JP5441718B2 - 複合材料、及びその製造方法 - Google Patents
複合材料、及びその製造方法 Download PDFInfo
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- JP5441718B2 JP5441718B2 JP2009550281A JP2009550281A JP5441718B2 JP 5441718 B2 JP5441718 B2 JP 5441718B2 JP 2009550281 A JP2009550281 A JP 2009550281A JP 2009550281 A JP2009550281 A JP 2009550281A JP 5441718 B2 JP5441718 B2 JP 5441718B2
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- 125000001931 aliphatic group Chemical group 0.000 description 4
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- WYKYCHHWIJXDAO-UHFFFAOYSA-N tert-butyl 2-ethylhexaneperoxoate Chemical compound CCCCC(CC)C(=O)OOC(C)(C)C WYKYCHHWIJXDAO-UHFFFAOYSA-N 0.000 description 1
- VSJBBIJIXZVVLQ-UHFFFAOYSA-N tert-butyl 3,5,5-trimethylhexaneperoxoate Chemical compound CC(C)(C)CC(C)CC(=O)OOC(C)(C)C VSJBBIJIXZVVLQ-UHFFFAOYSA-N 0.000 description 1
- ZUSDEBDNDIJDMZ-UHFFFAOYSA-N tert-butyl 7-methyloctaneperoxoate Chemical compound CC(C)CCCCCC(=O)OOC(C)(C)C ZUSDEBDNDIJDMZ-UHFFFAOYSA-N 0.000 description 1
- 150000003512 tertiary amines Chemical class 0.000 description 1
- 239000004408 titanium dioxide Substances 0.000 description 1
- 150000003613 toluenes Chemical class 0.000 description 1
- 239000013638 trimer Substances 0.000 description 1
- PUVAFTRIIUSGLK-UHFFFAOYSA-M trimethyl(oxiran-2-ylmethyl)azanium;chloride Chemical compound [Cl-].C[N+](C)(C)CC1CO1 PUVAFTRIIUSGLK-UHFFFAOYSA-M 0.000 description 1
- 229940005605 valeric acid Drugs 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
- 150000003738 xylenes Chemical class 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
- XOOUIPVCVHRTMJ-UHFFFAOYSA-L zinc stearate Chemical compound [Zn+2].CCCCCCCCCCCCCCCCCC([O-])=O.CCCCCCCCCCCCCCCCCC([O-])=O XOOUIPVCVHRTMJ-UHFFFAOYSA-L 0.000 description 1
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- C08L27/00—Compositions of homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a halogen; Compositions of derivatives of such polymers
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B27—WORKING OR PRESERVING WOOD OR SIMILAR MATERIAL; NAILING OR STAPLING MACHINES IN GENERAL
- B27N—MANUFACTURE BY DRY PROCESSES OF ARTICLES, WITH OR WITHOUT ORGANIC BINDING AGENTS, MADE FROM PARTICLES OR FIBRES CONSISTING OF WOOD OR OTHER LIGNOCELLULOSIC OR LIKE ORGANIC MATERIAL
- B27N3/00—Manufacture of substantially flat articles, e.g. boards, from particles or fibres
- B27N3/002—Manufacture of substantially flat articles, e.g. boards, from particles or fibres characterised by the type of binder
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B27—WORKING OR PRESERVING WOOD OR SIMILAR MATERIAL; NAILING OR STAPLING MACHINES IN GENERAL
- B27N—MANUFACTURE BY DRY PROCESSES OF ARTICLES, WITH OR WITHOUT ORGANIC BINDING AGENTS, MADE FROM PARTICLES OR FIBRES CONSISTING OF WOOD OR OTHER LIGNOCELLULOSIC OR LIKE ORGANIC MATERIAL
- B27N3/00—Manufacture of substantially flat articles, e.g. boards, from particles or fibres
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- C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
- C08L23/04—Homopolymers or copolymers of ethene
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- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
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- C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
- C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
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- C08L97/00—Compositions of lignin-containing materials
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- C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
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- C08L23/04—Homopolymers or copolymers of ethene
- C08L23/08—Copolymers of ethene
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- C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
- C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
- C08L23/04—Homopolymers or copolymers of ethene
- C08L23/08—Copolymers of ethene
- C08L23/0846—Copolymers of ethene with unsaturated hydrocarbons containing other atoms than carbon or hydrogen atoms
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- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
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- Y10T428/1348—Cellular material derived from plant or animal source [e.g., wood, cotton, wool, leather, etc.]
