JP2990278B2 - Stretching method of aliphatic polyester sheet - Google Patents
Stretching method of aliphatic polyester sheetInfo
- Publication number
- JP2990278B2 JP2990278B2 JP2797799A JP2797799A JP2990278B2 JP 2990278 B2 JP2990278 B2 JP 2990278B2 JP 2797799 A JP2797799 A JP 2797799A JP 2797799 A JP2797799 A JP 2797799A JP 2990278 B2 JP2990278 B2 JP 2990278B2
- Authority
- JP
- Japan
- Prior art keywords
- polylactic acid
- sheet
- plla
- stretching method
- polymer composition
- 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.)
- Expired - Lifetime
Links
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、成形が可能な脂肪
族ポリエステル系で使用後に、土壌中、水中で、分解可
能な新規な生分解性ポリエステルシートの延伸加工方法
に関するものである。さらに詳しくは、本発明は、例え
ば、農業、畜産、漁業用分野で使用されるシートや文
具、日用品に好適に利用できる新規な生分解性ポリエス
テルシートの延伸加工方法に関するものである。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a novel method for stretching a biodegradable polyester sheet which can be decomposed in soil or water after being used in a moldable aliphatic polyester system. More specifically, the present invention relates to a novel method for stretching a biodegradable polyester sheet that can be suitably used for, for example, sheets, stationery, and daily necessities used in the fields of agriculture, livestock, and fisheries.
【０００２】[0002]
【従来の技術】生分解性とは、材料が土壌中、又は、海
水、淡水などの水中で微生物や酵素によって分解され、
低分子になる現象である。従来から、脂肪族ポリエステ
ルの一部は生分解性を示すことが知られており、ポリ乳
酸は、この現象が顕著である。しかしながら、強度や弾
性率を向上させるためには、高融点成分であるポリ乳酸
の分子鎖を配向させる必要がある。通常の延伸加工法を
ポリ乳酸高分子組成物に適用し、均一な延伸を行うに
は、比較的厚みの薄いフィルム状のものである必要があ
った。このために、延伸後のフィルムの厚さに制限があ
り、力学的性質も満足な状況とはいえない。2. Description of the Related Art Biodegradability means that a material is decomposed by microorganisms or enzymes in soil or in water such as seawater or freshwater.
This is the phenomenon of becoming low molecular. Hitherto, it has been known that some aliphatic polyesters exhibit biodegradability, and this phenomenon is remarkable in polylactic acid. However, in order to improve strength and elastic modulus, it is necessary to orient the molecular chains of polylactic acid, which is a high melting point component. In order to apply a normal stretching method to the polylactic acid polymer composition and to perform uniform stretching, it was necessary to form a film having a relatively small thickness. For this reason, the thickness of the film after stretching is limited, and the mechanical properties are not satisfactory.
【０００３】[0003]
【発明が解決しようとする課題】本発明はポリ乳酸から
なり、生分解性を示し、かつ、厚みのあるシート状成形
物に高融点成分であるポリ乳酸の分子鎖配向を付与する
ための延伸方法を提供することをその課題とする。DISCLOSURE OF THE INVENTION The present invention relates to a stretching method for imparting the molecular chain orientation of polylactic acid, which is a high melting point component, to a thick sheet-like molded product made of polylactic acid, exhibiting biodegradability. The task is to provide a method.
