Multilayer carbon hybrid based electrodes for direct electrochemical detection of analgesics and biomolecules - Development of an electrochemical sensor for determination of analgesics in blood samples

Niklas Wester

Multilayer carbon hybrid based electrodes for direct electrochemical detection of analgesics and biomolecules - Development of an electrochemical sensor for determination of analgesics in blood samples

Julkaisun otsikon käännös: Monikerroksiset hiilipohjaiset hybridielektrodit sähkökemiallisessa analgeettien ja biomolekyylienhavaitsemisessa

Niklas Wester

Tutkimustuotos: Doctoral Thesis › Collection of Articles

Abstrakti

Kiinnostus vierimittauksiin sekä lääkkeiden ja biomolekyylien reaaliaikaiseen mittaamiseen kasvaa jatkuvasti. Lisäksi näiden analyyttien monitorointi puettavilla- sekä in vivo -antureilla on kiivaan tutkimuksen kohde. Nopeat vierimittaukset voivat parantaa potilaan hoitoa myrkytystapauksissa sekä mahdollistaa yksilöidyn terveydenhoidon. Neurotransmissioiden reaaliaikainen havaitseminen tutkimuksessa voi myös parantaa neurofysiologian ymmärrystä ja edelleen kehittää neurodegeneratiivisten sairauksien hoitoa. Sähkökemiallisten mittausten matalan hinnan, yksinkertaisen laitteiston ja pienen näytevolyymin vuoksi se on kilpailukykyinen menetelmä vierimittauksissa sekä puettavissa antureissa. Potilaiden vasteet analgeettisiin lääkkeisiin ovat usein yksilöllisiä. Tämän vuoksi annos, jolla ei ole analgeettista vaikutusta yhdellä potilaalla, voi aiheuttaa vaarallisia sivuvaikutuksia toisella. Lisäksi analgeettien väärinkäyttö on yleistä ja erityisesti opioidien aiheuttamiin yliannostuksiin kuolee pelkästään Yhdysvalloissa kymmeniä tuhansia ihmisiä vuosittain. Myös tahalliset ja tahattomat yliannostukset reseptivapailla lääkkeillä kuten parasetamolilla, ovat yleisiä. Näistä syistä kvantitatiivinen vierimittausmenetelmä analgeettien määrittämiseen kapillaariverinäytteestä voisi olla tehokas työkalu yliannostusten diagnoosissa. Vierimittausmenetelmän kehittäminen pienmolekyylien määrittämiseen käsittelemättömästä verinäytteestä on kuitenkin osoittautunut haastavaksi. Tässä työssä tutkimme tetraedrisestä amorfisesta hiilestä ja yksiseinämäisistä hiilinanoputkista valmistettujen ohutkalvojen käyttöä sähkökemiallisissa antureissa. Lisäksi tutkimme näiden materiaalien fysikaaliskemiallisia ominaisuuksia yhdistämällä synkrotronisäteilyyn perustuvan röntgenspektroskopian elektronimikroskopiaan, elektronidiffraktioon sekä perinteisiin spektroskooppisiin menetelmiin. Tutkittujen materiaalien hyvät elektroninsiirto-ominaisuudet ja matala taustavirta mahdollistavat dopamiinin ja analgeettien herkän mittaamisen. Materiaalien rajallinen selektiivisyys ja biolikaantuminen kuitenkin rajoittavat niiden käyttöä biologisissa näytteissä. Näitä ominaisuuksia sekä herkkyyttä voitiin kuitenkin parantaa hiilinanomateriaali- ja polymeeripinnoitteilla. Osoitamme, että nämä monikerroksiset elektrodit voidaan räätälöidä dopamiinin ja analgeettien havaitsemiseen. Lisäksi näillä elektrodeilla voidaan havaita analgeetteja ihmisen veriplasmassa ja kokoveressä ilman proteiinien saostusta. Tämän työn tulosten perusteella kyseisiä elektrodeja voidaan käyttää lääkeaineiden vapaan pitoisuuden määrittämiseen lähes reaaliajassa. Lopuksi, kehitimme massatuotantoon soveltuvan prosessin sähkökemiallisten mittaliuskojen valmistamiseen. Näiden anturien avulla voitiin mitata kliinisesti relevantteja konsentraatioita parasetamolia 20 µL verinäytteestä alle viidessä minuutissa.