Description
(A)天然繊維、
(B)少なくとも一種の熱可塑性ポリマー(熱可組性高分子)、
(C)モル質量Mnが最大で20000g/mol以下であり、
(a)エチレン、
(b)以下から選択される少なくとも一種の反応性コモノマー、
(b1)エチレン性不飽和C3〜C10モノカルボン酸、
(b2)エチレン性不飽和C4〜C10ジカルボン酸又はこれらの無水物、
(b3)エチレン性不飽和C3〜C10モノカルボン酸のエポキシエステル、
(b4)下記一般式I
R1は、水素、並びに非分岐状及び分岐状C1〜C10アルキルから選択され、
R2は、水素、並びに非分岐状及び分岐状C1〜C10アルキルから選択され、
R3は、同一又は異なり、水素、非分岐状及び分岐状C1〜C10アルキル、並びにC3〜C12シクロアルキルから選択され、ここで2個のR3基が相互に結合して3〜10員環を形成していてもよく、
Xは、酸素、硫黄、及びN−R4から選択され、
R4は、非分岐状及び分岐状C1〜C10アルキルから選択され、
A1は、C1〜C10アルキレン、C4〜C10シクロアルキレン、及びフェニレンから選択される2価の基である)
で示されるコモノマー、
(c)必要に応じて、少なくとも一種の他のコモノマー、
を共重合することにより得られる少なくとも一種のランダムコポリマー、
を含む複合材に関する。
(A)天然繊維、
(B)少なくとも一種の熱可塑性ポリマー(本発明ではポリマー(B)ともいう)、
(C)モル質量Mnが最大で20000g/mol以下であり、
(a)エチレン、
(b)以下から選択される少なくとも一種の反応性コモノマー、
(b1)エチレン性不飽和C3〜C10モノカルボン酸、
(b2)エチレン性不飽和C4〜C10ジカルボン酸、又はこれらの無水物、
(b3)エチレン性不飽和C3〜C10モノカルボン酸のエポキシエステル、
(b4)下記一般式I
R1は、水素、並びに非分岐状及び分岐状C1〜C10アルキルから選択され、
R2は、水素、並びに非分岐状及び分岐状C1〜C10アルキルから選択され、
R3は、同一又は異なり、水素、非分岐状及び分岐状C1〜C10アルキル、並びにC3〜C12シクロアルキルから選択され、ここで2個のR3基が相互に結合して3〜10員環を形成していてもよく、
Xは、酸素、硫黄、及びN−R4から選択され、
R4は、非分岐状及び分岐状C1〜C10アルキルから選択され、
A1は、C1〜C10アルキレン、C4〜C10シクロアルキレン、及びフェニレンから選択される2価の基である)
で示されるコモノマー、及び
(c)必要に応じて、少なくとも一種の他のコモノマー、
を共重合することにより得られる少なくとも一種のランダムコポリマー、
を含む。
(aa)無水物、特に無水マレイン酸とエチレンとのコポリマーなどの無水ポリマー、
(bb)エポキシド、特にグリシジル(メタ)アクリレートなどのエチレンとエチレン性不飽和エポキシドとのコポリマー、
との反応などによる、少なくとも一個の末端基が変性されたポリエステルが挙げられる。
(a)エチレン、
(b)以下から選択される少なくとも一種の反応性コモノマー、
(b1)エチレン性不飽和C3〜C10モノカルボン酸、
(b2)エチレン性不飽和C4〜C10ジカルボン酸又はその無水物、
(b3)エチレン性不飽和C3〜C10モノカルボン酸のエポキシエステル、
(b4)下記一般式I
R1は、水素並びに非分岐状及び分岐状のC1〜C10アルキルから選択され、
R2は、水素並びに非分岐状及び分岐状のC1〜C10アルキルから選択され、
R3は、同一又は異なり、水素、非分岐状及び分岐状のC1〜C10アルキル、並びにC3〜C12シクロアルキルから選択され、ここで、2個のR3基は相互に結合して3〜10員環を形成していてもよく、
Xは、酸素、硫黄、及びN−R4から選択され、
R4は、非分岐状及び分岐状のC1〜C10アルキルから選択され、
A1は、C1〜C10アルキレン、C4〜C10シクロアルキレン、及びフェニレンから選択される2価の基である)
で示されるコモノマー、および
(c)必要に応じて、少なくとも一個の他のコモノマー、
を共重合させることにより得られる。
R1及びR2は、同一又は異なり;
