JP7455187B2 - 電気化学fetセンサ - Google Patents
電気化学fetセンサ Download PDFInfo
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- JP7455187B2 JP7455187B2 JP2022502031A JP2022502031A JP7455187B2 JP 7455187 B2 JP7455187 B2 JP 7455187B2 JP 2022502031 A JP2022502031 A JP 2022502031A JP 2022502031 A JP2022502031 A JP 2022502031A JP 7455187 B2 JP7455187 B2 JP 7455187B2
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- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/403—Cells and electrode assemblies
- G01N27/414—Ion-sensitive or chemical field-effect transistors, i.e. ISFETS or CHEMFETS
- G01N27/4148—Integrated circuits therefor, e.g. fabricated by CMOS processing
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/416—Systems
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N33/00—Investigating or analysing materials by specific methods not covered by groups G01N1/00 - G01N31/00
- G01N33/48—Biological material, e.g. blood, urine; Haemocytometers
- G01N33/50—Chemical analysis of biological material, e.g. blood, urine; Testing involving biospecific ligand binding methods; Immunological testing
- G01N33/53—Immunoassay; Biospecific binding assay; Materials therefor
- G01N33/543—Immunoassay; Biospecific binding assay; Materials therefor with an insoluble carrier for immobilising immunochemicals
- G01N33/54366—Apparatus specially adapted for solid-phase testing
- G01N33/54373—Apparatus specially adapted for solid-phase testing involving physiochemical end-point determination, e.g. wave-guides, FETS, gratings
- G01N33/5438—Electrodes
Description
分析物溶液と接触して配置されるように構成された作用電極と、
ソース端子、ドレイン端子、および複数のナノワイヤを備える増幅器であって、前記複数のナノワイヤのそれぞれが、前記ソース端子を前記ドレイン端子に電気的に接続する増幅器と、
第1の側および前記第1の側の反対側の第2の側を有する絶縁体と、を備え、
前記作用電極は、前記絶縁体の前記第1の側に配置され、
(a)前記ソース端子、(b)前記ドレイン端子、および(c)前記複数のナノワイヤが、前記絶縁体の前記第2の側に配置され、
これにより、前記絶縁体は、前記作用電極と、(a)前記ソース端子、(b)前記ドレイン端子、または(c)前記複数のナノワイヤのいずれかとの間の直接的な電気的接触を防ぐように構成され、
これにより、前記絶縁体は、前記分析物溶液と、(a)前記ソース端子、(b)前記ドレイン端子、または(c)前記複数のナノワイヤのいずれかとの間の直接接触を防ぐように構成され、
前記作用電極は、電子伝達メディエーターが前記分析物溶液中に存在する場合、前記複数のナノワイヤの位置での電界の変化が誘発されるように構成され、
前記複数のナノワイヤは、電界が変化すると、前記ソース端子と前記ドレイン端子との間の電流の対応する変化が誘導されるように構成される。
前記複数のマイクロプローブのぞれぞれは、分析物溶液に挿入されるように構成された先端と、前記先端に配置されたセンサとを含み、
各センサは、分析物溶液と接触して配置されるように構成された作用電極と、増幅器とを備え、
