JP5865619B2 - 水系金属表面処理剤及びその処理剤で処理してなる金属材料 - Google Patents
水系金属表面処理剤及びその処理剤で処理してなる金属材料 Download PDFInfo
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- JP5865619B2 JP5865619B2 JP2011157012A JP2011157012A JP5865619B2 JP 5865619 B2 JP5865619 B2 JP 5865619B2 JP 2011157012 A JP2011157012 A JP 2011157012A JP 2011157012 A JP2011157012 A JP 2011157012A JP 5865619 B2 JP5865619 B2 JP 5865619B2
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- 238000004381 surface treatment Methods 0.000 claims description 60
- 150000001875 compounds Chemical class 0.000 claims description 50
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- 125000003504 2-oxazolinyl group Chemical group O1C(=NCC1)* 0.000 claims description 25
- 229910010272 inorganic material Inorganic materials 0.000 claims description 20
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 claims description 18
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims description 18
- 229910052782 aluminium Inorganic materials 0.000 claims description 15
- 229910052712 strontium Inorganic materials 0.000 claims description 14
- IQPQWNKOIGAROB-UHFFFAOYSA-N isocyanate group Chemical group [N-]=C=O IQPQWNKOIGAROB-UHFFFAOYSA-N 0.000 claims description 13
- 229910052725 zinc Inorganic materials 0.000 claims description 13
- 229910052791 calcium Inorganic materials 0.000 claims description 12
- 229910052749 magnesium Inorganic materials 0.000 claims description 12
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- 229910052748 manganese Inorganic materials 0.000 claims description 9
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- 229910052744 lithium Inorganic materials 0.000 description 6
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- SITVSCPRJNYAGV-UHFFFAOYSA-L tellurite Chemical compound [O-][Te]([O-])=O SITVSCPRJNYAGV-UHFFFAOYSA-L 0.000 description 3
- QPBYLOWPSRZOFX-UHFFFAOYSA-J tin(iv) iodide Chemical compound I[Sn](I)(I)I QPBYLOWPSRZOFX-UHFFFAOYSA-J 0.000 description 3
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- 229910000016 manganese(II) carbonate Inorganic materials 0.000 description 1
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- AOSHTALYABIEJR-UHFFFAOYSA-N neodymium(3+) hexanitrate Chemical class [Nd+3].[Nd+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O AOSHTALYABIEJR-UHFFFAOYSA-N 0.000 description 1
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- YAZJAPBTUDGMKO-UHFFFAOYSA-L potassium selenate Chemical compound [K+].[K+].[O-][Se]([O-])(=O)=O YAZJAPBTUDGMKO-UHFFFAOYSA-L 0.000 description 1
- BFPJYWDBBLZXOM-UHFFFAOYSA-L potassium tellurite Chemical compound [K+].[K+].[O-][Te]([O-])=O BFPJYWDBBLZXOM-UHFFFAOYSA-L 0.000 description 1
- CRQUBUILMSLSHI-UHFFFAOYSA-M potassium;hydrogen selenite Chemical compound [K+].O[Se]([O-])=O CRQUBUILMSLSHI-UHFFFAOYSA-M 0.000 description 1
