラックやシリカなどの補強性充填剤を任意の割合で配合することができる。その含有量は、ジエン系ゴム成分100重量部あたり、20〜60重量部であることが好ましい。これらの補強性充填剤が20重量部未満では、加工性が悪くなる傾向があり、60重量部をこえると、硬くなり過ぎる傾向がある。   Furthermore, reinforcing fillers such as carbon black and silica can be blended in the rubber composition of the present invention at an arbitrary ratio. The content is preferably 20 to 60 parts by weight per 100 parts by weight of the diene rubber component. If these reinforcing fillers are less than 20 parts by weight, the workability tends to deteriorate, and if they exceed 60 parts by weight, they tend to be too hard.

本発明のゴム組成物には、シランカップリング剤が好ましく用いられる。シランカップリング剤としては、たとえば、ビス(3−トリエトキシシリルプロピル)テトラスルフィド、ビス(2−トリエトキシシリルエチル)テトラスルフィド、ビス(3−トリメトキシシリルプロピル)テトラスルフィド、ビス(2−トリメトキシシリルエチル)テトラスルフィド、3−メルカプトプロピルトリメトキシシラン、3−メルカプトプロピルトリエトキシシラン、2−メルカプトエチルトリメトキシシラン、2−メルカプトエチルトリエトキシシラン、3−ニトロプロピルトリメトキシシラン、3−ニトロプロピルトリエトキシシラン、3−クロロプロピルトリメトキシシラン、3−クロロプロピルトリエトキシシラン、2−クロロエチルトリメトキシシラン、2−クロロエチルトリエトキシシラン、3−トリメトキシシリルプロピル−N,N−ジメチルチオカルバモイルテトラスルフィド、3−トリエトキシシリルプロピル−N,N−ジメチルチオカルバモイルテトラスルフィド、2−トリエトキシシリルエチル−N,N−ジメチルチオカルバモイルテトラスルフィド、3−トリメトキシシリルプロピルベンゾチアゾールテトラスルフィド、3−トリエトキシシリルプロピルベンゾチアゾールテトラスルフィド、3−トリエトキシシリルプロピルメタクリレートモノスルフィド、3−トリメトキシシリルプロピルメタクリレートモノスルフィドなどがあげられる。これらは単独で用いてもよく、2種以上を組み合わせて用いてもよい。これらのうちでは、カップリング剤添加効果とコストの両立の点から、ビス(3−トリエトキシシリルプロピル)テトラスルフィドなどが好ましい。   A silane coupling agent is preferably used in the rubber composition of the present invention. Examples of the silane coupling agent include bis (3-triethoxysilylpropyl) tetrasulfide, bis (2-triethoxysilylethyl) tetrasulfide, bis (3-trimethoxysilylpropyl) tetrasulfide, and bis (2-triethoxy). Methoxysilylethyl) tetrasulfide, 3-mercaptopropyltrimethoxysilane, 3-mercaptopropyltriethoxysilane, 2-mercaptoethyltrimethoxysilane, 2-mercaptoethyltriethoxysilane, 3-nitropropyltrimethoxysilane, 3-nitro Propyltriethoxysilane, 3-chloropropyltrimethoxysilane, 3-chloropropyltriethoxysilane, 2-chloroethyltrimethoxysilane, 2-chloroethyltriethoxysilane, 3-trimethoxysilane Rupropyl-N, N-dimethylthiocarbamoyl tetrasulfide, 3-triethoxysilylpropyl-N, N-dimethylthiocarbamoyl tetrasulfide, 2-triethoxysilylethyl-N, N-dimethylthiocarbamoyl tetrasulfide, 3-trimethoxy Examples thereof include silylpropyl benzothiazole tetrasulfide, 3-triethoxysilylpropyl benzothiazole tetrasulfide, 3-triethoxysilylpropyl methacrylate monosulfide, and 3-trimethoxysilylpropyl methacrylate monosulfide. These may be used alone or in combination of two or more. Of these, bis (3-triethoxysilylpropyl) tetrasulfide is preferable from the viewpoint of both the effect of adding a coupling agent and the cost.

前記シランカップリング剤の含有量は、澱粉、セルロースおよびシリカの合計含有量に対して1〜20重量%であることが好ましい。シランカップリング剤の含有量が1重量%未満では、耐摩耗性の改善効果が小さい傾向があり、20重量%をこえて配合しても、改善効果に変化がなく、高コストになる傾向がある。   The content of the silane coupling agent is preferably 1 to 20% by weight with respect to the total content of starch, cellulose and silica. If the content of the silane coupling agent is less than 1% by weight, the effect of improving the wear resistance tends to be small, and even if blended over 20% by weight, the improvement effect does not change and tends to be expensive. is there.

また、本発明のゴム組成物には、軟化剤、加硫剤、加硫促進剤、老化防止剤など通常タイヤ用ゴム組成物に配合されている各種添加剤を配合することができる。   The rubber composition of the present invention may contain various additives usually blended in a tire rubber composition such as a softening agent, a vulcanizing agent, a vulcanization accelerator, and an antioxidant.

