JP5341053B2 - Light diffusing laminated resin plate and manufacturing method thereof - Google Patents
Light diffusing laminated resin plate and manufacturing method thereof Download PDFInfo
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本発明は、良好な外観を有する光拡散性積層樹脂板およびその製造方法に関する。より詳細には、表示装置の保護板、照明カバー、照明看板、建材分野における積層紙（障子紙、襖紙、壁紙など）、和紙調照明カバーなどに好適に用いられる、良好な外観を有する光拡散性積層樹脂板およびその製造方法に関する。 The present invention relates to a light diffusing laminated resin plate having a good appearance and a method for producing the same. More specifically, light having a good appearance that is suitably used for protective plates of display devices, lighting covers, lighting signs, laminated paper in the field of building materials (such as shoji paper, paperboard, wallpaper, etc.), Japanese paper lighting covers, etc. The present invention relates to a diffusive laminated resin plate and a method for producing the same.
従来、照明カバー、透過型ディスプレイ用の光拡散板、看板などの部材として、アクリル系樹脂、スチレン系樹脂、ポリカーボネート、塩化ビニル系樹脂などの透明樹脂に、有機系光拡散剤または無機系光拡散剤を分散させた光拡散板が広く用いられている。 Conventionally, as materials for lighting covers, light diffusion plates for transmissive displays, signboards, etc., transparent resins such as acrylic resins, styrene resins, polycarbonates, vinyl chloride resins, organic light diffusing agents or inorganic light diffusion A light diffusing plate in which an agent is dispersed is widely used.
このような光拡散板は、光を拡散させることを主眼としている。しかし、近年、照明カバーや各種ディスプレイ用の光拡散板としては、光を拡散させるとともに、光を有効に利用することが望まれている。すなわち、所定の方向に光を十分に拡散させ、しかも光源が透けない（光源のエネルギーを有効に利用できる）光拡散板が望まれている。 Such a light diffusion plate is mainly intended to diffuse light. However, in recent years, it has been desired that a light diffusing plate for lighting covers and various displays effectively diffuses light and effectively uses light. That is, there is a demand for a light diffusing plate that sufficiently diffuses light in a predetermined direction and that does not allow the light source to pass therethrough (the energy of the light source can be used effectively).
特許文献１には、２層の樹脂層に含有されるそれぞれの光拡散剤の粒径が２倍以上異なる光拡散性積層樹脂板が開示されている。また、特許文献２には、光を拡散させる粒子として、扁平率、屈折率、平均粒径など所定の条件を満たす架橋重合体粒子を含有した基材層および表面層からなる光源保護カバー用光拡散性積層樹脂板が開示されている。これらの光拡散性積層樹脂板は、所定の方向に光を十分に拡散させることができ、さらに光源のエネルギーを有効に利用することができる。 Patent Document 1 discloses a light diffusing laminated resin plate in which the particle sizes of the respective light diffusing agents contained in the two resin layers are two or more times different. Patent Document 2 discloses light for a light source protective cover comprising a base material layer and a surface layer containing cross-linked polymer particles satisfying predetermined conditions such as flatness, refractive index, and average particle diameter as light diffusing particles. A diffusive laminated resin plate is disclosed. These light diffusing laminated resin plates can sufficiently diffuse light in a predetermined direction, and can further effectively use the energy of the light source.
しかし、これらの光拡散性積層樹脂板は、使用時に最も端の部分である切断面（端面）の外観が良好ではないという問題がある。 However, these light-diffusing laminated resin plates have a problem that the appearance of the cut surface (end surface) which is the end portion at the time of use is not good.
光拡散性積層樹脂板の基材層または表面層の光拡散剤濃度が高くなると、光拡散剤が凝集して大粒子径の凝集体が発生する。例えば、凝集体が表面層に存在すると、目視で確認され、このような光拡散性積層樹脂板はブツ欠陥として扱われる。さらに、従来の光拡散性積層樹脂板は、製造時に発煙が生じ、発煙物がロール(冷却ロール等)に付着してロール汚れが発生し、生産性の低下を招く場合がある。これは、光拡散剤（特に無機系粒子）が、水分を含みやすく、また微粒子表面に凝集を防止するための処理（例えば、ステアリン酸のような高級脂肪酸の塗布など）が施されている場合が多く、そのため、高温溶融下において高級脂肪酸も加熱されて揮発・蒸散することにより発煙が生じ、光拡散性積層樹脂板の製造時にその発煙物がロールに付着してロール汚れが発生することがあるからである。また、光拡散剤として有機系微粒子を用いる場合、微粒子の製造段階で添加される分散剤など種々の要因で、ロール汚れが発生する場合がある。 When the concentration of the light diffusing agent in the base layer or the surface layer of the light diffusing laminated resin plate is increased, the light diffusing agent is aggregated to generate aggregates having a large particle size. For example, the presence of aggregates in the surface layer is visually confirmed, and such a light diffusing laminated resin plate is treated as a defect. Furthermore, the conventional light diffusing laminated resin plate may generate smoke during production, and the smoke generated may adhere to a roll (cooling roll or the like) to cause roll contamination, resulting in a decrease in productivity. This is because the light diffusing agent (particularly inorganic particles) is likely to contain moisture, and the surface of the fine particles is subjected to a treatment for preventing aggregation (for example, application of a higher fatty acid such as stearic acid). Therefore, higher fatty acids are also heated and volatilized and evaporated under high temperature melting, resulting in smoke generation, and when the light diffusing laminated resin plate is produced, the smoke generation material may adhere to the roll and cause roll dirt. Because there is. When organic fine particles are used as the light diffusing agent, roll stains may occur due to various factors such as a dispersant added in the fine particle production stage.
本発明の目的は、発煙などによる生産性の低下やブツの発生を抑制し、かつ良好な鏡面性を保ちつつ、端面の外観が良好な光拡散性積層樹脂板を提供することにある。 An object of the present invention is to provide a light-diffusing laminated resin plate having a good end face appearance while suppressing a decrease in productivity due to fuming or the like and generation of fuzz, and maintaining a good specularity.