【０００４】[0004]
【課題を解決するための手段】本発明者らは、前記課題
を解決すべく鋭意検討した結果、本発明を完成するに至
った。すなわち、以下のことを見出したことによるもの
である。ポリ乳酸とポリ（ε−カプロラクトン）を主成
分とする高分子ブレンド組成物からなるシートを下式
（１）の温度Ｔｓ（℃）に加熱した一対のロールの間隙
から引き抜いて、一軸方向に３倍以上の延伸比を与える
高配向延伸加工方法が提供される。 [Tg(PLLA) × W(PLLA) + ｛Tm (PCL)−40｝×W(PCL)]/1
00 ＜ Ts ≦[{Tm(PLLA) - 80｝× W(PLLA) + ｛Tm (PC
L)−30｝×W(PCL)]/100 （２） ［但し、Ｔｇ（ＰＬＬ
Ａ）は、ポリ乳酸のガラス転移温度（℃）であり、Ｗ
（ＰＬＬＡ）はポリ乳酸の重量％、Ｔｍ（ＰＣＬ）は、
ポリ（ε−カプロラクトン）の融点（℃）、Ｗ（ＰＣ
Ｌ）は、ポリ（ε−カプロラクトン）の重量％、Ｔｍ
（ＰＬＬＡ）は、ポリ乳酸の融点である。］ 本発明の高配向延伸加工方法にいては、ポリ（ε−カプ
ロラクトン）を含まないもの、即ちその含有量が０の場
合である。この条件下に、前記（２）の式を整理する
と、以下の式（１）が得られる。即ち、本発明によれ
ば、ポリ乳酸からなる高分子組成物のシートを、下式
（１）の温度Ｔｓ（℃）に加熱した一対のロールの間隙
からを引き抜いて、一軸方向に３倍以上の延伸比を与え
る高配向延伸加工方法が提供される。 Tg(PLLA) ＜ Ts ≦ {Tm(PLLA) - 80｝ （１） ［但し、式中、Ｔｇ（ＰＬＬＡ）は、ポリ乳酸のガラス
転移温度（℃）であり、Ｔｍ（ＰＬＬＡ）は、ポリ乳酸
の融点である。］Means for Solving the Problems The present inventors have made intensive studies to solve the above-mentioned problems, and as a result, completed the present invention. That is, it is because they have found the following. A sheet made of a polymer blend composition containing polylactic acid and poly (ε-caprolactone) as main components is pulled out from a gap between a pair of rolls heated to a temperature Ts (° C.) of the following formula (1), and 3 A highly oriented stretching method for providing a stretching ratio of at least twice is provided. [Tg (PLLA) × W (PLLA) + ｛Tm (PCL) −40｝ × W (PCL)] / 1
00 <Ts ≤ [{Tm (PLLA)-80｝ × W (PLLA) + ｛Tm (PC
L) -30｝ × W (PCL)] / 100 (2) [However, Tg (PLL
A) is the glass transition temperature (° C.) of polylactic acid;
(PLLA) is the weight% of polylactic acid, Tm (PCL) is
Melting point (° C) of poly (ε-caprolactone), W (PC
L) is the weight percentage of poly (ε-caprolactone), Tm
(PLLA) is the melting point of polylactic acid. In the method for highly oriented stretching according to the present invention, the method does not include poly (ε-caprolactone), that is, the case where the content is 0. When the above equation (2) is rearranged under this condition, the following equation (1) is obtained. That is, according to the present invention, a sheet of the polymer composition made of polylactic acid is pulled out from a gap between a pair of rolls heated to a temperature Ts (° C.) of the following formula (1), and is three times or more in one axial direction. A highly oriented stretching method for providing a stretching ratio of Tg (PLLA) <Ts ≦ {Tm (PLLA) −80｝ (1) [where Tg (PLLA) is the glass transition temperature (° C.) of polylactic acid, and Tm (PLLA) is polylactic acid. Melting point. ]
【０００５】[0005]
【発明の実施の形態】本発明においては、ポリ乳酸から
なる高分子組成物からなるシートを被処理原料として用
いる。この場合、前記高分子組成物としては、ポリ乳酸
を、二軸押出機を用いて、溶融混練することで得られる
ポリ乳酸からなる高分子組成物であって、該ポリ乳酸の
含有量は１００重量％である。本発明の延伸加工方法に
おいては、前記高分子組成物シートを一対のロールの間
隙から引き抜いて、一軸方向に３倍以上の延伸比を与
え、高融点成分であるポリ乳酸の分子鎖を高度に配向さ
せるが、この場合、そのロール引き抜き方法それ自体は
ポリエチレン等の高分子の延伸に適用され、公知の方法
である（たとえば特開昭５９−２２０３２９）。また、
ポリ乳酸が、生分解性を示すことは公知である。しかし
ながら、本発明者等の知る限りロール引き抜き法を脂肪
族ポリエステルの延伸加工に適用した報告はなされてお
らず、勿論それにより得られるブレンド成形物に適用し
た報告もされていない。ポリ乳酸を主成分とする高分子
組成物からなるシートを本発明による温度条件に加熱し
た一対のロールの間隙から引き抜いて、一軸方向に３倍
以上の延伸比を与え、高融点成分のポリ乳酸の分子鎖を
高度に配向させる延伸加工方法は本発明者らによって初
めて見い出されたものである。次に添付図面によって、
本発明の方法を説明する。図１は、本発明の実施態様を
示すローラ部分である。始めに、シート３をローラ１の
内部に取り付けたヒータで所定の温度に加熱した一対の
ロ−ラ１，１の間から張力を加えて引き抜き、目的のシ
ート４を得る。このローラの間隙は調節可能であり、種
々の厚さのシートを得ることができる。本発明の方法で
用いられる、ポリ乳酸には、そのＬ−体、Ｄ−体及びＤ
Ｌ−体が包含されるが、本発明の場合、Ｌ−体を７０〜
１００重量％含有するもの、又は、Ｄ−体を７０〜１０
０重量％含有するもの、好ましくは、ポリ（Ｌ−乳酸）
の使用が好ましい。ＤＬ−体の含有量が高いと結晶性の
