JPS62230872A - Ink for heat transfer - Google Patents
Ink for heat transferInfo
- Publication number
- JPS62230872A JPS62230872A JP61073267A JP7326786A JPS62230872A JP S62230872 A JPS62230872 A JP S62230872A JP 61073267 A JP61073267 A JP 61073267A JP 7326786 A JP7326786 A JP 7326786A JP S62230872 A JPS62230872 A JP S62230872A
- Authority
- JP
- Japan
- Prior art keywords
- ink
- thermoplastic
- thermal transfer
- wax
- heat transfer
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
- 229920002725 thermoplastic elastomer Polymers 0.000 claims abstract description 23
- 239000000126 substance Substances 0.000 claims abstract description 22
- 239000003086 colorant Substances 0.000 claims abstract description 8
- 239000000049 pigment Substances 0.000 claims abstract description 5
- 229920001169 thermoplastic Polymers 0.000 claims abstract description 5
- 239000004416 thermosoftening plastic Substances 0.000 claims abstract description 5
- 239000000203 mixture Substances 0.000 claims description 13
- 229920005992 thermoplastic resin Polymers 0.000 claims description 6
- 230000001747 exhibiting effect Effects 0.000 claims 1
- 238000002156 mixing Methods 0.000 abstract 1
- 239000001993 wax Substances 0.000 description 17
- 239000004203 carnauba wax Substances 0.000 description 4
- 235000013869 carnauba wax Nutrition 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 239000012188 paraffin wax Substances 0.000 description 4
- 239000004698 Polyethylene Substances 0.000 description 3
- 239000006229 carbon black Substances 0.000 description 3
- 239000000975 dye Substances 0.000 description 3
- 229920000728 polyester Polymers 0.000 description 3
- -1 polyethylene Polymers 0.000 description 3
- 229920000573 polyethylene Polymers 0.000 description 3
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 229920001971 elastomer Polymers 0.000 description 2
- 239000005038 ethylene vinyl acetate Substances 0.000 description 2
- 239000000155 melt Substances 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- 239000004200 microcrystalline wax Substances 0.000 description 2
- 235000019808 microcrystalline wax Nutrition 0.000 description 2
- 229920003023 plastic Polymers 0.000 description 2
- 239000004033 plastic Substances 0.000 description 2
- 229920001200 poly(ethylene-vinyl acetate) Polymers 0.000 description 2
- 239000005060 rubber Substances 0.000 description 2
- JOYRKODLDBILNP-UHFFFAOYSA-N Ethyl urethane Chemical compound CCOC(N)=O JOYRKODLDBILNP-UHFFFAOYSA-N 0.000 description 1
- 239000005977 Ethylene Substances 0.000 description 1
- BZHJMEDXRYGGRV-UHFFFAOYSA-N Vinyl chloride Chemical compound ClC=C BZHJMEDXRYGGRV-UHFFFAOYSA-N 0.000 description 1
- 150000001336 alkenes Chemical class 0.000 description 1
- DQXBYHZEEUGOBF-UHFFFAOYSA-N but-3-enoic acid;ethene Chemical compound C=C.OC(=O)CC=C DQXBYHZEEUGOBF-UHFFFAOYSA-N 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 229920001577 copolymer Polymers 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 239000013013 elastic material Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 229920006244 ethylene-ethyl acrylate Polymers 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 1
- 235000019809 paraffin wax Nutrition 0.000 description 1
- 235000019271 petrolatum Nutrition 0.000 description 1
- 239000004014 plasticizer Substances 0.000 description 1
- 229920002037 poly(vinyl butyral) polymer Polymers 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 229920003051 synthetic elastomer Polymers 0.000 description 1
- 229920003002 synthetic resin Polymers 0.000 description 1
- 239000000057 synthetic resin Substances 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B41—PRINTING; LINING MACHINES; TYPEWRITERS; STAMPS
- B41M—PRINTING, DUPLICATING, MARKING, OR COPYING PROCESSES; COLOUR PRINTING
- B41M5/00—Duplicating or marking methods; Sheet materials for use therein
- B41M5/26—Thermography ; Marking by high energetic means, e.g. laser otherwise than by burning, and characterised by the material used
- B41M5/382—Contact thermal transfer or sublimation processes
- B41M5/38207—Contact thermal transfer or sublimation processes characterised by aspects not provided for in groups B41M5/385 - B41M5/395
Landscapes
- Physics & Mathematics (AREA)
- Optics & Photonics (AREA)
- Impression-Transfer Materials And Handling Thereof (AREA)
- Thermal Transfer Or Thermal Recording In General (AREA)
- Inks, Pencil-Leads, Or Crayons (AREA)
Abstract
Description
【発明の詳細な説明】
〔産業上の利用分野〕
この発明は熱転写型プリンターに供する熱転写記録シー
トに用いる熱転写用インクに関する。DETAILED DESCRIPTION OF THE INVENTION [Industrial Field of Application] This invention relates to a thermal transfer ink used for a thermal transfer recording sheet used in a thermal transfer printer.