本発明者らは、上記課題を解決すべく鋭意検討を重ねた結果、本発明を完成するに至った。 As a result of intensive studies to solve the above problems, the present inventors have completed the present invention.
本発明の光拡散性積層樹脂板は、以下の構成からなる。
（1）０．１１重量％〜２０重量％の光拡散剤（ａ）を含有するメタクリル樹脂（Ａ）からなる基材層の少なくとも一方の面に、０．１重量％〜１０重量％の光拡散剤（ｂ）を含有するメタクリル樹脂（Ｂ）からなる表面層が積層されてなる光拡散性積層樹脂板であって、該樹脂板が０．５ｍｍ〜１０ｍｍの厚みを有し、かつ以下の（Ｉ）〜（ＩＶ）を満たす、ことを特徴とする光拡散性積層樹脂板。
（I）光拡散剤（ａ）および光拡散剤（ｂ）が、同種の光拡散剤であること、
（II）メタクリル樹脂（Ａ）に含有される光拡散剤（ａ）の割合が、メタクリル樹脂（Ｂ）に含有される光拡散剤（ｂ）の割合よりも多いこと、
（III）表面層の厚みが、光拡散性積層樹脂板の厚みの１／１０以下であること、および
（IV）基材層の表面層側表面と、表面層の基材層側表面とは接していること。
（2）前記表面層が、前記基材層の両面に積層されてなる（1）に記載の光拡散性積層樹脂板。
（3）前記光拡散剤（ａ）が、硫酸バリウム、炭酸カルシウム、酸化チタン、架橋アクリル系樹脂粒子、架橋メタクリル酸メチル−スチレン共重合体樹脂粒子、およびシリコーン樹脂粒子からなる群より選択される少なくとも１種である、（1）または（2）に記載の光拡散性積層樹脂板。
（4）前記基材層と前記表面層とが、共押出成形で積層一体化される工程を含む、（1）から（3）のいずれかに記載の光拡散性積層樹脂板の製造方法。
The light diffusing laminated resin plate of this invention consists of the following structures.
(1) 0.1% by weight to 10% by weight of light on at least one surface of the base material layer made of the methacrylic resin (A) containing 0.11% by weight to 20% by weight of the light diffusing agent (a). A light-diffusing laminated resin plate in which a surface layer made of a methacrylic resin (B) containing a diffusing agent (b) is laminated, the resin plate having a thickness of 0.5 mm to 10 mm, and the following A light-diffusing laminated resin plate satisfying (I) to (IV).
(I) The light diffusing agent (a) and the light diffusing agent (b) are the same kind of light diffusing agent,
(II) The proportion of the light diffusing agent (a) contained in the methacrylic resin (A) is larger than the proportion of the light diffusing agent (b) contained in the methacrylic resin (B).
(III) The thickness of the surface layer is 1/10 or less of the thickness of the light diffusing laminated resin plate, and (IV) the surface layer side surface of the base material layer and the base material layer side surface of the surface layer Be in contact.
(2) The light-diffusing laminated resin plate according to (1), wherein the surface layer is laminated on both surfaces of the base material layer.
(3) The light diffusing agent (a) is selected from the group consisting of barium sulfate, calcium carbonate, titanium oxide, crosslinked acrylic resin particles, crosslinked methyl methacrylate-styrene copolymer resin particles, and silicone resin particles. The light diffusing laminated resin plate according to (1) or (2), which is at least one kind.
(4) The method for producing a light-diffusing laminated resin plate according to any one of (1) to (3), including a step in which the base material layer and the surface layer are laminated and integrated by coextrusion molding.
本発明の光拡散性積層樹脂板の製造方法は、上記基材層と上記表面層とが、共押出成形により成形され、積層一体化される工程を含む、ことを特徴とする。 The method for producing a light diffusing laminated resin plate of the present invention is characterized in that the substrate layer and the surface layer are formed by coextrusion molding and laminated and integrated.
本発明の光拡散性積層樹脂板は、表面層の拡散剤濃度を、基材層の拡散剤濃度よりも低い特定の範囲とし、さらに、光拡散性積層樹脂板が特定の厚みを有し、かつ基材層の厚みと表面層の厚みとの比が特定の範囲であるため、表面層に存在する拡散剤に起因する発煙が増加したり、ロールへの密着性が低下したりすることがなく、ブツの発生も抑制され、かつ良好な鏡面性を保つことができる。加えて、表面層の光拡散剤と基材層の光拡散剤とが同種のものであり、基材層の表面層側表面と表面層の基材層側表面とが接しているため、端面が良好な外観を有する。したがって、本発明によれば、発煙などによる生産性の低下やブツの発生を抑制し、かつ良好な鏡面性を保ちつつ、端面の外観が良好な光拡散性積層樹脂板を提供することができる。 The light diffusing laminated resin plate of the present invention has a specific range in which the diffusing agent concentration of the surface layer is lower than the diffusing agent concentration of the base material layer, and the light diffusing laminated resin plate has a specific thickness, And since the ratio between the thickness of the base material layer and the thickness of the surface layer is in a specific range, smoke generated due to the diffusing agent present in the surface layer may increase or the adhesion to the roll may decrease. In addition, the occurrence of unevenness is suppressed, and good specularity can be maintained. In addition, since the light diffusing agent of the surface layer and the light diffusing agent of the base material layer are of the same type, the surface layer side surface of the base material layer and the surface layer side surface of the surface layer are in contact with each other. Has a good appearance. Therefore, according to the present invention, it is possible to provide a light diffusing laminated resin plate having a good end face appearance while suppressing a decrease in productivity due to fuming or the like and generation of irregularities, and maintaining good specularity. .