低下が生じるので、あまり好ましいものではない。DESCRIPTION OF THE PREFERRED EMBODIMENTS In the present invention, a sheet composed of a polymer composition composed of polylactic acid is used as a raw material to be treated. In this case, the polymer composition is a polymer composition of polylactic acid obtained by melt-kneading polylactic acid using a twin screw extruder, and the content of the polylactic acid is 100. % By weight. In the stretching method of the present invention, the polymer composition sheet is pulled out from a gap between a pair of rolls to give a stretching ratio of 3 times or more in a uniaxial direction, and the molecular chain of polylactic acid, which is a high melting point component, is highly enhanced. In this case, the roll drawing method itself is applied to stretching of a polymer such as polyethylene, and is a known method (for example, JP-A-59-220329). Also,
It is known that polylactic acid exhibits biodegradability. However, to the knowledge of the present inventors, there has been no report on applying the roll drawing method to the stretching of aliphatic polyesters, and of course, no report has been found on the application to a blend molded product obtained by the method. A sheet made of a polymer composition containing polylactic acid as a main component is pulled out from a gap between a pair of rolls heated to a temperature condition according to the present invention, and a stretching ratio of 3 times or more is provided in a uniaxial direction, and polylactic acid as a high melting point component is obtained. A stretching method for highly orienting the molecular chain has been found for the first time by the present inventors. Next, according to the attached drawings,
The method of the present invention will be described. FIG. 1 is a roller portion showing an embodiment of the present invention. First, the sheet 3 is pulled out by applying tension between a pair of rollers 1 and 1 heated to a predetermined temperature by a heater mounted inside the roller 1 to obtain a target sheet 4. The gap between the rollers is adjustable so that sheets of various thicknesses can be obtained. The polylactic acid used in the method of the present invention includes its L-form, D-form and D-form.
The L-form is included, and in the case of the present invention, the L-form is 70 to
100 to 100% by weight, or 70 to 10% of D-form
0% by weight, preferably poly (L-lactic acid)
The use of is preferred. If the content of the DL-form is high, the crystallinity is reduced, so that it is not very preferable.
【０００６】本発明の生分解性高分子組成物を成形する
には、ポリ乳酸を、二軸押出機を用いて、溶融混練する
ことで得られる高分子組成物であって、ポリＬ乳酸の融
点（Ｔｍ）である１７４℃以上の温度、好ましくは、１
９０℃から２５０℃の範囲で溶融混練したのち、押出成
形する。これによりシート状に得ることができる。こう
して得られたシートを延伸加工後に希望するシート厚み
にロール間隙を設定したロールの間から引き抜くことに
より、一軸方向に３倍以上の延伸比を与える。これによ
り、高融点成分のポリ乳酸の分子鎖の配向したシートを
得ることができる。シートの一軸方向に与える延伸比は
３倍以上、好ましくは４倍以上である。その上限値は、
通常、６倍程度である。[0006] In order to mold the biodegradable polymer composition of the present invention, a polylactic acid is a polymer composition obtained by melt-kneading using a twin screw extruder. A temperature of 174 ° C. or more, which is the melting point (Tm), preferably 1
After melt-kneading in the range of 90 ° C. to 250 ° C., extrusion molding is performed. Thereby, a sheet can be obtained. The sheet thus obtained is drawn out from between the rolls having a roll gap set to a desired sheet thickness after the drawing process, thereby giving a stretch ratio of 3 times or more in the uniaxial direction. As a result, a sheet in which the molecular chains of the polylactic acid having a high melting point are oriented can be obtained. The stretching ratio given in the uniaxial direction of the sheet is 3 times or more, preferably 4 times or more. The upper limit is
Usually, it is about six times.
【０００７】[0007]
【実施例】次に本発明を実施例によりさらに詳細に説明
する。Next, the present invention will be described in more detail with reference to examples.
