Strong attractions and repulsions mediated by monovalent salts
Abstract
Controlling interactions between proteins and nanoparticles in electrolyte solutions is crucial for advancing biological sciences and biotechnology. The assembly of charged nanoparticles (NPs) and proteins in aqueous solutions can be directed by modifying the salt concentration. High concentrations of monovalent salt can induce the solubilization or crystallization of NPs and proteins. By using a multiscale coarse-grained molecular dynamics approach, we show that, due to ionic correlations in the electrolyte, NPs pairs at high monovalent salt concentrations interact via remarkably strong long-range attractions or repulsions, which can be split into three regimes depending on the surface charge densities of the NPs. NPs with zero-to-low surface charge densities interact via a long-range attraction that is stronger and has a similar range to the depletion attraction induced by polymers with radius of gyrations comparable to the NP diameter. On the other hand, moderately charged NPs with smooth surfaces as well as DNA-functionalized NPs with no possibility of hybridization between them interact via a strong repulsion of range and strength larger than the repulsion predicted by models that neglect ionic correlations, including the Derjaguin–Landau–Vervey–Overbeek (DLVO) model. Interactions between strongly charged NPs (>2 e/nm 2 ), both types smooth and DNA-functionalized NPs, show an attractivemore »
- Authors:
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1402121
- Grant/Contract Number:
- 3J-30081-0056A/3J-30081-0056B
- Resource Type:
- Published Article
- Journal Name:
- Proceedings of the National Academy of Sciences of the United States of America
- Additional Journal Information:
- Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 114 Journal Issue: 45; Journal ID: ISSN 0027-8424
- Publisher:
- Proceedings of the National Academy of Sciences
- Country of Publication:
- United States
- Language:
- English
Citation Formats
Li, Yaohua, Girard, Martin, Shen, Meng, Millan, Jaime Andres, and Olvera de la Cruz, Monica. Strong attractions and repulsions mediated by monovalent salts. United States: N. p., 2017.
Web. https://doi.org/10.1073/pnas.1713168114.
Li, Yaohua, Girard, Martin, Shen, Meng, Millan, Jaime Andres, & Olvera de la Cruz, Monica. Strong attractions and repulsions mediated by monovalent salts. United States. https://doi.org/10.1073/pnas.1713168114
Li, Yaohua, Girard, Martin, Shen, Meng, Millan, Jaime Andres, and Olvera de la Cruz, Monica. Mon .
"Strong attractions and repulsions mediated by monovalent salts". United States. https://doi.org/10.1073/pnas.1713168114.
@article{osti_1402121,
title = {Strong attractions and repulsions mediated by monovalent salts},
author = {Li, Yaohua and Girard, Martin and Shen, Meng and Millan, Jaime Andres and Olvera de la Cruz, Monica},
abstractNote = {Controlling interactions between proteins and nanoparticles in electrolyte solutions is crucial for advancing biological sciences and biotechnology. The assembly of charged nanoparticles (NPs) and proteins in aqueous solutions can be directed by modifying the salt concentration. High concentrations of monovalent salt can induce the solubilization or crystallization of NPs and proteins. By using a multiscale coarse-grained molecular dynamics approach, we show that, due to ionic correlations in the electrolyte, NPs pairs at high monovalent salt concentrations interact via remarkably strong long-range attractions or repulsions, which can be split into three regimes depending on the surface charge densities of the NPs. NPs with zero-to-low surface charge densities interact via a long-range attraction that is stronger and has a similar range to the depletion attraction induced by polymers with radius of gyrations comparable to the NP diameter. On the other hand, moderately charged NPs with smooth surfaces as well as DNA-functionalized NPs with no possibility of hybridization between them interact via a strong repulsion of range and strength larger than the repulsion predicted by models that neglect ionic correlations, including the Derjaguin–Landau–Vervey–Overbeek (DLVO) model. Interactions between strongly charged NPs (>2 e/nm 2 ), both types smooth and DNA-functionalized NPs, show an attractive potential well at intermediate-to-high salt concentrations, which demonstrates that electrolytes can induce aggregation of strongly charged NPs. Our work provides an improved understanding of the role of ionic correlations in NP assembly and design rules to utilize the salting-out process to crystallize NPs.},
doi = {10.1073/pnas.1713168114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 45,
volume = 114,
place = {United States},
year = {2017},
month = {10}
}
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Works referenced in this record:
Ueber die Anwendung des Satzes vom Virial in der kinetischen Theorie der Gase
journal, January 1881
- Lorentz, H. A.
