Fluorescence-Based Observation of Transient Electrochemical and Electrokinetic Effects at Nanoconfined Bipolar Electrodes

Karen Scida, Alexander Eden, Netzahualcóyotl Arroyo-Currás, Sean Mackenzie, Yesil Satik, Carl D. Meinhart, Jan C.T. Eijkel, Sumita Pennathur*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

3 Citations (Scopus)

Abstract

Bipolar electrodes (BPEs) are conductors that, when exposed to an electric field, polarize and promote the accumulation of counterionic charge near their poles. The rich physics of electrokinetic behavior near BPEs has not yet been rigorously studied, with our current understanding of such bipolar effects being restricted to steady-state conditions (under constant applied fields). Here, we reveal the dynamic electrokinetic and electrochemical phenomena that occur near nanoconfined BPEs throughout all stages of a reaction. Specifically, we demonstrate, both experimentally and through numerical modeling, that the removal of an electric field produces solution-phase charge imbalances in the vicinity of the BPE poles. These imbalances induce intense and short-lived nonequilibrium electric fields that drive the rapid transport of ions toward specific BPE locations. To determine the origin of these electrokinetic effects, we monitored the movement and fluorescent behavior (enhancement or quenching) of charged fluorophores within well-defined nanofluidic architectures via real-time optical detection. By systematically varying the nature of the fluorophore, the concentration of the electrolyte, the strength of the applied field, and oxide growth on the BPE surface, we dissect the ion transport events that occur in the aftermath of field-induced polarization. The results contained in this work provide new insights into transient bipolar electrokinetics that improve our understanding of current analytical platforms and can drive the development of new micro- and nanoelectrochemical systems.

Original languageEnglish
Pages (from-to)13777-13786
Number of pages10
JournalACS Applied Materials and Interfaces
Volume11
Issue number14
DOIs
Publication statusPublished - 18 Mar 2019

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Fluorescence
Electrodes
Fluorophores
Electric fields
Poles
Ions
Nanofluidics
Oxides
Electrolytes
Quenching
Physics
Polarization

Keywords

  • UT-Hybrid-D
  • electric double layer
  • electrochemistry
  • electrokinetics
  • fluorescence
  • nanoconfinement
  • water electrolysis
  • bipolar electrode

Cite this

Scida, K., Eden, A., Arroyo-Currás, N., Mackenzie, S., Satik, Y., Meinhart, C. D., ... Pennathur, S. (2019). Fluorescence-Based Observation of Transient Electrochemical and Electrokinetic Effects at Nanoconfined Bipolar Electrodes. ACS Applied Materials and Interfaces, 11(14), 13777-13786. https://doi.org/10.1021/acsami.9b01339
Scida, Karen ; Eden, Alexander ; Arroyo-Currás, Netzahualcóyotl ; Mackenzie, Sean ; Satik, Yesil ; Meinhart, Carl D. ; Eijkel, Jan C.T. ; Pennathur, Sumita. / Fluorescence-Based Observation of Transient Electrochemical and Electrokinetic Effects at Nanoconfined Bipolar Electrodes. In: ACS Applied Materials and Interfaces. 2019 ; Vol. 11, No. 14. pp. 13777-13786.
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abstract = "Bipolar electrodes (BPEs) are conductors that, when exposed to an electric field, polarize and promote the accumulation of counterionic charge near their poles. The rich physics of electrokinetic behavior near BPEs has not yet been rigorously studied, with our current understanding of such bipolar effects being restricted to steady-state conditions (under constant applied fields). Here, we reveal the dynamic electrokinetic and electrochemical phenomena that occur near nanoconfined BPEs throughout all stages of a reaction. Specifically, we demonstrate, both experimentally and through numerical modeling, that the removal of an electric field produces solution-phase charge imbalances in the vicinity of the BPE poles. These imbalances induce intense and short-lived nonequilibrium electric fields that drive the rapid transport of ions toward specific BPE locations. To determine the origin of these electrokinetic effects, we monitored the movement and fluorescent behavior (enhancement or quenching) of charged fluorophores within well-defined nanofluidic architectures via real-time optical detection. By systematically varying the nature of the fluorophore, the concentration of the electrolyte, the strength of the applied field, and oxide growth on the BPE surface, we dissect the ion transport events that occur in the aftermath of field-induced polarization. The results contained in this work provide new insights into transient bipolar electrokinetics that improve our understanding of current analytical platforms and can drive the development of new micro- and nanoelectrochemical systems.",
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Fluorescence-Based Observation of Transient Electrochemical and Electrokinetic Effects at Nanoconfined Bipolar Electrodes. / Scida, Karen; Eden, Alexander; Arroyo-Currás, Netzahualcóyotl; Mackenzie, Sean; Satik, Yesil; Meinhart, Carl D.; Eijkel, Jan C.T.; Pennathur, Sumita.