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- AABBHSMFGKYLKE-SNAWJCMRSA-N propan-2-yl (e)-but-2-enoate Chemical compound C\C=C\C(=O)OC(C)C AABBHSMFGKYLKE-SNAWJCMRSA-N 0.000 description 1
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- ATZNZKKJTNCSHB-UHFFFAOYSA-K scandium(3+) triformate Chemical compound [Sc+3].[O-]C=O.[O-]C=O.[O-]C=O ATZNZKKJTNCSHB-UHFFFAOYSA-K 0.000 description 1
- DBTMQFKUVICLQN-UHFFFAOYSA-K scandium(3+);triacetate Chemical compound [Sc+3].CC([O-])=O.CC([O-])=O.CC([O-])=O DBTMQFKUVICLQN-UHFFFAOYSA-K 0.000 description 1
- HUIHCQPFSRNMNM-UHFFFAOYSA-K scandium(3+);triiodide Chemical compound [Sc+3].[I-].[I-].[I-] HUIHCQPFSRNMNM-UHFFFAOYSA-K 0.000 description 1
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- TVXXNOYZHKPKGW-UHFFFAOYSA-N sodium molybdate (anhydrous) Chemical compound [Na+].[Na+].[O-][Mo]([O-])(=O)=O TVXXNOYZHKPKGW-UHFFFAOYSA-N 0.000 description 1
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- 229960001763 zinc sulfate Drugs 0.000 description 1
- HTOFKHJTNDESBL-UHFFFAOYSA-L zinc tellurite Chemical compound [Zn+2].[O-][Te]([O-])=O HTOFKHJTNDESBL-UHFFFAOYSA-L 0.000 description 1
- VRGNUPCISFMPEM-ZVGUSBNCSA-L zinc;(2r,3r)-2,3-dihydroxybutanedioate Chemical compound [Zn+2].[O-]C(=O)[C@H](O)[C@@H](O)C([O-])=O VRGNUPCISFMPEM-ZVGUSBNCSA-L 0.000 description 1
- WDHVIZKSFZNHJB-UHFFFAOYSA-L zinc;butanoate Chemical compound [Zn+2].CCCC([O-])=O.CCCC([O-])=O WDHVIZKSFZNHJB-UHFFFAOYSA-L 0.000 description 1
- VOSQOLXQDQZVCL-UHFFFAOYSA-L zinc;chloride;hydroxide Chemical compound [OH-].[Cl-].[Zn+2] VOSQOLXQDQZVCL-UHFFFAOYSA-L 0.000 description 1
- JDLYKQWJXAQNNS-UHFFFAOYSA-L zinc;dibenzoate Chemical compound [Zn+2].[O-]C(=O)C1=CC=CC=C1.[O-]C(=O)C1=CC=CC=C1 JDLYKQWJXAQNNS-UHFFFAOYSA-L 0.000 description 1
- ZPEJZWGMHAKWNL-UHFFFAOYSA-L zinc;oxalate Chemical compound [Zn+2].[O-]C(=O)C([O-])=O ZPEJZWGMHAKWNL-UHFFFAOYSA-L 0.000 description 1
- NHXVNEDMKGDNPR-UHFFFAOYSA-N zinc;pentane-2,4-dione Chemical compound [Zn+2].CC(=O)[CH-]C(C)=O.CC(=O)[CH-]C(C)=O NHXVNEDMKGDNPR-UHFFFAOYSA-N 0.000 description 1
- PEUPCBAALXHYHP-UHFFFAOYSA-L zinc;selenite Chemical compound [Zn+2].[O-][Se]([O-])=O PEUPCBAALXHYHP-UHFFFAOYSA-L 0.000 description 1
- 229910000166 zirconium phosphate Inorganic materials 0.000 description 1
- XJUNLJFOHNHSAR-UHFFFAOYSA-J zirconium(4+);dicarbonate Chemical compound [Zr+4].[O-]C([O-])=O.[O-]C([O-])=O XJUNLJFOHNHSAR-UHFFFAOYSA-J 0.000 description 1
- ZXAUZSQITFJWPS-UHFFFAOYSA-J zirconium(4+);disulfate Chemical compound [Zr+4].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O ZXAUZSQITFJWPS-UHFFFAOYSA-J 0.000 description 1
- 229910000350 zirconium(IV) sulfate Inorganic materials 0.000 description 1
