Printing "smart" Inks of Redox-Responsive Organometallic Polymers on Microelectrode Arrays for Molecular Sensing

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Abstract

Printing arrays of responsive spots for multiplexed sensing with electrochemical readout requires new molecules and precise, high-throughput deposition of active compounds on microelectrodes with spatial control. We have designed and developed new redox-responsive polymers, featuring a poly(ferrocenylsilane) (PFS) backbone and side groups with disulfide units, which allow an efficient and stable bonding to Au substrates, using sulfur-gold coupling chemistry in a "grafting-to" approach. The polymer molecules can be employed for area selective molecular sensing following their deposition by high-precision inkjet printing. The new PFS derivatives, which serve as "molecular inks", were characterized by 1H NMR, 13C NMR, and FTIR spectroscopies and by gel permeation chromatography. The viscosity and surface tension of the inks were assessed by rheology and pendant drop contact angle measurements, respectively. Commercial microelectrode arrays were modified with the new PFS ink by using inkjet printing in the "drop-on-demand" mode. FTIR spectroscopy, AFM, and EDX-SEM confirmed a successful, spatially localized PFS modification of the individual electrodes within the sensing cells of the microelectrode arrays. The potential application of these devices to act as an electrochemical sensor array was demonstrated with a model analyte, ascorbic acid, by using cyclic voltammetry and amperometric measurements.

Original languageEnglish
Pages (from-to)37060-37068
Number of pages9
JournalACS applied materials & interfaces
Volume11
Issue number40
Early online date16 Sep 2019
DOIs
Publication statusPublished - 9 Oct 2019

Fingerprint

Microelectrodes
Organometallics
Ink
Printing
Polymers
Nuclear magnetic resonance
Spectroscopy
Electrochemical sensors
Molecules
Ascorbic acid
Sensor arrays
Gel permeation chromatography
Angle measurement
Rheology
Sulfur
Gold
Disulfides
Ascorbic Acid
Cyclic voltammetry
Contact angle

Keywords

  • inkjet printing
  • electrochemical sensors
  • poly(ferrocenylsilane) (PFS)
  • microelectrode array (MEA) chip
  • drop-on-demand (DoD)

Cite this

@article{de6f26d7cfef4fb1aed2e8b4321b4b97,
title = "Printing {"}smart{"} Inks of Redox-Responsive Organometallic Polymers on Microelectrode Arrays for Molecular Sensing",
abstract = "Printing arrays of responsive spots for multiplexed sensing with electrochemical readout requires new molecules and precise, high-throughput deposition of active compounds on microelectrodes with spatial control. We have designed and developed new redox-responsive polymers, featuring a poly(ferrocenylsilane) (PFS) backbone and side groups with disulfide units, which allow an efficient and stable bonding to Au substrates, using sulfur-gold coupling chemistry in a {"}grafting-to{"} approach. The polymer molecules can be employed for area selective molecular sensing following their deposition by high-precision inkjet printing. The new PFS derivatives, which serve as {"}molecular inks{"}, were characterized by 1H NMR, 13C NMR, and FTIR spectroscopies and by gel permeation chromatography. The viscosity and surface tension of the inks were assessed by rheology and pendant drop contact angle measurements, respectively. Commercial microelectrode arrays were modified with the new PFS ink by using inkjet printing in the {"}drop-on-demand{"} mode. FTIR spectroscopy, AFM, and EDX-SEM confirmed a successful, spatially localized PFS modification of the individual electrodes within the sensing cells of the microelectrode arrays. The potential application of these devices to act as an electrochemical sensor array was demonstrated with a model analyte, ascorbic acid, by using cyclic voltammetry and amperometric measurements.",
keywords = "inkjet printing, electrochemical sensors, poly(ferrocenylsilane) (PFS), microelectrode array (MEA) chip, drop-on-demand (DoD)",
author = "Marco Cirelli and Jinmeng Hao and T.C. Bor and Joost Duvigneau and Niels Benson and R. Akkerman and Hempenius, {Mark A.} and Julius Vancso",
note = "ACS deal",
year = "2019",
month = "10",
day = "9",
doi = "10.1021/acsami.9b11927",
language = "English",
volume = "11",
pages = "37060--37068",
journal = "ACS applied materials & interfaces",
issn = "1944-8244",
publisher = "American Chemical Society",
number = "40",