本発明の光拡散性積層樹脂板は、０．１１重量％〜２０重量％の光拡散剤（ａ）を含有するメタクリル樹脂（Ａ）からなる表面層の少なくとも一方の面に、０．１重量％〜１０重量％の光拡散剤（ｂ）を含有するメタクリル樹脂（Ｂ）からなる樹脂層が積層されてなる。本発明の光拡散性積層樹脂板は、０．５ｍｍ〜１０ｍｍの厚みを有し、好ましくは１ｍｍ〜８ｍｍ、より好ましくは２ｍｍ〜５ｍｍの厚みを有する。 The light diffusing laminated resin plate of the present invention has 0.1 wt% on at least one surface of the surface layer made of methacrylic resin (A) containing 0.11 wt% to 20 wt% of the light diffusing agent (a). A resin layer made of a methacrylic resin (B) containing 10% to 10% by weight of a light diffusing agent (b) is laminated. The light diffusable laminated resin plate of the present invention has a thickness of 0.5 mm to 10 mm, preferably 1 mm to 8 mm, more preferably 2 mm to 5 mm.
本発明において、メタクリル樹脂（Ａ）、（Ｂ）とは、その構成単位としてメタクリル酸またはメタクリル酸エステル（例えば、メタクリル酸メチル、メタクリル酸エチルなど）を、５０重量％以上含有する樹脂（ホモポリマーおよびコポリマー）のことをいう。メタクリル樹脂の分子量は特に限定されない。 In the present invention, the methacrylic resins (A) and (B) are resins (homopolymers) containing 50% by weight or more of methacrylic acid or methacrylic acid ester (for example, methyl methacrylate, ethyl methacrylate, etc.) as a structural unit. And copolymer). The molecular weight of the methacrylic resin is not particularly limited.
このようなメタクリル樹脂（Ａ）、（Ｂ）としては、例えば、メタクリル酸のホモポリマー、メタクリル酸エステル（メタクリル酸メチル、メタクリル酸エチルなど）のホモポリマー、メタクリル酸またはメタクリル酸エステルと共重合可能な不飽和単量体とのコポリマーなどが挙げられる。 Such methacrylic resins (A) and (B) can be copolymerized with, for example, a homopolymer of methacrylic acid, a homopolymer of methacrylic acid ester (such as methyl methacrylate or ethyl methacrylate), methacrylic acid or methacrylic acid ester And copolymers with other unsaturated monomers.
メタクリル酸またはメタクリル酸エステルと共重合可能な不飽和単量体としては、例えば、アクリル酸、アクリル酸エステル（例えば、アクリル酸メチル、アクリル酸エチルなど）、主となるメタクリル酸エステルとは異なるメタクリル酸エステル、スチレン、α−メチルスチレン、アクリロニトリル、メタクリロニトリル、無水マレイン酸、フェニルマレイミド、シクロヘキシルマレイミドなどが挙げられる。 Examples of unsaturated monomers copolymerizable with methacrylic acid or methacrylic acid esters include acrylic acid, acrylic acid esters (for example, methyl acrylate and ethyl acrylate), and methacrylic acid different from the main methacrylic acid ester. Examples include acid esters, styrene, α-methylstyrene, acrylonitrile, methacrylonitrile, maleic anhydride, phenylmaleimide, cyclohexylmaleimide, and the like.
このようなメタクリル樹脂は、単独で用いてもよく、２種以上を混合して用いてもよい。また、メタクリル樹脂（Ａ）とメタクリル樹脂（Ｂ）とは、同一の樹脂であってもよく、異なる樹脂であってもよい。メタクリル樹脂（Ａ）とメタクリル樹脂（Ｂ）とが異なる場合としては、例えば分子量による違い、ホモポリマーとコポリマーの違い、コポリマーにおけるメタクリル酸エステルとの共重合成分の違い、共重合成分の含有割合の違いなどが挙げられるが、メタクリル樹脂（Ａ）の屈折率とメタクリル樹脂（Ｂ）の屈折率との差の絶対値は小さい方が好ましい。 Such methacrylic resins may be used alone or in combination of two or more. The methacrylic resin (A) and the methacrylic resin (B) may be the same resin or different resins. Examples of cases where the methacrylic resin (A) and the methacrylic resin (B) are different include, for example, differences in molecular weight, differences between homopolymers and copolymers, differences in copolymerization components with methacrylic acid esters in the copolymers, Although the difference etc. are mentioned, the one where the absolute value of the difference of the refractive index of a methacryl resin (A) and the refractive index of a methacryl resin (B) is smaller is preferable.
本発明に用いられる光拡散剤としては、例えば、硫酸バリウム、炭酸カルシウム、酸化チタン、水酸化アルミニウム、シリカ、硝子、タルク、マイカ、ホワイトカーボン、酸化マグネシウム、酸化亜鉛などの無機粒子；架橋アクリル系樹脂粒子；架橋アクリル−スチレン共重合体系樹脂粒子；シリコーン樹脂粒子などが挙げられる。 Examples of the light diffusing agent used in the present invention include inorganic particles such as barium sulfate, calcium carbonate, titanium oxide, aluminum hydroxide, silica, glass, talc, mica, white carbon, magnesium oxide, and zinc oxide; Resin particles; Crosslinked acrylic-styrene copolymer resin particles; Silicone resin particles and the like.
これらの中でも、コスト、樹脂との混練性、得られる光拡散性積層樹脂板の色合いなどの点から、硫酸バリウム、炭酸カルシウム、酸化チタン、架橋アクリル系樹脂粒子、架橋メタクリル酸メチル−スチレン共重合体樹脂粒子、およびシリコーン樹脂粒子が好ましく、硫酸バリウム、炭酸カルシウム、酸化チタン、架橋メタクリル酸メチル−スチレン共重合体粒子がより好ましい。光拡散剤は、単独で用いてもよく、２種以上を混合して用いてもよい。 Among these, barium sulfate, calcium carbonate, titanium oxide, cross-linked acrylic resin particles, cross-linked methyl methacrylate-styrene co-polymer in terms of cost, kneadability with resin, and color of the resulting light-diffusing laminated resin plate Combined resin particles and silicone resin particles are preferable, and barium sulfate, calcium carbonate, titanium oxide, and crosslinked methyl methacrylate-styrene copolymer particles are more preferable. A light-diffusion agent may be used independently and may mix and use 2 or more types.