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 description 1
- ATYZRBBOXUWECY-UHFFFAOYSA-N zirconium;hydrate Chemical compound O.[Zr] ATYZRBBOXUWECY-UHFFFAOYSA-N 0.000 description 1
- 239000004711 α-olefin Substances 0.000 description 1
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Description
本発明に係る水系金属表面処理剤は、図1に示すように、基材である金属材料1(以下、「基材金属1」という。)の表面に、ラミネートフィルム又は樹脂塗膜3の下地用の表面処理皮膜2を形成するための処理剤である。その特徴は、有機化合物(A)と、架橋性有機化合物(B1)及び架橋性無機化合物(B2)から選ばれる1種又は2種以上の架橋性化合物(B)とを含有することにある。「含有する」とは、水系金属表面処理剤中に有機化合物(A)及び架橋性化合物(B)以外の化合物を含んでいてもよいことを意味している。そうした化合物としては、例えば、界面活性剤、消泡剤、レベリング剤、防菌防ばい剤、着色剤等を挙げることができる。これらの化合物を、本発明の趣旨及び皮膜性能を損なわない範囲で含有することができる。
有機化合物(A)は、官能基であるカルボキシル基及び/又は水酸基を含有する化合物である。これらのカルボキシル基及び/又は水酸基(これらを「官能基」ともいう。)を有する有機化合物(A)は、後述する架橋性化合物(B)と反応して、得られる表面処理皮膜の密着性及び耐薬品密着維持性を高めることができる。有機化合物(A)が含有する上記のカルボキシル基及び/又は水酸基は、分子量30〜300に1個の割合で1分子中に2個以上含まれている。この割合で上記カルボキシル基及び/又は水酸基を含む有機化合物(A)は、架橋性化合物(B)との間でより反応しやすくなる。その結果、水系金属表面処理剤で処理して得られる表面処理皮膜が緻密となり、耐薬品密着維持性をより高めることができる。カルボキシル基及び/又は水酸基の含有割合は、分子量30〜150に1個の割合で1分子中に2個以上有していることがより好ましい。
ヘキサヒドロキシベンゼン、ピロガロール、1,2,4−トリヒドロキシベンゼン、フロログルシノール、カテコール、レソルシノール、ヒドロキノン、5−メチルピロガロール、2−メチルレソルシノール、5−メチルレソルシノール、2,5−ジメチルレソルシノール、3−メチルカテコール、4−メチルカテコール、メチルヒドロキノン、2,6−ジメチルヒドロキノン、5−メトキシレソルシノール、3−メトキシカテコール、メトキシヒドロキノン、2,5−ジヒドロキシ−1,4−ベンゾキノン、没食子酸、ピロガロール−4−カルボン酸、2−ヒドロキシ安息香酸、3−ヒドロキシ安息香酸、4−ヒドロキシ安息香酸、2,3−ジヒドロキシ安息香酸、2,4−ジヒドロキシ安息香酸、2,5−ジヒドロキシ安息香酸、2,6−ジヒドロキシ安息香酸、3,4−ジヒドロキシ安息香酸、3,5−ジヒドロキシ安息香酸、2,4,6−トリヒドロキシ安息香酸、2,6−ジヒドロキシ−4−メチル安息香酸、4−ヒドロキシ−3,5−ジメチル安息香酸、1,4−ジヒドロキシ−2−ナフトエ酸、没食子酸メチル、2,4−ジヒドロキシ安息香酸メチル、2,6−ジヒドロキシ安息香酸メチル、3,4−ジヒドロキシ安息香酸メチル、3,5−ジヒドロキシ安息香酸メチル、3,4−ジヒドロキシ安息香酸エチル、4,6−ジアミノレソルシノール二塩酸塩、4,6−ジアミノレソルシノール、2−ニトロレソルシノール、4−ニトロカテコール、メリット酸、ベンゼンペンタカルボン酸、ピロメリット酸、トリメリット酸、ヘミメリット酸、トリメシン酸、フタル酸、イソフタル酸、テレフタル酸、1,4−ナフタレンジカルボン酸、2,3−ナフタレンジカルボン酸、2,6−ナフタレンジカルボン酸、4−メチルフタル酸、5−メチルイソフタル酸、2,5−ジメチルテレフタル酸、4−ヒドロキシフタル酸、5−ヒドロキシイソフタル酸、4−ニトロフタル酸、5−ニトロイソフタル酸、5−アミノイソフタル酸、4−アミノサリチル酸、4−アミノ−3−ヒドロキシ安息香酸、L−アスコルビン酸等の環状有機化合物;
タンニン酸等の加水分解性タンニン;カキタンニン、テアフラビン、テアルビジン等の縮合型タンニン;等を挙げることができる。
架橋性化合物(B)は、架橋性有機化合物(B1)及び架橋性無機化合物(B2)から選ばれる1種又は2種以上の化合物である。水系金属表面処理剤が架橋性化合物(B)を含むことによって、その水系金属表面処理剤を処理して得られる表面処理皮膜の密着性及び耐薬品密着維持性を高めることができる。
架橋性有機化合物(B1)は、有機化合物(A)が有するカルボキシル基及び/又は水酸基と反応しうる構造単位を有する有機化合物である。「反応しうる」とは、有機化合物(A)が有するカルボキシル基及び水酸基の両方又はいずれか一方に接触してそれらに反応することができるという意味である。「構造単位」とは、官能基又は単一結合単位のことである。「有する」とは、これらの構造単位以外に他の官能基や結合単位を有していてもよいという意味である。架橋性有機化合物(B1)としては、例えば、カルボジイミド結合、オキサゾリン基、グリシジルエーテル基、イソシアネート基及びメチロール基から選ばれる1種又は2種以上の構造単位を有する有機化合物を挙げることができる。
架橋性無機化合物(B2)は、有機化合物(A)が有する官能基であるカルボキシル基及び/又は水酸基と反応しうる元素を含む化合物である。「反応しうる」とは、カルボキシル基及び水酸基の両方又はいずれか一方に接触してそれらに反応することができるという意味である。「含む」とは、これらの元素以外に他の元素を有していてもよいことを意味している。
硝酸アルミニウム、硫酸アルミニウム、硫酸カリウムアルミニウム、硫酸ナトリウムアルミニウム、硫酸アンモニウムアルミニウム、リン酸アルミニウム、炭酸アルミニウム、酸化アルミニウム、水酸化アルミニウム、酸化アルミニウム、フッ化アルミニウム、ヨウ化アルミニウム、酢酸アルミニウム、安息香酸アルミニウム、クエン酸アルミニウム、グルコン酸アルミニウム、セレン酸アルミニウム、蓚酸アルミニウム、酒石酸アルミニウム、乳酸アルミニウム、パルチミン酸アルミニウム等のアルミニウム塩等;