熱転写プリンターに供される熱転写インクは熱溶融性で
あり、熱転写時に固体−液体一固体の相変化を鋭敏に行
わせるために従来からインク組成の主成分は炭化水素を
主体とする天然ワックスおよび／または合成ワックスに
顔料、染料等の着色剤を分散したものであり、これに皮
膜強化、接着性向上のために多少の合成樹脂や可塑剤を
添加していた＠
〔発明が解決しようとする問題点〕
上記のように従来の熱転写用インク成分がワックスであ
るために溶融時の粘度が低く、第２図に示めすように高
圧力の印字では溶融したインク７か変形し均一かつ十分
な濃度か出ないという欠点があった。Thermal transfer ink used in thermal transfer printers is heat-melting, and the main components of the ink composition have traditionally been natural waxes and/or hydrocarbons, in order to achieve a sharp phase change between solid-liquid-solid during thermal transfer. Alternatively, it is a product in which coloring agents such as pigments and dyes are dispersed in synthetic wax, and some amount of synthetic resin or plasticizer is added to this to strengthen the film and improve adhesion. Points] As mentioned above, since the conventional thermal transfer ink component is wax, the viscosity when melted is low, and as shown in Figure 2, when printing under high pressure, the molten ink 7 deforms, resulting in a uniform and sufficient density. There was a drawback that it did not come out.
特に低平滑紙では平滑紙に対し紙表面の凹凸が大きいた
めにインク面との接触率が小さく、印字の際にインクと
の接触面積を大きくするためにす−マルヘッド１を高圧
力で押圧する必要がある。In particular, with low-smooth paper, the contact ratio with the ink surface is small because the paper surface has large irregularities compared to smooth paper, so in order to increase the contact area with the ink during printing, the multi-head 1 is pressed with high pressure. There is a need.
ついには紙表面の凹部と凸部で非常に大きな圧力差が生
ずるため高圧部５から低圧部６ヘインク７が押し出され
、一定のインク厚が得られずインク濃度が不均一となり
像が不鮮明となる。Eventually, a very large pressure difference occurs between the concave and convex portions of the paper surface, and the ink 7 is pushed from the high pressure section 5 to the low pressure section 6, making it impossible to obtain a constant ink thickness, resulting in uneven ink concentration and a blurred image. .
また単にインクの硬度を上げるだけでは熱転写記録シー
トの柔軟性が無くなったり、粘度が高過ぎるといった問
題が生ずる。Furthermore, simply increasing the hardness of the ink causes problems such as the thermal transfer recording sheet losing its flexibility and having too high a viscosity.