さらに、本発明の光拡散性積層樹脂板は、以下の（Ｉ）〜（ＩＶ）の要件を満たす必要がある：
（I）光拡散剤（ａ）および光拡散剤（ｂ）が、同種の光拡散剤であること、
（II）メタクリル樹脂（Ａ）に含有される光拡散剤（ａ）の割合が、メタクリル樹脂（Ｂ）に含有される光拡散剤（ｂ）の割合よりも多いこと、
（III）表面層の厚みが、光拡散性積層樹脂板の厚みの１／１０以下であること、および
（IV）基材層の表面層側表面と、表面層の基材層側表面とは接していること。
Furthermore, the light-diffusing laminated resin plate of the present invention needs to satisfy the following requirements (I) to (IV):
(I) The light diffusing agent (a) and the light diffusing agent (b) are the same kind of light diffusing agent,
(II) The proportion of the light diffusing agent (a) contained in the methacrylic resin (A) is larger than the proportion of the light diffusing agent (b) contained in the methacrylic resin (B).
(III) The thickness of the surface layer is 1/10 or less of the thickness of the light diffusing laminated resin plate, and (IV) the surface layer side surface of the base material layer and the base material layer side surface of the surface layer Be in contact.
本発明においては、光拡散剤（ａ）および光拡散剤（ｂ）は、同種の光拡散剤が用いられる。ここで、「同種の光拡散剤」とは、例えば、硫酸バリウム同士や炭酸カルシウム同士のように、同じ種類に分類される光拡散剤のことをいい、平均粒径が同一であっても異なっていてもよく、さらに、無機粒子の場合には結晶構造などが、有機粒子の場合には分子量などが同一であっても異なっていてもよい。光拡散剤（ａ）および光拡散剤（ｂ）は、均一な光拡散性が得られ、かつ端面の外観が良好になるという点で、同一の光拡散剤を用いることが好ましい。 In the present invention, the same kind of light diffusing agent is used for the light diffusing agent (a) and the light diffusing agent (b). Here, “the same kind of light diffusing agent” refers to light diffusing agents classified into the same type, for example, barium sulfates or calcium carbonates, and are different even if the average particle diameter is the same. Further, in the case of inorganic particles, the crystal structure and the like may be the same or different in the case of organic particles. The light diffusing agent (a) and the light diffusing agent (b) are preferably the same light diffusing agent in that uniform light diffusibility is obtained and the appearance of the end face is improved.
光拡散剤（ａ）および光拡散剤（ｂ）として、異種の光拡散剤を用いた場合（例えば、光拡散剤（ａ）として硫酸バリウムを用い、光拡散剤（ｂ）として炭酸カルシウムを用いた場合など）、光拡散性積層樹脂板の端面において、基材層と表面層との界面が明瞭に識別できるようになり、光拡散性積層樹脂板の外観が悪くなるため好ましくない。 When different light diffusing agents are used as the light diffusing agent (a) and the light diffusing agent (b) (for example, barium sulfate is used as the light diffusing agent (a), and calcium carbonate is used as the light diffusing agent (b). Etc.), the interface between the base material layer and the surface layer can be clearly identified on the end face of the light diffusing laminated resin plate, and the appearance of the light diffusing laminated resin plate is deteriorated.
本発明においては、光拡散剤（ａ）は、メタクリル樹脂（Ａ）に、０．１１重量％〜２０重量％、光拡散剤（ｂ）は、メタクリル樹脂（Ｂ）に、０．１重量％〜１０重量％の割合で含有され、メタクリル樹脂（Ａ）に含有される光拡散剤（ａ）の割合が、メタクリル樹脂（Ｂ）に含有される光拡散剤（ｂ）の割合よりも多くする必要がある。すなわち、基材層に含有される光拡散剤の割合が、表面層に含有される光拡散剤の割合よりも多くする必要がある。 In the present invention, the light diffusing agent (a) is 0.11 wt% to 20 wt% in the methacrylic resin (A), and the light diffusing agent (b) is 0.1 wt% in the methacrylic resin (B). The proportion of the light diffusing agent (a) contained in the methacrylic resin (A) is greater than the proportion of the light diffusing agent (b) contained in the methacrylic resin (B). There is a need. That is, the ratio of the light diffusing agent contained in the base material layer needs to be larger than the ratio of the light diffusing agent contained in the surface layer.
光拡散剤（ａ）は、メタクリル樹脂（Ａ）に、好ましくは０．５重量％〜１０重量％、より好ましくは０．８重量％〜５重量％の割合で含有される。光拡散剤（ｂ）は、メタクリル樹脂（Ｂ）に、好ましくは０．１重量％〜５重量％、より好ましくは０．１〜１．８重量％の割合で含有される。光拡散剤（ａ）および光拡散剤（ｂ）のそれぞれにおいて、２種以上の光拡散剤を用いる場合は、これらの合計含有量がそれぞれ上記範囲となるようにすればよい。 The light diffusing agent (a) is preferably contained in the methacrylic resin (A) in a proportion of 0.5 wt% to 10 wt%, more preferably 0.8 wt% to 5 wt%. The light diffusing agent (b) is preferably contained in the methacrylic resin (B) in a proportion of 0.1 to 5% by weight, more preferably 0.1 to 1.8% by weight. In the case where two or more kinds of light diffusing agents are used in each of the light diffusing agent (a) and the light diffusing agent (b), the total content thereof may be set in the above range.
光拡散剤（ａ）の含有割合が０．１１重量％未満の場合、あるいは光拡散剤（ｂ）の含有割合が０．１重量％未満の場合、十分な光拡散効果が得られない。一方、光拡散剤（ａ）の含有割合が２０重量％を超える場合、得られる光拡散性積層樹脂板の引張強度や耐衝撃性が低下する傾向にある。光拡散剤（ｂ）の含有割合が１０重量％を超える場合、光拡散性積層樹脂板の表面が粗くなり、例えば製造時にロールへの密着性が低下し、密着していない部分から発煙して発煙物がロールに付着してロール汚れが発生する。 When the content ratio of the light diffusing agent (a) is less than 0.11% by weight or when the content ratio of the light diffusing agent (b) is less than 0.1% by weight, a sufficient light diffusion effect cannot be obtained. On the other hand, when the content ratio of the light diffusing agent (a) exceeds 20% by weight, the tensile strength and impact resistance of the obtained light diffusing laminated resin plate tend to be lowered. When the content ratio of the light diffusing agent (b) exceeds 10% by weight, the surface of the light diffusing laminated resin plate becomes rough, for example, the adhesion to the roll is lowered during production, and smoke is emitted from a non-adhered part. Smoke material adheres to the roll and causes roll contamination.
本発明においては、表面層の厚みが光拡散性積層樹脂板の厚みの１／１０以下である。１／１０を超える場合、光拡散性積層樹脂板の端面の外観が損なわれる点で好ましくない。表面層の厚みは、光拡散性積層樹脂板の厚みの、好ましくは１／１２以下、より好ましくは１／１５以下である。また、表面層の厚みの下限値は、成形可能な厚みであればよいが、得られる表面層の厚みを均一にできる点や、基材層において光拡散剤の凝集体が発生しても、得られる光拡散性積層樹脂板の表面においてブツとして認識されないようにできる点を考慮して、好ましくは０．０２ｍｍ以上、より好ましくは０．０３ｍｍ以上であるのがよい。 In the present invention, the thickness of the surface layer is 1/10 or less of the thickness of the light diffusing laminated resin plate. When exceeding 1/10, it is unpreferable at the point by which the external appearance of the end surface of a light diffusable laminated resin board is impaired. The thickness of the surface layer is preferably 1/12 or less, more preferably 1/15 or less, of the thickness of the light diffusing laminated resin plate. Further, the lower limit of the thickness of the surface layer may be any thickness that can be molded, even if the thickness of the resulting surface layer can be made uniform, or even if an aggregate of the light diffusing agent is generated in the base material layer, In consideration of the point that the surface of the obtained light diffusing laminated resin plate can be prevented from being recognized as blisters, it is preferably 0.02 mm or more, more preferably 0.03 mm or more.
表面層は、基材層の少なくとも一方の面に積層されるが、好ましくは基材層の両面に積層される。表面層が基材層の両面に積層される場合、表面層はいずれも同一の厚みであってもよく、異なる厚みであってもよい。なお、表面層が基材層の両面に積層される場合、両方の表面層の合計厚みが上記の割合（光拡散性積層樹脂板の全厚に対する表面層の厚みの割合が１／１０以下）を満たす必要がある。 The surface layer is laminated on at least one surface of the base material layer, but is preferably laminated on both surfaces of the base material layer. When a surface layer is laminated | stacked on both surfaces of a base material layer, all may have the same thickness and a different thickness. In addition, when a surface layer is laminated | stacked on both surfaces of a base material layer, the total thickness of both surface layers is said ratio (The ratio of the thickness of the surface layer with respect to the total thickness of a light diffusable laminated resin board is 1/10 or less) It is necessary to satisfy.
本発明においては、基材層と表面層とが、接着剤層を介することなく接している。このように、基材層と樹脂層とが、接着剤層を介することなく接触することによって、基材層と表面層との界面がほとんど視認できなくなり、端面の外観が良好（ほぼ単層に見える）な光拡散性積層樹脂板が得られる。 In the present invention, the base material layer and the surface layer are in contact with each other without interposing the adhesive layer. Thus, when the base material layer and the resin layer are in contact with each other without an adhesive layer, the interface between the base material layer and the surface layer becomes almost invisible, and the end face has a good appearance (almost a single layer). A visible light diffusing laminated resin plate is obtained.
基材層と樹脂層とが、接着剤層を介することなく接触するように積層する方法としては、例えば、共押出成形法、溶融押出ラミネート法、積層一体化ラミネート法、コーティング法などが挙げられる。本発明の光拡散性積層樹脂板は、特に、基材層と表面層とを共押出成形で積層一体化することにより、好適に得られる。この共押出成形は、２基または３基の一軸または二軸の押出機を用いて、基材層の材料（光拡散剤（ａ）を含有するメタクリル樹脂（Ａ））と表面層の材料（光拡散剤（ｂ）を含有するメタクリル樹脂（Ｂ））とを、それぞれ溶融混練した後、フィードブロックダイ、マルチマニホールドダイなどを介して積層することにより行われる。 Examples of the method of laminating so that the base material layer and the resin layer are in contact with each other without an adhesive layer include, for example, a co-extrusion molding method, a melt extrusion laminating method, a laminated integrated laminating method, and a coating method. . The light diffusing laminated resin plate of the present invention can be suitably obtained by laminating and integrating the base material layer and the surface layer by coextrusion molding. This co-extrusion molding is carried out using a two- or three-unit uniaxial or biaxial extruder, and a base layer material (methacrylic resin (A) containing a light diffusing agent (a)) and a surface layer material ( The methacrylic resin (B) containing the light diffusing agent (b) is melt-kneaded and then laminated through a feed block die, a multi-manifold die or the like.
積層一体化されたシート状またはフィルム状の溶融樹脂を、例えば、ロールユニットなどを用いて冷却固化し、本発明の光拡散性積層樹脂板が得られる。 The sheet-like or film-like molten resin laminated and integrated is cooled and solidified using, for example, a roll unit to obtain the light-diffusing laminated resin plate of the present invention.