ビス(アセチルアセトナト)ジアクアカルシウム(II)、安息香酸カルシウム、クエン酸カルシウム、メタスズ酸カルシウム、セレン酸カルシウム、タングステン酸カルシウム、炭酸カルシウム、四ホウ酸カルシウム、モリブデン酸カルシウム、マレイン酸カルシウム、リンゴ酸カルシウム、ニリン酸カルシウム、フッ化カルシウム、ホスフィン酸カルシウム、硝酸カルシウム、水酸化カルシウム、酸化カルシウム、シュウ酸カルシウム、酸化カルシウム、酢酸カルシウム等のカルシウム塩等;
ビス(アセチルアセトナト)ジアクアマンガン(II)、四酸化三マンガン、酸化マンガン(II)、酸化マンガン(III)、酸化マンガン(IV)、臭化マンガン(II)、蓚酸マンガン(II)、過マンガン酸(VII)、過マンガン酸カリウム(VII)、過マンガン酸ナトリウム(VII)、リン酸二水素マンガン(II)、硝酸マンガン(II)、硫酸マンガン(II)、硫酸マンガン(III)、硫酸マンガン(IV)、フッ化マンガン(II)、フッ化マンガン(III)、炭酸マンガン(II)、酢酸マンガン(II)、酢酸マンガン(III)、硫酸アンモニウムマンガン(II)、ヨウ化マンガン(II)、水酸化マンガン(II)等のマンガン塩等又はマンガン酸塩等;
ビス(アセチルアセトナト)ジアクアコバルト(II)、トリス(アセチルアセトナト)コバルト(III)、スルファミン酸コバルト(II)、塩化コバルト(II)、クロロペンタアンミンコバルト塩化物(III)、ヘキサアンミンコバルト塩化物(III)、ジアンミンテトラニトロコバルト(III)酸アンモニウム、硫酸コバルト(II)、硫酸アンモニウムコバルト、硝酸コバルト(II)、酸化コバルト二アルミニウム、水酸化コバルト(II)、酸化コバルト(II)、リン酸コバルト、酢酸コバルト(II)、蟻酸コバルト(II)、四酸化三コバルト、臭化コバルト(II)、蓚酸コバルト(II)、セレン酸コバルト(II)、タングステン酸コバルト(II)、ヒドロキシ炭酸第一コバルト(II)、モリブデン酸コバルト(II)、ヨウ化コバルト(II)、リン酸コバルト(II)等のコバルト塩等;
二スルファミン酸ニッケル(II)、安息香酸ニッケル(II)、硝酸ニッケル(II)、硫酸ニッケル(II)、炭酸ニッケル(II)、ニッケルアセチルアセトネート(II)、塩化ニッケル(II)、ヘキサアンミンニッケル塩化物、酸化ニッケル、水酸化ニッケル(II)、酸化ニッケル(II)、酢酸ニッケル、クエン酸ニッケル(II)、コハク酸ニッケル(II)、臭化ニッケル(II)、蓚酸ニッケル(II)、酒石酸ニッケル(II)、セレン酸ニッケル(II)、ヒドロキシ炭酸ニッケル(II)、乳酸ニッケル(II)、モリブデン酸ニッケル(II)、ヨウ化ニッケル(II)、二リン酸ニッケル(II)等のニッケル塩等;
蟻酸クロム(III)、フッ化クロム(III)、硝酸クロム(III)、硫酸クロム(III)、蓚酸クロム(III)、酢酸クロム(III)、重燐酸クロム(III)、水酸化クロム(III)、酸化クロム(III)、臭化クロム(III)、ヨウ化クロム(III)等のクロム塩等;
ビス(アセチルアセトナト)亜鉛(II)、安息香酸亜鉛(II)、ヒドロキシ塩化亜鉛(II)、蟻酸亜鉛(II)、クエン酸亜鉛(II)、臭化亜鉛(II)、蓚酸亜鉛(II)、酒石酸亜鉛(II)、メタスズ酸亜鉛(II)、セレン酸亜鉛(II)、タングステン酸亜鉛(II)、フッ化亜鉛(II)、モリブデン酸亜鉛(II)、酪酸亜鉛(II)、ニリン酸亜鉛(II)、硫酸亜鉛(II)、炭酸亜鉛(II)、塩化亜鉛(II)、ヨウ化亜鉛(II)、水酸化亜鉛(II)、酸化亜鉛(II)等の亜鉛塩等;
ビス(アセチルアセトナト)ジアクア鉄(II)、トリス(アセチルアセトナト)鉄(III)、三蓚酸鉄三カリウム、蟻酸鉄(II)、四バナジン酸鉄(III)、臭化鉄(III)、酒石酸鉄(III)、乳酸鉄(II)、フッ化鉄(II)、フッ化鉄(III)、塩化鉄(II)、塩化鉄(III)、ヨウ化鉄(II)、ヨウ化鉄(III)、硫酸鉄(II)、硫酸鉄(III)、硝酸鉄(II)、硝酸鉄(III)、酢酸鉄(II)、酢酸鉄(III)、クエン酸鉄(II)クエン酸鉄(III)、グリシン鉄(II)、グリシン鉄(III)、蓚酸鉄(II)、蓚酸鉄(III)、ピコリン酸鉄(II)、ピコリン酸鉄(III)、L−フェニルアラニン鉄(II)、L−フェニルアラニン鉄(III)、マロン酸鉄(II)、マロン酸鉄(III)、水酸化鉄(II)、水酸化鉄(III)、酸化鉄(II)、酸化鉄(III)、四酸化三鉄等の鉄塩等;
ビス(アセチルアセトナト)ジアクアストロンチウム(II)、蟻酸ストロンチウム(II)、クエン酸ストロンチウム(II)タングステン酸ストロンチウム、メタスズ酸ストロンチウム、酸化ストロンチウム(IV)、酸化ストロンチウム(II)、蓚酸ストロンチウム、メタニオブ酸ストロンチウム、モリブデン酸ストロンチウム、ヨウ化ストロンチウム、硝酸ストロンチウム、硫酸ストロンチウム、炭酸ストロンチウム、酢酸ストロンチウム、塩化ストロンチウム、リン酸ストロンチウム、乳酸ストロンチウム等のストロンチウム塩等;
オキシ二蓚酸チタン二アンモニウム、オキシ二蓚酸チタン二カリウム、酸化チタン(II)、酸化チタン(III)、酸化チタン(IV)、オキシ硫酸第二チタン、塩基性リン酸チタン、臭化チタン(IV)、メタチタン酸、メタチタン酸亜鉛(II)、チタン酸アルミニウム(III)、メタチタン酸カリウム、メタチタン三コバルト(II)、チタン酸ジルコニウム、メタチタン酸ストロンチウム、メタチタン三鉄(III)、メタチタン酸銅(II)、チタン酸ナトリウム、二チタン酸ネオジム(III)、メタチタン酸バリウム、メタチタン酸ビスマス(III)、メタチタン酸マグネシウム、チタン酸マグネシウム、メタチタン酸マンガン(II)、二チタン酸ランタン(III)、メタチタン酸リチウム、ヘキサフルオロチタン(IV)酸アンモニウム、ヘキサフルオロチタン(IV)酸カリウム、ヨウ化チタン(IV)、硫酸チタン(III)、硫酸チタン(IV)、塩化チタン、硝酸チタン、硫酸チタニル、フッ化チタン(III)、フッ化チタン(IV)、ヘキサフルオロチタン酸、乳酸チタン、ペルオキソチタン酸、チタンラウレート、チタニウムアセチルアセトネート、水酸化チタン(IV)等のチタン塩等又はチタン酸塩等;