【０００８】実施例１ 原料のポリ乳酸として、島津製作所製ラクティ１０１２
を用いた。このものの融点（ＤＳＣのピーク温度）は１
７４℃で、ガラス転移温度は６８℃であった。これを真
空下で２４時間以上乾燥したのち、室温度でポリ乳酸１
００重量％である組成物を二軸押出機内で温度２０５℃
に加熱溶融、混練したのち、幅６０ｍｍ、隙間１．０５
ｍｍのＴダイからシート状に押出し、水中で冷却後に巻
き取った。こうして得られた厚さ約１ｍｍのシートを所
定の温度（６８℃）に加熱した外径１２０ｍｍ、幅１５
０ｍｍの一対のクロムメッキした鋼製ローラを用い、ロ
ールの間隙から引き出して延伸加工したところ、表面状
態の良好なシートを得ることができた。Example 1 As a raw material polylactic acid, Lacty 1012 manufactured by Shimadzu Corporation was used.
Was used. Its melting point (peak temperature of DSC) is 1
At 74 ° C, the glass transition temperature was 68 ° C. After drying this under vacuum for 24 hours or more, the polylactic acid 1
In a twin-screw extruder at a temperature of 205 ° C.
After heating and kneading, a width of 60 mm and a gap of 1.05
It was extruded into a sheet form from a T-die having a diameter of mm, cooled in water and wound up. The thus obtained sheet having a thickness of about 1 mm was heated to a predetermined temperature (68 ° C.) and had an outer diameter of 120 mm and a width of 15 mm.
Using a pair of 0 mm chrome-plated steel rollers, the sheet was drawn out from the gap between the rolls and stretched, whereby a sheet having a good surface condition could be obtained.
【０００９】[0009]
【表１】 [Table 1]
【００１０】[0010]
【発明の効果】本発明のポリ乳酸を主成分とする高分子
組成物からなるシートは、フィルム状に比べて厚さが大
きいにもかかわらず、均一な分子鎖の配向を示し、延伸
後の表面も平滑であり、高い強度を示す。本発明の延伸
加工方法が厚みの大きいシートの延伸に適用でき、か
つ、良好な延伸シートを与えることができる理由は、ロ
ール温度の範囲を適切に選ぶことによって、ロールの間
隙から引き出され変形したブレンドのシートが高度に分
子鎖配向することにより、破断や流動することなく、平
滑な表面を有するシート形状を維持できることにある。
本発明によって延伸加工してシート成形物は、弾性率、
強度が高く、例えば、農業、漁業用分野での、生分解性
を必要とする部品、部材等に好適に利用できる。また、
玩具や、日用品に好適に利用できる。The sheet composed of the polymer composition containing polylactic acid as the main component of the present invention shows a uniform molecular chain orientation despite its thickness being larger than that of a film, The surface is also smooth and shows high strength. The reason why the stretching method of the present invention can be applied to stretching of a sheet having a large thickness, and that a good stretched sheet can be obtained is that by appropriately selecting the range of the roll temperature, the sheet is drawn from the gap between the rolls and deformed. An object of the present invention is to maintain a shape of a sheet having a smooth surface without breaking or flowing due to a highly oriented molecular chain of a sheet of the blend.
The sheet molding obtained by stretching according to the present invention has an elastic modulus,
It has high strength and can be suitably used for parts and members that require biodegradability in the fields of agriculture and fisheries, for example. Also,
It can be suitably used for toys and daily necessities.
【図１】本発明に用いるロール引き抜き延伸加工装置の
構造を示す断面図。FIG. 1 is a sectional view showing the structure of a roll drawing and stretching apparatus used in the present invention.
