JP2019511594A - エチレンコポリマーを含む積層フィルム - Google Patents
エチレンコポリマーを含む積層フィルム Download PDFInfo
- Publication number
- JP2019511594A JP2019511594A JP2018544486A JP2018544486A JP2019511594A JP 2019511594 A JP2019511594 A JP 2019511594A JP 2018544486 A JP2018544486 A JP 2018544486A JP 2018544486 A JP2018544486 A JP 2018544486A JP 2019511594 A JP2019511594 A JP 2019511594A
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- Prior art keywords
- polymer composition
- ethylene
- copolymer
- composition according
- polymer
- 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.)
- Granted
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- 229920001038 ethylene copolymer Polymers 0.000 title description 5
- 229920000642 polymer Polymers 0.000 claims abstract description 121
- 239000000203 mixture Substances 0.000 claims abstract description 103
- BLRPTPMANUNPDV-UHFFFAOYSA-N Silane Chemical group [SiH4] BLRPTPMANUNPDV-UHFFFAOYSA-N 0.000 claims abstract description 81
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 claims abstract description 62
- 239000005977 Ethylene Substances 0.000 claims abstract description 62
- 229920001577 copolymer Polymers 0.000 claims abstract description 51
- 229920002397 thermoplastic olefin Polymers 0.000 claims abstract description 15
- 239000000758 substrate Substances 0.000 claims abstract description 10
- 229920000034 Plastomer Polymers 0.000 claims description 22
- 238000000034 method Methods 0.000 claims description 22
- 230000008569 process Effects 0.000 claims description 22
- 239000011521 glass Substances 0.000 claims description 20
- 239000003054 catalyst Substances 0.000 claims description 16
- 238000003475 lamination Methods 0.000 claims description 15
- 150000002978 peroxides Chemical class 0.000 claims description 15
- -1 polyethylene Polymers 0.000 claims description 15
- 238000009833 condensation Methods 0.000 claims description 14
- 230000005494 condensation Effects 0.000 claims description 14
- 238000010998 test method Methods 0.000 claims description 11
- 229920001169 thermoplastic Polymers 0.000 claims description 7
- 239000004416 thermosoftening plastic Substances 0.000 claims description 7
- 239000004594 Masterbatch (MB) Substances 0.000 claims description 6
- 239000007788 liquid Substances 0.000 claims description 5
- 229920000573 polyethylene Polymers 0.000 claims description 5
- 239000004698 Polyethylene Substances 0.000 claims description 4
- 238000002156 mixing Methods 0.000 claims description 3
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- 239000003963 antioxidant agent Substances 0.000 claims description 2
- 238000002347 injection Methods 0.000 claims description 2
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- 229910000077 silane Inorganic materials 0.000 abstract description 10