In: ACS Applied Materials and Interfaces, Vol. 11, No. 14, 18.03.2019, p. 13777-13786.

Research output: Contribution to journalArticleAcademicpeer-review

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T1 - Fluorescence-Based Observation of Transient Electrochemical and Electrokinetic Effects at Nanoconfined Bipolar Electrodes

AU - Scida, Karen

AU - Eden, Alexander

AU - Arroyo-Currás, Netzahualcóyotl

AU - Mackenzie, Sean

AU - Satik, Yesil

AU - Meinhart, Carl D.

AU - Eijkel, Jan C.T.

AU - Pennathur, Sumita

N1 - ACS deal

PY - 2019/3/18

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N2 - Bipolar electrodes (BPEs) are conductors that, when exposed to an electric field, polarize and promote the accumulation of counterionic charge near their poles. The rich physics of electrokinetic behavior near BPEs has not yet been rigorously studied, with our current understanding of such bipolar effects being restricted to steady-state conditions (under constant applied fields). Here, we reveal the dynamic electrokinetic and electrochemical phenomena that occur near nanoconfined BPEs throughout all stages of a reaction. Specifically, we demonstrate, both experimentally and through numerical modeling, that the removal of an electric field produces solution-phase charge imbalances in the vicinity of the BPE poles. These imbalances induce intense and short-lived nonequilibrium electric fields that drive the rapid transport of ions toward specific BPE locations. To determine the origin of these electrokinetic effects, we monitored the movement and fluorescent behavior (enhancement or quenching) of charged fluorophores within well-defined nanofluidic architectures via real-time optical detection. By systematically varying the nature of the fluorophore, the concentration of the electrolyte, the strength of the applied field, and oxide growth on the BPE surface, we dissect the ion transport events that occur in the aftermath of field-induced polarization. The results contained in this work provide new insights into transient bipolar electrokinetics that improve our understanding of current analytical platforms and can drive the development of new micro- and nanoelectrochemical systems.

AB - Bipolar electrodes (BPEs) are conductors that, when exposed to an electric field, polarize and promote the accumulation of counterionic charge near their poles. The rich physics of electrokinetic behavior near BPEs has not yet been rigorously studied, with our current understanding of such bipolar effects being restricted to steady-state conditions (under constant applied fields). Here, we reveal the dynamic electrokinetic and electrochemical phenomena that occur near nanoconfined BPEs throughout all stages of a reaction. Specifically, we demonstrate, both experimentally and through numerical modeling, that the removal of an electric field produces solution-phase charge imbalances in the vicinity of the BPE poles. These imbalances induce intense and short-lived nonequilibrium electric fields that drive the rapid transport of ions toward specific BPE locations. To determine the origin of these electrokinetic effects, we monitored the movement and fluorescent behavior (enhancement or quenching) of charged fluorophores within well-defined nanofluidic architectures via real-time optical detection. By systematically varying the nature of the fluorophore, the concentration of the electrolyte, the strength of the applied field, and oxide growth on the BPE surface, we dissect the ion transport events that occur in the aftermath of field-induced polarization. The results contained in this work provide new insights into transient bipolar electrokinetics that improve our understanding of current analytical platforms and can drive the development of new micro- and nanoelectrochemical systems.

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KW - electric double layer

KW - electrochemistry

KW - electrokinetics

KW - fluorescence

KW - nanoconfinement

KW - water electrolysis

KW - bipolar electrode

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DO - 10.1021/acsami.9b01339

M3 - Article

C2 - 30880379

AN - SCOPUS:85064201739

VL - 11

SP - 13777

EP - 13786

JO - ACS applied materials & interfaces

JF - ACS applied materials & interfaces

SN - 1944-8244

IS - 14

ER -