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Electrodialytic crystallization to enable zero liquid discharge

Nature Water volume 1, pages 547–554 (2023)Cite this article

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Abstract

The management of hypersaline brines (that is, wastewater of high salinity) is a technical challenge that has received increasing attention due to their growing volume, environmental impacts and increasingly stringent regulations. Here we present electrodialytic crystallization (EDC) as a new process to achieve brine crystallization without evaporation. In an EDC process, the brine stream recirculating between an electrodialysis cell and a crystallizer remains oversaturated via continuous electromigration of ions from the feed stream across the ion exchange membranes. We first used Na2SO4 as the model salt to demonstrate the feasibility of EDC and to perform a systematic investigation of how crystallization kinetics and crystal size distribution depend on current density and crystallization mode. We then elucidated the criterion of crystallizability and showed how it depends on salt species, membrane properties and operating conditions. Lastly, we analysed the energy consumption of an EDC-reverse osmosis treatment train for achieving zero liquid discharge of a Na2SO4 brine. Overall, this study provides a proof of concept for EDC as an electric-field driven and non-evaporative crystallization process, and lays the foundation for its future technical development and optimization.

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Fig. 1: The concept of EDC.
Fig. 2: Proof of concept for EDC with experiments of Na2SO4 crystallization.
Fig. 3: The variation of crystal size produced by EDC under different current densities.
Fig. 4: Crystallization of different salts in EDC.
Fig. 5: Energy consumption analysis of EDC and EDC-RO system for ZLD.

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Source data are provided with this paper.

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No code is used in the current study.

References

  1. Tong, T. Z. & Elimelech, M. The global rise of zero liquid discharge for wastewater management: drivers, technologies, and future directions. Environ. Sci. Technol. 50, 6846–6855 (2016).

    Article  CAS  PubMed  Google Scholar 

  2. Shah, K. M. et al. Drivers, challenges, and emerging technologies for desalination of high-salinity brines: a critical review. Desalination 538, 115827 (2022).

    Article  CAS  Google Scholar 

  3. Karanikola, V., Boo, C., Rolf, J. & Elimelech, M. Engineered slippery surface to mitigate gypsum scaling in membrane distillation for treatment of hypersaline industrial wastewaters. Environ. Sci. Technol. 52, 14362–14370 (2018).

    Article  CAS  PubMed  Google Scholar 

  4. Tian, W. D., Wang, X., Fan, C. Y. & Cui, Z. Optimal treatment of hypersaline industrial wastewater via bipolar membrane electrodialysis. ACS Sustain. Chem. Eng. 7, 12358–12368 (2019).

    CAS  Google Scholar 

  5. Chang, H. Q. et al. Potential and implemented membrane-based technologies for the treatment and reuse of flowback and produced water from shale gas and oil plays: a review. Desalination 455, 34–57 (2019).

    Article  CAS  Google Scholar 

  6. Tong, T. Z., Carlson, K. H., Robbins, C. A., Zhang, Z. Y. & Du, X. W. Membrane-based treatment of shale oil and gas wastewater: the current state of knowledge. Front. Environ. Sci. Eng. 13, 63 (2019).

    Article  Google Scholar 

  7. Shemer, H. & Semiat, R. Sustainable RO desalination—energy demand and environmental impact. Desalination 424, 10–16 (2017).

    Article  CAS  Google Scholar 

  8. Ellsworth, W. L. Injection-induced earthquakes. Science 341, 1225942 (2013).

    Article  PubMed  Google Scholar 

  9. Scanlon, B. R., Weingarten, M. B., Murray, K. E. & Reedy, R. C. Managing basin-scale fluid budgets to reduce injection-induced seismicity from the recent U.S. shale oil revolution. Seismol. Res. Lett. 90, 171–182 (2018).

    Article  Google Scholar 

  10. Davenport, D. M., Deshmukh, A., Werber, J. R. & Elimelech, M. High-pressure reverse osmosis for energy-efficient hypersaline brine desalination: current status, design considerations, and research needs. Environ. Sci. Technol. Lett. 5, 467–475 (2018).

    Article  CAS  Google Scholar 

  11. Mauter, M. S. & Fiske, P. S. Desalination for a circular water economy. Energy Environ. Sci. 13, 3180–3184 (2020).

    Article  CAS  Google Scholar 

  12. Wang, R. & Lin, S. Thermodynamics and energy efficiency of zero liquid discharge. ACS ES&T Eng. 2, 1491–1503 (2022).

    Article  CAS  Google Scholar 

  13. Mickley, M. Survey of High-Recovery and Zero Liquid Discharge Technologies for Water Utilities (WateReuse, 2008).

  14. Burbano, A. & Brankhuber, P. Demonstration of Membrane Zero Liquid Discharge for Drinking Water Systems—A Literature Review (The Water Research Foundation, 2014).

  15. McGinnis, R. L., Hancock, N. T., Nowosielski-Slepowron, M. S. & McGurgan, G. D. Pilot demonstration of the NH3/CO2 forward osmosis desalination process on high salinity brines. Desalination 312, 67–74 (2013).

    Article  CAS  Google Scholar 

  16. What is zero liquid discharge & why is it important? Saltworks https://www.saltworkstech.com/articles/what-is-zero-liquid-discharge-why-is-it-important/ (2018).