テトラキス(アセチルアセトナト)ジルコニウム(IV)、塩化酸化ジルコニウム(IV)、塩化ジルコニウム(IV)、ケイ酸ジルコニウム、酢酸酸化ジルコニウム(IV)、酸化ジルコニウム(IV)、硝酸酸化ジルコニウム(IV)、メタジルコニウム酸セシウム、メタジルコニウム酸リチウム、メタジルコニウム酸亜鉛(II)、メタジルコニウム酸アルミニウム(III)、メタジルコニウム酸カルシウム、メタジルコニウム酸コバルト(II)、メタジルコニウム酸ストロンチウム、メタジルコニウム酸銅(II)、メタジルコニウム酸ナトリウム、メタジルコニウム酸ニッケル(II)、メタジルコニウム酸バリウム、メタジルコニウム酸ビスマス(III)、メタジルコニウム酸マグネシウム、オキシ炭酸ジルコニウム、ヘキサフルオロジルコニウム(IV)酸アンモニウム、ヘキサフルオロジルコニウム(IV)酸カリウム、ヨウ化ジルコニウム、リン酸二水素酸化ジルコニウム(IV)、塩基性炭酸ジルコニウム、炭酸ジルコニウムアンモニウム、炭酸ジルコニルアンモニウム、硝酸ジルコニウム、硝酸ジルコニル、硫酸ジルコニウム(IV)、硫酸ジルコニル、ヘキサフルオロジルコニウム酸、オキシリン酸ジルコニウム、ピロリン酸ジルコニウム、リン酸二水素ジルコニル、オキシ塩化ジルコニウム、フッ化ジルコニウム、酢酸ジルコニル、酸化ジルコニウム、水酸化ジルコニウム等のジルコニウム塩等;
ヘキサフルオロケイ酸、シリカ等のケイ酸塩等;
塩化タングステン(VI)、酸化タングステン酸鉄(III)、塩化タングステン(VI)、オキシ二塩化タングステン、二酸化タングステン、三酸化タングステン、メタタングステン酸、メタタングステン酸アンモニウム、メタタングステン酸ナトリウム、パラタングステン酸、パラタングステン酸アンモニウム、パラタングステン酸ナトリウム、タングステン酸亜鉛(II)、タングステン酸カリウム、タングステン酸カルシウム、タングステン酸コバルト(II)、タングステン酸ストロンチウム、タングステン酸セシウム、タングステン酸銅(II)、タングステン酸ニッケル、タングステン酸バリウム、タングステン酸マグネシウム、タングステン酸マンガン(II)、タングステン酸リチウム、リンタングステン酸、リンタングステン酸アンモニウム、リンタングステン酸ナトリウム等のタングステン塩等又はタングステン酸塩等;
トリス(アセチルアセトナト)セリウム(III)、塩化セリウム(III)、酸化セリウム(III)、酸化セリウム(IV)、臭化セリウム(III)、蓚酸セリウム(III)、水酸化セリウム(IV)、硫酸第二セリウムアンモニウム(IV)、硫酸第一セリウムアンモニウム(III)、炭酸セリウム(III)、硫酸セリウム、酢酸セリウム(III)、硝酸セリウム(III)、硫酸セリウム(IV)、フッ化セリウム(III)、ヨウ化セリウム(III)、リン酸セリウム(III)等のセリウム塩等;
塩化モリブデン(V)、酸化モリブデン(IV)、酸化モリブデン(VI)、モリブデン酸亜鉛(II)、モリブデン酸カリウム、モリブデン酸カルシウム、モリブデン酸コバルト(II)、モリブデン酸セシウム、モリブデン酸ニッケル(II)、モリブデン酸バリウム、モリブデン酸ビスマス(III)、モリブデン酸マグネシウム、モリブデン酸リチウム、パラモリブデン酸リチウム、モリブデン酸ストロンチウム、リンモリブデン酸、リンモリブデン酸アンモニウム、リンモリブデン酸ナトリウム、モリブデン酸、モリブデン酸アンモニウム、パラモリブデン酸アンモニウム、モリブデン酸ナトリウム等のモリブデン塩等又はモリブデン酸塩等;
オキシ二塩化バナジウム、オキシ三塩化バナジウム、三塩化バナジウム、酸化バナジウム、四バナジン酸鉄(III)、臭化バナジウム(III)、オキシ蓚酸バナジウム、ヨウ化バナジウム(II)、五酸化バナジウム、メタバナジン酸、ピロバナジン酸ナトリウム、バナジン酸ナトリウム、メタバナジン酸アンモニウム、メタバナジン酸ナトリウム、メタバナジン酸カリウム、オキシ三塩化バナジウム、三酸化バナジウム、二酸化バナジウム、オキシ硫酸バナジウム、バナジウムオキシアセチルアセテート、バナジウムアセチルアセテート、リンバナドモリブデン酸等のバナジウム塩等又はバナジン酸塩等;
塩化スズ(II)、酢酸スズ(II)、蓚酸スズ(II)、酒石酸スズ(II)、酸化スズ(IV)、硝酸スズ、硫酸スズ、フッ化スズ(II)、ヨウ化スズ(II)、ヨウ化スズ(IV)、ピロリン酸スズ(II)、メタスズ酸、メタスズ酸亜鉛、メタスズ酸カルシウム、メタスズ酸ストロンチウム、メタスズ酸バリウム、メタスズ酸マグネシウム等のスズ塩又はスズ酸塩等;
安息香酸ビスマス(III)、塩化酸化ビスマス(III)、クエン酸ビスマス(III)、オキシ酢酸ビスマス(III)、酸化酒石酸ビスマス(III)、酸化ビスマス(III)、オキシ硫酸二ビスマス、臭化ビスマス(III)、酒石酸ビスマス(III)、水酸化ビスマス(III)、オキシ炭酸二ビスマス、ジルコニウム酸ビスマス(III)、オキシ硝酸ビスマス、四チタン酸ビスマス(III)、三チタン酸ビスマス(III)、フッ化ビスマス(III)、モリブデン酸ビスマス(III)、ヨウ化ビスマス(III)、硝酸ビスマス(III)、塩化ビスマス(III)、硫酸ビスマス(III)、酢酸ビスマス(III)、リン酸ビスマス(III)等のビスマス塩等;
塩化タンタル(V)、酸化タンタル(V)、臭化タンタル(V)、タンタル酸、六タンタル酸カリウム、メタタンタル酸ストロンチウム、メタタンタル酸ナトリウム、メタタンタル酸リチウム、ヨウ化タンタル(V)、タンタルオキシアセチルアセトネート、メタタンタル酸、メタタンタル酸アンモニウム、ヘプタフルオロタンタル酸カリウム等のタンタル塩等又はタンタル酸塩等;
テルル酸、メタテルル酸アンモニウム、メタテルル酸カリウム、メタテルル酸ナトリウム、ヨウ化テルル(IV)、テルル酸カリウム、テルル酸ナトリウム、亜テルル酸、亜テルル酸カリウム、亜テルル酸ナトリウム、亜テルル酸バリウム、亜テルル酸リチウム、塩化テルル(IV)、酸化テルル(IV)、臭化テルル(IV)、水酸化硝酸三酸化二テルル、亜テルル酸亜鉛等のテルル塩等又はテルル酸塩等;
トリス(アセチルアセトナト)インジウム(III)、アミド硫酸インジウム(III)、二塩化インジウム、塩化インジウム(I)、塩化インジウム(III)、酢酸インジウム(III)、臭化インジウム(III)、ヨウ化インジウム(III)、硝酸インジウム(III)、硫酸インジウム(III)、フッ化インジウム(III)、酸化インジウム(III)、水酸化インジウム(III)等のインジウム塩等;