１ ローラ ２ 加熱ヒーター ３ 原料シート ４ 引き抜いて延伸加工したシート DESCRIPTION OF SYMBOLS 1 Roller 2 Heater 3 Material sheet 4 Sheet drawn and drawn
───────────────────────────────────────────────────── フロントページの続き (51)Int.Cl.6 識別記号 ＦＩ Ｂ２９Ｌ 7:00 (72)発明者 レオン テベイク 茨城県つくば市東１丁目１番 工業技術 院物質工学工業技術研究所内 (58)調査した分野(Int.Cl.6，ＤＢ名) B29C 55/18,55/30,55/06 C08J 5/18 CFD C08L 67/04 ──────────────────────────────────────────────────の Continued on the front page (51) Int.Cl. 6 Identification code FI B29L 7:00 (72) Inventor Leon Tebake 1-1-1 Higashi, Tsukuba, Ibaraki Pref. Field (Int.Cl. 6 , DB name) B29C 55 / 18,55 / 30,55 / 06 C08J 5/18 CFD C08L 67/04
Claims (4)
を、下式（１）の温度Ｔｓ（℃）に加熱した一対のロー
ルの間隙から引き抜いて、一軸方向に３倍以上の延伸比
を与えることを特徴とする高配向延伸加工方法。 Tg(PLLA) ＜ Ts ≦ {Tm(PLLA) - 80｝ （１） ［但し、Ｔｇ（ＰＬＬＡ）は、ポリ乳酸のガラス転移温
度（℃）であり、Ｔｍ（ＰＬＬＡ）は、ポリ乳酸の融点
である。］1. A sheet of a polymer composition comprising polylactic acid is pulled out from a gap between a pair of rolls heated to a temperature Ts (° C.) of the following formula (1), and a stretching ratio of at least three times in a uniaxial direction is obtained. A highly oriented stretching method. Tg (PLLA) <Ts ≦ {Tm (PLLA) -80｝ (1) [where Tg (PLLA) is the glass transition temperature (° C.) of polylactic acid, and Tm (PLLA) is the melting point of polylactic acid. is there. ]
１００重量％含有することを特徴とする請求項１記載の
高配向延伸加工方法。2. The polylactic acid according to claim 1, wherein the poly (lactic acid) is 70 to
2. The highly oriented stretching method according to claim 1, wherein the content is 100% by weight.
１００重量％含有することを特徴とする請求項１記載の
高配向延伸加工方法。3. The polylactic acid has a poly (D-lactic acid) content of 70 to
2. The highly oriented stretching method according to claim 1, wherein the content is 100% by weight.
軸押出機を用いて、溶融混練することで得られるポリ乳
酸を主成分とする高分子組成物であることを特徴とする
請求項１記載の高配向延伸加工方法。4. The polymer composition according to claim 1, wherein the polymer composition is polylactic acid, and the polymer composition is mainly composed of polylactic acid and obtained by melt-kneading using a twin screw extruder. The highly oriented stretching method according to claim 1.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2797799A JP2990278B2 (en) | 1999-02-04 | 1999-02-04 | Stretching method of aliphatic polyester sheet |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2797799A JP2990278B2 (en) | 1999-02-04 | 1999-02-04 | Stretching method of aliphatic polyester sheet |
Related Parent Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP10069628 Division | 1998-03-19 | 1998-03-19 |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH11268116A JPH11268116A (en) | 1999-10-05 |
| JP2990278B2 true JP2990278B2 (en) | 1999-12-13 |
Family
ID=12235932
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP2797799A Expired - Lifetime JP2990278B2 (en) | 1999-02-04 | 1999-02-04 | Stretching method of aliphatic polyester sheet |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2990278B2 (en) |
Families Citing this family (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP4960660B2 (en) * | 2006-07-19 | 2012-06-27 | 積水化学工業株式会社 | Method for producing stretched thermoplastic polyester resin sheet |
| JP4960661B2 (en) * | 2006-07-19 | 2012-06-27 | 積水化学工業株式会社 | Method for producing stretched thermoplastic polyester resin sheet |
| JP4874845B2 (en) * | 2007-03-27 | 2012-02-15 | 積水化学工業株式会社 | Method for producing drawing-drawn thermoplastic resin sheet |
| JP5064895B2 (en) * | 2007-06-06 | 2012-10-31 | 積水化学工業株式会社 | Method for producing stretched thermoplastic polyester resin sheet |
| EP2493978A4 (en) * | 2009-10-29 | 2014-01-15 | Sole Gear Design Inc | Compositions comprising polylactic acid, bentonite, and gum arabic |
| AU2010312244A1 (en) * | 2009-10-29 | 2012-05-17 | Sole Gear Design Inc. | Compositions comprising polylactic acid and gum arabic |
| CN111212721B (en) * | 2017-09-08 | 2022-04-26 | 宙斯有限公司 | Polymeric tube with controlled orientation |
| CN116474179A (en) | 2017-09-08 | 2023-07-25 | 宙斯有限公司 | Polymer tube with controlled orientation |
-
1999
- 1999-02-04 JP JP2797799A patent/JP2990278B2/en not_active Expired - Lifetime
Also Published As
| Publication number | Publication date |
|---|---|
| JPH11268116A (en) | 1999-10-05 |
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