前記増幅器は、ソース端末と、ドレイン端子、および複数の前記ナノワイヤを備え、
前記ナノワイヤのそれぞれが、前記ソース端子を前記ドレイン端子に電気的に接続し、
前記ナノワイヤのそれぞれは、1から500ナノメートルの範囲の直径を有し、
前記作用電極は、前記絶縁体の前記第1の側に配置され、
(a)前記ソース端子、(b)前記ドレイン端子、および(c)前記複数のナノワイヤは、前記絶縁体の前記第2の側に配置され、
前記絶縁体は、前記作用電極と、(a)前記ソース端子、(b)前記ドレイン端子、または(c)前記複数のナノワイヤのいずれかとの間の直接的な電気的接触を防ぐように構成され、
それによって、前記絶縁体は、分析物溶液と、(a)前記ソース端子、(b)前記ドレイン端子、または(c)前記複数のナノワイヤのいずれかとの間の直接接触を防ぐように構成され、
前記作用電極は、電子伝達メディエーターが分析物溶液中に存在する場合、前記複数のナノワイヤの位置での電界の変化が誘発されるように構成され、
前記複数のナノワイヤは、電界が変化すると、前記ソース端子と前記ドレイン端子との間の電流の対応する変化が誘導されるように構成される。
センシングデバイスの第1のマイクロプローブの先端および第2のマイクロプローブの先端を前記分析物溶液に挿入し、
前記第1および第2のマイクロプローブのそれぞれは、先端に配置されたセンサを含むみ、
各センサは、
分析物溶液と接触して配置されるように構成された作用電極と、
ソース端子、ドレイン端子、および複数のナノワイヤを備える増幅器であって、前記ナノワイヤのそれぞれが、前記ソース端子を、前記ドレイン端子に電気的に接続する増幅器と、
第1の側および前記第1の側の反対側の第2の側を有する絶縁体と、を備え、
前記作用電極は、前記絶縁体の第1の側に配置され、
(a)前記ソース端子、(b)前記ドレイン端子、および(c)複数の前記ナノワイヤは、前記絶縁体の前記第2の側に配置され、
これにより、前記絶縁体は、前記作用電極と、(a)前記ソース端子、(b)ドレイン端子、または(c)前記複数のナノワイヤのいずれかとの間の直接的な電気的接触を防ぐように構成され、
これにより、前記絶縁体は、前記分析物溶液と、(a)前記ソース端子、(b)ドレイン端子、または(c)前記複数のナノワイヤのいずれかとの直接接触を防ぐように構成され、
前記第1のマイクロプローブの前記センサの前記作用電極は、その中に埋め込まれたヒドロゲルを含み、前記ヒドロゲルは、グルコースオキシダーゼを含み、
前記第1のマイクロプローブの前記センサの前記複数のナノワイヤの位置で、
(a)過酸化水素を形成する、グルコースオキシダーゼと分析物溶液中のグルコースとの反応により、および
(b)前記第1のマイクロプローブの前記センサの前記作動電極と、
(1)前記分析物溶液中に存在するレドックス種との、および
(2)前記グルコースオキシダーゼと前記グルコースとの反応によって形成される、
過酸化水素とのレドックス反応により、第1の電界に第1の変動を誘発し、
前記第2のマイクロプローブの前記センサの前記作用電極と、前記分析物溶液中に存在する前記レドックス種とのレドックス反応によって、前記第2のマイクロプローブの前記センサの前記複数のナノワイヤの位置で第2の電界に第2の変動を誘発し、
前記第1のマイクロプローブの前記センサの前記ソース端子と、前記第1のマイクロプローブの前記センサの前記ドレイン端子との間に、第1の電流の第1の変動を誘発し、前記第1の電流の前記第1の変動は、前記第1の電界の前記第1の変動に対応し、
前記第2のマイクロプローブの前記センサの前記ソース端子と、前記第2のマイクロプローブの前記センサの前記ドレイン端子との間に、第2の電流の第2の変動を誘発し、前記第2の電流の第2の変動は、前記第2の電界の前記第2の変動に対応し、
前記第1の電流の前記第1の変動と、前記第2の電流の前記第2の変動との間の差に基づいて、前記分析物溶液中に存在するグルコースの量を決定する。
センシングデバイスの先端に配置されたセンサを分析物溶液に挿入し、
前記センサは、
前記分析物溶液と接触して配置されるように構成された作用電極と、
ソース端子、ドレイン端子、および複数のナノワイヤを備える増幅器であって、前記複数のナノワイヤのそれぞれが、前記ソース端子を前記ドレイン端子に電気的に接続する増幅器と、
第1の側および前記第1の側の反対側の第2の側を有する絶縁体と、を備え、
前記作用電極は、前記絶縁体の前記第1の側に配置され、
(a)前記ソース端子、(b)前記ドレイン端子、および(c)前記複数のナノワイヤは、前記絶縁体の前記第2の側に配置され、
これにより、前記絶縁体は、前記作用電極と、(a)前記ソース端子、(b)ドレイン端子、または(c)前記複数のナノワイヤのいずれかとの間の直接的な電気的接触を防ぐように構成され、
これにより、前記絶縁体は、前記分析物溶液と、(a)前記ソース端子、(b)ドレイン端子、または(c)前記複数のナノワイヤのいずれかとの直接接触を防ぐように構成され、
前記作用電極は、前記化学種が前記分析物溶液中に存在する場合、前記複数のナノワイヤの位置での電界の変化が誘発されるように構成され、
