Ion selectivity in capacitive deionization with functionalized electrode: Theory and experimental validation

Oyarzun, Diego I.; Hemmatifar, Ali; Palko, James W.; Stadermann, Michael; Santiago, Juan G.

doi:10.1016/j.wroa.2018.100008

Title: Ion selectivity in capacitive deionization with functionalized electrode: Theory and experimental validation

Journal Article · 04 November 2018 · Water Research. X

DOI: https://doi.org/10.1016/j.wroa.2018.100008 · OSTI ID:1512611

Oyarzun, Diego I. ^[1];

^[1]; Palko, James W. ^[2]; Stadermann, Michael ^[3]; Santiago, Juan G. ^[1]

Stanford Univ., CA (United States). Dept. of Mechanical Engineering
Univ. of California, Merced, CA (United States). Dept. of Mechanical Engineering
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Capacitive deionization (CDI) is a promising technique for salt removal and may have potential for highly selective removal of ion species. In this work, we take advantage of functional groups usually used with ionic exchange resins and apply these to CDI. To this end, we functionalize activated carbon with a quaternary amines surfactant and use this surface to selectively and passively (no applied field) trap nitrate ions. We then set the cell voltage to a constant value to regenerate these electrodes, resulting in an inverted capacitive deionization (i-CDI) operation. Unlike resins, we avoid use of concentrated chemicals for regeneration. We measure the selectivity of nitrate versus chloride ions as a function of regeneration voltage and initial chloride concentration. We experimentally demonstrate up to about 6.5-fold (observable) selectivity in a cycle with a regeneration voltage of 0.4 V. We also demonstrate a novel multi-pass, air-flush i-CDI operation to selectively enrich nitrate with high water recovery. We further present a dynamic, multi-species electrosorption and equilibrium solution-to-surface chemical reaction model and validate the model with detailed measurements. Our i-CDI system exhibits higher nitrate selectivity at lower voltages; making it possible to reduce NaNO₃ concentrations from ~170 ppm to below the limit of maximum allowed values for nitrate in drinking water of about 50 ppm NaNO₃.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: CONICYT-BECAS CHILE; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1512611

Report Number(s):: LLNL-JRNL--773303; 965471

Journal Information:: Water Research. X, Journal Name: Water Research. X Journal Issue: C Vol. 1; ISSN 2589-9147

