JP2018099504A - 生体電極組成物、生体電極、及び生体電極の製造方法 - Google Patents
生体電極組成物、生体電極、及び生体電極の製造方法 Download PDFInfo
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- JP2018099504A JP2018099504A JP2017205300A JP2017205300A JP2018099504A JP 2018099504 A JP2018099504 A JP 2018099504A JP 2017205300 A JP2017205300 A JP 2017205300A JP 2017205300 A JP2017205300 A JP 2017205300A JP 2018099504 A JP2018099504 A JP 2018099504A
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Abstract
【解決手段】イオン性の繰り返し単位aが、下記一般式(1−1)及び(1−2)で示される部分構造のうちいずれかもしくは両方を有するナトリウム塩、カリウム塩、アンモニウム塩の繰り返し単位生体電極組成物。
【選択図】なし
Description
本発明の生体電極組成物は、粘着機能を有するポリマー型イオン性材料として、イオン性の繰り返し単位aと、(メタ)アクリレートの繰り返し単位bとの両方を有する高分子化合物を含有する。以下、各成分について、さらに詳細に説明する。
本発明の生体電極組成物における高分子化合物は、導電性材料として配合されるポリマー型の塩であり、イオン性の繰り返し単位aと、(メタ)アクリレートの繰り返し単位bとの両方を有する。
なお、例えば、a+b+c=1とは、繰り返し単位a、b、cを含む高分子化合物において、繰り返し単位a、b、cの合計量が全繰り返し単位の合計量に対して100モル%であることを示し、a+b+c<1とは、繰り返し単位a、b、cの合計量が全繰り返し単位の合計量に対して100モル%未満であり、a、b、c以外に他の繰り返し単位を有していることを示す。
また、本発明の生体電極組成物には、有機溶剤を添加することができる。有機溶剤としては、具体的には、トルエン、キシレン、クメン、1,2,3−トリメチルベンゼン、1,2,4−トリメチルベンゼン、1,3,5−トリメチルベンゼン、スチレン、αメチルスチレン、ブチルベンゼン、sec−ブチルベンゼン、イソブチルベンゼン、シメン、ジエチルベンゼン、2−エチル−p−キシレン、2−プロピルトルエン、3−プロピルトルエン、4−プロピルトルエン、1,2,3,5−テトラメチルベンゼン、1,2,4,5−テトラメチルベンゼン、テトラヒドロナフタレン、4−フェニル−1−ブテン、tert−アミルベンゼン、アミルベンゼン、2−tert−ブチルトルエン、3−tert−ブチルトルエン、4−tert−ブチルトルエン、5−イソプロピル−m−キシレン、3−メチルエチルベンゼン、tert−ブチル−3−エチルベンゼン、4−tert−ブチル−o−キシレン、5−tert−ブチル−m−キシレン、tert−ブチル−p−キシレン、1,2−ジイソプロピルベンゼン、1,3−ジイソプロピルベンゼン、1,4−ジイソプロピルベンゼン、ジプロピルベンゼン、3,9−ドデカジイン、ペンタメチルベンゼン、ヘキサメチルベンゼン、ヘキシルベンゼン、1,3,5−トリエチルベンゼン等の芳香族系炭化水素系溶剤、n−ヘプタン、イソヘプタン、3−メチルヘキサン、2,3−ジメチルペンタン、3−エチルペンタン、1,6−ヘプタジエン、5−メチル−1−ヘキシン、ノルボルナン、ノルボルネン、ジシクロペンタジエン、1−メチル−1,4−シクロヘキサジエン、1−ヘプチン、2−ヘプチン、シクロヘプタン、シクロヘプテン、1,3−ジメチルシクロペンタン、エチルシクロペンタン、メチルシクロヘキサン、1−メチル−1−シクロヘキセン、3−メチル−1−シクロヘキセン、メチレンシクロヘキサン、4−メチル−1−シクロヘキセン、2−メチル−1−ヘキセン、2−メチル−2−ヘキセン、1−ヘプテン、2−ヘプテン、3−ヘプテン、n−オクタン、2,2−ジメチルヘキサン、2,3−ジメチルヘキサン、2,4−ジメチルヘキサン、2,5−ジメチルヘキサン、3,3−ジメチルヘキサン、3,4−ジメチルヘキサン、3−エチル−2−メチルペンタン、3−エチル−3−メチルペンタン、2−メチルヘプタン、3−メチルヘプタン、4−メチルヘプタン、2,2,3−トリメチルペンタン、2,2,4−トリメチルペンタン、シクロオクタン、シクロオクテン、1,2−ジメチルシクロヘキサン、1,3−ジメチルシクロヘキサン、1,4−ジメチルシクロヘキサン、エチルシクロヘキサン、ビニルシクロヘキサン、イソプロピルシクロペンタン、2,2−ジメチル−3−ヘキセン、2,4−ジメチル−1−ヘキセン、2,5−ジメチル−1−ヘキセン、2,5−ジメチル−2−ヘキセン、3,3−ジメチル−1−ヘキセン、3,4−ジメチル−1−ヘキセン、4,4−ジメチル−1−ヘキセン、2−エチル−1−ヘキセン、2−メチル−1−ヘプテン、1−オクテン、2−オクテン、3−オクテン、4−オクテン、1,7−オクタジエン、1−オクチン、2−オクチン、3−オクチン、4−オクチン、n−ノナン、2,3−ジメチルヘプタン、2,4−ジメチルヘプタン、2,5−ジメチルヘプタン、3,3−ジメチルヘプタン、3,4−ジメチルヘプタン、3,5−ジメチルヘプタン、4−エチルヘプタン、2−メチルオクタン、3−メチルオクタン、4−メチルオクタン、2,2,4,4−テトラメチルペンタン、2,2,4−トリメチルヘキサン、2,2,5−トリメチルヘキサン、2,2−ジメチル−3−ヘプテン、2,3−ジメチル−3−ヘプテン、2,4−ジメチル−1−ヘプテン、2,6−ジメチル−1−ヘプテン、2,6−ジメチル−3−ヘプテン、3,5−ジメチル−3−ヘプテン、2,4,4−トリメチル−1−ヘキセン、3,5,5−トリメチル−1−ヘキセン、1−エチル−2−メチルシクロヘキサン、1−エチル−3−メチルシクロヘキサン、1−エチル−4−メチルシクロヘキサン、プロピルシクロヘキサン、イソプロピルシクロヘキサン、1,1,3−トリメチルシクロヘキサン、1,1,4−トリメチルシクロヘキサン、1,2,3−トリメチルシクロヘキサン、1,2,4−トリメチルシクロヘキサン、1,3,5−トリメチルシクロヘキサン、アリルシクロヘキサン、ヒドリンダン、1,8−ノナジエン、1−ノニン、2−ノニン、3−ノニン、4−ノニン、1−ノネン、2−ノネン、3−ノネン、4―ノネン、n−デカン、3,3−ジメチルオクタン、3,5−ジメチルオクタン、4,4−ジメチルオクタン、3−エチル−3−メチルヘプタン、2−メチルノナン、3−メチルノナン、4−メチルノナン、tert−ブチルシクロヘキサン、ブチルシクロヘキサン、イソブチルシクロヘキサン、4−イソプロピル−1−メチルシクロヘキサン、ペンチルシクロペンタン、1,1,3,5−テトラメチルシクロヘキサン、シクロドデカン、1−デセン、2−デセン、3−デセン、4−デセン、5−デセン、1,9−デカジエン、デカヒドロナフタレン、1−デシン、2−デシン、3−デシン、4−デシン、5−デシン、1,5,9−デカトリエン、2,6−ジメチル−2,4,6−オクタトリエン、リモネン、ミルセン、1,2,3,4,5−ペンタメチルシクロペンタジエン、α−フェランドレン、ピネン、テルピネン、テトラヒドロジシクロペンタジエン、5,6−ジヒドロジシクロペンタジエン、ジシクロペンタジエン、1,4−デカジイン、1,5−デカジイン、1,9−デカジイン、2,8−デカジイン、4,6−デカジイン、n−ウンデカン、アミルシクロヘキサン、1−ウンデセン、1,10−ウンデカジエン、1−ウンデシン、3−ウンデシン、5−ウンデシン、トリシクロ[6.2.1.02,7]ウンデカ−4−エン、n−ドデカン、2−メチルウンデカン、3−メチルウンデカン、4−メチルウンデカン、5−メチルウンデカン、2,2,4,6,6−ペンタメチルヘプタン、1,3−ジメチルアダマンタン、1−エチルアダマンタン、1,5,9−シクロドデカトリエン、1,2,4−トリビニルシクロヘキサン、イソパラフィン等の脂肪族炭化水素系溶剤、シクロヘキサノン、シクロペンタノン、2−オクタノン、2−ノナノン、2−ヘプタノン、3−ヘプタノン、4−ヘプタノン、2−ヘキサノン、3−ヘキサノン、ジイソブチルケトン、メチルシクロヘキサノン、メチルn−ペンチルケトン等のケトン系溶剤、3−メトキシブタノール、3−メチル−3−メトキシブタノール、1−メトキシ−2−プロパノール、1−エトキシ−2−プロパノール等のアルコール系溶剤、プロピレングリコールモノメチルエーテル、エチレングリコールモノメチルエーテル、プロピレングリコールモノエチルエーテル、エチレングリコールモノエチルエーテル、プロピレングリコールジメチルエーテル、ジエチレングリコールジメチルエーテル、ジイソプロピルエーテル、ジイソブチルエーテル、ジイソペンチルエーテル、ジ−n−ペンチルエーテル、メチルシクロペンチルエーテル、メチルシクロヘキシルエーテル、ジ−n−ブチルエーテル、ジ−secブチルエーテル、ジイソペンチルエーテル、ジ−sec−ペンチルエーテル、ジ−tert−アミルエーテル、ジ−n−ヘキシルエーテル、アニソール等のエーテル系溶剤、プロピレングリコールモノメチルエーテルアセテート、プロピレングリコールモノエチルエーテルアセテート、乳酸エチル、ピルビン酸エチル、酢酸ブチル、3−メトキシプロピオン酸メチル、3−エトキシプロピオン酸エチル、酢酸tert−ブチル、プロピオン酸tert−ブチル、プロピレングリコールモノtert−ブチルエーテルアセテート等のエステル系溶剤、γ−ブチロラクトン等のラクトン系溶剤等を挙げることができる。
本発明の生体電極組成物には、導電性をさらに高めるために、導電性向上剤として、カーボン材料を添加することができる。カーボン材料としては、カーボンブラック、カーボンナノチューブ等を挙げることができる。カーボンナノチューブは単層、多層のいずれであってもよく、表面が有機基で修飾されていても構わない。カーボン材料の添加量は、高分子化合物100質量部に対して1〜50質量部の範囲とすることが好ましい。
また、本発明の生体電極組成物には、カーボン材料以外の導電性向上剤を添加することもできる。具体的には、樹脂を金、銀、白金等の貴金属や銅、ニッケルでコートした粒子や、金、銀、白金等のナノ粒子、インジウムスズの酸化物(ITO)、インジウム亜鉛酸化物(IZO)、スズ酸化物、亜鉛酸化物等の金属酸化物の粒子等を挙げることができる。特には、ITO粒子、又は銀、金、白金、銅、及びニッケルから選ばれる金属でコートされた粒子が好ましい。
生体電極を肌から剥がした後に、肌に生体接触層が付着することがないようにするために、架橋剤を添加することができる。本発明で使用可能な架橋剤の具体例を列挙すると、メチロール基、アルコキシメチル基、アシロキシメチル基から選ばれる少なくとも一つの基で置換されたメラミン化合物、グアナミン化合物、グリコールウリル化合物、又はウレア化合物、エポキシ化合物、イソシアネート化合物、アジド化合物、アルケニルエーテル基等の二重結合を含む化合物等を挙げることができる。これらは添加剤として用いてもよいが、高分子化合物の側鎖にペンダント基として導入してもよい。また、ヒドロキシ基を含む化合物も架橋剤として用いることができる。
