JP7408561B2 - 多層構造体及びそれを用いた包装材 - Google Patents
多層構造体及びそれを用いた包装材 Download PDFInfo
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- JP7408561B2 JP7408561B2 JP2020551089A JP2020551089A JP7408561B2 JP 7408561 B2 JP7408561 B2 JP 7408561B2 JP 2020551089 A JP2020551089 A JP 2020551089A JP 2020551089 A JP2020551089 A JP 2020551089A JP 7408561 B2 JP7408561 B2 JP 7408561B2
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Description
[1]硬質層(A)と、樹脂組成物層(B1)または樹脂組成物層(B2)とを有する多層構造体であって、硬質層(A)の突き刺し強度が40N/mm以上150N/mm以下であり、樹脂組成物層(B1)を構成する樹脂が、融点Tm1が170℃以上であるエチレン-ビニルアルコール共重合体(b1)(以下、EVOH(b1)と称することがある)と融点Tm2が170℃未満であるエチレン-ビニルアルコール共重合体(b2)(以下、EVOH(b2)と称することがある)からなり、樹脂組成物層(B2)を構成する樹脂が、下記式(I)で表される一級水酸基を持つ変性基を含有する変性EVOHからなる、多層構造体;
[2]EVOH(b1)に対するEVOH(b2)の質量比(b2/b1)が1/99~50/50である、[1]の多層構造体;
[3]EVOH(b2)のエチレン含有量(モル%)とEVOH(b1)のエチレン含有量(モル%)の差の絶対値|b2-b1|が5以上である、[1]又は[2]の多層構造体;
[4]硬質層(A)がオレフィン系重合体を含む、[1]~[3]のいずれかの多層構造体;
[5]前記オレフィン系重合体が直鎖状低密度ポリエチレンである、[4]の多層構造体;
[6]直鎖状低密度ポリエチレンが、メタロセン触媒を用いて重合されたエチレン重合体又は共重合体である、[5]の多層構造体;
[7]前記オレフィン系重合体が植物由来ポリエチレンを含む、[4]~[6]のいずれかの多層構造体;
[8]前記オレフィン系重合体がエチレン-不飽和カルボン酸共重合体アイオノマーである、[4]の多層構造体;
[9]前記オレフィン系重合体の密度が0.940以下である、[4]~[7]のいずれかの多層構造体;
[10]前記オレフィン系重合体の融点が130℃以下である、[4]~[9]のいずれかの多層構造体;
[11]前記オレフィン系重合体のメルトフローレート(190℃、2160g)(以下、メルトフローレートをMFRと称することがある)が5.0g/10分未満である、[4]~[10]のいずれかの多層構造体;
[12]樹脂組成物層(B1)または樹脂組成物層(B2)が2つの硬質層(A)の間に配置されてなる、[1]~[11]のいずれかの多層構造体;
[13]硬質層(A)と、樹脂組成物層(B1)または樹脂組成物層(B2)との間に、さらに接着性樹脂層(C)を有する、[1]~[12]のいずれかの多層構造体;
[14]接着性樹脂層(C)/樹脂組成物層(B1)または樹脂組成物層(B2)/接着性樹脂層(C)の層構成を有する、[13]の多層構造体;
[15][1]~[14]のいずれかの多層構造体からなる包装材;
[16][1]~[14]のいずれかの多層構造体の回収物を含む、回収組成物;
[17][1]~[14]のいずれかの多層構造体の回収物を溶融混錬する、回収組成物の製造方法を提供することにより解決される。
硬質層(A)の突き刺し強度は40N/mm以上150N/mm以下である。突き刺し強度が上記範囲であることで、本発明の多層構造体を用いた包装材で包装された食品等を運搬する際に、該包装材におけるピンホールの発生を防ぐことができる。突き刺し強度は45N/mm以上が好ましく、50N/mm以上がより好ましく、55N/mm以上がさらに好ましく、65N/mm以上が特に好ましい。また、突き刺し強度は120N/mm以下が好ましく、100N/mm以下がより好ましく、75N/mm以下がさらに好ましい。本明細書における硬質層(A)の突き刺し強度は、硬質層(A)と同じ組成の単層フィルムからなる試験片を、23℃、50%RH条件下で24時間調湿した後、同条件下で、先端直径1mmの針が、50mm/minの速度で試験片を突き抜けた時の荷重を測定し、その平均値を試験片厚み(mm)で除することにより算出される値(N/mm)である。
樹脂組成物層(B1)を構成する樹脂は、EVOH(b1)とEVOH(b2)からなる。EVOH(b1)の融点Tm1が170℃よりも小さい場合には、得られる多層構造体の突き刺し強度とガスバリア性が低下する。また、EVOH(b2)の融点Tm2が170℃以上の場合には、得られる多層構造体の熱成形性が低下する。樹脂組成物層(B1)を構成する樹脂は、EVOH(b1)とEVOH(b2)のみからなることが好ましい。
樹脂組成物層(B2)を構成する樹脂は、下記式(I)で表される一級水酸基を持つ変性基を含有する変性EVOHを含む。この変性EVOHがエチレン単位及びビニルアルコール単位に加えて、一級水酸基を持つ変性基を含有することによって、得られる多層構造体の熱成形性が向上するとともに、樹脂組成物層(B2)と後述する接着性樹脂層(C)との接着性が向上する。
本発明の多層構造体は、硬質層(A)と樹脂組成物層(B1)又は樹脂組成物層(B2)との間に、さらに接着性樹脂層(C)を有することが好ましい。接着性樹脂層(C)に用いられる接着性樹脂としては、例えば不飽和カルボン酸又はその無水物をオレフィン系重合体に付加反応やグラフト反応等により化学的に結合させて得られるカルボキシル基を含有する変性オレフィン系重合体を挙げることができる。不飽和カルボン酸又はその無水物としては、マレイン酸、無水マレイン酸、フマル酸、アクリル酸、メタクリル酸、クロトン酸、イタコン酸、シトラコン酸、ヘキサヒドロ無水フタル酸等が挙げられ、中でも、無水マレイン酸が好適に用いられる。具体的には、無水マレイン酸グラフト変性ポリエチレン、無水マレイン酸グラフト変性ポリプロピレン、無水マレイン酸グラフト変性エチレン-プロピレン共重合体、無水マレイン酸グラフト変性エチレン-エチルアクリレート共重合体、無水マレイン酸グラフト変性エチレン-酢酸ビニル共重合体等から選ばれた1種又は2種以上の混合物が好適なものとして挙げられる。
本発明の多層構造体は、樹脂組成物層(B1)又は樹脂組成物層(B2)が2つの硬質層(A)の間に配置されてなることが好ましい。この場合、硬質層(A)と、樹脂組成物層(B1)又は(B2)の間に任意の他の層を設けても良い。
共押出多層キャスト製膜装置を用いて、硬質層(A)がメタロセン触媒を用いて重合された直鎖状低密度ポリエチレン(mLLDPE-1;プライムポリマー社製「エボリューSP0510」)からなり、樹脂組成物層(B1)がEVOH(b1)としてEVOH(エチレン含有量27モル%、ケン化度99.9モル%、融点190℃)を80質量部、及びEVOH(b2)としてEVOH(エチレン含有量44モル%、ケン化度99.9モル%、融点165℃)を20質量部配合した樹脂組成物からなり、接着性樹脂層(C)が無水マレイン酸変性ポリエチレン(三井化学社製「AdmerNF518」)からなる多層構造体((A)/(C)/(B1)/(C)/(A)=41μm/6μm/6μm/6μm/41μmの層厚みと層構成を有する5層共押出多層キャストフィルム)を得た。このときの製膜条件は以下に示す。