Country of Publication:: United States

Language:: English

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Investigation of fluoride removal from low-salinity groundwater by single-pass constant-voltage capacitive deionization Tang, Wangwang; Kovalsky, Peter; Cao, Baichuan Water Research, Vol. 99 https://doi.org/10.1016/j.watres.2016.04.047	journal	August 2016
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Fluoride Removal from Brackish Groundwaters by Constant Current Capacitive Deionization (CDI) Tang, Wangwang; Kovalsky, Peter; Cao, Baichuan Environmental Science & Technology, Vol. 50, Issue 19 https://doi.org/10.1021/acs.est.6b03307	journal	September 2016
Two-Dimensional Porous Electrode Model for Capacitive Deionization Hemmatifar, Ali; Stadermann, Michael; Santiago, Juan G. The Journal of Physical Chemistry C, Vol. 119, Issue 44 https://doi.org/10.1021/acs.jpcc.5b05847	journal	October 2015
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A comparative study of electrosorption selectivity of ions by activated carbon electrodes in capacitive deionization Hou, Chia-Hung; Huang, Cheng-Ye Desalination, Vol. 314 https://doi.org/10.1016/j.desal.2012.12.029	journal	April 2013
Enhancement of nitrate removal from a solution of mixed nitrate, chloride and sulfate ions using a nitrate-selective carbon electrode Yeo, Jin-Hee; Choi, Jae-Hwan Desalination, Vol. 320 https://doi.org/10.1016/j.desal.2013.04.013	journal	July 2013
A short review on reverse osmosis pretreatment technologies Jamaly, S.; Darwish, N. N.; Ahmed, I. Desalination, Vol. 354 https://doi.org/10.1016/j.desal.2014.09.017	journal	December 2014
On-line method to study dynamics of ion adsorption from mixtures of salts in capacitive deionization Dykstra, J. E.; Dijkstra, J.; van der Wal, A. Desalination, Vol. 390 https://doi.org/10.1016/j.desal.2016.04.001	journal	July 2016
Effects of the hydration ratio on the electrosorption selectivity of ions during capacitive deionization Li, Yingzhen; Zhang, Chang; Jiang, Yanping Desalination, Vol. 399 https://doi.org/10.1016/j.desal.2016.09.011	journal	December 2016
Capacitive deionization with wire-shaped electrodes Mubita, T. M.; Porada, S.; Biesheuvel, P. M. Electrochimica Acta, Vol. 270 https://doi.org/10.1016/j.electacta.2018.03.082	journal	April 2018
Selective lithium recovery from aqueous solution using a modified membrane capacitive deionization system Lee, Dong-Hee; Ryu, Taegong; Shin, Junho Hydrometallurgy, Vol. 173 https://doi.org/10.1016/j.hydromet.2017.09.005	journal	November 2017
Time-dependent ion selectivity in capacitive charging of porous electrodes Zhao, R.; van Soestbergen, M.; Rijnaarts, H. H. M. Journal of Colloid and Interface Science, Vol. 384, Issue 1 https://doi.org/10.1016/j.jcis.2012.06.022	journal	October 2012
Exploring the impact of pore size distribution on the performance of carbon electrodes for capacitive deionization Han, Linchen; Karthikeyan, K. G.; Anderson, Marc A. Journal of Colloid and Interface Science, Vol. 430 https://doi.org/10.1016/j.jcis.2014.05.015	journal	September 2014
Nitrate removal from aqueous solution by Arundo donax L. reed based anion exchange resin Xu, Xing; Gao, Baoyu; Zhao, Yaqing Journal of Hazardous Materials, Vol. 203-204 https://doi.org/10.1016/j.jhazmat.2011.11.094	journal	February 2012
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Selective removal of nitrate ions by controlling the applied current in membrane capacitive deionization (MCDI) Kim, Yu-Jin; Kim, Jin-Hyun; Choi, Jae-Hwan Journal of Membrane Science, Vol. 429 https://doi.org/10.1016/j.memsci.2012.11.064	journal	February 2013
A comprehensive review of hybrid forward osmosis systems: Performance, applications and future prospects Chekli, Laura; Phuntsho, Sherub; Kim, Jung Eun Journal of Membrane Science, Vol. 497 https://doi.org/10.1016/j.memsci.2015.09.041	journal	January 2016
Enhanced both water flux and salt rejection of reverse osmosis membrane through combining isophthaloyl dichloride with biphenyl tetraacyl chloride as organic phase monomer for seawater desalination Zhao, Yali; Zhang, Zhiguang; Dai, Lei Journal of Membrane Science, Vol. 522 https://doi.org/10.1016/j.memsci.2016.09.022	journal	January 2017
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Adsorption and capacitive regeneration of nitrate using inverted capacitive deionization with surfactant functionalized carbon electrodes Oyarzun, Diego I.; Hemmatifar, Ali; Palko, James W. Separation and Purification Technology, Vol. 194 https://doi.org/10.1016/j.seppur.2017.11.027	journal	April 2018
Investigation on removal of hardness ions by capacitive deionization (CDI) for water softening applications Seo, Seok-Jun; Jeon, Hongrae; Lee, Jae Kwang Water Research, Vol. 44, Issue 7 https://doi.org/10.1016/j.watres.2009.10.020	journal	April 2010