以下、実施例および比較例を挙げて本発明を具体的に説明するが、本発明はこれらの実施例に限定されるものではない。 EXAMPLES Hereinafter, although an Example and a comparative example are given and this invention is demonstrated concretely, this invention is not limited to these Examples.
（実施例１）
（光拡散性積層樹脂板の調製）
ＰＭＭＡ樹脂ペレット（住友化学（株）製、スミペックスＥＸ）に、光拡散剤として炭酸カルシウム（丸尾カルシウム（株）製、カルテックスＲＲ、重量平均粒子径５μｍ、屈折率１．５７〜１．６０）を２重量％の割合となるように添加し、スーパーミキサーで混合した。得られた混合物を二軸押出機で溶融混練してメタクリル樹脂（Ａ）のペレットを調製した。
Example 1
(Preparation of light diffusing laminated resin plate)
Calcium carbonate (Maruo Calcium Co., Ltd., Caltex RR, weight average particle diameter 5 μm, refractive index 1.57 to 1.60) as a light diffusing agent on PMMA resin pellets (Sumitomo EX, manufactured by Sumitomo Chemical Co., Ltd.) It added so that it might become a 2 weight% ratio, and it mixed with the super mixer. The resulting mixture was melt-kneaded with a twin screw extruder to prepare methacrylic resin (A) pellets.
メタクリル樹脂（Ａ）とは別に、上記スミペックスＥＸに、カルテックスＲＲを０．１重量％の割合となるように添加し、スーパーミキサーで混合した。得られた混合物を二軸押出機で溶融混練してメタクリル樹脂（Ｂ）のペレットを調製した。 Separately from the methacrylic resin (A), Caltex RR was added to the Sumipex EX at a ratio of 0.1% by weight and mixed with a super mixer. The resulting mixture was melt-kneaded with a twin screw extruder to prepare methacrylic resin (B) pellets.
次いで、得られたメタクリル樹脂（Ａ）のペレットを、東芝機械（株）製の６５ｍｍφ一軸押出機で、そして得られたメタクリル樹脂（Ｂ）のペレットを、東芝機械（株）製の４５ｍｍφ一軸押出機でそれぞれ溶融し、フィードブロック法にて、２７５℃に設定したＴ型ダイスを介して押し出すことによりメタクリル樹脂（Ａ）の両表面にメタクリル樹脂（Ｂ）を溶融積層一体化させ積層シートを作製した。なお、溶融積層一体化は、メタクリル樹脂（Ａ）からなる層の両表面に積層されたメタクリル樹脂（Ｂ）からなる層がそれぞれ同一の厚みとなるようにし、かつ、積層シートの全厚に対して、該積層シートにおけるメタクリル樹脂（Ｂ）からなる層の合計厚みが１／３０となるように行った。得られた積層シートを、一対の表面が平滑な金属製のロールの間に挟み込んで成形し、全厚３ｍｍの光拡散性積層樹脂板（メタクリル樹脂（Ｂ）からなる表面層の１層当たりの厚み：０．０５ｍｍ）を調製した。 Next, the obtained methacrylic resin (A) pellets were manufactured by Toshiba Machine Co., Ltd. 65 mmφ single screw extruder, and the obtained methacrylic resin (B) pellets were manufactured by Toshiba Machine Co., Ltd. 45 mmφ single screw extruder. Each sheet is melted by a machine, and extruded through a T-type die set at 275 ° C. by a feed block method, so that the methacrylic resin (B) is fused and integrated on both surfaces of the methacrylic resin (A) to produce a laminated sheet. did. The melt lamination integration is performed so that the layers made of methacrylic resin (B) laminated on both surfaces of the layer made of methacrylic resin (A) have the same thickness, and the total thickness of the laminated sheet. Thus, the total thickness of the layers made of the methacrylic resin (B) in the laminated sheet was 1/30. The obtained laminated sheet was sandwiched between a pair of metal rolls having smooth surfaces, and formed into a light diffusing laminated resin plate (methacrylic resin (B) having a total thickness of 3 mm per layer. (Thickness: 0.05 mm) was prepared.
（実施例２〜８）
光拡散剤の種類および含有割合を、それぞれ表１に記載の種類および含有割合にしたこと以外は、実施例１と同様にして光拡散性積層樹脂板を調製した。なお、硫酸バリウムについては、日本化学工業（株）製「ＡＤ硫酸バリウム（重量平均粒子径１．４μｍ、屈折率１．６４）」を用い、酸化チタンについては、石原産業（株）製「タイペークＲ８３０（ルチル型、重量平均粒子径０．２５μｍ、屈折率２．７２）」を用い、そしてＭＳ系架橋粒子（メタクリル酸メチル−スチレン共重合架橋微粒子）については、積水化成品工業（株）製「テクポリマーＸＸ−２４Ｋ（重量平均粒子径５μｍ、屈折率１．５２）」を用いた。
(Examples 2 to 8)
A light diffusing laminated resin plate was prepared in the same manner as in Example 1 except that the type and content ratio of the light diffusing agent were changed to the types and content ratios shown in Table 1, respectively. As for barium sulfate, “AD barium sulfate (weight average particle diameter: 1.4 μm, refractive index: 1.64)” manufactured by Nippon Chemical Industry Co., Ltd. was used. For titanium oxide, “Taipeku” manufactured by Ishihara Sangyo Co., Ltd. was used. R830 (rutile type, weight average particle diameter 0.25 μm, refractive index 2.72) ”and MS-based crosslinked particles (methyl methacrylate-styrene copolymer crosslinked fine particles) manufactured by Sekisui Plastics Co., Ltd. “Techpolymer XX-24K (weight average particle diameter 5 μm, refractive index 1.52)” was used.