R1は、水素、及び非分岐状又は分岐状C1〜C10アルキル、例えば、メチル、エチル、n−プロピル、イソプロピル、n−ブチル、イソブチル、sec−ブチル、tert−ブチル、n−ペンチル、イソペンチル、sec−ペンチル、ネオペンチル、1,2−ジメチルプロピル、イソアミル、n−ヘキシル、イソヘキシル、sec−ヘキシル、n−ヘプチル、n−オクチル、2−エチルヘキシル、n−ノニル、n−デシルなど;特に好ましくは、C1〜C4アルキル、例えば、メチル、エチル、n−プロピル、イソプロピル、n−ブチル、イソブチル、sec−ブチル、及びtert−ブチルなど、特にメチルから選択され;
R2は、非分岐状又は分岐状C1〜C10アルキル、例えば、メチル、エチル、n−プロピル、イソプロピル、n−ブチル、イソブチル、sec−ブチル、tert−ブチル、n−ペンチル、イソペンチル、sec−ペンチル、ネオペンチル、1,2−ジメチルプロピル、イソアミル、n−ヘキシル、イソヘキシル、sec−ヘキシル、n−ヘプチル、n−オクチル、2−エチルヘキシル、n−ノニル、n−デシルなど;特に好ましくは、C1〜C4アルキル、例えば、メチル、エチル、n−プロピル、イソプロピル、n−ブチル、イソブチル、sec−ブチル、及びtert−ブチルなど、特にメチル;及び
特に好ましくは水素から選択される。
C3〜C12シクロアルキル、例えば、シクロプロピル、シクロブチル、シクロペンチル、シクロヘキシル、シクロへプチル、シクロオクチル、シクロノニル、シクロデシル、シクロウンデシル、及びシクロドデシルなど;好ましくは、シクロペンチル、シクロへキシル、及びシクロへプチルから選択され、
ここで、2個のR3が相互に結合して、必要に応じてC1〜C4アルキル基で置換された3〜10員環、好ましくは5〜7員環を形成していてもよく、且つ
N(R3)2基は、
A1は、2価の基、例えば、
C1〜C10アルキレン、例えば、−CH2−、−CH(CH3)−、−(CH2)2−、−CH2−CH(CH3)−、cis−及びtrans−CH(CH3)−CH(CH3)−、−(CH2)3−、−CH2−CH(C2H5)−、−(CH2)4−、−(CH2)5−、−(CH2)6−、−(CH2)7−、−(CH2)8−、−(CH2)9−、−(CH2)10−など;好ましくは、C2〜C4アルキレン、例えば、−(CH2)2−、−CH2−CH(CH3)−、−(CH2)3−、−(CH2)4−、及び−CH2−CH(C2H5)−など;特に好ましくは、−(CH2)2−、−(CH2)3−、−(CH2)4−、最も好ましくは−(CH2)2−、
C4〜C10シクロアルキレン、例えば、異性体的に純粋な形態又は異性体混合物で、
マレイン酸モノ及びジメチル、マレイン酸モノ及びジエチル、フマル酸モノ及びジメチル、フマル酸モノ及びジエチル、イタコン酸モノ及びジメチル、マレイン酸モノ及びジ−n−ブチル、及びマレイン酸モノ及びジ−2−エチルヘキシルなどのエチレン性不飽和C4〜C10ジカルボン酸のモノ及びジC1〜C10アルキルエステル、
C1〜C10カルボン酸のビニルエステル又はアリルエステル、好ましくは酢酸又はプロピオン酸のビニルエステル又はアリルエステル、特に好ましくはプロピオン酸ビニル、最も好ましくは酢酸ビニル。
C1〜C6アルキル、例えば、メチル、エチル、n−プロピル、イソプロピル、n−ブチル、イソブチル、sec−ブチル、tert−ブチル、n−ペンチル、イソペンチル、sec−ペンチル、ネオペンチル、1,2−ジメチルプロピル、イソアミル、n−ヘキシル、イソヘキシル、sec−ヘキシル、特に好ましくはC1〜C4アルキル、例えば、メチル、エチル、n−プロピル、イソプロピル、n−ブチル、イソブチル、sec−ブチル、及びtert−ブチル;
C3〜C12シクロアルキル、例えば、シクロプロピル、シクロブチル、シクロペンチル、シクロヘキシル、シクロへプチル、シクロオクチル、シクロノニル、シクロデシル、シクロウンデシル、及びシクロドデシル;好ましくはシクロペンチル、シクロヘキシル、及びシクロへプチチル。
−ジデカノイルペルオキシド、2,5−ジメチル−2,5−ジ(2−エチルヘキサノイルペルオキシ)ヘキサン、tert−アミルペルオキシピバレート、tert−ブチルペルオキシピバレート、tert−アミル2−エチルペルオキシヘキサノアート、ジベンゾイルペルオキシド、tert−ブチル2−エチルペルオキシヘキサノアート、tert−ブチルジエチルペルオキシアセテート、tert−ブチルジエチルペルオキシイソブチラート、異性体混合物として1,4−ジ(tert−ブチルペルオキシカルボニル)シクロヘキサン、tert−ブチルペルイソノナノアート、1,1−ジ(tert−ブチルペルオキシ)−3,3,5−トリメチルシクロヘキサン、1,1−ジ(tert−ブチルペルオキシ)シクロヘキサン、メチルイソブチルケトンペルオキシド、tert−ブチルペルオキシイソプロピルカーボネート、2,2−ジ−tert−ブチルペルオキシブタン、又はtert−ブチルペルオキシアセテート;