- Annalen der Physik, Vol. 248, Issue 1
Direct observation of crystallization and aggregation in a phase-separating colloid-polymer suspension
journal, July 2001
- de Hoog, E. H. A.; Kegel, W. K.; van Blaaderen, A.
- Physical Review E, Vol. 64, Issue 2
Stability and Aggregation of Metal Oxide Nanoparticles in Natural Aqueous Matrices
journal, March 2010
- Keller, Arturo A.; Wang, Hongtao; Zhou, Dongxu
- Environmental Science & Technology, Vol. 44, Issue 6
General nonequilibrium theory of colloid dynamics
journal, December 2010
- Ramírez-González, Pedro; Medina-Noyola, Magdaleno
- Physical Review E, Vol. 82, Issue 6
Criticality in ionic fluids: Debye-Hückel theory, Bjerrum, and beyond
journal, December 1993
- Fisher, Michael E.; Levin, Yan
- Physical Review Letters, Vol. 71, Issue 23
Attraction between Like-Charged Macroions by Coulomb Depletion
journal, August 1998
- Allahyarov, E.; D'Amico, I.; Löwen, H.
- Physical Review Letters, Vol. 81, Issue 6
Transferability of Coarse Grained Potentials: Implicit Solvent Models for Hydrated Ions
journal, May 2011
- Shen, Jia-Wei; Li, Chunli; van der Vegt, Nico F. A.
- Journal of Chemical Theory and Computation, Vol. 7, Issue 6
Concentration Fluctuations and Capacitive Response in Dense Ionic Solutions
journal, June 2016
- Uralcan, Betul; Aksay, Ilhan A.; Debenedetti, Pablo G.
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 13
Osmotic coefficients of atomistic NaCl (aq) force fields
journal, April 2006
- Hess, Berk; Holm, Christian; van der Vegt, Nico
- The Journal of Chemical Physics, Vol. 124, Issue 16
Theory of the stability of lyophobic colloids
journal, April 1955
- Verwey, E. J. W.; Overbeek, J. Th. G.
- Journal of Colloid Science, Vol. 10, Issue 2
Flexible Linear Polyelectrolytes in Multivalent Salt Solutions: Solubility Conditions
journal, August 2000
- Solis, F. J.; de la Cruz, M. Olvera
- EPJ direct, Vol. 2, Issue 1
Patterns of protein-protein interactions in salt solutions and implications for protein crystallization
journal, September 2007
- Dumetz, André C.; Snellinger-O'Brien, Ann M.; Kaler, Eric W.
- Protein Science, Vol. 16, Issue 9
Electrostatics at the nanoscale
journal, January 2011
- Walker, David A.; Kowalczyk, Bartlomiej; de la Cruz, Monica Olvera
- Nanoscale, Vol. 3, Issue 4
Modeling the Crystallization of Spherical Nucleic Acid Nanoparticle Conjugates with Molecular Dynamics Simulations
journal, April 2012
- Li, Ting I. N. G.; Sknepnek, Rastko; Macfarlane, Robert J.
- Nano Letters, Vol. 12, Issue 5
Ion Specificity and the Theory of Stability of Colloidal Suspensions
journal, April 2011
- dos Santos, Alexandre P.; Levin, Yan
- Physical Review Letters, Vol. 106, Issue 16
Precipitation of DNA by Polyamines: A Polyelectrolyte Behavior
journal, January 1998
- Raspaud, E.; Olvera de la Cruz, M.; Sikorav, J. -L.
- Biophysical Journal, Vol. 74, Issue 1
Revisiting the hydration structure of aqueous Na +
journal, February 2017
- Galib, M.; Baer, M. D.; Skinner, L. B.
- The Journal of Chemical Physics, Vol. 146, Issue 8
Scaling Analysis of the Screening Length in Concentrated Electrolytes
journal, July 2017
- Lee, Alpha A.; Perez-Martinez, Carla S.; Smith, Alexander M.
