Selective fluoride removal from groundwater using CNT-CeO2 electrodes in capacitive deionization (CDI)
Name
LIU_CEJ_CDI_Manuscript_revised_clean.pdf
Description
Accepted version
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26.16 MB
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Checksum (MD5)
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Author(s)
Liu, Xun
Rehman, Danyal
Shu, Yufei
Liu, Bei
Wang, Li
Li, Li
Wang, Mengxia
Wang, Kunkun
Han, Qi
Zang, Linlin
Date Issued
February 2024
Journal
Chemical Engineering Journal
Publisher
Elsevier BV
Citation
Liu, Xun, Rehman, Danyal, Shu, Yufei, Liu, Bei, Wang, Li et al. 2024. "Selective fluoride removal from groundwater using CNT-CeO2 electrodes in capacitive deionization (CDI)." Chemical Engineering Journal, 482.
Version
Author's final manuscript
Abstract
Selective capacitive deionization (SCDI) is a promising process for preferentially removing specific ions from waters with complex compositions. The selectivity towards certain species in CDI is most frequently achieved through novel electrode materials with high affinities towards targeted species. In this study, we investigate the selective removal of fluoride ions from groundwater containing concentrated co-existing chloride ions. A carbon nanotube-CeO2 (CNT-CeO2) electrode is employed for the electro-sorption of fluoride ions. Our findings are compelling: when processing a mixed F−/Cl− solution comprising 10 mg/L F− and 100 mg/L Cl−, the CNT-CeO2 electrode is seen to reduce the concentration of F− ions to 1.5 mg/L in just 150 min, amounting to an 85 % F− removal efficiency, while the Cl− removal efficiency remains below 2 %. Importantly, this translates to a F−/Cl− separation factor of up to 4.16 when using the CeO2-based electrodes, which is 40 times higher than that achieved with conventional activated carbon (AC) electrodes. Furthermore, the energy consumption for treating actual groundwater using scaled-up equipment is impressively low at approximately 0.2 kWh/m3. The high affinity of CNT-CeO2 towards fluoride is attributed to the intercalation Faraday capacitance initiated by the reaction between F− with CeO2, as verified by the electrochemical quartz crystal microbalance (EQCM). Moreover, EQCM results show a substantial increase in both mass and current as the potential increased beyond 0.8 V vs Ag/AgCl, implying that the current surge is not a result of water splitting but rather the adsorption of F− onto the CNT-CeO2 electrode. The addition of CNTs substantially increases the conductivity of CeO2 electrodes and restricts the aggregation of CeO2, thereby accelerating ion diffusion and promoting selective adsorption characteristics. Importantly, our electro-driven approach demonstrates excellent adsorption–desorption over 20 cycles. This comprehensive study advances the technological development of selective CDI, while providing new insights for fluoride removal in groundwater.
MIT Department
Massachusetts Institute of Technology. Department of Mechanical Engineering
Massachusetts Institute of Technology. Center for Computational Science and Engineering
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Creative Commons Attribution-Noncommercial-ShareAlike
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DOI of Published Version
https://doi.org/10.1016/j.cej.2024.149097
