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Langmuir Article cleaning, or replacement due to the low cost of the porous materials themselves. By combining microfiltration and deionization in one step, shock ED may also enable more compact, portable point-of-use systems. Besides filtration by size, suspended particles are also strongly filtered by charge. Co-ionic particles (with the same charge as the pore walls and the membrane) are repelled by the shock,22 but counterionic particles are accelerated through the depleted region by the large electric field and sent to the outlet if they are blocked by the membrane. Some of these advantages are also possessed by microfluidic desalination devices with aligned flow and current in individual microchannels23 but with higher fabrication costs and smaller flow rates (even with massive parallelization). By decoupling the flow and current directions using porous media, it is possible to extend deionization and filtering cheaply over macroscopic volumes. Selective ion exchange and separation may also be possible by shock ED. In contrast to existing methods for heavy metal removal based on adsorption in nanocrystals,8 functionalized porous media,56,57 and biosorbents,6,7 shock ED is not limited to particular ions and exhibits ion selectivity (based on surface transport in porous media), which could be used to fractionate different metal ions and/or charged macromolecules by splitting streams in cross-flow through the cell. Multivalent/ monovalent ion separation can also be achieved by electro- osmotic convection in nanochannels58 or by the capacitive charging of porous electrodes,59 but shock ED could enable c■ontinuous, scalable separations based on both size and charge. ASSOCIATED CONTENT *S Supporting Information Sweep rate effect for linear sweep voltammetry. Reproducibility of the measured current−voltage curves. Comparison of current−voltage curves with and without a glass frit. Chronoamperometry measurement during the deionization extraction. Impedance measurement for solution conductivity. Measurement of pH , calculation of surface charge density, and pK effect. Surface chemical modifications. This material is available free of charge via the Internet at http://pubs.acs.org. ■ AUTHOR INFORMATION Corresponding Author *E-mail: bazant@mit.edu. Present Addresses §Department of Surgery, Beth Israel Deaconess Medical Center, Harvard Medical School, Boston, Massachusetts 02215, United States, and Wyss Institute of Biologically Inspired Engineering, Harvard University, Boston, Massachu- setts 02215, United States. ∥Department of Mechanical Engineering, Stanford University, Stanford, California 94304, United States. ⊥Blaustein Institutes for Desert Research, Ben-Gurion Uni- versity of the Negev, Sede Boqer Campus, 84990 Israel. Notes The authors declare no competing financial interest. ■ ACKNOWLEDGMENTS This work was supported by a grant from Weatherford International through the MIT Energy Initiative. B.Z. and M.Z.B. also acknowledge support from the USA-Israel Binational Science Foundation (grant 2010199) and J.-H.H. acknowledges support from the Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (2012R1A6A3A03039224). We thank P. Morley and A. Gallant at the MIT Central Machine Shop for producing the prototype. ■ (1) Shannon, M. A.; Bohn, P. W.; Elimelech, M.; Georgiadis, J. G.; Marioas, B. J.; Mayes, A. M. Science and technology for water purification in the coming decades. Nature 2008, 452, 301−310. (2) Humplik, T.; Lee, J.; O’Hern, S. C.; Fellman, B. A.; Baig, M. A.; Hassan, S. F.; Atieh, M. A.; Rahman, F.; Laoui, T.; Karnik, R.; Wang, E. N. Nanostructured materials for water desalination. Nanotechnology 2011, 22, 292001. (3) Greenlee, L. F.; Lawler, D. F.; Freeman, B. D.; Marrot, B.; Moulin, P. Reverse osmosis desalination: water sources, technology, and today’s challenges. Water Res. 2009, 43, 2317−2348. (4) Potts, D. E.; Ahlert, R. C.; Wang, S. S. A critical review of fouling of reverse osmosis membranes. Desalination 1981, 36, 235−264. (5) Schultz, A. Hydraulic Fracturing and Natural Gas Drilling: Questions and Concerns; Nova Science Publishers: New York, 2011. (6) Volesky, B.; Holant, Z. R. Biosorption of heavy metals. Biotechnol. Prog. 1995, 11, 235−250. (7) Wan Ngah, W. S.; Hanafiah, M. A. Removal of heavy metal ions from wastewater by chemically modified plant wastes as adsorbents: a review. Bioresour. Technol. 2008, 99, 3935−3948. (8) Yavuz, C. T.; Mayo, J. T.; Yu, W. W.; Prakash, A.; Falkner, J. C.; Yean, S.; Cong, L.; Shipley, H. J.; Kan, A.; Tomson, M.; Natelson, D.; Colvin, V. L. Low-field magnetic separation of monodisperse Fe3O4 nanocrystals. Science 2006, 314, 964−967. (9) Probstein, R. Physicochemical Hydrodynamics, 2nd ed.; John Wiley & Sons: New York, 1994. (10) Nikonenko, V.; Pismenskaya, N.; Belova, E.; Sistat, P.; Huguet, P.; Pourcelly, G.; Larchet, C. Intensive current transfer in membrane systems: Modeling, mechanisms and application in electrodialysis. Adv. Colloid Interface Sci. 2010, 160, 101−123. (11) Porada, S.; Zhao, R.; van der Wal, A.; Presser, V.; Biesheuvel, P. Review on the science and technology of water desalination by capacitive deionization. Prog. Mater. Sci. 2013, 58, 1388−1442. (12) Dydek, E. V.; Zaltzman, B.; Rubinstein, I.; Deng, D. S.; Mani, A.; Bazant, M. Z. Overlimiting current in a microchannel. Phys. Rev. Lett. 2011, 107, 118301. (13) Rubinstein, I.; Warshawsky, A.; Schechtman, L.; Kedem, O. Elimination of acid-base generation (water-splitting) in electrodialysis. Desalination 1984, 51, 55−60. (14) Andersen, M. B.; van Soestbergen, M.; Mani, A.; Bruus, H.; Biesheuvel, P. M.; Bazant, M. Z. Current induced membrane discharge. Phys. Rev. Lett. 2012, 109, 108301. (15) Rubinstein, I.; Staude, E.; Kedem, O. Role of the membrane surface in concentration polarization at ion-exchange membrane. Desalination 1988, 69, 101−114. (16) Zaltzman, B.; Rubinstein, I. Electro-osmotic slip and electro- convective instability. J. Fluid Mech. 2007, 579, 173−226. (17) Rubinstein, S.; Manukyan, G.; Staicu, A.; Rubinstein, I.; Zaltzman, B.; Lammertink, R.; Mugele, F.; Wessling, M. Direct observation of a nonequilibrium electro-osmotic instability. Phys. Rev. Lett. 2008, 101, 236101. (18) Yossifon, G.; Chang, H.-C. Selection of non-equilibrium over- limiting currents: universal depletion layer formation dynamics and vortex instability. Phys. Rev. Lett. 2008, 101, 254501. (19) Yaroshchuk, A.; Zholkovskiy, E.; Pogodin, S.; Baulin, V. Coupled concentration polarization and electroosmotic circulation near micro/nanointerfaces: Taylor-Aris model of hydrodynamic dispersion and limits of its applicability. Langmuir 2011, 27, 11710− 11721. (20) Kim, S. J.; Wang, Y.; Lee, J. H.; Jang, H.; Han, J. Concentration polarization and nonlinear electrokinetic flow near a nanofluidic channel. Phys. Rev. Lett. 2007, 99, 044501. 16176 dx.doi.org/10.1021/la4040547 | Langmuir 2013, 29, 16167−16177 REFERENCESPDF Image | Overlimiting Current and Shock Electrodialysis in Porous Media
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