Ion correlations drive charge overscreening and heterogeneous nucleation at solid–aqueous electrolyte interfaces

Lee, Sang Soo; Koishi, Ayumi; Bourg, Ian C.; Fenter, Paul

doi:10.1073/pnas.2105154118

Title: Ion correlations drive charge overscreening and heterogeneous nucleation at solid–aqueous electrolyte interfaces

Journal Article · 04 August 2021 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.2105154118 · OSTI ID:1812112

^[1];

^[2];

^[1]

Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL 60439,
Department of Civil and Environmental Engineering, Princeton University, Princeton, NJ 08544,, High Meadows Environmental Institute, Princeton University, Princeton, NJ 08544

Significance Ion distributions at charged solid–water interfaces, referred to as the electrical double layer (EDL), are poorly understood at high ion concentrations, in part due to the lack of molecular-scale descriptions of the interactions between adsorbed hydrated ions. Here, direct visualization of the salinity-dependent evolution of EDL structure reveals molecular origins of nonclassical transformation of the EDL, in which charge overscreening and heterogeneous nucleation are driven by ion–ion correlations at the interfaces. This manifestation of the atomistic basis of nonclassical behaviors provides a much-needed understanding of the impact of ion cooperativity at charged interfaces for the development of predictive models for element transport in natural environments and advanced technologies for material growth and synthesis in saline environments.

View Journal Article

Cite

Export

Save

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Princeton Univ., NJ (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; SC0018419

OSTI ID:: 1812112

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 32 Vol. 118; ISSN 0027-8424

Publisher:: Proceedings of the National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

References (47)