共押出条件
硬質層(A)の押出温度:供給部/圧縮部/計量部/ダイ=170/220/220/220℃
樹脂組成物層(B1)の押出温度:供給部/圧縮部/計量部/ダイ=170/220/220/220℃
接着樹脂層(C)の押出温度:供給部/圧縮部/計量部/ダイ=170/220/220/220℃
押出機:
・硬質層(A) 32φ押出機 GT-32-A型(株式会社プラスチック工学研究所製)
・接着性樹脂 25φ押出機 P25-18-AC型(大阪精機工作株式会社製)
・樹脂組成物 20φ押出機 ラボ機ME型CO-EXT(株式会社東洋精機製)
Tダイ:300mm幅3種5層用(株式会社プラスチック工学研究所製)
冷却ロールの温度:60℃
引取速度:3m/分
20mmφ単軸押出機(押出温度200℃)を用いて、硬質層(A)に使用される樹脂からなる厚み100μmの単層フィルムを製膜し、当該単層フィルムを試験片として用いた。当該試験片を23℃、50%RH条件下で24時間調湿した後、同条件下で、先端直径1mmの針が、50mm/minの速度で試験片を突き抜けた時の荷重を測定し、その平均値を試験片厚み(mm)で除することにより突き刺し強度(N/mm)を算出した。
得られた多層構造体を熱成形機(浅野製作所製:真空圧空深絞り成形機「FX-0431-3型」)にて、シート温度を110℃にして、圧縮空気(気圧5kgf/cm2)により丸カップ形状の包装材(金型形状:上部75mmφ、下部60mmφ、深さ37mm、絞り比S=0.5)に熱成形した。得られた包装材を目視で観察し、熱成形性を評価した。成形条件及び評価の基準を以下に示す。
ヒーター温度:600℃
プラグ:45φ×65mm
金型温度:40℃
A:外観異常なし
B:一部白化不良あり
C:破断箇所あり
得られた多層構造体をJIS Z 1707に準拠し、23℃、50%RHの条件下で調湿した後、直径10cmの円形にカットして試験片を得た。治具を用いて試験片を固定し、AUTOGRAPH(島津製作所製「AGS-H」)で直径1.0mm、先端形状が半径0.5mmの半円形である針を50mm/分の速度で試験片に突き刺すことで、針が貫通するまでの最大応力(N)を測定して、多層構造体の突き刺し強度とした。
酸素透過量測定装置(MOCON社製「MOCON OX-TRAN2/20型」)を用い、20℃、65%RH条件下でJIS K 7126-2(等圧法;2006年)に準じて、得られた多層構造体の酸素透過度(OTR)を測定し、その平均値を求めた。
多層構造体を粉砕して得られた回収物を20mmφ押出機を用いて、厚み20μmのフィルムに製膜した。得られたフィルムの単位面積当たりに見られるブツの個数(個数/m2)を計測した。ブツの個数が少ないほど、リサイクル性に優れると評価した。
A:500個/m2未満
B:500個/m2以上、750個/m2未満
C:750個/m2以上、1000個/m2未満
D:1000個/m2以上
硬質層(A)、樹脂組成物層(B1)、及び接着性樹脂層(C)を表1に示す通りとしたこと以外は実施例1と同様にして、多層構造体及び包装材を得た後、各種評価を行った。結果を表1に示す。なお、硬質層(A)として、実施例2ではエチレン-メタクリル酸共重合体アイオノマーである三井デュポンケミカル社製「ハイミラン1706」を用いた。実施例3ではメタロセン触媒を用いて重合された直鎖状低密度ポリエチレンであるプライムポリマー社製「エボリューSP1510」を用いた。実施例6ではメタロセン触媒を用いて重合された直鎖状低密度ポリエチレンであるプライムポリマー社製「エボリューSP4510」を用いた。