Dynamic and weak electric double layers in ultrathin nanopores

Heiranian, Mohammad; Noh, Yechan; Aluru, Narayana R.

doi:10.1063/5.0048011

Dynamic and weak electric double layers in ultrathin nanopores

Journal Article · Thu Apr 01 00:00:00 EDT 2021 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0048011· OSTI ID:1852832

^[1]; Noh, Yechan ^[2]; ^[2]

University of Illinois at Urbana-Champaign, IL (United States); Univ. of Illinois at Urbana-Champaign, IL (United States)
University of Illinois at Urbana-Champaign, IL (United States)

The unique properties of aqueous electrolytes in ultrathin nanopores have drawn a great deal of attention in a variety of applications, such as power generation, water desalination, and disease diagnosis. Inside the nanopore, at the interface, properties of ions differ from those predicted by the classical ionic layering models (e.g., Gouy–Chapman electric double layer) when the thickness of the nanopore approaches the size of a single atom (e.g., nanopores in a single-layer graphene membrane). Here, using extensive molecular dynamics simulations, the structure and dynamics of aqueous ions inside nanopores are studied for different thicknesses, diameters, and surface charge densities of carbon-based nanopores [ultrathin graphene and finite-thickness carbon nanotubes (CNTs)]. The ion concentration and diffusion coefficient in ultrathin nanopores show no indication of the formation of a Stern layer (an immobile counter-ionic layer) as the counter-ions and nanopore atoms are weakly correlated in time compared to the strong correlation observed in thick nanopores. The weak correlation observed in ultrathin nanopores is indicative of a weak adsorption of counter-ions onto the surface compared to that of thick pores. The vanishing counter-ion adsorption (ion–wall correlation) in ultrathin nanopores leads to several orders of magnitude shorter ionic residence times (picoseconds) compared to the residence times in thick CNTs (seconds). The results of this study will help better understand the structure and dynamics of aqueous ions in ultrathin nanopores.

View Accepted Manuscript (DOE)

Research Organization:: Massachusetts Institute of Technology (MIT), Cambridge, MA (United States); University of Illinois at Urbana-Champaign, IL (United States)

Sponsoring Organization:: National science Foundation (NSF); State of Illinois; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019112

OSTI ID:: 1852832

Alternate ID(s):: OSTI ID: 1773569

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 13 Vol. 154; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (37)