前記複数のナノワイヤは、電界が変化すると、前記ソース端子と前記ドレイン端子との間の電流の対応する変化が誘発されるように構成され、
前記ソース端子と前記ドレイン端子との間の電流の最小変動が、望ましくない前記化学種の存在によって誘導されるように、(a)バックゲート電圧と、(b)作用電極電圧と、(c)ソース電圧を調整する。
センシングデバイスの先端に配置されたセンサを分析物溶液に挿入し、
前記センサは、
前記分析物溶液と接触して配置されるように構成された作用電極と、
ソース端末、ドレイン端子、および複数のナノワイヤを備える増幅器であって、前記複数のナノワイヤのそれぞれが、前記ソース端子を前記ドレイン端子に電気的に接続する増幅器と、
第1の側および前記第1の側の反対側の第2の側を有する絶縁体と、を備え、
前記作用電極は、前記絶縁体の前記第1の側に配置され、
(a)前記ソース端子、(b)前記ドレイン端子、および(c)前記複数のナノワイヤは、前記絶縁体の前記第2の側に配置され、
これにより、前記絶縁体は、前記作用電極と、(a)前記ソース端子、(b)前記ドレイン端子、または(c)前記複数のナノワイヤのいずれかとの間の直接的な電気的接触を防ぐように構成され、
これによって、前記絶縁体は、前記分析物溶液と、(a)前記ソース端子、(b)前記ドレイン端子、または(c)前記複数のナノワイヤのいずれかとの間の直接接触を防ぐように構成され、
前記作用電極は、化学種が分析物溶液中に存在する場合、前記複数のナノワイヤの位置での電界の変化が誘発されるように構成され、
前記複数のナノワイヤは、電界が変化すると、前記ソース端子と前記ドレイン端子との間の電流の対応する変化が誘発されるように構成され、
前記ソース端子と前記ドレイン端子の間の電流の最大変動が分析物の存在によって引き起こされるように。(a)バックゲート電圧、(b)作用電極電圧、および(c)ソース電圧を調整して、特定の分析物のセンサのパフォーマンスグラフで特異点を特定する。
本開示のいくつかの実施形態の一態様によれば、作用電極、絶縁体、およびFET増幅器を含む、メディエーターを含まない、レドックス調整可能な、電気化学的FET増幅センシングシステム(FETセンシングシステム)が提供される。本開示の実施形態による、FETセンシングシステムは、サンプル、例えば、生物学的サンプル中の分析物の存在および/または量を検出するように構成される。
または50ナノメートルから1000ナノメートル、または75ナノメートルから1000ナノメートル、または100ナノメートルから1000ナノメートル、または150ナノメートルから1000ナノメートル、または200ナノメートルから1000ナノメートル、または300ナノメートルから1000ナノメートル、または500ナノメートルから1000ナノメートル、または700ナノメートルから1000ナノメートル、または800ナノメートルから1000ナノメートル、または900ナノメートルから1000ナノメートルの非円形断面主寸法を有する。
または5ナノメートルから300ナノメートル、または5ナノメートルから200ナノメートル、または5ナノメートルから150ナノメートル、または5ナノメートルから100ナノメートル、または5ナノメートルから50ナノメートル、または5ナノメートルから25ナノメートル、または5ナノメートルから10ナノメートルの非円形主要寸法を有する。
本発明におけるキャリブレーションプロセスの1つの目的は、作用電極の性能がロバストで十分に敏感である電圧値または電圧値範囲を特定することである。場合によっては、校正プロセスにより、作用電極のこの性能レベルをサポートするバックゲート電極の電圧値または電圧値範囲も特定される。
図16~20は、本開示の例示的な実施形態による、マルチマイクロプローブセンシングチップ132を示している。図16~19に見られるように、センシングチップ132は、センシングチップ132のブリッジ部分134から外向きに延びる少なくとも1つのセンシングマイクロプローブ136を含む。少なくとも1つのセンシングマイクロプローブ136は、マイクロプローブ142の先端をブリッジ部分134に接続する本体140を有する。マイクロプローブの先端142は、円錐形、円筒形、管状形、およびピラミッド形を含むがこれらに限定されない任意の形状を有することができる。一実施形態では、少なくとも1つのマイクロプローブ136の先端142は、それが低侵襲性の皮膚貫通マイクロプローブを形成するように鋭利である。本発明のいくつかの実施形態では、少なくとも1つのマイクロプローブ136は真っ直ぐであるが、真っ直ぐではない形状(例えば、湾曲したマイクロプローブ、フック形状のマイクロプローブ、またはセミフック形状のマイクロプローブ)も企図される。少なくとも1つのマイクロプローブ136は、マイクロプローブアレイのブリッジ部分134から垂直に突出することができる。本発明のいくつかの実施形態では、少なくとも1つのマイクロプローブ136は、センシングチップ132のブリッジ部分134に取り付けられた、またはそれと一体のベース138を有し、本体140は、センシングチップ132のブリッジ部分134から離れて延びる。先端142は、基部138の遠位にある本体140の遠位にある。