そこで本発明はこの問題を解決しようとするもので、そ
の目的は転写記録シートの柔軟性低下、インクの高粘度
化を防ぎ、低平滑紙に高圧力で転写しても鮮明な印字像
が得られるような熱転写用インクを提供するところにあ
る。The present invention aims to solve this problem, and its purpose is to prevent the transfer recording sheet from decreasing in flexibility and the ink from increasing in viscosity, and to ensure that clear printed images can be obtained even when transferred to low-smooth paper under high pressure. The purpose of the present invention is to provide a thermal transfer ink that can be used for thermal transfer.
本発明の熱転写用インクは、熱可塑性有機物質と着色剤
と熱可塑性ゴム弾性物質を含む熱転写インクであり、具
体的には上記熱可塑性有機物質としてワックスまたはワ
ックスと熱可塑性樹脂との混合物を用い、着色剤として
は顔料および／または油性染料を用い、また熱可塑性ゴ
ム弾性物質としてハ熱可塑性ゴムおよび／または熱可塑
性エラストマーを用いるものである。The thermal transfer ink of the present invention is a thermal transfer ink containing a thermoplastic organic substance, a colorant, and a thermoplastic rubber elastic substance, and specifically, a wax or a mixture of a wax and a thermoplastic resin is used as the thermoplastic organic substance. A pigment and/or an oil-based dye is used as the coloring agent, and a thermoplastic rubber and/or a thermoplastic elastomer is used as the thermoplastic rubber elastic substance.
上記のように熱可塑性ゴム弾性物質を熱転写用インクの
成分に用いるとインクにゴム弾性が与えられ、第１図の
ように高圧力で低平滑紙に印字してもインクがつぶれた
り押し出されたりする塑性変形が無く、インク厚が均一
になり濃度むらの無い鮮明な印字が得られる。また高温
では普通の熱可塑性樹脂と同様に溶融し塗工に適した粘
度を与え、しかも固化したインクに柔軟性を与える。As mentioned above, when a thermoplastic rubber elastic substance is used as a component of thermal transfer ink, rubber elasticity is imparted to the ink, and as shown in Figure 1, even when printing on low-smooth paper under high pressure, the ink does not get crushed or pushed out. There is no plastic deformation, the ink thickness becomes uniform, and clear prints with no density unevenness can be obtained. At high temperatures, it melts like a normal thermoplastic resin, giving it a viscosity suitable for coating, and also gives flexibility to the solidified ink.
この発明に用いられる熱可塑性ゴム弾性物質としては、
熱可塑性ゴム、またはスチレン系、オレフィン、ｆｂ、
塩化ビニール系、ウレタン系、ポリエステル系、ポリ了
ミド系等の各熱可塑性エラストマーがあり、単独または
混合で用いられるものでありその使用量はインクの０．
３重量％〜１０重量％である。また軟化温度は５０℃〜
１５０すが適当である。The thermoplastic rubber elastic material used in this invention is as follows:
thermoplastic rubber, or styrenic, olefin, fb,
There are various thermoplastic elastomers such as vinyl chloride type, urethane type, polyester type, polyester type, etc., which can be used alone or as a mixture, and the amount used is 0.5% of the ink.
It is 3% to 10% by weight. Also, the softening temperature is 50℃ ~
150 is appropriate.
この発明に用いられるワックスと熱可塑性樹脂の軟化温
度は５０℃〜３００℃が適当である。The appropriate softening temperature of the wax and thermoplastic resin used in this invention is 50°C to 300°C.
ワックスとしては天然系ワックス、合成ワックスのいず
れも用いられる。As the wax, both natural wax and synthetic wax can be used.
天然系ワックスとして、カルナバワックス、パラフィン
ワックス、マイクロクリスタリンワックス等が挙げられ
る。Examples of natural waxes include carnauba wax, paraffin wax, and microcrystalline wax.
合成ワックスとしてはポリエチレンワックス等がある。Synthetic waxes include polyethylene wax and the like.
これらのワックスは単独または混合して用いられ、その
使用量は６５〜９０重量％が適当である。These waxes may be used alone or in combination, and the appropriate amount is 65 to 90% by weight.