- Physical Review Letters, Vol. 119, Issue 2
Interaction between particles suspended in solutions of macromolecules
journal, December 1958
- Asakura, Sho; Oosawa, Fumio
- Journal of Polymer Science, Vol. 33, Issue 126
Stable colloids in molten inorganic salts
journal, February 2017
- Zhang, Hao; Dasbiswas, Kinjal; Ludwig, Nicholas B.
- Nature, Vol. 542, Issue 7641
The Electrostatic Screening Length in Concentrated Electrolytes Increases with Concentration
journal, May 2016
- Smith, Alexander M.; Lee, Alpha A.; Perkin, Susan
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 12
Protein-protein and protein-salt interactions in aqueous protein solutions containing concentrated electrolytes
journal, January 1998
- Curtis, R. A.; Prausnitz, J. M.; Blanch, H. W.
- Biotechnology and Bioengineering, Vol. 57, Issue 1
Fluids of Clusters in Attractive Colloids
journal, January 2006
- Lu, Peter J.; Conrad, Jacinta C.; Wyss, Hans M.
- Physical Review Letters, Vol. 96, Issue 2
Empirical potential Monte Carlo simulation of fluid structure
journal, January 1996
- Soper, A. K.
- Chemical Physics, Vol. 202, Issue 2-3
Precipitation of highly charged polyelectrolyte solutions in the presence of multivalent salts
journal, October 1995
- de la Cruz, M. Olvera; Belloni, L.; Delsanti, M.
- The Journal of Chemical Physics, Vol. 103, Issue 13
Phase diagram of dilute polyelectrolytes: Collapse and redissolution by association of counterions and co-ions
journal, November 2002
- Solis, Francisco J.
- The Journal of Chemical Physics, Vol. 117, Issue 19
Ionic structure in liquids confined by dielectric interfaces
journal, November 2015
- Jing, Yufei; Jadhao, Vikram; Zwanikken, Jos W.
- The Journal of Chemical Physics, Vol. 143, Issue 19
Specific Ion Effects: Why DLVO Theory Fails for Biology and Colloid Systems
journal, October 2001
- Boström, M.; Williams, D. R. M.; Ninham, B. W.
- Physical Review Letters, Vol. 87, Issue 16
A DNA-based method for rationally assembling nanoparticles into macroscopic materials
journal, August 1996
- Mirkin, Chad A.; Letsinger, Robert L.; Mucic, Robert C.
- Nature, Vol. 382, Issue 6592, p. 607-609
Electrolyte-Mediated Assembly of Charged Nanoparticles
journal, April 2016
- Kewalramani, Sumit; Guerrero-García, Guillermo I.; Moreau, Liane M.
- ACS Central Science, Vol. 2, Issue 4
Advanced protein crystallization using water-soluble ionic liquids as crystallization additives
journal, August 2007
- Hekmat, Dariusch; Hebel, Dirk; Joswig, Sebastian
- Biotechnology Letters, Vol. 29, Issue 11
Interfacial Ordering and Accompanying Divergent Capacitance at Ionic Liquid-Metal Interfaces
journal, December 2015
- Limmer, David T.
- Physical Review Letters, Vol. 115, Issue 25
Gelation of particles with short-range attraction
journal, May 2008
- Lu, Peter J.; Zaccarelli, Emanuela; Ciulla, Fabio
- Nature, Vol. 453, Issue 7194
Potential of mean force between identical charged nanoparticles immersed in a size-asymmetric monovalent electrolyte
journal, October 2011
- Guerrero-García, Guillermo Iván; González-Mozuelos, Pedro; de la Cruz, Mónica Olvera
- The Journal of Chemical Physics, Vol. 135, Issue 16
Phase behavior of polyelectrolyte solutions with salt
journal, January 2009
- Lee, Chi-Lun; Muthukumar, Murugappan
- The Journal of Chemical Physics, Vol. 130, Issue 2
Colloidal charge renormalization in suspensions containing multivalent electrolyte
journal, March 2010
- dos Santos, Alexandre P.; Diehl, Alexandre; Levin, Yan
- The Journal of Chemical Physics, Vol. 132, Issue 10
Macroion Attraction Due to Electrostatic Correlation between Screening Counterions. 1. Mobile Surface-Adsorbed Ions and Diffuse Ion Cloud
journal, January 1996
- Rouzina, Ioulia; Bloomfield, Victor A.