- BAPJBEWLBFYGME-UHFFFAOYSA-N Methyl acrylate Chemical compound COC(=O)C=C BAPJBEWLBFYGME-UHFFFAOYSA-N 0.000 description 36
- 239000000523 sample Substances 0.000 description 21
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- 239000005038 ethylene vinyl acetate Substances 0.000 description 13
- 238000012360 testing method Methods 0.000 description 13
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 13
- CQEYYJKEWSMYFG-UHFFFAOYSA-N butyl acrylate Chemical compound CCCCOC(=O)C=C CQEYYJKEWSMYFG-UHFFFAOYSA-N 0.000 description 11
- 230000003287 optical effect Effects 0.000 description 11
- 229920002037 poly(vinyl butyral) polymer Polymers 0.000 description 11
- 229920000098 polyolefin Polymers 0.000 description 11
- DQXBYHZEEUGOBF-UHFFFAOYSA-N but-3-enoic acid;ethene Chemical compound C=C.OC(=O)CC=C DQXBYHZEEUGOBF-UHFFFAOYSA-N 0.000 description 10
- 229920001200 poly(ethylene-vinyl acetate) Polymers 0.000 description 10
- NLZUEZXRPGMBCV-UHFFFAOYSA-N Butylhydroxytoluene Chemical group CC1=CC(C(C)(C)C)=C(O)C(C(C)(C)C)=C1 NLZUEZXRPGMBCV-UHFFFAOYSA-N 0.000 description 9
- 230000008901 benefit Effects 0.000 description 9
- 238000010521 absorption reaction Methods 0.000 description 7
- NKSJNEHGWDZZQF-UHFFFAOYSA-N ethenyl(trimethoxy)silane Chemical compound CO[Si](OC)(OC)C=C NKSJNEHGWDZZQF-UHFFFAOYSA-N 0.000 description 7
- 239000000155 melt Substances 0.000 description 7
- 239000000654 additive Substances 0.000 description 6
- 230000005540 biological transmission Effects 0.000 description 6
- 150000001875 compounds Chemical class 0.000 description 6
- 238000007334 copolymerization reaction Methods 0.000 description 6
- 238000004132 cross linking Methods 0.000 description 6
- 230000010354 integration Effects 0.000 description 6
- 239000012968 metallocene catalyst Substances 0.000 description 6
- 229920002725 thermoplastic elastomer Polymers 0.000 description 6
- KWKAKUADMBZCLK-UHFFFAOYSA-N 1-octene Chemical compound CCCCCCC=C KWKAKUADMBZCLK-UHFFFAOYSA-N 0.000 description 5
- 229920006362 Teflon® Polymers 0.000 description 5
- XTXRWKRVRITETP-UHFFFAOYSA-N Vinyl acetate Chemical compound CC(=O)OC=C XTXRWKRVRITETP-UHFFFAOYSA-N 0.000 description 5
- 150000003254 radicals Chemical class 0.000 description 5
- 229920005989 resin Polymers 0.000 description 5
- 239000011347 resin Substances 0.000 description 5
- 239000003381 stabilizer Substances 0.000 description 5
- 229920001897 terpolymer Polymers 0.000 description 5
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 4
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- 238000010348 incorporation Methods 0.000 description 4
- 238000006116 polymerization reaction Methods 0.000 description 4
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- 230000035699 permeability Effects 0.000 description 3
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- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 3