図35~36に示される本発明のいくつかの実施形態では、マルチマイクロプローブセンシングチップ132は、センシングシステム180に組み込まれる。本発明のいくつかの実施形態では、センシングシステム180は、複数の生体分析物の存在、不在、または量を監視することを可能にするパッチまたは取り外し可能なインプラントとして構成される。図35に示されるように、本発明のいくつかの実施形態では、センシングシステム180は、対象(ヒトまたは動物)の皮膚に接触するための皮膚接触面184を有するセンサパッチ182を備える。本発明のいくつかの実施形態では、センサパッチ182は、1つまたは複数のセンシングマイクロプローブ136が皮膚接触面から外向きに突出するように、マルチマイクロプローブセンシングチップ132を保持するように構成される。例示的な実施形態では、少なくとも1つのマイクロプローブ136は、センサパッチ182の表面184から垂直に、または表面184から鋭角で突出することができる。本発明のいくつかの実施形態では、回路がセンサパッチ182に取り付けられている。本発明のいくつかの実施形態では、回路は、マイクロプローブに対して基板の反対側に配置される。
Claims (12)
- 分析物溶液と接触して配置されるように構成された作用電極と、
ソース端子、ドレイン端子、および複数のナノワイヤを備える電界効果トランジスタ増幅器であって、前記複数のナノワイヤのそれぞれが、前記ソース端子を前記ドレイン端子に電気的に接続する電界効果トランジスタ増幅器と、
第1の側と、当該第1の側の反対側の第2の側とを有する絶縁体と、を備え、
前記作用電極は、前記絶縁体の前記第1の側に配置され、
前記電界効果トランジスタ増幅器が、前記絶縁体の前記第2の側に配置され、
これにより、前記絶縁体は、前記作用電極と、前記電界効果トランジスタ増幅器との間の直接的な電気的接触を防ぐように構成され、
これにより、前記絶縁体は、前記分析物溶液と、前記電界効果トランジスタ増幅器との間の直接接触を防ぐように構成され、
前記作用電極は、化学種が前記分析物溶液中に存在する場合、前記電界効果トランジスタ増幅器の位置での電界の変化が誘発されるように構成され、
前記電界効果トランジスタ増幅器は、電界が変化すると、前記ソース端子と前記ドレイン端子との間の電流の対応する変化が誘導されるように構成される、
センサ。 - 前記作用電極、前記電界効果タトランジスタ増幅器、および前記絶縁体は、積み重ねられた構成である、
請求項1に記載のセンサ。 - 前記作用電極、前記電界効果トランジスタ増幅器、および前記絶縁体は、平面内に並んで構成されている、
請求項1に記載のセンサ。 - 前記作用電極材料が少なくとも1つの貴金属を備える、
請求項1に記載のセンサ。 - 前記作用電極材料が金属を備える、
請求項1に記載のセンサ。 - 前記センサの全体のサイズは、0.00005mm2から0.005mm2である、
請求項1に記載のセンサ。 - 前記作用電極の露出部分は、1ミクロンから1,000ミクロンの主寸法を有する、
請求項1に記載のセンサ。 - 前記複数のナノワイヤは、1から100個のナノワイヤを備える、
請求項1に記載のセンサ。 - 前記センサは、前記作用電極上に配置されたヒドロゲルをさらに備え、前記ヒドロゲルは、前記分析物溶液中の分析物と相互作用するように構成された少なくとも1つの酵素を含む、
請求項1に記載のセンサ。 - 前記酵素は、グルコースオキシダーゼ、乳酸塩オキシダーゼ、3-ヒドロキシ酪酸デヒドロゲナーゼ、コレステロールオキシダーゼ、ピルビン酸オキシダーゼ、グリセロールオキシダーゼ、アルコールオキシダーゼ、グルタミナーゼオキシダーゼ、L-グルタミン酸オキシダーゼ、キサンチンオキシダーゼ、L-グルタミン酸、コリンオキシダーゼ、サルコシンオキシダーゼ、アスコルビン酸オキシダーゼ、クレアチニナーゼ、クレアチナーゼ、ペルオキシダーゼ、ラクケース、チロシナーゼ、3-ヒドロキシブチレートデヒドロゲナーゼ、グルコースデヒドロゲナーゼ、乳酸デヒドロゲナーゼ、アルコールデヒドロゲナーゼ、またはグルタミン酸デヒドロゲナーゼの1つを含む、
請求項9に記載のセンサ。 - 前記ヒドロゲルは、β-d-グルコース、L-乳酸、グルタミン、コレステロール、グリセロール、ピルビン酸、エタノールL-グルタミン酸、コリンアセチルコリン、1-アスコルビン酸、コルチゾール、クレアチニン、クレアチニン、2-ヒドロキシ酪酸、3-ヒドロキシ酪酸またはアセト酢酸の少なくとも1つと相互作用する酵素を含む、
請求項9に記載のセンサ。 - 前記化学種は、過酸化水素、ニコチンアミドアデニンジヌクレオチド(NADH)、アスコルビン酸、カフェイン、アセトアミノフェン、フラビンアデニンジヌクレオチド(FAD)、フラビンモノヌクレオチド(FMN)またはキノン補因子のうちの1つである、
請求項9に記載のセンサ。
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