DNA condensation by multivalent cations Bloomfield, Victor A. Biopolymers, Vol. 44, Issue 3 https://doi.org/10.1002/(SICI)1097-0282(1997)44:3<269::AID-BIP6>3.0.CO;2-T	journal	January 1997
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Adsorption of hydrolyzable metal ions at the oxide—water interface. III. A thermodynamic model of adsorption James, Robert O.; Healy, Thomas W. Journal of Colloid and Interface Science, Vol. 40, Issue 1 https://doi.org/10.1016/0021-9797(72)90174-9	journal	July 1972
Numerical integration of the cartesian equations of motion of a system with constraints: molecular dynamics of n-alkanes Ryckaert, Jean-Paul; Ciccotti, Giovanni; Berendsen, Herman J. C. Journal of Computational Physics, Vol. 23, Issue 3 https://doi.org/10.1016/0021-9991(77)90098-5	journal	March 1977
DNA binding to mica correlates with cationic radius: assay by atomic force microscopy Hansma, H. G.; Laney, D. E. Biophysical Journal, Vol. 70, Issue 4 https://doi.org/10.1016/S0006-3495(96)79757-6	journal	April 1996
Interpretation and prediction of triple-layer model capacitances and the structure of the oxide-electrolyte-water interface Sverjensky, Dimitri A. Geochimica et Cosmochimica Acta, Vol. 65, Issue 21 https://doi.org/10.1016/S0016-7037(01)00709-8	journal	November 2001
Cation sorption on the muscovite (001) surface in chloride solutions using high-resolution X-ray reflectivity Schlegel, Michel L.; Nagy, Kathryn. L.; Fenter, Paul Geochimica et Cosmochimica Acta, Vol. 70, Issue 14 https://doi.org/10.1016/j.gca.2006.04.011	journal	July 2006
Changes in adsorption free energy and speciation during competitive adsorption between monovalent cations at the muscovite (001)-water interface Lee, Sang Soo; Fenter, Paul; Nagy, Kathryn L. Geochimica et Cosmochimica Acta, Vol. 123 https://doi.org/10.1016/j.gca.2013.07.033	journal	December 2013
van der Waals heteroepitaxy on muscovite Yen, Min; Bitla, Yugandhar; Chu, Ying-Hao Materials Chemistry and Physics, Vol. 234 https://doi.org/10.1016/j.matchemphys.2019.05.053	journal	August 2019
Stern Layer Structure and Energetics at Mica–Water Interfaces Bourg, Ian C.; Lee, Sang Soo; Fenter, Paul The Journal of Physical Chemistry C, Vol. 121, Issue 17 https://doi.org/10.1021/acs.jpcc.7b01828	journal	April 2017
Effect of pH on the Formation of Gibbsite-Layer Films at the Muscovite (001)–Water Interface Lee, Sang Soo; Schmidt, Moritz; Sturchio, Neil C. The Journal of Physical Chemistry C, Vol. 123, Issue 11 https://doi.org/10.1021/acs.jpcc.8b12122	journal	February 2019
Concentration-Dependent Adsorption of CsI at the Muscovite–Electrolyte Interface Brugman, Sander J. T.; Townsend, Eleanor R.; Smets, Mireille M. H. Langmuir, Vol. 34, Issue 13 https://doi.org/10.1021/acs.langmuir.8b00038	journal	March 2018
Formation of a Solid Electrolyte Interphase in Hydrate-Melt Electrolytes Ko, Seongjae; Yamada, Yuki; Yamada, Atsuo ACS Applied Materials & Interfaces, Vol. 11, Issue 49 https://doi.org/10.1021/acsami.9b13662	journal	November 2019
The missing term in effective pair potentials Berendsen, H. J. C.; Grigera, J. R.; Straatsma, T. P. The Journal of Physical Chemistry, Vol. 91, Issue 24 https://doi.org/10.1021/j100308a038	journal	November 1987
Mechanism and Thermodynamics of Ion Selectivity in Aqueous Solutions of 18-Crown-6 Ether: A Molecular Dynamics Study Dang, Liem X. Journal of the American Chemical Society, Vol. 117, Issue 26 https://doi.org/10.1021/ja00131a018	journal	July 1995
Density, viscosity, and electrolytic conductivity of concentrated aqueous electrolyte solutions at several temperatures. Alkaline-earth chlorides, lanthanum chloride, sodium chloride, sodium nitrate, sodium bromide, potassium nitrate, potassium bromide, and cadmium nitrate Isono, Toshiaki Journal of Chemical & Engineering Data, Vol. 29, Issue 1 https://doi.org/10.1021/je00035a016	journal	January 1984
Temperature Dependence of the Density of Aqueous Alkali Halide Salt Solutions by Experiment and Molecular Simulation Reiser, Steffen; Horsch, Martin; Hasse, Hans Journal of Chemical & Engineering Data, Vol. 59, Issue 11 https://doi.org/10.1021/je500420g	journal	August 2014
Molecular Models of Hydroxide, Oxyhydroxide, and Clay Phases and the Development of a General Force Field Cygan, Randall T.; Liang, Jian-Jie; Kalinichev, Andrey G. The Journal of Physical Chemistry B, Vol. 108, Issue 4 https://doi.org/10.1021/jp0363287	journal	January 2004
The Electric Double Layer Has a Life of Its Own Merlet, Céline; Limmer, David T.; Salanne, Mathieu The Journal of Physical Chemistry C, Vol. 118, Issue 32 https://doi.org/10.1021/jp503224w	journal	June 2014
Determination of Alkali and Halide Monovalent Ion Parameters for Use in Explicitly Solvated Biomolecular Simulations Joung, In Suk; Cheatham, Thomas E. The Journal of Physical Chemistry B, Vol. 112, Issue 30 https://doi.org/10.1021/jp8001614	journal	July 2008
Monovalent Ion Adsorption at the Muscovite (001)–Solution Interface: Relationships among Ion Coverage and Speciation, Interfacial Water Structure, and Substrate Relaxation Lee, Sang Soo; Fenter, Paul; Nagy, Kathryn L. Langmuir, Vol. 28, Issue 23 https://doi.org/10.1021/la300032h	journal	May 2012
Thermodynamics, Interfacial Structure, and pH Hysteresis of Rb ⁺ and Sr ²⁺ Adsorption at the Muscovite (001)−Solution Interface Park, Changyong; Fenter, Paul A.; Sturchio, Neil C. Langmuir, Vol. 24, Issue 24 https://doi.org/10.1021/la802446m	journal	December 2008