- The Journal of Physical Chemistry, Vol. 100, Issue 23
Tunable soft structure in charged fluids confined by dielectric interfaces
journal, March 2013
- Zwanikken, J. W.; Olvera de la Cruz, M.
- Proceedings of the National Academy of Sciences, Vol. 110, Issue 14
Salting-Out and Salting-In of Polyelectrolyte Solutions: A Liquid-State Theory Study
journal, December 2016
- Zhang, Pengfei; Alsaifi, Nayef M.; Wu, Jianzhong
- Macromolecules, Vol. 49, Issue 24
Nonadditivity of nanoparticle interactions
journal, October 2015
- Silvera Batista, C. A.; Larson, R. G.; Kotov, N. A.
- Science, Vol. 350, Issue 6257
Effect of Counterion Size on Short Range Repulsive Forces at High Ionic Strengths
journal, June 1997
- Colic, Miroslav; Franks, George V.; Fisher, Matthew L.
- Langmuir, Vol. 13, Issue 12
Dynamics and Statics of DNA-Programmable Nanoparticle Self-Assembly and Crystallization
journal, May 2011
- Knorowski, C.; Burleigh, S.; Travesset, A.
- Physical Review Letters, Vol. 106, Issue 21
Electrolytes between dielectric charged surfaces: Simulations and theory
journal, May 2015
- dos Santos, Alexandre P.; Levin, Yan
- The Journal of Chemical Physics, Vol. 142, Issue 19
Molecular thermodynamics for salt-induce protein precipitation
journal, September 1995
- Chiew, Y. C.; Kuehner, D.; Blanch, H. W.
- AIChE Journal, Vol. 41, Issue 9
Water structure, dynamics, and vibrational spectroscopy in sodium bromide solutions
journal, October 2009
- Lin, Y. -S.; Auer, B. M.; Skinner, J. L.
- The Journal of Chemical Physics, Vol. 131, Issue 14
DLVO and hydration forces between mica surfaces in Li+, Na+, K+, and Cs+ electrolyte solutions: A correlation of double-layer and hydration forces with surface cation exchange properties
journal, October 1981
- Pashley, R. M.
- Journal of Colloid and Interface Science, Vol. 83, Issue 2
Introduction to protein crystallization
journal, November 2004
- Mcpherson, A.
- Methods, Vol. 34, Issue 3
Dressed ion theory for bulk symmetric electrolytes in the restricted primitive model
journal, January 1995
- Ennis, Jonathan; Kjellander, Roland; Mitchell, D. John
- The Journal of Chemical Physics, Vol. 102, Issue 2
Self-assembly of coarse-grained ionic surfactants accelerated by graphics processing units
journal, January 2012
- LeBard, David N.; Levine, Benjamin G.; Mertmann, Philipp
- Soft Matter, Vol. 8, Issue 8
Cation-induced toroidal condensation of DNA
journal, December 1980
- Widom, Jonathan; Baldwin, Robert L.
- Journal of Molecular Biology, Vol. 144, Issue 4
Molecular multivalent electrolytes: microstructure and screening
lengths
journal, February 2005
- González-Mozuelos, P.; Yeom, M. S.; Olvera de la Cruz, M.
- The European Physical Journal E, Vol. 16, Issue 2
Electrostatic Attraction and Phase Separation in Solutions of Like-Charged Colloidal Particles
journal, November 1999
- Linse, Per; Lobaskin, Vladimir
- Physical Review Letters, Vol. 83, Issue 20
Modeling Multibody Effects in Ionic Solutions with a Concentration Dependent Dielectric Permittivity
journal, April 2006
- Hess, Berk; Holm, Christian; van der Vegt, Nico
- Physical Review Letters, Vol. 96, Issue 14
Large Counterions Boost the Solubility and Renormalized Charge of Suspended Nanoparticles
journal, October 2013
- Guerrero-García, Guillermo Iván; González-Mozuelos, Pedro; Olvera de la Cruz, Monica
- ACS Nano, Vol. 7, Issue 11
Van der Waals Picture of Liquids, Solids, and Phase Transformations
journal, May 1983
- Chandler, D.; Weeks, J. D.; Andersen, H. C.
- Science, Vol. 220, Issue 4599
Charge oscillations in Debye-Hückel theory
journal, September 1997
- Lee, B. P.; Fisher, M. E.
- Europhysics Letters (EPL), Vol. 39, Issue 6