実施例7では植物由来のエチレンを原料とする植物由来ポリエチレン(メタロセン触媒を用いて重合された直鎖状低密度ポリエチレン)であるブラスケム社製「SLL318」を用いた。比較例2及び比較例5では、無水マレイン酸変性ポリエチレンの代わりにポリアミド樹脂(BASF社製「Ultramid C40L」)を用いて、接着性樹脂層(C)の代わりにポリアミド樹脂からなる層を形成した。EVOH(b1)として、実施例8ではEVOH(エチレン含有量32モル%、ケン化度99.9モル%、融点183℃)を用いて樹脂組成物層(B1)を形成した。実施例9では表2に記載の式(I)においてXがCH2OH、R1が単結合で表される一級水酸基を持つ変性基を含有する変性EVOH(エチレン含有量27モル%、ケン化度99.9モル%、変性度1.0モル%)を用いて樹脂組成物層(B1)の代わりに樹脂組成物層(B2)を形成した。
Claims (17)
- 硬質層(A)と、樹脂組成物層(B1)または樹脂組成物層(B2)とを有し、ポリアミド系樹脂層を有さない多層構造体であって、
硬質層(A)の突き刺し強度が40N/mm以上150N/mm以下であり、
樹脂組成物層(B1)を構成する樹脂が、融点Tm1が170℃以上であるエチレン-ビニルアルコール共重合体(b1)と融点Tm2が170℃未満であるエチレン-ビニルアルコール共重合体(b2)からなり、
樹脂組成物層(B2)を構成する樹脂が、下記式(I)で表される一級水酸基を持つ変性基を含有する変性エチレン-ビニルアルコール共重合体からなる、多層構造体。
- エチレン-ビニルアルコール共重合体(b1)に対するエチレン-ビニルアルコール共重合体(b2)の質量比(b2/b1)が1/99~50/50である、請求項1に記載の多層構造体。
- エチレン-ビニルアルコール共重合体(b2)のエチレン含有量(モル%)とエチレン-ビニルアルコール共重合体(b1)のエチレン含有量(モル%)の差の絶対値|b2-b1|が5以上である、請求項1又は2に記載の多層構造体。
- 硬質層(A)がオレフィン系重合体を含む、請求項1~3のいずれかに記載の多層構造体。
- 前記オレフィン系重合体が直鎖状低密度ポリエチレンである、請求項4に記載の多層構造体。
- 前記直鎖状低密度ポリエチレンが、メタロセン触媒を用いて重合されたエチレン重合体又は共重合体である、請求項5に記載の多層構造体。
- 前記オレフィン系重合体が植物由来ポリエチレンを含む、請求項4~6のいずれかに記載の多層構造体。
- 前記オレフィン系重合体がエチレン-不飽和カルボン酸共重合体アイオノマーである、請求項4に記載の多層構造体。
- 前記オレフィン系重合体の密度が0.940以下である、請求項4~7のいずれかに記載の多層構造体。
- 前記オレフィン系重合体の融点が130℃以下である、請求項4~9のいずれかに記載の多層構造体。
- 前記オレフィン系重合体のメルトフローレート(190℃、2160g)が5.0g/10分未満である、請求項4~10のいずれかに記載の多層構造体。
- 樹脂組成物層(B1)または樹脂組成物層(B2)が2つの硬質層(A)の間に配置されてなる、請求項1~11のいずれかに記載の多層構造体。
- 硬質層(A)と、樹脂組成物層(B1)または樹脂組成物層(B2)との間に、さらに接着性樹脂層(C)を有する、請求項1~12のいずれかに記載の多層構造体。
- 接着性樹脂層(C)/樹脂組成物層(B1)または樹脂組成物層(B2)/接着性樹脂層(C)の層構成を有する、請求項13に記載の多層構造体。
- 請求項1~14のいずれかに記載の多層構造体からなる、包装材。
- 請求項1~14のいずれかに記載の多層構造体の回収物を含む、回収組成物。
- 請求項1~14のいずれかに記載の多層構造体の回収物を溶融混錬する、回収組成物の製造方法。
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