−tert−ブチルペルオキシベンゾアート、ジ−tert−アミルペルオキシド、ジクミルペルオキシド、異性体ジ(tert−ブチルペルオキシイソプロピル)ベンゼン、2,5−ジメチル−2,5−ジ(tert−ブチルペルオキシヘキサン、tert−ブチルクミルペルオキシド、2,5−ジメチル−2,5−ジ−tert−ブチルペルオキシ)ヘキサ−3−イン、ジ−tert−ブチルペルオキシド、1,3−ジイソプロピルベンゼンモノハイドロペルオキシド、クメンハイドロペルオキシド、又はtert−ブチルハイドロペルオキシド;又は
−EP−A0813550などに記載されている二量体又は三量体ケトンペルオキシド。
30〜90質量%、好ましくは40〜85質量%の量の天然繊維(A)、
9〜69質量%、好ましくは12〜57質量%の量の熱可塑性ポリマー(B)、
1〜10質量%、好ましくは3〜5質量%の量のコポリマー(C)、
を含む。
(a)60〜98質量%、好ましくは70〜97質量%のエチレン、
(b)2〜40質量%、好ましくは3〜30質量%の、
(b1)エチレン性不飽和C3〜C10モノカルボン酸、
(b2)エチレン性不飽和C4〜C10ジカルボン酸又はその無水物、
(b3)エチレン性不飽和C3〜C10モノカルボン酸のエポキシエステル、
(b4)一般式I
R1は、水素並びに非分岐状及び分岐状のC1〜C10アルキルから選択され、
R2は、水素並びに非分岐状及び分岐状のC1〜C10アルキルから選択され、
R3は、同一又は異なり、水素、非分岐状及び分岐状のC1〜C10アルキル、並びにC3〜C12シクロアルキルから選択され、ここで2個のR3基は、相互に結合して3〜10員環を形成していてもよく、
Xは、酸素、硫黄及びN−R4から選択され、
R4は、非分岐状及び分岐状のC1〜C10アルキルから選択され、
A1は、C1〜C10アルキレン、C4〜C10シクロアルキレン、及びフェニレンから選択される2価の基である)で示されるコモノマー、
から選択される反応性コモノマー、及び
(c)0〜30質量%、好ましくは0.1〜30質量%の一種以上の他のモノマー、
を含む。
エチレン、及びグリシジルメタクリレート(b3.1)、メタクリル酸(b1.1)、又は無水マレイン酸(b2.1)から選択されるコモノマーを、文献(M.Buback等、Chem.Ing.Tech.1994、66、510)に記載されている高圧オートクレーブ方式で表1に従って共重合した。このため、表1に記載した量のエチレンを1700barの反応圧力で高圧オートクレーブ中に供給した。これとは別に、実施例(C1)〜(C.9)及び(C.11)では、最初に表1に記載した量のコモノマーを260barの中間圧力で圧縮し、次に1700barの反応圧力で供給した。これとは別に、実施例(C.1)〜(C.10)ではイソドデカン中にtert−アミルペルオキシピバレートを含む開始剤溶液、又は実施例(C.11)ではイソドデカンにtert−ブチルペルオキシピバレートを含む開始剤溶液(量及び濃度は表1の通り)を、1700barの反応圧力で高圧オートクレーブ中に供給した。これとは別に、最初に、表1の濃度でイソドデンカン中にプロピオンアルデヒドを含む表1に記載した量の調節剤を、260barの中間圧力で圧縮し、次に他の圧縮器により高圧オートクレーブへ供給した。反応温度は220℃であった。これにより、表1に従ってコポリマー(C.1)〜(C.11)が得られ、これらの分析データを表2に示す。コポリマー(C.1)〜(C.11)のモル質量Mnは常に20000g/mol以下であった。
c(PA):ID中のPAの濃度(体積部)、1:純PA、
c(PO):ID中のPOの濃度(mol/l)。
本発明で用いたコポリマー(C.1)〜(C.9)におけるエチレン及びグリシジルメタクリレートの含有量は、IP分光法により測定した。このため、較正IR曲線をNMR分光法により得られたデータから得た。