熱可塑性樹脂としては、上記ワックスと相溶するもので
あれば何でもよく、具体的にはエチレンビニルアセテー
ト共重合体、エチレンエチルアクリレート共重合体、ポ
リエチレン、ポリビニルブチラール、ポリエステル等が
挙げられる。Any thermoplastic resin may be used as long as it is compatible with the wax, and specific examples include ethylene vinyl acetate copolymer, ethylene ethyl acrylate copolymer, polyethylene, polyvinyl butyral, and polyester.
これらの熱可塑性樹脂の使用量は５〜２０重量％が適当
である。The appropriate amount of these thermoplastic resins to be used is 5 to 20% by weight.
この発明で用いられる着色剤は顔料と油性染料であり、
これらも単独または混合して用いることができる。その
使用量は０５〜３０重量−である。The colorants used in this invention are pigments and oil dyes,
These can also be used alone or in combination. The amount used is 0.5-30% by weight.
以下、この発明を実施例によって、具体的に説明する。 Hereinafter, the present invention will be specifically explained with reference to Examples.
以下の実施例中に示すインクの成分の！（％）はすべて
重ｉｔ％である。Of the components of the ink shown in the examples below! All (%) are weight %.
実施例１
インクの組成
パラフィンワックス １３０’ｌ’
〔日本製蝋（株）製〕 ４０％
カルナバワックス １号 ２４％ポリエチレンワ
ックス 〔サニワックス１６５Ｆ、三菱化成工業（株）
製〕２４％カーボンブラック ［ＭＡ−１００、三菱化
成工業（株）製〕 ８％オイルブラック
ＨＢＢ （５ｏｌｖｅｎｔＢｌａｃｋ ３ 、オリエ
ント化学工業（株）製〕２％
熱可塑性ゴム 〔クレイトン（）１６５７シエル化学（
株）製〕 ２％上記組成の混合物をプラネタ
リ−ミキサーにより予備分散しく１２０℃、３０分）、
冷却固化後、粉砕してから３本ロールミルにより本分散
して（後ロールと中ロール、１２０℃、前ロールは水冷
して１５回通し）黒色の熱転写用インクをつくったＯ
比較例１
上記実施例１における熱可塑性ゴムを除いた他は実施例
１と同じ成分の混合物を同じ方法で分散処理をして熱転
写インクをつくったＯ
実施例２
インクの組成
パラフィンワックス １３０°ＩＰ
〔日本製蝋（株）製〕 ４０％
カルナバワックス １号 ２０％酸化ワックス
（：Ｎ５Ｐ−６０１０、日本製蝋（株）製〕
２０％
エチレンビニルアセテート共ｍ合体
〔エバフレックス４１０、三井ポリケミカル（株）製〕
８％
カーボンブラック ［ＭＡ−１００、三菱化成工業（株
）製〕 １０％熱可塑性エラストマー 〔タ
フプレン１２０、旭化成工業（株）製〕 ２
％比較例２
実施例２の熱可塑性エラストマーを除いた他は上記実施
例２と同じ成分の混合物を同じ方法で分散処理をして熱
転写用インクをつくったＯ実施例５
インクの組成
パラフィンワックス １３０°Ｆ
〔日本製蝋（株）製〕 ２６％
マイクロクリスタリンワックス ｌ：ｕｌ−Ｍｉｃ−１
０７０、日本製蝋（株）製〕２６％
カルナバワックス １号 ２０％エチレンエチル
共重合体 ［ＮＵＯ−６０７０、日本ユニカー（株）製
〕１６％
カーボンブラック ＣＭＡ−１００、三菱化成工業（株
）製〕 ６％
オイルブラック ＨＢＥ ［５ｏｌｖｅｎｔＢ１ａｃ
ｋ３、オリエント化学工業（株）製〕４％
熱可塑性エラストマー ［、ｒＳＲＲＢ８１０、日本合
成ゴム（株）製〕 ２％
比較例６
実施例乙のインク組成のうち、熱可塑性エラストマーを
除いた他は実施例３と同じ成分の混合物を同じ方法で分
散処理をして熱転写用インクをつくった〇
上記実施例１，２．３および比較例１，２．３より得ら
れた各インクを１００℃にて加熱溶融して厚さ４μのＰ
ＫＴフィルムにワイヤーバー法で塗布し、インク厚６μ
の熱転写用インクシートをつくった０
この熱転写インクシートを用い・ベック平滑度８秒のボ
ンド紙に熱印加ｆｉｌＯＤＰ工において、１、０ ｍＪ
／ｄｏｔで、ヘッド圧力１００ ？ ７ｃｍ３００ ？
７ｃｍ、５００ ？ ／ ｃｍのそれぞれにて転写し
た。その結果を表に示す０
○：インクがつぶれず均一な厚さで転写されている。Example 1 Composition of ink Paraffin wax 130'l' [manufactured by Nippon Seiwa Co., Ltd.] 40% Carnauba wax No. 1 24% polyethylene wax [Saniwax 165F, Mitsubishi Chemical Industries, Ltd.]
