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Title: Electrostatics of Nanoparticle–Wall Interactions within Nanochannels: Role of Double-Layer Structure and Ion–Ion Correlations

Abstract

We perform computational investigations of the electrolyte-mediated interactions of charged nanoparticles with the walls of nanochannels. We investigate the role of discrete ion effects, valence, and electrolyte strength on nanoparticle- wall interactions. We find for some of the multivalent charge regimes that the like-charged nanoparticles and walls can have attractive interactions. We study in detail these interactions and the free-energy profile for the nanoparticle-wall separation. We find there are energy barriers and energy minima giving preferred nanoparticle locations in the channel near the center and at a distance near to but separated from the channel walls. We characterize contributions from surface overcharging, condensed layers, and overlap of ion double layers. We perform our investigations using coarse-grained particle-level simulations with Brownian dynamics, classical density functional theory, and the mean-field Poisson-Boltzmann theory. We discuss the implications of our results for phenomena in nanoscale devices.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Department of Mathematics and Department of Mechanical Engineering, University of California at Santa Barbara, Santa Barbara, California 93106, United States
  2. Center for Integrated Nanotechnologies, Sandia National Laboratories, Albuquerque, New Mexico 87185, United States
Publication Date:
Research Org.:
Univ. of California, Santa Barbara, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR)
OSTI Identifier:
1471273
Alternate Identifier(s):
OSTI ID: 1508631
Grant/Contract Number:  
SC0009254; NA0003525; DMS-0956210; DMS-1616353
Resource Type:
Published Article
Journal Name:
ACS Omega
Additional Journal Information:
Journal Name: ACS Omega Journal Volume: 3 Journal Issue: 9; Journal ID: ISSN 2470-1343
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 42 ENGINEERING; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 97 MATHEMATICS AND COMPUTING

Citation Formats

Sidhu, Inderbir S., Frischknecht, Amalie L., and Atzberger, Paul J. Electrostatics of Nanoparticle–Wall Interactions within Nanochannels: Role of Double-Layer Structure and Ion–Ion Correlations. United States: N. p., 2018. Web. doi:10.1021/acsomega.8b01393.
Sidhu, Inderbir S., Frischknecht, Amalie L., & Atzberger, Paul J. Electrostatics of Nanoparticle–Wall Interactions within Nanochannels: Role of Double-Layer Structure and Ion–Ion Correlations. United States. https://doi.org/10.1021/acsomega.8b01393
Sidhu, Inderbir S., Frischknecht, Amalie L., and Atzberger, Paul J. Tue . "Electrostatics of Nanoparticle–Wall Interactions within Nanochannels: Role of Double-Layer Structure and Ion–Ion Correlations". United States. https://doi.org/10.1021/acsomega.8b01393.
@article{osti_1471273,
title = {Electrostatics of Nanoparticle–Wall Interactions within Nanochannels: Role of Double-Layer Structure and Ion–Ion Correlations},
author = {Sidhu, Inderbir S. and Frischknecht, Amalie L. and Atzberger, Paul J.},
abstractNote = {We perform computational investigations of the electrolyte-mediated interactions of charged nanoparticles with the walls of nanochannels. We investigate the role of discrete ion effects, valence, and electrolyte strength on nanoparticle- wall interactions. We find for some of the multivalent charge regimes that the like-charged nanoparticles and walls can have attractive interactions. We study in detail these interactions and the free-energy profile for the nanoparticle-wall separation. We find there are energy barriers and energy minima giving preferred nanoparticle locations in the channel near the center and at a distance near to but separated from the channel walls. We characterize contributions from surface overcharging, condensed layers, and overlap of ion double layers. We perform our investigations using coarse-grained particle-level simulations with Brownian dynamics, classical density functional theory, and the mean-field Poisson-Boltzmann theory. We discuss the implications of our results for phenomena in nanoscale devices.},
doi = {10.1021/acsomega.8b01393},
journal = {ACS Omega},
number = 9,
volume = 3,
place = {United States},
year = {2018},
month = {9}
}

Journal Article:
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https://doi.org/10.1021/acsomega.8b01393

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