また、本発明では、導電性基材と該導電性基材上に形成された生体接触層とを有する生体電極であって、前記生体接触層が、上述の本発明の生体電極組成物の硬化物である生体電極を提供する。
本発明の生体電極は、導電性基材を有するものである。この導電性基材は、通常、センサーデバイス等と電気的に接続されており、生体から生体接触層を介して取り出した電気信号をセンサーデバイス等まで伝導させる。
本発明の生体電極は、導電性基材上に形成された生体接触層を有するものである。この生体接触層は、生体電極を使用する際に、実際に生体と接触する部分であり、導電性及び粘着性を有する。生体接触層は、上述の本発明の生体電極組成物の硬化物であり、即ち、上述の粘着性機能を有する高分子化合物、さらには必要に応じてカーボン材料等の添加剤を含有する粘着性の樹脂層である。
また、本発明では、導電性基材と該導電性基材上に形成された生体接触層とを有する生体電極の製造方法であって、前記導電性基材上に、上述の本発明の生体電極組成物を塗布し、硬化させることで前記生体接触層を形成する生体電極の製造方法を提供する。
Mw=20,900
Mw/Mn=2.21
Mw=27,400
Mw/Mn=1.94
Mw=30,600
Mw/Mn=1.88
Mw=26,600
Mw/Mn=1.86
Mw=80,900
Mw/Mn=4.33
Mw=35,600
Mw/Mn=2.34
Mw=35,700
Mw/Mn=2.33
Mw=30,900
Mw/Mn=2.66
Mw=51,600
Mw/Mn=2.55
Mw=75,600
Mw/Mn=5.38
Mw=65,600
Mw/Mn=5.36
Mw=16,300
Mw/Mn=1.75
Mw=29,600
Mw/Mn=1.89
Mw=29,800
Mw/Mn=2.10
Mw=116,000
Mw/Mn=2.20
Mw=44,900
Mw/Mn=2.59
Mw=57,900
Mw/Mn=1.89
カーボンブラック:デンカ社製 デンカブラックHS−100
カーボンナノチューブ:Sigma−Aldrich社製 Multi−walled 直径60〜100nm、長さ5μm
金コート粒子:積水化学社製 ミクロパールAU(直径100μm)
銀コート粒子:三菱マテリアル社製 銀コート粉(直径30μm)
ITO粒子:三菱マテリアル社製 ITO粉(直径0.03μm)
表1に記載の組成で、高分子化合物溶液、比較塩、及び添加剤(導電性向上剤、架橋剤)をブレンドし、生体電極組成物溶液(生体電極組成物溶液1〜18、比較生体電極組成物溶液1〜5)を調製した。
直径3cm、厚さ0.2mmのアルミニウム製の円板の上にアプリケーターを用いて生体電極組成物溶液を塗布し、室温で6時間風乾した後、オーブンを用いて窒素雰囲気下130℃で30分間ベークして硬化させて、1つの生体電極組成物溶液につき生体電極を4枚作製した。このようにして得られた生体電極は、図3(a)、(b)に示されるように、一方の面には生体接触層3を有し、他方の面には導電性基材としてアルミニウム製の円板7を有するものであった。次に、図3(b)に示されるように、生体接触層で覆われていない側のアルミニウム製の円板7の表面に銅配線8を粘着テープで貼り付けて引き出し電極とし、これをインピーダンス測定装置に接続した。図4に示されるように、人の腕の肌と生体接触層側が接触するように生体電極1’を2枚貼り付けて、その間隔を15cmとした。ソーラトロン社製の交流インピーダンス測定装置SI1260を用い、周波数を変えながら初期インピーダンスを測定した。次に、残りの2枚の生体電極を純水中に1時間浸漬し、水を乾燥させた後、上記と同様の方法で肌上のインピーダンスを測定した。周波数1,000Hzにおけるインピーダンスを表2に示す。