[Manufactured by Mitsubishi Chemical Industries, Ltd.] 24% carbon black [MA-100, manufactured by Mitsubishi Chemical Industries, Ltd.] 8% oil black
HBB (5olventBlack 3, manufactured by Orient Chemical Industry Co., Ltd.) 2% thermoplastic rubber [Clayton () 1657 Shell Chemical (
Co., Ltd.] 2% A mixture having the above composition was pre-dispersed using a planetary mixer at 120°C for 30 minutes),
After cooling and solidifying, the ink was pulverized and then dispersed using a three-roll mill (rear roll and middle roll, 120°C, front roll was water-cooled and passed 15 times) to make a black thermal transfer ink.Comparative Example 1 The above implementation A thermal transfer ink was prepared by dispersing a mixture of the same components as in Example 1 in the same manner except for the thermoplastic rubber in Example 1. Example 2 Composition of ink Paraffin wax 130°IP [Nippon Wax ( Co., Ltd.] 40% carnauba wax No. 1 20% oxidized wax
(:N5P-6010, manufactured by Nippon Seiro Co., Ltd.)
20% ethylene vinyl acetate co-m combination [Evaflex 410, manufactured by Mitsui Polychemical Co., Ltd.]
8% carbon black [MA-100, manufactured by Mitsubishi Chemical Industries, Ltd.] 10% thermoplastic elastomer [Tuffprene 120, manufactured by Asahi Kasei Industries, Ltd.] 2
% Comparative Example 2 A thermal transfer ink was prepared by dispersing a mixture of the same components as in Example 2 in the same manner as in Example 2 except for the thermoplastic elastomer of Example 2. Example 5 Ink composition Paraffin wax 130 °F [Manufactured by Nippon Seiwa Co., Ltd.] 26% Microcrystalline wax l:ul-Mic-1
070, manufactured by Nippon Seiro Co., Ltd.] 26% Carnauba wax No. 1 20% ethylene ethyl copolymer [NUO-6070, manufactured by Nippon Unicar Co., Ltd.] 16% Carbon black CMA-100, manufactured by Mitsubishi Chemical Industries, Ltd. ] 6% Oil Black HBE [5olventB1ac
k3, manufactured by Orient Chemical Industry Co., Ltd.] 4% Thermoplastic elastomer [, rSRRB810, manufactured by Japan Synthetic Rubber Co., Ltd.] 2% Comparative Example 6 The ink composition of Example B except for the thermoplastic elastomer was used. A thermal transfer ink was prepared by dispersing a mixture of the same components as in Example 3 using the same method. Each ink obtained from the above Examples 1 and 2.3 and Comparative Examples 1 and 2.3 was heated at 100°C. Heat-melted P with a thickness of 4μ
Coated on KT film using wire bar method, ink thickness 6μ
I made a thermal transfer ink sheet of
/dot, head pressure 100? 7cm300?