ビス(アセチルアセトナト)ジアクアバリウム(II)、亜セレン酸バリウム、亜テルル酸バリウム、安息香酸バリウム、アルミン酸バリウム、塩化バリウム、蟻酸バリウム、クエン酸バリウム、酸化バリウム、臭化バリウム、蓚酸バリウム、酒石酸バリウム、メタジルコニウム酸バリウム、水酸化バリウム、メタスズ酸バリウム、タングステン酸バリウム、メタチタン酸バリウム、メタニオブ酸バリウム、乳酸バリウム、メタホウ酸バリウム、モリブデン酸バリウム、ヨウ化バリウム、リン酸水素バリウム、炭酸バリウム、フッ化バリウム等のバリウム塩等;
テトラキス(アセチルアセトナト)ハフニウム(IV)、塩化ハフニウム(IV)、酸化ハフニウム(IV)、ヨウ化ハフニウム(IV)、硫酸ハフニウム(IV)、硝酸ハフニウム(IV)、オキシ蓚酸ハフニウム(IV)、フルオロハフニウム酸、フルオロハフニウム酸塩、フッ化ハフニウム等のハフニウム塩等又はハフニウム酸塩等;
亜セレン酸カリウム、亜セレン酸水素カリウム、亜セレン酸三水素セシウム、亜セレン酸水素ナトリウム、亜セレン酸水素リチウム、亜セレン酸銅(II)、亜セレン酸ナトリウム、亜セレン酸バリウム、オキシ塩化セレン、塩化セレン(I)、塩化セレン(IV)、酸化セレン(IV)、セレン酸アルミニウム、セレン酸、亜セレン酸亜鉛、セレン酸カリウム、セレン酸アンモニウム、セレン酸カルシウム、セレン酸セシウム、セレン酸コバルト、セレン酸銅(II)、セレン酸ニッケル、セレン酸ナトリウム、セレン酸バリウム、セレン酸亜鉛等のセレン塩等又はセレン酸塩等;
塩化スカンジウム(III)、蟻酸スカンジウム(III)、酢酸スカンジウム(III)、硝酸スカンジウム(III)、酸化スカンジウム(III)、フッ化スカンジウム(III)、ヨウ化スカンジウム(III)、硫酸スカンジウム(III)等のスカンジウム塩等;
酸化ニオブ(II)、酸化ニオブ(V)、五(蓚酸水素)ニオブ、水酸化ニオブ(V)、ニオブオキシアセチルアセトネート、メタニオブ酸、メタニオブ酸カルシウム、メタニオブ酸ストロンチウム、メタニオブ酸バリウム、メタニオブ酸マグネシウム、メタニオブ酸リチウム、メタニオブ酸アンモニウム、メタニオブ酸ナトリウム、五塩化ニオブ等のニオブ塩等又はニオブ酸塩等;
アミド硫酸銅(II)、安息香酸銅(II)、テトラアンミン銅(II)硝酸塩、クエン酸銅(II)、酸化銅(I)、臭化銅(I)、蓚酸銅(II)、蟻酸銅(II)、酢酸銅(II)、プロピオン酸銅(II)、吉草酸銅(II)、グルコン酸銅(II)、酒石酸銅(II)、塩化銅(II)、臭化銅(II)、水酸化銅(II)、酢酸銅(II)、硝酸銅(II)、硫酸銅(II)、炭酸銅(II)、酸化銅(II)、ヒドロキシ硝酸第二銅、タングステン酸銅(II)、炭酸水酸化銅(II)、乳酸銅(II)、フッ化銅(II)、ヨウ化銅(I)等の銅塩等;
トリス(アセチルアセトナト)イットリウム(III)、塩化イットリウム(III)、蟻酸イットリウム(III)、クエン酸イットリウム(III)、酢酸イットリウム(III)、酸化イットリウム(III)、蓚酸イットリウム(III)、硝酸イットリウム(III)、炭酸イットリウム(III)、フッ化イットリウム(III)、ヨウ化イットリウム(III)、硫酸イットリウム(III)、リン酸イットリウム(III)等のイットリウム塩等;
トリス(アセチルアセトナト)ランタン(III)、塩化ランタン(III)、蟻酸ランタン(III)、酢酸ランタン(III)、酸化ランタン(III)、蓚酸ランタン(III)、硝酸ランタン(III)、炭酸ランタン(III)、フッ化ランタン(III)、二チタン酸ランタン(III)、硫酸ランタン(III)、リン酸ランタン(III)、ヨウ化ランタン(III)等のランタン塩等;
トリス(アセチルアセトナト)ネオジム(III)、塩化ネオジム(III)、蟻酸ネオジム(III)、酢酸ネオジム(III)、酸化ネオジム(III)、臭化ネオジム(III)、蓚酸ネオジム(III)、硝酸ネオジム(III)、炭酸ネオジム(III)、二チタン酸ネオジム(III)、フッ化ネオジム(III)、ヨウ化ネオジム(III)、硫酸ネオジム(III)、リン酸ネオジム(III)等のネオジウム塩等;を挙げることができる。これらの化合物は無水物であってもよいし、水和物であってもよい。また、単独で使用してもよいし、2種以上組み合わせて使用してもよい。さらに、水系金属表面処理剤溶剤中に溶解していてもよいし、分散していてもよい。
本発明に係る水系金属表面処理剤は、金属材料表面に塗布する際の作業性を良くするために、必要に応じて各種の溶剤を含有することができる。
本発明に係る水系金属表面処理剤は、界面活性剤、消泡剤、レベリング剤、防菌防ばい剤、着色剤等を、本発明の趣旨及び皮膜性能を損なわない範囲で含有することができる。
本発明に係る水系金属表面処理剤の製造方法は、特に限定されない。例えば、有機化合物(A)と架橋性化合物(B)は、任意に含まれる添加剤及び任意に含まれる溶剤等と混ぜ、混合ミキサー等の攪拌機を用いて十分に混合することによって調製することができる。
本発明に係る金属材料10は、図1に示すように、基材金属1と、その表面に本発明に係る水系金属表面処理剤を塗布して形成された表面処理皮膜2を有する。「塗布」とは、後述する塗布工程によって、基材金属1の表面に水系金属表面処理剤を塗ることをいう。「有する」とは、基材金属1及び表面処理皮膜2以外に他の構成を有していてもよいことを意味している。例えば、表面処理皮膜2の上にラミネート加工によって形成された樹脂フィルム3を有していてもよい。表面処理皮膜2は、上記した本発明に係る水系金属表面処理剤を基材金属1に塗布して形成されるので、密着性及び耐薬品密着維持性に優れている。
水系金属表面処理剤を用いた金属表面の処理方法は、水系金属表面処理剤を基材金属の表面に塗布する塗布工程と、塗布工程の後、水洗することなく乾燥し、表面処理皮膜を形成する乾燥工程とによって形成することができる。
塗布工程は、水系金属表面処理剤を基材金属の表面に塗布する工程である。塗布する方法は、特に限定されず、例えば、スプレーコート、ディップコート、ロールコート、カーテンコート、スピンコート、又はこれらを組み合わせた方法を用いることができる。水系金属表面処理剤の使用条件は、特に限定されない。例えば、塗布する際の水系金属表面処理剤及び金属材料の温度は、10℃〜90℃であることが好ましく、20℃〜60℃であることがより好ましい。温度が60℃以下であると、無駄なエネルギーの使用を抑制することができる。また、塗布する時間及び塗布する量は、得られる表面処理皮膜の求められる膜厚に応じて適宜設定することができる。