- UKRDPEFKFJNXQM-UHFFFAOYSA-N vinylsilane Chemical compound [SiH3]C=C UKRDPEFKFJNXQM-UHFFFAOYSA-N 0.000 description 3
- 125000003903 2-propenyl group Chemical group [H]C([*])([H])C([H])=C([H])[H] 0.000 description 2
- NIXOWILDQLNWCW-UHFFFAOYSA-M Acrylate Chemical compound [O-]C(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-M 0.000 description 2
- CERQOIWHTDAKMF-UHFFFAOYSA-N Methacrylic acid Chemical compound CC(=C)C(O)=O CERQOIWHTDAKMF-UHFFFAOYSA-N 0.000 description 2
- 238000005481 NMR spectroscopy Methods 0.000 description 2
- 125000004369 butenyl group Chemical group C(=CCC)* 0.000 description 2
- 125000004432 carbon atom Chemical group C* 0.000 description 2
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- FWDBOZPQNFPOLF-UHFFFAOYSA-N ethenyl(triethoxy)silane Chemical compound CCO[Si](OCC)(OCC)C=C FWDBOZPQNFPOLF-UHFFFAOYSA-N 0.000 description 2
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- 125000001183 hydrocarbyl group Chemical group 0.000 description 2
- 239000003999 initiator Substances 0.000 description 2
- 125000000555 isopropenyl group Chemical group [H]\C([H])=C(\*)C([H])([H])[H] 0.000 description 2
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 2
- TVMXDCGIABBOFY-UHFFFAOYSA-N n-Octanol Natural products CCCCCCCC TVMXDCGIABBOFY-UHFFFAOYSA-N 0.000 description 2
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- 229920006395 saturated elastomer Polymers 0.000 description 2
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- 229920002554 vinyl polymer Polymers 0.000 description 2
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 description 1
- NIXOWILDQLNWCW-UHFFFAOYSA-N 2-Propenoic acid Natural products OC(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 description 1
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 1
- 241000252095 Congridae Species 0.000 description 1
- 239000004971 Cross linker Substances 0.000 description 1
- JIGUQPWFLRLWPJ-UHFFFAOYSA-N Ethyl acrylate Chemical compound CCOC(=O)C=C JIGUQPWFLRLWPJ-UHFFFAOYSA-N 0.000 description 1
- 238000003109 Karl Fischer titration Methods 0.000 description 1
- 241000071353 Listera borealis Species 0.000 description 1
- 150000001252 acrylic acid derivatives Chemical class 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 239000002318 adhesion promoter Substances 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- 150000001336 alkenes Chemical class 0.000 description 1
- 125000003282 alkyl amino group Chemical group 0.000 description 1
- 125000001769 aryl amino group Chemical group 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000003086 colorant Substances 0.000 description 1
- 230000008602 contraction Effects 0.000 description 1
