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Title: Quasi-Steady-State Polarization Reveals the Interplay of Capacitive and Faradaic Processes in Capacitive Deionization

Abstract

Abstract We employ slow cyclic voltammetry to study the quasi‐steady‐state capacitive deionization (CDI) of aerated 10 mM NaCl from V cell =−0.2 to 2 V. The method allows for the deconvolution of capacitive and faradaic processes, which are significant even at low voltage, in conjunction with pH, conductivity, dissolved oxygen (DO), and electrode potential measurements. The pH at three locations and effluent DO data identify asymmetric electrosorption in the cell configured with pristine activated carbon electrodes, where charge is irreversibly consumed to produce H + /OH instead of reversibly adsorbing Cl /Na + . Implementing a reference electrode resolves ion adsorption as a function of the individual potential at each electrode. Near‐electrode pH probes reveal pH environments that diverge by up to 8 units during cell polarization and allow more accurate calculation of faradaic redox potentials in a flow‐by CDI cell. In the aerated NaCl solution that will be relevant to industrial‐scale water treatment, we find that DO reduction occurs to a greater degree than Na + adsorption at the cathode until DO removal becomes mass transfer limited at <−0.2 V vs. SHE. Two cell architectures – flow‐by and flow‐through – corroborate our findings. Finally, we reconcile all measurements to generatemore » a map displaying how the potential is partitioned amongst the capacitive and faradaic processes occurring during CDI operation over a 2.2 V window.« less

Authors:
 [1];  [1];  [1];  [1];  [1]
  1. Univ. of Kentucky, Lexington, KY (United States)
Publication Date:
Research Org.:
West Virginia Univ., Morgantown, WV (United States)
Sponsoring Org.:
USDOE Office of Policy and International Affairs (PO); USDOE
OSTI Identifier:
1533132
Alternate Identifier(s):
OSTI ID: 1389886
Grant/Contract Number:  
PI0000017
Resource Type:
Accepted Manuscript
Journal Name:
ChemElectroChem
Additional Journal Information:
Journal Volume: 4; Journal Issue: 9; Journal ID: ISSN 2196-0216
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Electrochemistry; oxygen reduction; capacitors; electrodes; capacitive deionization; electrochemical water treatment

Citation Formats

Holubowitch, Nicolas, Omosebi, Ayokunle, Gao, Xin, Landon, James, and Liu, Kunlei. Quasi-Steady-State Polarization Reveals the Interplay of Capacitive and Faradaic Processes in Capacitive Deionization. United States: N. p., 2017. Web. doi:10.1002/celc.201700082.
Holubowitch, Nicolas, Omosebi, Ayokunle, Gao, Xin, Landon, James, & Liu, Kunlei. Quasi-Steady-State Polarization Reveals the Interplay of Capacitive and Faradaic Processes in Capacitive Deionization. United States. https://doi.org/10.1002/celc.201700082
Holubowitch, Nicolas, Omosebi, Ayokunle, Gao, Xin, Landon, James, and Liu, Kunlei. Thu . "Quasi-Steady-State Polarization Reveals the Interplay of Capacitive and Faradaic Processes in Capacitive Deionization". United States. https://doi.org/10.1002/celc.201700082. https://www.osti.gov/servlets/purl/1533132.
@article{osti_1533132,
title = {Quasi-Steady-State Polarization Reveals the Interplay of Capacitive and Faradaic Processes in Capacitive Deionization},
author = {Holubowitch, Nicolas and Omosebi, Ayokunle and Gao, Xin and Landon, James and Liu, Kunlei},
abstractNote = {Abstract We employ slow cyclic voltammetry to study the quasi‐steady‐state capacitive deionization (CDI) of aerated 10 mM NaCl from V cell =−0.2 to 2 V. The method allows for the deconvolution of capacitive and faradaic processes, which are significant even at low voltage, in conjunction with pH, conductivity, dissolved oxygen (DO), and electrode potential measurements. The pH at three locations and effluent DO data identify asymmetric electrosorption in the cell configured with pristine activated carbon electrodes, where charge is irreversibly consumed to produce H + /OH − instead of reversibly adsorbing Cl − /Na + . Implementing a reference electrode resolves ion adsorption as a function of the individual potential at each electrode. Near‐electrode pH probes reveal pH environments that diverge by up to 8 units during cell polarization and allow more accurate calculation of faradaic redox potentials in a flow‐by CDI cell. In the aerated NaCl solution that will be relevant to industrial‐scale water treatment, we find that DO reduction occurs to a greater degree than Na + adsorption at the cathode until DO removal becomes mass transfer limited at <−0.2 V vs. SHE. Two cell architectures – flow‐by and flow‐through – corroborate our findings. Finally, we reconcile all measurements to generate a map displaying how the potential is partitioned amongst the capacitive and faradaic processes occurring during CDI operation over a 2.2 V window.},
doi = {10.1002/celc.201700082},
journal = {ChemElectroChem},
number = 9,
volume = 4,
place = {United States},
year = {Thu May 11 00:00:00 EDT 2017},
month = {Thu May 11 00:00:00 EDT 2017}
}

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