生体電極組成物溶液を、アプリケーターを用いて厚さ100μmのPEN(ポリエチレンナフタレート)基板上に塗布し、室温で6時間風乾後、オーブンを用いて窒素雰囲気下130℃で30分間ベークして硬化させて、粘着フィルムを作製した。この粘着フィルムから25mm幅のテープを切り取り、これをステンレス版(SUS304)に圧着させ、室温で20時間放置した後、引っ張り試験機を用い角度180度、300mm/分の速度で粘着剤が付いたテープをステンレス版から引きはがすのに要する力(N/25mm)を測定した。結果を表2に示す。
上記の導電性評価試験で作製した生体電極において、生体接触層の厚さをマイクロメーターを用いて測定した。結果を表2に示す。
4…カーボン材料、 5…高分子化合物(樹脂)、 6…生体、
7…アルミニウム製の円板、 8…銅配線。
Claims (9)
- イオン性の繰り返し単位aと、(メタ)アクリレートの繰り返し単位bとの両方を有する高分子化合物を含有する生体電極組成物であって、
前記イオン性の繰り返し単位aが、下記一般式(1−1)及び(1−2)で示される部分構造のうちいずれかもしくは両方を有するナトリウム塩、カリウム塩、アンモニウム塩の繰り返し単位であり、前記(メタ)アクリレートの繰り返し単位bが、下記一般式(2)で示される繰り返し単位であることを特徴とする生体電極組成物。
- 前記繰り返し単位aが、下記一般式(3)で示される繰り返し単位a1〜a5から選ばれる1種以上であることを特徴とする請求項1に記載の生体電極組成物。
- 前記高分子化合物が、さらに、前記繰り返し単位a及び前記繰り返し単位b以外に、フッ素原子又はケイ素原子を有する繰り返し単位c及びヒドロキシ基、カルボキシル基、オキシラン基、オキセタン基から選ばれる1種以上の基を有する繰り返し単位dのいずれかもしくは両方を共重合した高分子化合物であることを特徴とする請求項1又は請求項2に記載の生体電極組成物。
- 前記生体電極組成物が、さらに、カーボン材料、ITO粒子、又は銀、金、白金、銅、及びニッケルから選ばれる金属でコートされた粒子を含有するものであることを特徴とする請求項1から請求項3のいずれか一項に記載の生体電極組成物。
- 前記カーボン材料が、カーボンブラック及びカーボンナノチューブのいずれかもしくは両方であることを特徴とする請求項4に記載の生体電極組成物。
- 導電性基材と該導電性基材上に形成された生体接触層とを有する生体電極であって、
前記生体接触層が、請求項1から請求項5のいずれか一項に記載の生体電極組成物の硬化物であることを特徴とする生体電極。 - 前記導電性基材が、金、銀、塩化銀、白金、アルミニウム、マグネシウム、スズ、タングステン、鉄、銅、ニッケル、ステンレス、クロム、チタン、及び炭素から選ばれる1種以上を含むものであることを特徴とする請求項6に記載の生体電極。
- 導電性基材と該導電性基材上に形成された生体接触層とを有する生体電極の製造方法であって、
前記導電性基材上に、請求項1から請求項5のいずれか一項に記載の生体電極組成物を塗布し、硬化させることで前記生体接触層を形成することを特徴とする生体電極の製造方法。 - 前記導電性基材として、金、銀、塩化銀、白金、アルミニウム、マグネシウム、スズ、タングステン、鉄、銅、ニッケル、ステンレス、クロム、チタン、及び炭素から選ばれる1種以上を含むものを用いることを特徴とする請求項8に記載の生体電極の製造方法。
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