7cm, 500? / cm, respectively. The results are shown in the table: 0: The ink was transferred with a uniform thickness without being crushed.
△：わずかにインクが変形している。Δ: Ink is slightly deformed.
Ｘ：完全にインクが変形している。X: The ink is completely deformed.
以上述べたように本発明の熱転写インクは、熱可塑性ゴ
ム弾性物質を含むためにゴム弾性を有し、高圧力で低平
滑紙に印字してもインクがつぶれたり押し出されたりす
る塑性変形を防ぐことができる。しかるに、低平滑紙に
対しても均一な濃度の鮮明な印字ができる。As described above, the thermal transfer ink of the present invention has rubber elasticity because it contains a thermoplastic rubber elastic substance, and prevents plastic deformation such as crushing or extrusion of the ink even when printing on low-smooth paper under high pressure. be able to. However, clear printing with uniform density is possible even on low-smooth paper.
また高温では溶融し、塗工に適した粘度を与え、また固
化時にはインクに柔軟性を与えるという効果を有する。Furthermore, it melts at high temperatures, giving it a viscosity suitable for coating, and has the effect of giving flexibility to the ink when it solidifies.
第１図は本発明の熱転写インクの転写メカニズムを示す
図。
第２図は従来の熱転写インクの転写メカニズムを示す図
。
１・・・・・・サーマルヘッド
２・・・・・・インク層
３・・・・・・インク支持層 −
４・・・・・・被転写紙
５・・・・・・高圧力部
６・・・・・・低圧力部
以 上
出願人 セイコーエプソン株式会社
第１図
第２図FIG. 1 is a diagram showing the transfer mechanism of the thermal transfer ink of the present invention. FIG. 2 is a diagram showing a transfer mechanism of a conventional thermal transfer ink. 1... Thermal head 2... Ink layer 3... Ink support layer - 4... Transfer paper 5... High pressure section 6・・・・・・Low pressure section and above Applicant: Seiko Epson Corporation Figure 1 Figure 2
Claims (1)
ム弾性物質を含むことを特徴とする熱転写用インク。 ２、熱可塑性を示す有機物質がワックスまたは、ワック
スと熱可塑性樹脂との混合物である特許請求の範囲第１
項記載の熱転写用インク。 ３、着色剤が顔料および／または油溶性染料である特許
請求の範囲第１項記載の熱転写用インク。 ４、熱可塑性ゴム弾性物質が熱可塑性ゴムおよび／また
は熱可塑性エラストマーである特許請求の範囲第１項記
載の熱転写用インク。[Scope of Claims] 1. A thermal transfer ink comprising at least a thermoplastic organic substance, a colorant, and a thermoplastic rubber elastic substance. 2. Claim 1, wherein the organic substance exhibiting thermoplasticity is wax or a mixture of wax and thermoplastic resin.
Thermal transfer ink described in section. 3. The thermal transfer ink according to claim 1, wherein the colorant is a pigment and/or an oil-soluble dye. 4. The thermal transfer ink according to claim 1, wherein the thermoplastic rubber elastic substance is a thermoplastic rubber and/or a thermoplastic elastomer.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP61073267A JPS62230872A (en) | 1986-03-31 | 1986-03-31 | Ink for heat transfer |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP61073267A JPS62230872A (en) | 1986-03-31 | 1986-03-31 | Ink for heat transfer |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPS62230872A true JPS62230872A (en) | 1987-10-09 |
Family
ID=13513222
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP61073267A Pending JPS62230872A (en) | 1986-03-31 | 1986-03-31 | Ink for heat transfer |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS62230872A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH06301239A (en) * | 1993-04-14 | 1994-10-28 | Nippon Shokubai Co Ltd | Carbon black graft polymer composition, its production and use |
-
1986
- 1986-03-31 JP JP61073267A patent/JPS62230872A/en active Pending
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH06301239A (en) * | 1993-04-14 | 1994-10-28 | Nippon Shokubai Co Ltd | Carbon black graft polymer composition, its production and use |
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