使用材料:
Sabic(登録商標)HDPE M30053S HDPE(190℃、2.16kg(MFR)で測定したメルトインデックス=3.5dg/分、密度=953kg/m3、及び溶融点(DIN53765に準拠したDSC試験)=132℃)を含む熱可塑性ポリマー(B.1)、及び
粒径が0.7〜1.2mmであり、かさ密度が100〜170g/リットルであり、850℃で4時間の処理後に約0.5%の残留物、JRS(Pettenmaier & Soehne GmbH + Co)製のLignocle(登録商標)グレードF9として商業的に利用可能な、針葉樹からの針葉樹繊維からなる天然繊維(A.1)。全混合物中の木材繊維の割合は、75質量%であった。
本発明の複合材又は比較材からなるプロファイルを、異方向回転2軸押出機(Weber Maschinenfabrik製 DS 7.22D)において製造した。表3の通り、(A.1)、(B.1)、比較コポリマー(C)、及び必要に応じて処理酸(D.1)を、押出機の主要な取入れ口に添加し、処理することにより、一工程ですぐに使用できるプロファイルを直接押出により得た。押出機は、40kg/hの処理量で1分あたり20回転で操作した。T1からT12の、質量流の方向における押出処理中の温度分布は、T1及びT2領域で190℃、T3〜T5領域で180℃、T6〜T11領域で170℃、T12領域で40℃であった。T1〜T12のうち、T1〜T5はバレルにおける温度、T6〜T7はアダプターフランジにおける温度、T8〜T11はダイにおける温度、T12はダイ末端の冷却プレートの温度である。
試験片を上記の通りに製造したプロファイルから鋸で切り取った。試験片の大きさは、80mm×10mm×4mmであった。
Claims (12)
- (A)30〜90質量%の天然繊維、
(B)9〜69質量%の少なくとも一種の熱可塑性ポリマー(B)、
(C)1〜10質量%の、モル質量Mnが最大で20000g/mol以下であり、
(a)60〜98質量%のエチレン、
(b)以下から選択される2〜40質量%の少なくとも一種の反応性コモノマー、
(b3)エチレン性不飽和C3〜C10モノカルボン酸のエポキシエステル、
を共重合することにより得られる少なくとも一種のランダムコポリマー、
を含む複合材。 - 天然繊維が、セルロース繊維、及び/又はリグノセルロース含有繊維から選択される請求項1に記載の複合材。
- 天然繊維が、木材繊維から選択される請求項1又は2に記載の複合材。
- 熱可塑性ポリマー(B)が、ポリエチレン、ポリプロピレン、及びポリ塩化ビニルから選択される請求項1〜3のいずれか1項に記載の複合材。
- 熱可塑性ポリマー(B)が、生物分解可能な熱可塑性物質から選択される請求項1〜4のいずれか1項に記載の複合材。
- 40〜85質量%の天然繊維(A)、
12〜57質量%の熱可塑性ポリマー(B)、
3〜5質量%のコポリマー(C)
を含む請求項1〜5のいずれか1項に記載の複合材。 - コポリマー(C)が、
(a)70〜97質量%のエチレン、
(b)以下から選択される3〜30質量%の少なくとも一種の反応性コモノマー、
(b3)エチレン性不飽和C3〜C10モノカルボン酸のエポキシエステル、
を、当該ポリマー中に組み込まれて含む請求項1〜6のいずれか1項に記載の複合材。 - 天然繊維(A)、溶融させた熱可塑性ポリマー(B)、及び溶融又は分散させたコポリマー(C)を相互に混合する工程を含む請求項1〜7のいずれか1項に記載の複合材の製造方法。
- 混合を押出機中で行う請求項8に記載の方法。
- 請求項1〜7のいずれか1項に記載の複合材を、中空体、家具、プロファイル部品、建築物の外装部品、及び建築物の内装部品として、又はこれらの製造に使用する方法。
- 請求項1〜7のいずれか1項に記載の複合材の少なくとも一種を用いた、中空体、家具、プロファイル部品、建築物の外装部品、及び建築物の内装部品の製造方法。
- 請求項1〜7のいずれか1項に記載の複合材の少なくとも一種を含む、又は請求項1〜7のいずれか1項に記載の複合材の少なくとも一種を用いて製造された、中空体、家具品目、プロファイル部品、建築物の内装部品、又は建築物の外装部品。
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