乾燥工程は、塗布工程後、水洗することなく乾燥し、表面処理皮膜を形成する工程である。乾燥温度は、使用する溶剤に合わせた温度とすることができる。例えば、水を溶剤として用いた場合には、50℃〜250℃の範囲であることが好ましい。乾燥装置は特に限定されないが、バッチ式、連続式又は熱風循環式の乾燥炉、コンベアー式熱風乾燥炉又はIHヒーターを用いた電磁誘導加熱炉等を用いることができ、その風量と風速等は任意に設定することができる。
用いた有機化合物(A)を以下に示す。なお、官能基含有量とは、有機化合物(A)の分子量を、1分子に含まれる、カルボキシル基及び/又は水酸基の合計含有量で割り付けた値である。
Ab:L−アスコルビン酸(分子量175、官能基含有量43.8)
Ac:酒石酸(分子量150、官能基含有量37.5)
Ad:ピロメリト酸(分子量254、官能基含有量63.5)
Ae:ブタンテトラカルボン酸(分子量234、官能基含有量58.5)
Af:ペンタエリスリトール(分子量136、官能基含有量34)
Ag:没食子酸(分子量188、官能基含有量47)
Ah:ポリエチレングリコール(分子量4000、官能基含有量2000)
Ai:ポリアクリル酸(分子量15000、官能基含有量72)
Aj:ポリマレイン酸(分子量20000、官能基含有量58)
(カルボジイミド結合を有する有機化合物I;記号B1a)
m−テトラメチルキシリレンジイソシアネート700部(2.87mol)を、3−メチル−1−フェニル−2−ホスホレン−1−オキシド(カルボジイミド化触媒)14部の存在下、180℃で32時間反応させて、両末端がイソシアネート基で縮合度12のポリカルボジイミド化合物を得た。得られたポリカルボジイミド化合物224部に、重合度12のポリオキシエチレンモノメチルエーテル115部を加え、100℃で48時間反応させて両末端のイソシアネート基を封止した。次いで、50℃で蒸留水509質量部を徐々に加えて、ポリカルボジイミド化合物水溶液B1aを得た。
ジフェニルメタンジイソシアネート338部(1.35mol)と、4,4’−ジシクロヘキシルメタンジイソシアネート354部(1.35mol)とを、3−メチル−1−フェニル−2−ホスホレン−1−オキシド(カルボジイミド化触媒)2.9部の存在下、180℃で32時間反応させて、両末端がイソシアネート基で縮合度12のポリカルボジイミド化合物を得た。得られたポリカルボジイミド化合物224部に、重合度12のポリオキシエチレンモノメチルエーテル115部を加え、100℃で48時間反応させて両末端のイソシアネート基を封止した。次いで、50℃で蒸留水509部を徐々に加え、ポリカルボジイミド化合物水溶液B1bを得た。
m−テトラメチルキシリレンジイソシアネート700部を、3−メチル−1−フェニル−2−ホスホレン−1−オキシド(カルボジイミド化触媒)14部の存在下、180℃で32時間反応させて、両末端がイソシアネート基で縮合度12のポリカルボジイミド化合物を得た。得られたポリカルボジイミド化合物224.4部と、3,3−ビス(ジメチルアミノ)プロピルアミン10.2部とを、80℃で1時間反応させた後、ジメチル硫酸12.6gを加え1時間攪拌した。次いで、蒸留水509.1gを50℃で徐々に加え、ポリカルボジイミド化合物水溶液B1cを得た。
攪拌機、還流冷却器、窒素導入管及び温度計を備えたフラスコに、脱イオン水220部、1−メトキシ‐2‐プロパノール380部、過硫酸ソーダ5部、2−イソプロペニル−2−オキサゾリン200部及びアクリル酸エチル200部を仕込み、ゆるやかに窒素ガスを流しながら50℃に加熱した。フラスコ内の温度を50±1℃に保ち、10時間攪拌を続けて反応を完結させた後冷却し、不揮発分40.0%の水溶性オキサゾリン基含有樹脂B1dを得た。この重合体の数平均分子量は約2万であり、重合体1g当たりのオキサゾリン基含有量は4.5mmol/gであった。
撹拌機、還流冷却器、窒素導入管及び温度計を備えた容量1リットルのセパフラスコに、脱イオン水228.1部、界面活性剤ノニルフェノールエトキシレート(エチレンオキサイド6モル付加)硫酸アンモニウム塩の25%水溶液1.23部及び7%アンモニア水溶液1.9部を仕込み、緩やかに窒素ガスを流しながら70℃に昇温させた。その後、このセパフラスコに、(メタ)アクリル酸ブチル283.5部、スチレン211.4部、ジビニルベンゼン0.6部、2−イソプロペニル−2−オキサゾリン55.1部、脱イオン水158.4部、界面活性剤ノニルフェノールエトキシレート(エチレンオキサイド6モル付加)硫酸アンモニウム塩の25%水溶液31.0部及び7%アンモニア水0.6部からなるプレエマルションの10質量%を初期仕込みとして添加した。その後、このセパフラスコに、過硫酸カリウム2.8部を純水34.4部に溶解させた開始剤水溶液をさらに添加し、重合を開始させた。さらに残りのプレエマルションを2.5時間かけて滴下し、撹拌しながら反応させ、滴下後80℃で2.5時間熟成させた。反応終了後、7%アンモニア水1.4部を添加し、pHを8.8に調節し、不揮発分55.6質量%のオキサゾリン基含有アクリル水分散体B1eを得た。理論オキサゾリン基当量は0.90mmol/gであった。
撹拌機、還流冷却器、窒素導入管及び温度計を備えた容量1リットルのセパフラスコに、脱イオン水228.1部、界面活性剤ノニルフェノールエトキシレート(エチレンオキサイド6モル付加)硫酸アンモニウム塩の25%水溶液1.23部、及び7%アンモニア水溶液1.9部を仕込み、緩やかに窒素ガスを流しながら70℃に昇温させた。70℃に昇温後、このセパフラスコに、一段目重合反応の材料として作製した(メタ)アクリル酸ブチル170.1部、スチレン159.9部、ジビニルベンゼン0.4部、脱イオン水95.0部、界面活性剤ノニルフェノールエトキシレート(エチレンオキサイド6モル付加)硫酸アンモニウム塩の25%水溶液18.6部及び7%アンモニア水0.4部からなるプレエマルション(以下、「一段目のプレエマルション」という。)の10質量%を初期仕込みとして添加した。その後、このセパフラスコに、過硫酸カリウム2.8部を純水34.4部に溶解させた開始剤水溶液を添加し、重合を開始させた。さらに、残りの一段目のプレエマルションを1.3時間かけて滴下し、撹拌しながら反応させた。