- 238000003869 coulometry Methods 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- 229920006037 cross link polymer Polymers 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 230000032798 delamination Effects 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 238000007580 dry-mixing Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 125000001301 ethoxy group Chemical group [H]C([H])([H])C([H])([H])O* 0.000 description 1
- 230000005284 excitation Effects 0.000 description 1
- 239000012467 final product Substances 0.000 description 1
- 238000009472 formulation Methods 0.000 description 1
- 229920000578 graft copolymer Polymers 0.000 description 1
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- 229920001519 homopolymer Polymers 0.000 description 1
- 229920000554 ionomer Polymers 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 239000000314 lubricant Substances 0.000 description 1
- 239000006078 metal deactivator Substances 0.000 description 1
- 125000000956 methoxy group Chemical group [H]C([H])([H])O* 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 150000002763 monocarboxylic acids Chemical class 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 230000009965 odorless effect Effects 0.000 description 1
- 125000000962 organic group Chemical group 0.000 description 1
- 230000003534 oscillatory effect Effects 0.000 description 1
- 230000035515 penetration Effects 0.000 description 1
- PNJWIWWMYCMZRO-UHFFFAOYSA-N pent‐4‐en‐2‐one Natural products CC(=O)CC=C PNJWIWWMYCMZRO-UHFFFAOYSA-N 0.000 description 1
- 238000005191 phase separation Methods 0.000 description 1
- 230000010363 phase shift Effects 0.000 description 1
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- 229920006254 polymer film Polymers 0.000 description 1
- 239000000047 product Substances 0.000 description 1
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- 230000009467 reduction Effects 0.000 description 1
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- 239000002904 solvent Substances 0.000 description 1
- 238000010183 spectrum analysis Methods 0.000 description 1
- 238000002834 transmittance Methods 0.000 description 1
- YUYCVXFAYWRXLS-UHFFFAOYSA-N trimethoxysilane Chemical group CO[SiH](OC)OC YUYCVXFAYWRXLS-UHFFFAOYSA-N 0.000 description 1
- 229920001567 vinyl ester resin Polymers 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
- 239000004711 α-olefin Substances 0.000 description 1
Classifications
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- C08L23/0846—Copolymers of ethene with unsaturated hydrocarbons containing other atoms than carbon or hydrogen atoms
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- B32B2307/00—Properties of the layers or laminate
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Abstract
【選択図】なし
Description
(A)10〜50wt%の、シラン基含有単位を有するエチレンのコポリマーと、
(B)少なくとも50wt%の、シラン基を含まない熱可塑性ポリオレフィンとを含み、
このポリマー組成物は、「テスト方法」に記載されるとおりに測定されるときに90℃にて1mm未満のクリープと、「テスト方法」に記載されるとおりに測定されるときに20N/cmより高い付着力とを有する。