（比較例１、３、および４）
光拡散剤の種類および含有割合を、それぞれ表１に記載の種類および含有割合にしたこと以外は、実施例１と同様にして光拡散性積層樹脂板を調製した。
(Comparative Examples 1, 3, and 4)
A light diffusing laminated resin plate was prepared in the same manner as in Example 1 except that the type and content ratio of the light diffusing agent were changed to the types and content ratios shown in Table 1, respectively.
（比較例２）
上記スミペックスＥＸに、カルテックスＲＲを２重量％の割合となるように添加し、スーパーミキサーで混合した。得られた混合物を二軸押出機で溶融混練してメタクリル樹脂（Ａ）のペレットを調製した。次いで、得られたメタクリル樹脂（Ａ）のペレットを、東芝機械株式会社製の６５ｍｍφ一軸押出機で、２７５℃に設定したＴ型ダイスを介して押し出して所定の厚みを有するメタクリル樹脂（Ａ）からなる単層シートを調製した。
(Comparative Example 2)
Caltex RR was added to the Sumipex EX so as to have a ratio of 2% by weight and mixed with a super mixer. The resulting mixture was melt-kneaded with a twin screw extruder to prepare methacrylic resin (A) pellets. Next, the obtained methacrylic resin (A) pellets were extruded through a T-type die set at 275 ° C. with a 65 mmφ single screw extruder manufactured by Toshiba Machine Co., Ltd., and from a methacrylic resin (A) having a predetermined thickness. A single layer sheet was prepared.
さらに、スミペックスＥＸに、カルテックスＲＲを０．２重量％の割合となるように添加し、スーパーミキサーで混合した。得られた混合物を二軸押出機で溶融混練してメタクリル樹脂（Ｂ）のペレットを調製した。次いで、得られたメタクリル樹脂（Ｂ）のペレットを、東芝機械株式会社製の６５ｍｍφ一軸押出機で、２７５℃に設定したＴ型ダイスを介して押し出して所定の厚みを有するメタクリル樹脂（Ｂ）からなる単層シートを調製した。 Further, Caltex RR was added to Sumipex EX at a ratio of 0.2% by weight and mixed with a super mixer. The resulting mixture was melt-kneaded with a twin screw extruder to prepare methacrylic resin (B) pellets. Next, the obtained methacrylic resin (B) pellets were extruded through a T-type die set at 275 ° C. with a 65 mmφ single screw extruder manufactured by Toshiba Machine Co., Ltd., and from a methacrylic resin (B) having a predetermined thickness. A single layer sheet was prepared.
次いで、メタクリル樹脂（Ａ）からなるシートの表面に、接着剤層（アクリル系重合型接着剤（住友化学株式会社製、セメント７））を介してメタクリル樹脂（Ｂ）からなるシートを置いた。ゴム弾性を有する２本のロールに挟み込んで、空気を抜きつつ貼り合わせて、メタクリル樹脂（Ａ）からなるシートとメタクリル樹脂（Ｂ）からなるシートとが接着するまで放置し、光拡散性積層樹脂板を得た。 Next, a sheet made of methacrylic resin (B) was placed on the surface of the sheet made of methacrylic resin (A) via an adhesive layer (acrylic polymerization type adhesive (Sumitomo Chemical Co., Ltd., cement 7)). Light diffusing laminated resin, sandwiched between two rolls having rubber elasticity, stuck together while releasing air, and left until the sheet made of methacrylic resin (A) and the sheet made of methacrylic resin (B) are bonded I got a plate.
（比較例５）
光拡散剤の種類および含有割合を、表１に記載の種類および含有割合にしたこと以外は、比較例２と同様にして光拡散性積層樹脂板を調製した。
(Comparative Example 5)
A light diffusing laminated resin plate was prepared in the same manner as in Comparative Example 2 except that the type and content ratio of the light diffusing agent were changed to those shown in Table 1.
（比較例６）
メタクリル樹脂（Ａ）に含有される光拡散剤（炭酸カルシウム）の含有割合を２．２重量％にし、メタクリル樹脂（Ｂ）に光拡散剤を含有しなかったこと以外は、実施例１と同様にして光拡散性積層樹脂板を調製した。
(Comparative Example 6)
Example 1 except that the content ratio of the light diffusing agent (calcium carbonate) contained in the methacrylic resin (A) was 2.2% by weight and the methacrylic resin (B) did not contain any light diffusing agent. Thus, a light diffusing laminated resin plate was prepared.
各実施例および比較例で得られた光拡散性積層樹脂板について、以下の評価方法にて、ブツ発生個数、鏡面性、発煙など生産性、および端面外観をそれぞれ調べた。 With respect to the light-diffusing laminated resin plates obtained in each of the examples and comparative examples, the number of occurrences of fluff, specularity, productivity such as smoke generation, and end face appearance were examined by the following evaluation methods.
＜ブツ発生個数＞
得られた光拡散性積層樹脂板の任意の部分をＡ４サイズの大きさに切り取り、目視でブツの個数を数え、以下の基準で評価した。
○：ブツの個数が５個未満（ブツがない、または極めて少ない）。
△：ブツの個数が５個以上２０個未満（ブツが少ない）。
×：ブツの個数が２０個以上（ブツが多い）。
<Number of occurrences>
Arbitrary portions of the obtained light diffusing laminated resin plate were cut into A4 size, and the number of spots was visually counted and evaluated according to the following criteria.
○: The number of buns is less than 5 (no buns or very few).
(Triangle | delta): The number of protrusions is 5 or more and less than 20 pieces (there are few defects).
X: The number of bumps is 20 or more (there are many bumps).
＜鏡面性＞
得られた光拡散性積層樹脂板の任意の部分を切り取り、表面に反射した蛍光灯の写り込みの様子を目視で観察し、以下の基準で評価した。
○：反射した蛍光灯の像が、明確である場合。
△：反射した蛍光灯の像が、ややぼやけている場合（光沢が失われている場合）。
×：反射した蛍光灯の像が、明らかにぼやけている場合。
<Specularity>
An arbitrary portion of the obtained light diffusing laminated resin plate was cut out, and the appearance of the fluorescent lamp reflected on the surface was visually observed and evaluated according to the following criteria.