Carbon Materials for Chemical Capacitive Energy Storage Zhai, Yunpu; Dou, Yuqian; Zhao, Dongyuan Advanced Materials, Vol. 23, Issue 42 https://doi.org/10.1002/adma.201100984	journal	September 2011
Ueber einige Gesetze der Vertheilung elektrischer Ströme in körperlichen Leitern mit Anwendung auf die thierisch-elektrischen Versuche Helmholtz, H. Annalen der Physik und Chemie, Vol. 165, Issue 6 https://doi.org/10.1002/andp.18531650603	journal	January 1853
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
Molecular dynamics simulations of the electric double layer capacitance of graphene electrodes in mono-valent aqueous electrolytes Jiang, Gengping; Cheng, Chi; Li, Dan Nano Research, Vol. 9, Issue 1 https://doi.org/10.1007/s12274-015-0978-5	journal	January 2016
Water management in proton exchange membrane fuel cells using integrated electroosmotic pumping Buie, Cullen R.; Posner, Jonathan D.; Fabian, Tibor Journal of Power Sources, Vol. 161, Issue 1 https://doi.org/10.1016/j.jpowsour.2006.03.021	journal	October 2006
Antibody Subclass Detection Using Graphene Nanopores Barati Farimani, Amir; Heiranian, Mohammad; Min, Kyoungmin The Journal of Physical Chemistry Letters, Vol. 8, Issue 7 https://doi.org/10.1021/acs.jpclett.7b00385	journal	March 2017
Nanofluidic Transport Theory with Enhancement Factors Approaching One Heiranian, Mohammad; Aluru, Narayana R. ACS Nano, Vol. 14, Issue 1 https://doi.org/10.1021/acsnano.9b04328	journal	December 2019
Graphitic Carbon–Water Nonbonded Interaction Parameters Wu, Yanbin; Aluru, N. R. The Journal of Physical Chemistry B, Vol. 117, Issue 29 https://doi.org/10.1021/jp402051t	journal	July 2013
Structure and Dynamics of an Electrolyte Confined in Charged Nanopores Cazade, Pierre-Andre; Hartkamp, Remco; Coasne, Benoit The Journal of Physical Chemistry C, Vol. 118, Issue 10 https://doi.org/10.1021/jp4098638	journal	March 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
Water Transport through Ultrathin Graphene Suk, Myung E.; Aluru, N. R. The Journal of Physical Chemistry Letters, Vol. 1, Issue 10, p. 1590-1594 https://doi.org/10.1021/jz100240r	journal	April 2010
Electromechanical Signatures for DNA Sequencing through a Mechanosensitive Nanopore Farimani, A. Barati; Heiranian, M.; Aluru, N. R. The Journal of Physical Chemistry Letters, Vol. 6, Issue 4 https://doi.org/10.1021/jz5025417	journal	February 2015
Hierarchical Multiscale Simulation of Electrokinetic Transport in Silica Nanochannels at the Point of Zero Charge Joseph, Sony; Aluru, N. R. Langmuir, Vol. 22, Issue 21 https://doi.org/10.1021/la0610147	journal	October 2006
Electrostatic Control of Ions and Molecules in Nanofluidic Transistors Karnik, Rohit; Fan, Rong; Yue, Min Nano Letters, Vol. 5, Issue 5 https://doi.org/10.1021/nl050493b	journal	May 2005
Why Are Carbon Nanotubes Fast Transporters of Water? Joseph, Sony; Aluru, N. R. Nano Letters, Vol. 8, Issue 2 https://doi.org/10.1021/nl072385q	journal	February 2008
Detection beyond the Debye Screening Length in a High-Frequency Nanoelectronic Biosensor Kulkarni, Girish S.; Zhong, Zhaohui Nano Letters, Vol. 12, Issue 2 https://doi.org/10.1021/nl203666a	journal	January 2012
Water Desalination across Nanoporous Graphene Cohen-Tanugi, David; Grossman, Jeffrey C. Nano Letters, Vol. 12, Issue 7, p. 3602-3608 https://doi.org/10.1021/nl3012853	journal	June 2012
Atomically Thin Molybdenum Disulfide Nanopores with High Sensitivity for DNA Translocation Liu, Ke; Feng, Jiandong; Kis, Andras ACS Nano, Vol. 8, Issue 3 https://doi.org/10.1021/nn406102h	journal	February 2014
Single-layer MoS2 nanopores as nanopower generators Feng, Jiandong; Graf, Michael; Liu, Ke Nature, Vol. 536, Issue 7615 https://doi.org/10.1038/nature18593	journal	July 2016
Ion selectivity of graphene nanopores Rollings, Ryan C.; Kuan, Aaron T.; Golovchenko, Jene A. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11408	journal	April 2016
Water desalination with a single-layer MoS2 nanopore Heiranian, Mohammad; Farimani, Amir Barati; Aluru, Narayana R. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9616	journal	October 2015
