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Title: Helical vortex formation in three-dimensional electrochemical systems with ion-selective membranes

Abstract

The rate of electric-field-driven transport across ion-selective membranes can exceed the limit predicted by Nernst (the limiting current), and encouraging this “overlimiting” phenomenon can improve efficiency in many electrochemical systems. Overlimiting behavior is the result of electroconvectively induced vortex formation near membrane surfaces, a conclusion supported so far by two-dimensional (2D) theory and numerical simulation, as well as experiments. We show that the third dimension plays a critical role in overlimiting behavior. In particular, the vortex pattern in shear flow through wider channels is helical rather than planar, a surprising result first observed in three-dimensional (3D) simulation and then verified experimentally. We present a complete experimental and numerical characterization of a device exhibiting this recently discovered 3D electrokinetic instability, and show that the number of parallel helical vortices is a jump-discontinuous function of width, as is the overlimiting current and overlimiting conductance. In addition, we show that overlimiting occurs at lower fields in wider channels, because the associated helical vortices are more readily triggered than the planar vortices associated with narrow channels (effective 2D systems). These unexpected width dependencies arise in realistic electrochemical desalination systems, and have important ramifications for design optimization.

Authors:
 [1];  [2];  [3];  [3];  [4];  [5]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Lab. of Electronics. Dept. of Electrical Engineering and Computer Science; Singapore-MIT Alliance for Research and Technology (SMART) (Singapore); Hanoi Univ. of Science and Technology (Vietnam). Dept. of Ship Engineering and Fluid Mechanics
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Lab. of Electronics. Dept. of Electrical Engineering and Computer Science; Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Lab. of Electronics. Dept. of Electrical Engineering and Computer Science
  4. Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
  5. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Lab. of Electronics. Dept. of Electrical Engineering and Computer Science. Dept. of Biological Engineering; Singapore-MIT Alliance for Research and Technology (SMART) (Singapore)
Publication Date:
Research Org.:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E); National Research Foundation of Korea (NRF); Ministry of Science, ICT and Future Planning (MSIP) of Korea
OSTI Identifier:
1505718
Alternate Identifier(s):
OSTI ID: 1242614
Grant/Contract Number:  
AR0000294; 2012R1A2A2A06047424
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review E
Additional Journal Information:
Journal Volume: 93; Journal Issue: 3; Journal ID: ISSN 2470-0045
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electrochemistry; vortex flows; membrane structures; nonlinear dynamics; polymers & soft matter; fluid dynamics

Citation Formats

Pham, Sang V., Kwon, Hyuckjin, Kim, Bumjoo, White, Jacob K., Lim, Geunbae, and Han, Jongyoon. Helical vortex formation in three-dimensional electrochemical systems with ion-selective membranes. United States: N. p., 2016. Web. doi:10.1103/physreve.93.033114.
Pham, Sang V., Kwon, Hyuckjin, Kim, Bumjoo, White, Jacob K., Lim, Geunbae, & Han, Jongyoon. Helical vortex formation in three-dimensional electrochemical systems with ion-selective membranes. United States. doi:10.1103/physreve.93.033114.
Pham, Sang V., Kwon, Hyuckjin, Kim, Bumjoo, White, Jacob K., Lim, Geunbae, and Han, Jongyoon. Mon . "Helical vortex formation in three-dimensional electrochemical systems with ion-selective membranes". United States. doi:10.1103/physreve.93.033114. https://www.osti.gov/servlets/purl/1505718.
@article{osti_1505718,
title = {Helical vortex formation in three-dimensional electrochemical systems with ion-selective membranes},
author = {Pham, Sang V. and Kwon, Hyuckjin and Kim, Bumjoo and White, Jacob K. and Lim, Geunbae and Han, Jongyoon},
abstractNote = {The rate of electric-field-driven transport across ion-selective membranes can exceed the limit predicted by Nernst (the limiting current), and encouraging this “overlimiting” phenomenon can improve efficiency in many electrochemical systems. Overlimiting behavior is the result of electroconvectively induced vortex formation near membrane surfaces, a conclusion supported so far by two-dimensional (2D) theory and numerical simulation, as well as experiments. We show that the third dimension plays a critical role in overlimiting behavior. In particular, the vortex pattern in shear flow through wider channels is helical rather than planar, a surprising result first observed in three-dimensional (3D) simulation and then verified experimentally. We present a complete experimental and numerical characterization of a device exhibiting this recently discovered 3D electrokinetic instability, and show that the number of parallel helical vortices is a jump-discontinuous function of width, as is the overlimiting current and overlimiting conductance. In addition, we show that overlimiting occurs at lower fields in wider channels, because the associated helical vortices are more readily triggered than the planar vortices associated with narrow channels (effective 2D systems). These unexpected width dependencies arise in realistic electrochemical desalination systems, and have important ramifications for design optimization.},
doi = {10.1103/physreve.93.033114},
journal = {Physical Review E},
number = 3,
volume = 93,
place = {United States},
year = {2016},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
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Citation Metrics:
Cited by: 5 works
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Figures / Tables:

FIG. 1 FIG. 1: (a) Schematic of ICP-desalination system including a microchannel with two CEMs located on top and bottom, and insulating sidewalls; electric field is introduced between the CEMs. (b) Design of ICP-desalination device used in the experiment.

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    Works referencing / citing this record:

    Influence of Rayleigh-Bénard convection on electrokinetic instability in overlimiting current conditions
    journal, March 2017


      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.