R1SiR2 qY3−q (I)
ここで
R1はエチレン不飽和ヒドロカルビル、ヒドロカルビルオキシ、または(メト)アクリルオキシヒドロカルビル基であり、
各R2は独立に脂肪族飽和ヒドロカルビル基であり、
同じであっても異なっていてもよいYは加水分解性有機基であり、
qは0、1または2である。
1.中程度の伸長に伸びることができ、かつ応力を取り除いた際に元の形状に近いものに戻り得ること。
2.特定の温度より上では溶融物として加工可能であり、かつ冷却の際には固体状態に戻ること。
3.顕著なクリープがないこと。
a)メルトフローレート
メルトフローレート(melt flow rate)MFR2は、エチレンホモポリマーおよびコポリマーに対して190℃および2.16kgの荷重にてISO 1133に従って測定した。
ポリマー組成物中のポリマーのコモノマー含有量を定量化するために、定量的核磁気共鳴(NMR:nuclear−magnetic resonance)分光法を用いた。
VA=(I*VA−(IArBHT)/2)/1
MA=I1MA/3
BA=I4BA/2
VTMS=I1VTMS/9
BHT=IArBHT/2
E=(1/4)*[Ibulk−5*VA−3*MA−10*BA−3*VTMS−21*BHT]
fM=M/(E+VA+MA+BA+VTMS)
M[mol%]=100*fM
M[wt%]=100*(fM*MW)/((fVA*86.09)+(fMA*86.09)+(fBA*128.17)+(fVTMS*148.23)+((1−fVA−fMA−fBA−fVTMS)*28.05))
randall89
J.Randall,Macromol.Sci.,Rev.Macromol.Chem.Phys.1989,C29,201。
サンプルから厚さ0.45mmのフィルムを調製した。このフィルムから、30mm*120mmの2つのサンプルを切り取った。30mm*150mm*3.85mm厚さの2つの平面ガラススライドをイソプロパノールで洗浄して乾燥したものを調製した。100mm*15mmの孔を有するテフロン(登録商標)(0.1mm厚さ)の2つのマスクも調製した。
ポリマーサンプルから0.45mmのフィルムを調製した。標準的な仕様に従ってフィルムを調整した。
0.45mmの厚さを有する押出しフィルムを付着力測定に用いた。イソプロパノールで洗浄して乾燥した標準的な窓ガラスに対して、付着強度を測定した。付着力テスト測定のためにガラスとフィルムとの間にテフロン(登録商標)ストライプを伴って、ガラスプレート(寸法30×300×4mm(b*l*d))上に2つのフィルムを積層することによって、付着サンプルを調製した。積層の前に、2つのフィルムの頂部にバックシートも置いた。完全自動ラミネータP.Energy L036LABを用いて、150℃にて15分間および800mbarの圧力にて積層を行った。積層後、テフロン(登録商標)ストライプを除去した。剥離強度測定のために、15mmの幅を有する試料をサンプルガラスからスライスした。Alwetron TCT 25引張り機において、90℃の剥離角度および100mm/minの剥離速度によって、付着力を測定した。1kNの荷重セルによる剥離(peal)力を常時測定しながら、最大100mmの伸長まで剥離テストを行った。この測定から最大、最小、および平均の力(N)を取った。平均の力を試料の幅(15mm)で割ることによって、付着力(N/cm)を測定した。
0.45mmの厚さおよび200mmの長さを有する押出しフィルムに対して、水吸収測定を行った。調査するフィルムを23℃および50%のRHの恒温室内で3週間調整した。カールフィッシャー滴定によって、サンプル中の総水分含有量の水吸収判定を行った。用いた機器は、Mettler DL39 Coulometric KF Titratorである。総水分含有量測定のために、サンプルを180℃まで加熱した。
動的剪断測定によってポリマー溶融物を特徴付けることは、ISO規格6721−1および6721−10に準拠する。この測定は、25mm平行プレートジオメトリを備えるAnton Paar MCR501応力制御回転レオメータにおいて行った。窒素雰囲気を用いて、歪みを線形粘弾性領域内に設定して、圧縮成形プレートに対する測定を行った。振動剪断テストは190℃にて、0.01〜600rad/sの周波数範囲を適用し、1.3mmの間隙を設定して行った。
γ(t)=γ0sin(ωt) (1)
σ(t)=σ0sin(ωt+δ) (2)
ここで
σ0およびγ0はそれぞれ応力および歪みの振幅であり、
ωは角周波数であり、
δは位相シフト(加えられた歪みと応力応答との間の損失角)であり、
tは時間である。
EI(x)=(G’’=x kPa)に対するG’[Pa] (9)
[1] Rheological characterization of polyethylene fractions Heino, E.L., Lehtinen, A., Tanner J., Seppala, J., Neste Oy, Porvoo, Finland, Theor. Appl. Rheol., Proc. Int. Congr. Rheol, 11th (1992), 1, 360−362
[2] The influence of molecular structure on some rheological properties of polyethylene, Heino, E.L., Borealis Polymers Oy, Porvoo, Finland, Annual Transactions of the Nordic Rheology Society, 1995.).
[3] Definition of terms relating to the non−ultimate mechanical properties of polymers, Pure & Appl. Chem., Vol. 70, No. 3, pp. 701−754, 1998.
パイロット規模押出し機(Prism TSE 24TC)において、異なる化合物を配合した。得られた混合物を以下の表に与えた条件で溶融混合し、ストリング状に押出してペレット化した。
付着力および透過率測定のために、Collin teach−line E 20T押出し機において、50mmの幅および0.45mmの厚さの寸法を有するフィルム(テープ)を押出した。以下の設定温度によってテープを生産した。
150/150/150℃および50rpm。