Materials for electrochemical capacitors Simon, Patrice; Gogotsi, Yury Nature Materials, Vol. 7, Issue 11 https://doi.org/10.1038/nmat2297	journal	November 2008
Nanopore sensors for nucleic acid analysis Venkatesan, Bala Murali; Bashir, Rashid Nature Nanotechnology, Vol. 6, Issue 10 https://doi.org/10.1038/nnano.2011.129	journal	September 2011
Graphene cleans up water Wang, Evelyn N.; Karnik, Rohit Nature Nanotechnology, Vol. 7, Issue 9 https://doi.org/10.1038/nnano.2012.153	journal	September 2012
Stochastic sensing of proteins with receptor-modified solid-state nanopores Wei, Ruoshan; Gatterdam, Volker; Wieneke, Ralph Nature Nanotechnology, Vol. 7, Issue 4 https://doi.org/10.1038/nnano.2012.24	journal	March 2012
Water desalination using nanoporous single-layer graphene Surwade, Sumedh P.; Smirnov, Sergei N.; Vlassiouk, Ivan V. Nature Nanotechnology, Vol. 10, Issue 5 https://doi.org/10.1038/nnano.2015.37	journal	March 2015
Ultrasensitive detection of nucleic acids using deformed graphene channel field effect biosensors Hwang, Michael Taeyoung; Heiranian, Mohammad; Kim, Yerim Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15330-9	journal	March 2020
Identification of amino acids with sensitive nanoporous MoS2: towards machine learning-based prediction Barati Farimani, Amir; Heiranian, Mohammad; Aluru, Narayana R. npj 2D Materials and Applications, Vol. 2, Issue 1 https://doi.org/10.1038/s41699-018-0060-8	journal	May 2018
Carbon-based materials as supercapacitor electrodes Zhang, Li Li; Zhao, X. S. Chemical Society Reviews, Vol. 38, Issue 9 https://doi.org/10.1039/b813846j	journal	January 2009
A unified formulation of the constant temperature molecular dynamics methods Nosé, Shuichi The Journal of Chemical Physics, Vol. 81, Issue 1 https://doi.org/10.1063/1.447334	journal	July 1984
Particle mesh Ewald: An N ⋅log( N ) method for Ewald sums in large systems Darden, Tom; York, Darrin; Pedersen, Lee The Journal of Chemical Physics, Vol. 98, Issue 12 https://doi.org/10.1063/1.464397	journal	June 1993
Water flow in carbon nanotubes: The effect of tube flexibility and thermostat Sam, Alan; Kannam, Sridhar Kumar; Hartkamp, Remco The Journal of Chemical Physics, Vol. 146, Issue 23 https://doi.org/10.1063/1.4985252	journal	June 2017
Ion exclusion by sub-2-nm carbon nanotube pores Fornasiero, F.; Park, H. G.; Holt, J. K. Proceedings of the National Academy of Sciences, Vol. 105, Issue 45 https://doi.org/10.1073/pnas.0710437105	journal	June 2008
Canonical dynamics: Equilibrium phase-space distributions Hoover, William G. Physical Review A, Vol. 31, Issue 3 https://doi.org/10.1103/PhysRevA.31.1695	journal	March 1985
Charge Inversion and Flow Reversal in a Nanochannel Electro-osmotic Flow Qiao, R.; Aluru, N. R. Physical Review Letters, Vol. 92, Issue 19 https://doi.org/10.1103/PhysRevLett.92.198301	journal	May 2004
Revisiting Sampson's theory for hydrodynamic transport in ultrathin nanopores Heiranian, Mohammad; Taqieddin, Amir; Aluru, Narayana R. Physical Review Research, Vol. 2, Issue 4 https://doi.org/10.1103/PhysRevResearch.2.043153	journal	October 2020
Fast Mass Transport Through Sub-2-Nanometer Carbon Nanotubes Holt, J. K. Science, Vol. 312, Issue 5776 https://doi.org/10.1126/science.1126298	journal	May 2006

Similar Records

Nonlinear ion transport mediated by induced charge in ultrathin nanoporous membranes

Journal Article · Mon Oct 25 20:00:00 EDT 2021 · Physical Review. E · OSTI ID:1980195

Zn2+ and Sr2+ Adsorption at the TiO2 (110)-Electrolyte Interface: Influence of Ionic Strength, Coverage, and Anions

Journal Article · Sat Dec 31 23:00:00 EST 2005 · J. Colloid Interface Sci. · OSTI ID:914158

Related Subjects

2D materials
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
desalination
electrical double layers
electrolytes
graphene
molecular dynamics
nanomaterials
nanotubes

Dynamic and weak electric double layers in ultrathin nanopores

Citation Formats

References (37)

Similar Records

Related Subjects