Assembly of thin films by means of successive deposition of alternate layers of DNA and poly(allylamine) Lvov, Yu.; Decher, G.; Sukhorukov, G. Macromolecules, Vol. 26, Issue 20 https://doi.org/10.1021/ma00072a016	journal	September 1993
Nanoscale Perturbations of Room Temperature Ionic Liquid Structure at Charged and Uncharged Interfaces Zhou, Hua; Rouha, Michael; Feng, Guang ACS Nano, Vol. 6, Issue 11 https://doi.org/10.1021/nn303355b	journal	October 2012
Superconcentrated electrolytes for a high-voltage lithium-ion battery Wang, Jianhui; Yamada, Yuki; Sodeyama, Keitaro Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms12032	journal	June 2016
Real-time observation of cation exchange kinetics and dynamics at the muscovite-water interface Lee, Sang Soo; Fenter, Paul; Nagy, Kathryn L. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15826	journal	June 2017
Highly confined ions store charge more efficiently in supercapacitors Merlet, C.; Péan, C.; Rotenberg, B. Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3701	journal	October 2013
Water-induced correlation between single ions imaged at the solid–liquid interface Ricci, Maria; Spijker, Peter; Voïtchovsky, Kislon Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5400	journal	July 2014
Face-selective electrostatic control of hydrothermal zinc oxide nanowire synthesis Joo, Jaebum; Chow, Brian Y.; Prakash, Manu Nature Materials, Vol. 10, Issue 8 https://doi.org/10.1038/nmat3069	journal	July 2011
Electrostatic control of block copolymer morphology Sing, Charles E.; Zwanikken, Jos W.; Olvera de la Cruz, Monica Nature Materials, Vol. 13, Issue 7 https://doi.org/10.1038/nmat4001	journal	June 2014
Charge inversion accompanies DNA condensation by multivalent ions Besteman, K.; Van Eijk, K.; Lemay, S. G. Nature Physics, Vol. 3, Issue 9 https://doi.org/10.1038/nphys697	journal	August 2007
Electrostatics at the nanoscale Walker, David A.; Kowalczyk, Bartlomiej; de la Cruz, Monica Olvera Nanoscale, Vol. 3, Issue 4 https://doi.org/10.1039/C0NR00698J	journal	January 2011
Photoelectron spectra of the hydrated iodine anion from molecular dynamics simulations Dang, Liem X.; Garrett, Bruce C. The Journal of Chemical Physics, Vol. 99, Issue 4 https://doi.org/10.1063/1.465203	journal	August 1993
Tuning ion correlations at an electrified soft interface Laanait, N.; Mihaylov, M.; Hou, B. Proceedings of the National Academy of Sciences, Vol. 109, Issue 50 https://doi.org/10.1073/pnas.1214204109	journal	November 2012
Electrostatic correlations: from plasma to biology Levin, Yan Reports on Progress in Physics, Vol. 65, Issue 11 https://doi.org/10.1088/0034-4885/65/11/201	journal	September 2002
Heteroepitaxial growth in aqueous solutions: Rubidium iodide on mica Lamelas, F. J.; Schmidt, J. D.; Xiong, May Physical Review B, Vol. 58, Issue 21 https://doi.org/10.1103/PhysRevB.58.14270	journal	December 1998
Screening of a macroion by multivalent ions: Correlation-induced inversion of charge Shklovskii, B. I. Physical Review E, Vol. 60, Issue 5 https://doi.org/10.1103/PhysRevE.60.5802	journal	November 1999
Double Layer in Ionic Liquids: Overscreening versus Crowding Bazant, Martin Z.; Storey, Brian D.; Kornyshev, Alexei A. Physical Review Letters, Vol. 106, Issue 4 https://doi.org/10.1103/PhysRevLett.106.046102	journal	January 2011
Scaling Analysis of the Screening Length in Concentrated Electrolytes Lee, Alpha A.; Perez-Martinez, Carla S.; Smith, Alexander M. Physical Review Letters, Vol. 119, Issue 2 https://doi.org/10.1103/PhysRevLett.119.026002	journal	July 2017
Interfacial Layering in the Electric Double Layer of Ionic Liquids de Souza, J. Pedro; Goodwin, Zachary A. H.; McEldrew, Michael Physical Review Letters, Vol. 125, Issue 11 https://doi.org/10.1103/PhysRevLett.125.116001	journal	September 2020
Hydration and Distribution of Ions at the Mica-Water Interface Park, Changyong; Fenter, Paul A.; Nagy, Kathryn L. Physical Review Letters, Vol. 97, Issue 1 https://doi.org/10.1103/PhysRevLett.97.016101	journal	July 2006
Phasing of resonant anomalous X-ray reflectivity spectra and direct Fourier synthesis of element-specific partial structures at buried interfaces Park, Changyong; Fenter, Paul A. Journal of Applied Crystallography, Vol. 40, Issue 2 https://doi.org/10.1107/S0021889806053131	journal	March 2007
Optimizing a flow-through X-ray transmission cell for studies of temporal and spatial variations of ion distributions at mineral–water interfaces Lee, Sang Soo; Fenter, Paul; Park, Changyong Journal of Synchrotron Radiation, Vol. 20, Issue 1 https://doi.org/10.1107/S0909049512041568	journal	November 2012
Molecular Layering of Fluorinated Ionic Liquids at a Charged Sapphire (0001) Surface Mezger, M.; Schroder, H.; Reichert, H. Science, Vol. 322, Issue 5900 https://doi.org/10.1126/science.1164502	journal	October 2008
Biomimetic Pathways for Assembling Inorganic Thin Films Aksay, I. A.; Trau, M.; Manne, S. Science, Vol. 273, Issue 5277 https://doi.org/10.1126/science.273.5277.892	journal	August 1996
Crystallization by particle attachment in synthetic, biogenic, and geologic environments De Yoreo, J. J.; Gilbert, P. U. P. A.; Sommerdijk, N. A. J. M. Science, Vol. 349, Issue 6247 https://doi.org/10.1126/science.aaa6760	journal	July 2015
Powder neutron diffraction study of 2M1 muscovite at room pressure and at 2 GPa [Powder neutron diffraction study of 2M1 muscovite at room pressure and at 2 GPa] Catti, Michele; Ferraris, Giovanni; Hull, Steve European Journal of Mineralogy, Vol. 6, Issue 2 https://doi.org/10.1127/ejm/6/2/0171	journal	March 1994