Julkaisun otsikon käännös	Monikerroksiset hiilipohjaiset hybridielektrodit sähkökemiallisessa analgeettien ja biomolekyylienhavaitsemisessa
Alkuperäiskieli	Englanti
Pätevyys	Tohtorintutkinto
Myöntävä instituutio	Aalto-yliopisto
Valvoja/neuvonantaja	Koskinen, Jari, Vastuuprofessori Laurila, Tomi, Ohjaaja
Kustantaja	Aalto University
Painoksen ISBN	978-952-64-0257-4
Sähköinen ISBN	978-952-64-0258-1
Tila	Julkaistu - 2021
OKM-julkaisutyyppi	G5 Tohtorinväitöskirja (artikkeli)

Tutkimusalat

amorfinen hiili
hiilinanoputket
sähkökemia
voltammteria
dopamiini
parasetamoli
morfiini
opioidit

Pääsy asiakirjaan

http://urn.fi/URN:ISBN:978-952-64-0258-1

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@phdthesis{0150c8f017d24a248ae7dc9e8263557b,

title = "Multilayer carbon hybrid based electrodes for direct electrochemical detection of analgesics and biomolecules - Development of an electrochemical sensor for determination of analgesics in blood samples",

abstract = "There is increasing interest in point-of-care (POC) determination of drugs and biomolecules, as well as real-time monitoring of these analytes, with wearable and in vivo sensors. Rapid response POC tests can improve patient safety in situations like poisoning and enable personalized treatments whereas real time detection of physiological processes such as neurotransmission events can improve our understanding of neurophysiology and enable novel treatments for neurological disorders. Electrochemical detection is an attractive technology for both POC in vitro diagnostics and wearable sensors alike, due to its low price, simple instrumentation and small required sample volume. Many analgesic drugs show highly individual dose response and thus a dose that causes dangerous side effects in one patient may lack analgesic effect in another. Analgesics are also some of the most abused prescription drugs. Opioid overdoses kill tens of thousands of people annually in the United states alone. Both intentional and unintentional poisoning of over-the-counter analgesics, such as paracetamol, also regularly occur. Therefore, a quantitative POC test for determination of analgesics in capillary blood samples, could be a powerful diagnostic tool for poisoning. However, the POC determination of small drug and biomolecules in unprocessed blood samples has proven to be difficult. In this thesis, we have investigated the use of tetrahedral amorphous carbon (ta-C) and single-walled carbon nanotube (SWCNT) thin films in electrochemical sensing. We have carried out extensive physicochemical characterization of these electrode materials. We combine synchrotron based x-ray spectroscopy with electron microscopy, diffraction and conventional spectroscopic techniques. Both the studied materials were found to support facile electron transfer and show low background currents enabling highly sensitive detection of dopamine and morphine. They, however, lack the fouling resistance and selectivity required for detection of dopamine and analgesics in complex biological samples. Modification with carbon nanomaterials or polymer membranes significantly improved the selectivity as well as reduced the electrode fouling, allowing for detection of dopamine and analgesics in blood samples without precipitation of proteins. We show that such multilayer electrodes can be tailored for the requirements of detection of neurotransmitters and analgesic drugs. Finally, we demonstrate a process for mass production of electrochemical test strips. These sensor strips were shown to be capable of detecting clinically meaningful concentrations of paracetamol from a 20 µL blood sample in less than 5 min. Based on these results we propose an electrochemical assay for quantitative detection of paracetamol.",

keywords = "amorphous carbon, ta-C, carbon nanotubes, SWCNT, electroanalytical chemistry, dopamine, paracetamol, morphine, opioids, amorfinen hiili, hiilinanoputket, s{\"a}hk{\"o}kemia, voltammteria, dopamiini, parasetamoli, morfiini, opioidit, amorphous carbon, ta-C, carbon nanotubes, SWCNT, electroanalytical chemistry, dopamine, paracetamol, morphine, opioids",

author = "Niklas Wester",

year = "2021",

language = "English",

isbn = "978-952-64-0257-4",

series = "Aalto University publication series DOCTORAL DISSERTATIONS",

publisher = "Aalto University",

number = "14",

address = "Finland",

school = "Aalto University",

}

TY - THES

T1 - Multilayer carbon hybrid based electrodes for direct electrochemical detection of analgesics and biomolecules - Development of an electrochemical sensor for determination of analgesics in blood samples