  17. Xu, T. & Huang, C. Electrodialysis-based separation technologies: a critical review. AlChE J. 54, 3147–3159 (2008).

    Article  CAS  Google Scholar 

  18. Strathmann, H. Electrodialysis, a mature technology with a multitude of new applications. Desalination 264, 268–288 (2010).

    Article  CAS  Google Scholar 

  19. Zhang, X. et al. Near-zero liquid discharge of desulfurization wastewater by electrodialysis-reverse osmosis hybrid system. J. Water Process. Eng. 40, 101962 (2021).

    Article  Google Scholar 

  20. Reig, M. et al. Concentration of NaCl from seawater reverse osmosis brines for the chlor-alkali industry by electrodialysis. Desalination 342, 107–117 (2014).

    Article  CAS  Google Scholar 

  21. Jiang, C., Wang, Y., Zhang, Z. & Xu, T. Electrodialysis of concentrated brine from RO plant to produce coarse salt and freshwater. J. Membr. Sci. 450, 323–330 (2014).

    Article  CAS  Google Scholar 

  22. Lin, S. Energy efficiency of desalination: fundamental insights from intuitive interpretation. Environ. Sci. Technol. 54, 76–84 (2019).

    Article  PubMed  Google Scholar 

  23. Tong, T., Wallace, A. F., Zhao, S. & Wang, Z. Mineral scaling in membrane desalination: mechanisms, mitigation strategies, and feasibility of scaling-resistant membranes. J. Membr. Sci. 579, 52–69 (2019).

    Article  CAS  Google Scholar 

  24. Rolf, J. et al. Inorganic scaling in membrane desalination: models, mechanisms, and characterization methods. Environ. Sci. Technol. 56, 7484–7511 (2022).

    Article  CAS  PubMed  Google Scholar 

  25. Tedesco, M., Hamelers, H. V. M. & Biesheuvel, P. M. Nernst–Planck transport theory for (reverse) electrodialysis: II. Effect of water transport through ion-exchange membranes. J. Membr. Sci. 531, 172–182 (2017).

    Article  CAS  Google Scholar 

  26. Jiang, C., Wang, Q., Li, Y., Wang, Y. & Xu, T. Water electro-transport with hydrated cations in electrodialysis. Desalination 365, 204–212 (2015).

    Article  CAS  Google Scholar 

  27. Porada, S., van Egmond, W. J., Post, J. W., Saakes, M. & Hamelers, H. V. M. Tailoring ion exchange membranes to enable low osmotic water transport and energy efficient electrodialysis. J. Membr. Sci. 552, 22–30 (2018).

    Article  CAS  Google Scholar 

  28. Epsztein, R., Shaulsky, E., Qin, M. & Elimelech, M. Activation behavior for ion permeation in ion-exchange membranes: role of ion dehydration in selective transport. J. Membr. Sci. 580, 316–326 (2019).

    Article  CAS  Google Scholar 

  29. Sun, B., Zhang, M., Huang, S., Wang, J. & Zhang, X. Limiting concentration during batch electrodialysis process for concentrating high salinity solutions: A theoretical and experimental study. Desalination 498, 114793 (2021).

    Article  CAS  Google Scholar 

  30. Kingsbury, R. et al. Influence of water uptake, charge, manning parameter, and contact angle on water and salt transport in commercial ion exchange membranes. Ind. Eng. Chem. Res. 58, 18663–18674 (2019).

    Article  CAS  Google Scholar 

  31. Jones, A. G. Crystallization Process Systems (Elsevier, 2002).

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Acknowledgements

This material is based on the work supported by the National Alliance for Water Innovation (NAWI), funded by the US Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE), Advanced Manufacturing Office, under Funding Opportunity Announcement Number DE-FOA-0001905. The views expressed herein do not necessarily represent the views of the US Department of Energy or the US Government.

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Author notes

  1. These authors contributed equally: Xudong Zhang, Yiqun Yao, Thomas Horseman.

Authors and Affiliations

  1. Department of Civil and Environmental Engineering, Vanderbilt University, Nashville, TN, USA

    Xudong Zhang, Ruoyu Wang, Sizhuo Zhang & Shihong Lin

  2. Department of Civil and Environmental Engineering, Colorado State University, Fort Collins, CO, USA

    Yiqun Yao, Yiming Yin & Tiezheng Tong

  3. Department of Chemical and Biomolecular Engineering, Vanderbilt University, Nashville, TN, USA

    Thomas Horseman & Shihong Lin

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  1. Xudong Zhang
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Contributions

S.L. and T.T. conceived the idea and designed the research. X.Z., Y. Yao. and T.H. carried out the experiment. R.W. performed the energy consumption analysis. All authors participated in the discussion and writing of the paper.

Corresponding authors

Correspondence to Tiezheng Tong or Shihong Lin.

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We are in the process of filing a provisional patent application based on this work.

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Nature Water thanks Mohammed Elhashimi, How Yong Ng and Natasha Wright for their contribution to the peer review of this work.

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Zhang, X., Yao, Y., Horseman, T. et al. Electrodialytic crystallization to enable zero liquid discharge. Nat Water 1, 547–554 (2023). https://doi.org/10.1038/s44221-023-00095-4

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