}

Printing "smart" Inks of Redox-Responsive Organometallic Polymers on Microelectrode Arrays for Molecular Sensing. / Cirelli, Marco ; Hao, Jinmeng ; Bor, T.C.; Duvigneau, Joost ; Benson, Niels; Akkerman, R.; Hempenius, Mark A.; Vancso, Julius.

In: ACS applied materials & interfaces, Vol. 11, No. 40, 09.10.2019, p. 37060-37068.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Printing "smart" Inks of Redox-Responsive Organometallic Polymers on Microelectrode Arrays for Molecular Sensing

AU - Cirelli, Marco

AU - Hao, Jinmeng

AU - Bor, T.C.

AU - Duvigneau, Joost

AU - Benson, Niels

AU - Akkerman, R.

AU - Hempenius, Mark A.

AU - Vancso, Julius

N1 - ACS deal

PY - 2019/10/9

Y1 - 2019/10/9

N2 - Printing arrays of responsive spots for multiplexed sensing with electrochemical readout requires new molecules and precise, high-throughput deposition of active compounds on microelectrodes with spatial control. We have designed and developed new redox-responsive polymers, featuring a poly(ferrocenylsilane) (PFS) backbone and side groups with disulfide units, which allow an efficient and stable bonding to Au substrates, using sulfur-gold coupling chemistry in a "grafting-to" approach. The polymer molecules can be employed for area selective molecular sensing following their deposition by high-precision inkjet printing. The new PFS derivatives, which serve as "molecular inks", were characterized by 1H NMR, 13C NMR, and FTIR spectroscopies and by gel permeation chromatography. The viscosity and surface tension of the inks were assessed by rheology and pendant drop contact angle measurements, respectively. Commercial microelectrode arrays were modified with the new PFS ink by using inkjet printing in the "drop-on-demand" mode. FTIR spectroscopy, AFM, and EDX-SEM confirmed a successful, spatially localized PFS modification of the individual electrodes within the sensing cells of the microelectrode arrays. The potential application of these devices to act as an electrochemical sensor array was demonstrated with a model analyte, ascorbic acid, by using cyclic voltammetry and amperometric measurements.

AB - Printing arrays of responsive spots for multiplexed sensing with electrochemical readout requires new molecules and precise, high-throughput deposition of active compounds on microelectrodes with spatial control. We have designed and developed new redox-responsive polymers, featuring a poly(ferrocenylsilane) (PFS) backbone and side groups with disulfide units, which allow an efficient and stable bonding to Au substrates, using sulfur-gold coupling chemistry in a "grafting-to" approach. The polymer molecules can be employed for area selective molecular sensing following their deposition by high-precision inkjet printing. The new PFS derivatives, which serve as "molecular inks", were characterized by 1H NMR, 13C NMR, and FTIR spectroscopies and by gel permeation chromatography. The viscosity and surface tension of the inks were assessed by rheology and pendant drop contact angle measurements, respectively. Commercial microelectrode arrays were modified with the new PFS ink by using inkjet printing in the "drop-on-demand" mode. FTIR spectroscopy, AFM, and EDX-SEM confirmed a successful, spatially localized PFS modification of the individual electrodes within the sensing cells of the microelectrode arrays. The potential application of these devices to act as an electrochemical sensor array was demonstrated with a model analyte, ascorbic acid, by using cyclic voltammetry and amperometric measurements.

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KW - microelectrode array (MEA) chip

KW - drop-on-demand (DoD)

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U2 - 10.1021/acsami.9b11927

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JO - ACS applied materials & interfaces

JF - ACS applied materials & interfaces

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IS - 40

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