AU - Wester, Niklas

PY - 2021

Y1 - 2021

N2 - There is increasing interest in point-of-care (POC) determination of drugs and biomolecules, as well as real-time monitoring of these analytes, with wearable and in vivo sensors. Rapid response POC tests can improve patient safety in situations like poisoning and enable personalized treatments whereas real time detection of physiological processes such as neurotransmission events can improve our understanding of neurophysiology and enable novel treatments for neurological disorders. Electrochemical detection is an attractive technology for both POC in vitro diagnostics and wearable sensors alike, due to its low price, simple instrumentation and small required sample volume. Many analgesic drugs show highly individual dose response and thus a dose that causes dangerous side effects in one patient may lack analgesic effect in another. Analgesics are also some of the most abused prescription drugs. Opioid overdoses kill tens of thousands of people annually in the United states alone. Both intentional and unintentional poisoning of over-the-counter analgesics, such as paracetamol, also regularly occur. Therefore, a quantitative POC test for determination of analgesics in capillary blood samples, could be a powerful diagnostic tool for poisoning. However, the POC determination of small drug and biomolecules in unprocessed blood samples has proven to be difficult. In this thesis, we have investigated the use of tetrahedral amorphous carbon (ta-C) and single-walled carbon nanotube (SWCNT) thin films in electrochemical sensing. We have carried out extensive physicochemical characterization of these electrode materials. We combine synchrotron based x-ray spectroscopy with electron microscopy, diffraction and conventional spectroscopic techniques. Both the studied materials were found to support facile electron transfer and show low background currents enabling highly sensitive detection of dopamine and morphine. They, however, lack the fouling resistance and selectivity required for detection of dopamine and analgesics in complex biological samples. Modification with carbon nanomaterials or polymer membranes significantly improved the selectivity as well as reduced the electrode fouling, allowing for detection of dopamine and analgesics in blood samples without precipitation of proteins. We show that such multilayer electrodes can be tailored for the requirements of detection of neurotransmitters and analgesic drugs. Finally, we demonstrate a process for mass production of electrochemical test strips. These sensor strips were shown to be capable of detecting clinically meaningful concentrations of paracetamol from a 20 µL blood sample in less than 5 min. Based on these results we propose an electrochemical assay for quantitative detection of paracetamol.

AB - There is increasing interest in point-of-care (POC) determination of drugs and biomolecules, as well as real-time monitoring of these analytes, with wearable and in vivo sensors. Rapid response POC tests can improve patient safety in situations like poisoning and enable personalized treatments whereas real time detection of physiological processes such as neurotransmission events can improve our understanding of neurophysiology and enable novel treatments for neurological disorders. Electrochemical detection is an attractive technology for both POC in vitro diagnostics and wearable sensors alike, due to its low price, simple instrumentation and small required sample volume. Many analgesic drugs show highly individual dose response and thus a dose that causes dangerous side effects in one patient may lack analgesic effect in another. Analgesics are also some of the most abused prescription drugs. Opioid overdoses kill tens of thousands of people annually in the United states alone. Both intentional and unintentional poisoning of over-the-counter analgesics, such as paracetamol, also regularly occur. Therefore, a quantitative POC test for determination of analgesics in capillary blood samples, could be a powerful diagnostic tool for poisoning. However, the POC determination of small drug and biomolecules in unprocessed blood samples has proven to be difficult. In this thesis, we have investigated the use of tetrahedral amorphous carbon (ta-C) and single-walled carbon nanotube (SWCNT) thin films in electrochemical sensing. We have carried out extensive physicochemical characterization of these electrode materials. We combine synchrotron based x-ray spectroscopy with electron microscopy, diffraction and conventional spectroscopic techniques. Both the studied materials were found to support facile electron transfer and show low background currents enabling highly sensitive detection of dopamine and morphine. They, however, lack the fouling resistance and selectivity required for detection of dopamine and analgesics in complex biological samples. Modification with carbon nanomaterials or polymer membranes significantly improved the selectivity as well as reduced the electrode fouling, allowing for detection of dopamine and analgesics in blood samples without precipitation of proteins. We show that such multilayer electrodes can be tailored for the requirements of detection of neurotransmitters and analgesic drugs. Finally, we demonstrate a process for mass production of electrochemical test strips. These sensor strips were shown to be capable of detecting clinically meaningful concentrations of paracetamol from a 20 µL blood sample in less than 5 min. Based on these results we propose an electrochemical assay for quantitative detection of paracetamol.

KW - amorphous carbon

KW - ta-C

KW - carbon nanotubes

KW - SWCNT

KW - electroanalytical chemistry

KW - dopamine

KW - paracetamol

KW - morphine

KW - opioids

KW - amorfinen hiili

KW - hiilinanoputket

KW - sähkökemia

KW - voltammteria

KW - dopamiini

KW - parasetamoli

KW - morfiini

KW - opioidit

KW - amorphous carbon

KW - ta-C

KW - carbon nanotubes

KW - SWCNT

KW - electroanalytical chemistry

KW - dopamine

KW - paracetamol

KW - morphine

KW - opioids

M3 - Doctoral Thesis

SN - 978-952-64-0257-4

T3 - Aalto University publication series DOCTORAL DISSERTATIONS

PB - Aalto University

ER -

Multilayer carbon hybrid based electrodes for direct electrochemical detection of analgesics and biomolecules - Development of an electrochemical sensor for determination of analgesics in blood samples

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