グリセロールポリグリシジルエーテル(3官能、エポキシ当量144、粘度170mPa・S)を用いた。
ヘキサメチレンジイソシアネート−アセト酢酸エチルブロック体を用いた。
メチロールメラミンを用いた。
用いた架橋性無機化合物(B2)を以下に示す。
B2b:ジルコニウムフッ化水素酸(濃度40.0質量%)
B2c:シリカゾル(表面電荷カチオン、粒子径10〜20nm、19.0質量%、pH=4.7)
B2d:乳酸チタン(濃度44.0質量%)
B2e:非晶質ジルコニアゾル(不揮発分濃度10.0質量%、粒子径10〜30nm、pH=2.8)
B2f:ケイフッ化水素酸(濃度40.0質量%)
B2g:フッ化クロム(III)(Cr濃度1.0質量%)
B2h:フッ化鉄(III)(Fe濃度2.5質量%)
B2i;酸化セレン(IV)
B2j;酸化セリウムゾル(不揮発分濃度15%、pH=3.5)
B2k;酢酸クロム(III)
有機化合物Aa〜Ajと、架橋性有機化合物B1a〜B1i及び架橋性無機化合物B2a〜B2kから選ばれる1種又は2種以上とを所定の含有量で組み合わせ、溶剤を水として、表1〜表6に示す実施例1〜91及び比較例1〜20の水系金属表面処理剤を準備した。なお、表1〜表6における「濃度」は、水系金属表面処理剤に含まれる各化合物の不揮発分濃度(質量%)を示す。また、「A濃度」は、水系金属表面処理剤中の全固形分に対する有機化合物(A)の含有量(質量%)を示し、「B1+B2濃度」は、水系金属表面処理剤中の全固形分に対する架橋性化合物(B)の含有量であって、架橋性有機化合物B1と架橋性無機化合物B2との合計含有量(質量%)を示す。なお、以下において、分子量が254を超える有機化合物Aa,Ahを用いた実施例1,3,6,9,12,24,38,39,43,67,71,72,73,77,85,88,及び91は、比較例である。
基材金属として用いた金属材料を以下に示す。
Cu:C1020P、厚さ0.3mm
Ni:純ニッケル板:(純度99質量%以上)、厚さ0.3mm
SUS:SUS304板、厚さ0.3mm
NiめっきCu:電気NiめっきCu板(厚さ0.3mm、Niめっき厚2μm)
これら金属材料から、表1〜表6の「基材」欄に示す金属材料を選択し、実施例1〜91及び比較例1〜24の基材金属として準備した。
(表面処理)
表1〜表6に示した実施例1〜91及び比較例1〜20の基材金属をファインクリーナー359E(日本パーカライジング株式会社製のアルカリ脱脂剤)の3%水溶液で65℃、1分間スプレー脱脂した後、水洗して表面を清浄した。続いて、金属材料の表面の水分を蒸発させるために、80℃で1分間、加熱乾燥した。脱脂洗浄した基材金属の表面に、それぞれ、表1〜表6に示した実施例1〜90及び比較例1〜20の水系金属表面処理剤を#3SUSマイヤーバーを用い、バーコートによって塗布し(塗布工程)、熱風循環式乾燥炉内で200℃、1分間乾燥し(乾燥工程)、表面処理皮膜を有する金属材料を得た。なお、同種の水系金属表面処理剤を用いて表面処理した金属材料をそれぞれ2つずつ準備し、以下に示すように、表面処理皮膜の上にそれぞれ別の方法でラミネート加工を施した。
2つずつ準備した表面処理皮膜を有する金属材料の1つについて、その表面処理皮膜の上に、ヒートラミネーションによるラミネート加工を施した。他の1つの表面処理皮膜の上に、ドライラミネーションによるラミネート加工を施した。表面処理皮膜を有しない金属材料についても、2つのうち1つの片側表面にヒートラミネーションを施し、他の1つの片側表面にドライラミネーションを施した。
ヒートラミネーションによって得たポリプロピレンフィルム積層金属材料と、ドライラミネーションによって得たポリプロピレンフィルム積層金属材料とを、それぞれ絞りしごき加工試験で深絞り加工した。直径160mmに打ち抜いた被覆金属板を絞り加工(1回目)し、直径100mmのカップを作製した。続いて、そのカップを直径75mmに再度絞り加工(2回目)し、さらに直径65mmに絞り加工(3回目)し、供試材である缶を作製した。なお、1回目の絞り加工、2回目の絞り加工、3回目の絞り加工におけるしごき(薄肉化分)率は、それぞれ、5%、15%、15%であった。
(密着性)
成形加工後の缶について、ポリプロピレンフィルムの剥離の有無(以下、「初期密着性」という。)を評価した。缶が作製でき、フィルムの剥離がなく初期密着性に優れるものを「3点」とし、フィルムの一部が剥離したものを「2点」とし、フィルムが全面剥離したものを「1点」とした。評価試験の結果を表7〜表9に示す。
耐薬品密着維持性のうち、ここでは、電解液に対する密着維持性(以下、「耐電解液密着維持性」という。)について評価した。詳しくは、次のようにして、成形加工後にさらに電解液に浸漬した後の缶について、ポリプロピレンフィルムの剥離の有無を評価した。
2 表面処理皮膜
3 樹脂フィルム(ラミネートフィルム)又は樹脂塗膜
10 表面処理皮膜を有する金属材料
Claims (4)
- カルボキシル基及び/又は水酸基を1分子中に2個以上含有し、分子量が254以下である有機化合物(A)と、前記カルボキシル基及び/又は前記水酸基と反応しうる構造単位を有する架橋性有機化合物(B1)及び前記カルボキシル基及び/又は前記水酸基と反応しうる元素を含む架橋性無機化合物(B2)から選ばれる1種又は2種以上の架橋性化合物(B)とを含有することを特徴とする水系金属表面処理剤。
- 前記架橋性有機化合物(B1)が、カルボジイミド結合、オキサゾリン基、グリシジルエーテル基、イソシアネート基及びメチロール基から選ばれる1種又は2種以上の構造単位を有する、請求項1に記載の水系金属表面処理剤。
- 前記架橋性無機化合物(B2)が、Mg、Al、Ca、Mn、Co、Ni、Cr(III)、Zn、Fe、Zr、Ti、Si、Sr、W、Ce、Mo、V、Sn、Bi、Ta、Te、In、Ba、Hf、Se、Sc、Nb、Cu、Y、Nd及びLaから選ばれる1種又は2種以上の元素を含む、請求項1又は2に記載の水系金属表面処理剤。
- 請求項1〜3のいずれか1項に記載の水系金属表面処理剤を金属材料表面に塗布して形成された表面処理皮膜を有することを特徴とする金属材料。
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