Similar Records

Molecular-Scale Structure of Electrode–Electrolyte Interfaces: The Case of Platinum in Aqueous Sulfuric Acid

Journal Article · 2018 · Journal of the American Chemical Society · OSTI ID:1543727

Wu, Cheng Hao; Pascal, Tod A.; Baskin, Artem; +7 more

Molecular-Scale Structure of Electrode–Electrolyte Interfaces: The Case of Platinum in Aqueous Sulfuric Acid

Journal Article · 2018 · Journal of the American Chemical Society · OSTI ID:1604655

Wu, Cheng Hao; Pascal, Tod A.; Baskin, Artem; +7 more

Direct Experimental Observations of Ion Distributions during Overcharging at the Muscovite–Water Interface by Adsorption of Rb⁺ and Halides (Cl^–, Br^–, I^–) at High Salinity

Journal Article · 2023 · ChemPhysChem · OSTI ID:2368837

Neumann, Julia; Lee, Sang Soo; Zhao, Eric J.; +1 more

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
54 ENVIRONMENTAL SCIENCES
58 GEOSCIENCES
77 NANOSCIENCE AND NANOTECHNOLOGY
EDL
X-ray reflectivity
adsorption
electrical double layer
ion cooperativity
ion-ion correlation
molecular dynamics
molecular dynamics simulation
muscovite mica
salinity
x-ray reflectivity

Title: Ion correlations drive charge overscreening and heterogeneous nucleation at solid–aqueous electrolyte interfaces

Citation Formats

References (47)

Similar Records

Related Subjects