Comparison of the removal of hydrophobic trace organic contaminants by forward osmosis and reverse osmosis Xie, Ming; Nghiem, Long D.; Price, William E. Water Research, Vol. 46, Issue 8 https://doi.org/10.1016/j.watres.2012.02.023	journal	May 2012
Selective removal of nitrate ion using a novel composite carbon electrode in capacitive deionization Kim, Yu-Jin; Choi, Jae-Hwan Water Research, Vol. 46, Issue 18 https://doi.org/10.1016/j.watres.2012.08.031	journal	November 2012
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Fluoride and nitrate removal from brackish groundwaters by batch-mode capacitive deionization Tang, Wangwang; Kovalsky, Peter; He, Di Water Research, Vol. 84 https://doi.org/10.1016/j.watres.2015.08.012	journal	November 2015
Investigation of fluoride removal from low-salinity groundwater by single-pass constant-voltage capacitive deionization Tang, Wangwang; Kovalsky, Peter; Cao, Baichuan Water Research, Vol. 99 https://doi.org/10.1016/j.watres.2016.04.047	journal	August 2016
Theory of pH changes in water desalination by capacitive deionization Dykstra, J. E.; Keesman, K. J.; Biesheuvel, P. M. Water Research, Vol. 119 https://doi.org/10.1016/j.watres.2017.04.039	journal	August 2017
Equilibria model for pH variations and ion adsorption in capacitive deionization electrodes Hemmatifar, Ali; Oyarzun, Diego I.; Palko, James W. Water Research, Vol. 122 https://doi.org/10.1016/j.watres.2017.05.036	journal	October 2017
Theory of water treatment by capacitive deionization with redox active porous electrodes He, Fan; Biesheuvel, P. M.; Bazant, Martin Z. Water Research, Vol. 132 https://doi.org/10.1016/j.watres.2017.12.073	journal	April 2018
Enhanced Salt Removal in an Inverted Capacitive Deionization Cell Using Amine Modified Microporous Carbon Cathodes Gao, Xin; Omosebi, Ayokunle; Landon, James Environmental Science & Technology, Vol. 49, Issue 18 https://doi.org/10.1021/acs.est.5b02320	journal	August 2015
Fluoride Removal from Brackish Groundwaters by Constant Current Capacitive Deionization (CDI) Tang, Wangwang; Kovalsky, Peter; Cao, Baichuan Environmental Science & Technology, Vol. 50, Issue 19 https://doi.org/10.1021/acs.est.6b03307	journal	September 2016
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Two-Dimensional Porous Electrode Model for Capacitive Deionization Hemmatifar, Ali; Stadermann, Michael; Santiago, Juan G. The Journal of Physical Chemistry C, Vol. 119, Issue 44 https://doi.org/10.1021/acs.jpcc.5b05847	journal	October 2015
Properties of Strongly Basic Anion Exchange Resins Wheaton, R. M.; Bauman, W. C. Industrial & Engineering Chemistry, Vol. 43, Issue 5 https://doi.org/10.1021/ie50497a027	journal	May 1951
Basic principles of electrolyte chemistry for microfluidic electrokinetics. Part II: Coupling between ion mobility, electrolysis, and acid–base equilibria Persat, Alexandre; Suss, Matthew E.; Santiago, Juan G. Lab on a Chip, Vol. 9, Issue 17 https://doi.org/10.1039/b906468k	journal	January 2009
Hybrid capacitive deionization with anion-exchange membranes for lithium extraction Siekierka, Anna; Bryjak, Marek E3S Web of Conferences, Vol. 22 https://doi.org/10.1051/e3sconf/20172200157	journal	January 2017
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Electrosorption of different cations and anions with membrane capacitive deionization based on carbon nanotube/nanofiber electrodes and ion-exchange membranes Nie, Chunyang; Zhan, Yankun; Pan, Likun Desalination and Water Treatment, Vol. 30, Issue 1-3 https://doi.org/10.5004/dwt.2011.2089	journal	June 2011
The use of activated carbon modified with polypyrrole as a supporting electrode for lithium ions adsorption in capacitive deionization Siekierka, Anna; Bryjak, Marek; Wolska, Joanna DESALINATION AND WATER TREATMENT, Vol. 64 https://doi.org/10.5004/dwt.2017.11387	journal	January 2017
Anion exchange membranes in lithium extraction by means of capacitive deionization system Siekierka, Anna; Wolska, Joanna; Bryjak, Marek DESALINATION AND WATER TREATMENT, Vol. 75 https://doi.org/10.5004/dwt.2017.20431	journal	January 2017

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Theoretical Analysis of Constant Voltage Mode Membrane Capacitive Deionization for Water Softening Zhang, Xin; Reible, Danny Membranes, Vol. 11, Issue 4 https://doi.org/10.3390/membranes11040231	journal	March 2021
Selective ion separation by capacitive deionization (CDI) based technologies: a state-of-the-art review Zhang, Xudong; Zuo, Kuichang; Zhang, Xiaori Environmental Science: Water Research & Technology, Vol. 6, Issue 2 https://doi.org/10.1039/c9ew00835g	journal	January 2020
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