EVS(1.9wt%):VTMS−エチレンコポリマーであって、高圧チューブ状リアクタによって従来の方式で従来の過酸化物イニシエータを用いて、最高温度285℃にて生成したものであり、ここではコポリマー中に1.9wt%のシラン含有量が得られるような量のビニルトリメトキシシラン(VTMS:vinyl trimethoxysilane)とエチレンモノマーとを反応させた。当業者に周知であるとおり、MFRを調節するためにCTAを用いた。ISO 1133(190℃、2.16kg)に従うメルトフローレート(MFR2@190℃)は1g/10minである。
表1は、より高い融解温度を有するEVS(1.9wt%)を加えたときのクリープ性能に対する影響を示す。20%のEVS(1.9wt%)をQueo 8201に加えることによって、サンプルは110℃におけるクリープテストに合格することになる。このテストにおける好ましい組成である20%EVS(1.9wt%)、80%Queo 8201は、クリープの問題を解決する一方で、光学性能に対する限定された影響を有する。
Claims (17)
- フィルム層に対するポリマー組成物であって、
(A)10〜50wt%の、シラン基含有単位を有するエチレンのコポリマーと、
(B)少なくとも50wt%の、シラン基を含まない熱可塑性ポリオレフィンとを含み、
前記ポリマー組成物は、「テスト方法」に記載されるとおりに測定されるときに90℃にて48時間で1mm未満のクリープと、「テスト方法」に記載されるとおりに測定されるときに20N/cmより高い付着力とを有する、ポリマー組成物。 - シラン基含有単位を有するエチレンの前記コポリマー(A)は、前記ポリマー組成物の総重量に基づいて10〜45wt%、好適には25〜45wt%の量である、請求項1に記載のポリマー組成物。
- シラン基含有単位を有するエチレンの前記コポリマー(A)は、「テスト方法」に記載されるとおりに910kg/m3より高い密度を有する、請求項1または2に記載のポリマー組成物。
- シラン基を含まない前記熱可塑性ポリオレフィン(B)は、前記ポリマー組成物の総重量に基づいて60〜90wt%、好適には55〜75wt%の量で存在する、請求項1〜3のいずれか一項に記載のポリマー組成物。
- シラン基を含まない前記熱可塑性ポリオレフィン(B)は熱可塑性エラストマーポリエチレン、好ましくはプラストマー(E)である、請求項1〜4のいずれか一項に記載のポリマー組成物。
- 前記ポリマー組成物中のシラン基の総量は1wt%未満、好ましくは0.75wt%である、請求項1〜5のいずれか一項に記載のポリマー組成物。
- 前記ポリマー組成物は、860〜910kg/m3の密度と、1〜10g/10minのMFR2とを有する、請求項1〜6のいずれか一項に記載のポリマー組成物。
- 前記ポリマー組成物は過酸化物を含まない、請求項1〜7のいずれか一項に記載のポリマー組成物。
- 前記ポリマー組成物は、前記ポリマー組成物の総重量に基づいて0.1〜5wt%の量で存在するUV安定剤および抗酸化剤を有する、請求項1〜8のいずれか一項に記載のポリマー組成物。
- 前記ポリマー組成物は縮合触媒(F)を含む、請求項1〜9のいずれか一項に記載のポリマー組成物。
- 縮合触媒(F)は、
− マスターバッチとして、
− または移動によって、
− または液体として、たとえばケーブル押出し機などの押出し機への直接注入によって、
− または前記縮合触媒を前記ポリマー組成物と混合し、混合物をたとえばフィルム押出し機などの押出し機に供給することによって加えられる、請求項1〜10のいずれか一項に記載のポリマー組成物。 - 請求項1〜11のいずれか一項に記載のポリマー組成物で作られたフィルム層であって、好ましくは積層のためのフィルム層である、フィルム層。
- 請求項1〜11のいずれか一項において定義されるポリマー組成物を含む少なくとも1つのフィルム層を含む積層物品であって、基体層と、少なくとも1つの層とを含み、前記少なくとも1つの層は請求項1〜11のいずれか一項に記載のポリマー組成物を含む、積層物品。
- 前記基体層はガラス層である、請求項13に記載の積層物品。
- 前記クリープは90℃にて1mm未満であり、付着力は20N/cmより高い、請求項13または14に記載の積層物品。
- 請求項1〜15のいずれか一項に記載のポリマー組成物を含む積層物品を生産するためのプロセスであって、前記ポリマー組成物は130℃から170℃にて積層される、プロセス。
- フィルム層に対するポリマー組成物であって、
(A)10〜50wt%の、シラン基含有単位を有するエチレンのコポリマーと、
(B)少なくとも50wt%の、シラン基を含まない熱可塑性ポリオレフィンとを含む、ポリマー組成物。
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- 2017-03-02 MX MX2018010287A patent/MX2018010287A/es unknown
- 2017-03-02 CA CA3014491A patent/CA3014491A1/en not_active Abandoned
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CN108779304A (zh) | 2018-11-09 |
AU2017236139B2 (en) | 2019-07-18 |
JP6742428B2 (ja) | 2020-08-19 |
WO2017162417A1 (en) | 2017-09-28 |
MX2018010287A (es) | 2018-09-27 |
EP3433316A1 (en) | 2019-01-30 |
EP3222662B1 (en) | 2020-06-03 |
EA201800503A1 (ru) | 2019-02-28 |
CA3014491A1 (en) | 2017-09-28 |
US11192349B2 (en) | 2021-12-07 |
ES2811973T3 (es) | 2021-03-15 |
AU2017236139A1 (en) | 2018-08-23 |
US20200290331A1 (en) | 2020-09-17 |
CN108779304B (zh) | 2020-12-18 |
EP3222662A1 (en) | 2017-09-27 |
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