○: When the reflected fluorescent lamp image is clear.
Δ: The reflected fluorescent light image is slightly blurred (when gloss is lost).
X: When the reflected fluorescent lamp image is clearly blurred.
＜発煙など生産性＞
光拡散性積層樹脂板の生産時に、Ｔ型ダイス出口から一対のロールに挟み込まれるまでの間の積層シートからの発煙、および成形時のロールの汚れを目視で観察し、以下の基準で評価した。
○：発煙などの生産上の問題が一切ない場合。
△：やや発煙が認められるが、生産上、問題になるレベルではない場合。
×：発煙し、ロール汚れなどが認められ、収率の低下などを招く恐れがある場合。
<Productivity such as smoke>
During the production of the light diffusing laminated resin plate, the smoke generation from the laminated sheet until it was sandwiched between the pair of rolls from the exit of the T-shaped die and the dirt on the roll during molding were visually observed and evaluated according to the following criteria: .
○: When there is no production problem such as smoke.
Δ: Smoke is slightly observed, but is not at a level that causes problems in production.
X: When smoke is generated, roll dirt is observed, and there is a risk of lowering the yield.
＜端面外観＞
得られた光拡散性積層樹脂板の任意の部分を切り取り、端面をプラビューティーで研磨加工した後、端面を目視で観察し、以下の基準で評価した。
○：基材層と表面層との界面が、目視上観察できない（単層に見える）場合。
△：基材層と表面層との界面が、目視上僅かに確認できる（ほぼ単層に見える）場合。
×：基材層と表面層との界面が、目視上明らかに確認できる（多層に見える）場合。
<End face appearance>
An arbitrary portion of the obtained light diffusing laminated resin plate was cut out and the end face was polished with plasticity, and then the end face was visually observed and evaluated according to the following criteria.
◯: When the interface between the base material layer and the surface layer cannot be observed visually (appears as a single layer).
(Triangle | delta): When the interface of a base material layer and a surface layer can be confirmed visually visually (it looks almost a single layer).
X: When the interface of a base material layer and a surface layer can be confirmed clearly visually (it looks multilayer).
試験結果を表１に示す。 The test results are shown in Table 1.
表１に示すように、本発明の光拡散性積層樹脂板は、発煙などによる生産性の低下やブツの発生を抑制し、かつ良好な鏡面性を保ちつつ、端面の外観が良好であることがわかる。 As shown in Table 1, the light diffusing laminated resin plate of the present invention has a good end face appearance while suppressing the decrease in productivity due to fuming and the like, and the generation of flaws and maintaining good specularity. I understand.
本発明によれば、発煙などによる生産性の低下やブツの発生を抑制し、かつ良好な鏡面性を保ちつつ、端面の外観が良好な光拡散性積層樹脂板を提供することができる。したがって、本発明は、表示装置の保護板、照明カバー、照明看板などで有用である。また、本発明の光拡散性積層樹脂板は、和紙などの両面に配置され、プレスなどで一体積層化することにより、破れず耐候性に優れ光沢感のある和紙風シートが得られる。このような和紙風シートは、障子紙、襖紙、壁紙などの建材分野、和紙調照明カバーなどに有用である。 ADVANTAGE OF THE INVENTION According to this invention, the light diffusable laminated resin board with the favorable external appearance of an end surface can be provided, suppressing the fall of productivity by generation | occurrence | production of smoke, etc., and generation | occurrence | production of fuzz, and maintaining favorable mirror surface property. Therefore, the present invention is useful for a protective plate, a lighting cover, a lighting signboard, and the like of a display device. Further, the light diffusing laminated resin plate of the present invention is disposed on both surfaces of Japanese paper or the like, and is integrally laminated with a press or the like, whereby a Japanese paper-like sheet having excellent weather resistance without tearing and having a glossy feeling can be obtained. Such a Japanese paper-like sheet is useful in the field of building materials such as shoji paper, paper, and wallpaper, and a Japanese paper-like lighting cover.
Claims (4)
該樹脂板が０．５ｍｍ〜１０ｍｍの厚みを有し、かつ以下の（Ｉ）〜（ＩＶ）を満たす、ことを特徴とする光拡散性積層樹脂板。
（I）光拡散剤（ａ）および光拡散剤（ｂ）が、同種の光拡散剤であること、
（II）メタクリル樹脂（Ａ）に含有される光拡散剤（ａ）の割合が、メタクリル樹脂（Ｂ）に含有される光拡散剤（ｂ）の割合よりも多いこと、
（III）表面層の厚みが、光拡散性積層樹脂板の厚みの１／１０以下であること、および
（IV）基材層の表面層側表面と、表面層の基材層側表面とは接していること。 0.1% by weight to 10% by weight of the light diffusing agent (a) is added to at least one surface of the base material layer made of the methacrylic resin (A) containing 0.11% by weight to 20% by weight of the light diffusing agent (a). a light diffusing laminated resin plate in which a surface layer made of a methacrylic resin (B) containing b) is laminated,
The light-diffusing laminated resin plate, wherein the resin plate has a thickness of 0.5 mm to 10 mm and satisfies the following (I) to (IV):
(I) The light diffusing agent (a) and the light diffusing agent (b) are the same kind of light diffusing agent,
(II) The proportion of the light diffusing agent (a) contained in the methacrylic resin (A) is larger than the proportion of the light diffusing agent (b) contained in the methacrylic resin (B).
(III) The thickness of the surface layer is 1/10 or less of the thickness of the light diffusing laminated resin plate, and (IV) the surface layer side surface of the base material layer and the base material layer side surface of the surface layer Be in contact.
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