以下に、実施例に基づいて本発明を具体的に説明するが、本発明はこれに制限されるものではない。   Hereinafter, the present invention will be specifically described based on examples, but the present invention is not limited thereto.

実施例1〜2および比較例1
(材料)
天然ゴム:RSS#3
シリカ:デグッサ社製のウルトラジルVN3(N2SA:210m2/g)
シランカップリング剤:ビス−(3−トリエトキシシリルプロピル)テトラスルフィド
澱粉:コーンスターチ
セルロース1:D−グルコースを主成分とする標準培地で、酢酸菌を静置培養により培養したバクテリアセルロース(繊維直径0.1μm)
セルロース2:日本製紙(株)製のセルロース繊維(繊維直径25μm)
亜鉛華:東邦亜鉛(株)製の銀嶺R
ステアリン酸:日本油脂(株)製の桐
硫黄:鶴見化学工業(株)製の硫黄
加硫促進剤1:N−t−ブチル−2−ベンゾチアゾリル−スルフェンアミド
加硫促進剤2:1,3−ジフェニルグアニジン
Examples 1-2 and Comparative Example 1
(material)
Natural rubber: RSS # 3
Silica: Ultrazil VN3 manufactured by Degussa (N 2 SA: 210 m 2 / g)
Silane coupling agent: Bis- (3-triethoxysilylpropyl) tetrasulfide starch: Corn starch cellulose 1: Bacterial cellulose (fiber diameter 0) in which acetic acid bacteria are cultured by stationary culture in a standard medium mainly composed of D-glucose. .1 μm)
Cellulose 2: Cellulose fiber manufactured by Nippon Paper Industries Co., Ltd. (fiber diameter 25 μm)
Zinc flower: Toho Zinc Co., Ltd.
Stearic acid: Paulownia sulfur manufactured by NOF Corporation: Sulfur vulcanization accelerator manufactured by Tsurumi Chemical Co., Ltd. 1: Nt-butyl-2-benzothiazolyl-sulfenamide vulcanization accelerator 2: 1, 3 -Diphenylguanidine

(製造方法)
表1に示した配合内容にしたがって、まず、加硫促進剤と硫黄を除く成分を1.7リットルの密閉型ミキサーで3〜5分間混練した。つぎに、硫黄と加硫促進剤を加えてオープンロールで混練した。得られた混練物を150℃で30分間プレス加硫することによって試験試料を得た。
(Production method)
According to the blending contents shown in Table 1, first, the vulcanization accelerator and the components excluding sulfur were kneaded for 3 to 5 minutes with a 1.7 liter closed mixer. Next, sulfur and a vulcanization accelerator were added and kneaded with an open roll. The obtained kneaded material was press vulcanized at 150 ° C. for 30 minutes to obtain a test sample.

(試験方法)
JIS K6264のランボーン摩耗試験に準拠して摩耗量を測定し、比較例1の摩耗量を100とする指数で示した。数値が大きいほど、耐摩耗性に優れていることを示す。
(Test method)
The amount of wear was measured according to the lambone wear test of JIS K6264, and the wear amount of Comparative Example 1 was represented by an index of 100. It shows that it is excellent in abrasion resistance, so that a numerical value is large.

(試験結果)
結果を表1に示す。表1から、澱粉とセルロースを両方配合した実施例1および2は、澱粉のみを配合した比較例1に比べて耐摩耗性が向上したことがわかる。とくに、繊維直径が小さいバクテリアセルロースを配合した実施例1は、耐摩耗性が大きく向上した。
(Test results)
The results are shown in Table 1. From Table 1, it can be seen that Examples 1 and 2 in which both starch and cellulose are blended have improved wear resistance compared to Comparative Example 1 in which only starch is blended. In particular, Example 1 in which bacterial cellulose having a small fiber diameter was blended greatly improved the wear resistance.

Figure 2005133025
Figure 2005133025

Claims (4)

ジエン系ゴム成分、澱粉およびセルロースからなるゴム組成物。 A rubber composition comprising a diene rubber component, starch and cellulose. セルロースの繊維直径が1μm以下である請求項1記載のゴム組成物。 The rubber composition according to claim 1, wherein the fiber diameter of the cellulose is 1 µm or less. ジエン系ゴム成分100重量部に対して、澱粉の含有量が5〜75重量部であり、セルロースの含有量が0.1〜40重量部である請求項1記載のゴム組成物。 The rubber composition according to claim 1, wherein the starch content is 5 to 75 parts by weight and the cellulose content is 0.1 to 40 parts by weight with respect to 100 parts by weight of the diene rubber component. セルロースがバクテリアセルロースである請求項1、2または3記載のゴム組成物。 The rubber composition according to claim 1, 2 or 3, wherein the cellulose is bacterial cellulose.
JP2003372908A 2003-10-31 2003-10-31 Rubber composition Pending JP2005133025A (en)

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