Imaging Arrangements of Discrete Ions at Liquid–Solid Interfaces

© The individual and collective behavior of ions near electrically charged interfaces is foundational to a variety of electrochemical phenomena encountered in biology, energy, and the environment. While many theories have been developed to predict the interfacial arrangements of counterions, direct...

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Main Authors: Li, Hao-Kun, Pedro de Souza, J, Zhang, Ze, Martis, Joel, Sendgikoski, Kyle, Cumings, John, Bazant, Martin Z, Majumdar, Arun
Other Authors: Massachusetts Institute of Technology. Department of Chemical Engineering
Format: Article
Language:English
Published: American Chemical Society (ACS) 2021
Online Access:https://hdl.handle.net/1721.1/133460
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author Li, Hao-Kun
Pedro de Souza, J
Zhang, Ze
Martis, Joel
Sendgikoski, Kyle
Cumings, John
Bazant, Martin Z
Majumdar, Arun
author2 Massachusetts Institute of Technology. Department of Chemical Engineering
author_facet Massachusetts Institute of Technology. Department of Chemical Engineering
Li, Hao-Kun
Pedro de Souza, J
Zhang, Ze
Martis, Joel
Sendgikoski, Kyle
Cumings, John
Bazant, Martin Z
Majumdar, Arun
author_sort Li, Hao-Kun
collection MIT
description © The individual and collective behavior of ions near electrically charged interfaces is foundational to a variety of electrochemical phenomena encountered in biology, energy, and the environment. While many theories have been developed to predict the interfacial arrangements of counterions, direct experimental observations and validations have remained elusive. Utilizing cryo-electron microscopy, here we directly visualize individual counterions and reveal their discrete interfacial layering. Comparison with simulations suggests the strong effects of finite ionic size and electrostatic interactions. We also uncover correlated ionic structures under extreme confinement, with the channel widths approaching the ionic diameter (∼1 nm). Our work reveals the roles of ionic size, valency, and confinement in determining the structures of liquid-solid interfaces and opens up new opportunities to study such systems at the single-ion level.
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spelling mit-1721.1/1334602023-02-16T20:53:52Z Imaging Arrangements of Discrete Ions at Liquid–Solid Interfaces Li, Hao-Kun Pedro de Souza, J Zhang, Ze Martis, Joel Sendgikoski, Kyle Cumings, John Bazant, Martin Z Majumdar, Arun Massachusetts Institute of Technology. Department of Chemical Engineering Massachusetts Institute of Technology. Department of Mathematics © The individual and collective behavior of ions near electrically charged interfaces is foundational to a variety of electrochemical phenomena encountered in biology, energy, and the environment. While many theories have been developed to predict the interfacial arrangements of counterions, direct experimental observations and validations have remained elusive. Utilizing cryo-electron microscopy, here we directly visualize individual counterions and reveal their discrete interfacial layering. Comparison with simulations suggests the strong effects of finite ionic size and electrostatic interactions. We also uncover correlated ionic structures under extreme confinement, with the channel widths approaching the ionic diameter (∼1 nm). Our work reveals the roles of ionic size, valency, and confinement in determining the structures of liquid-solid interfaces and opens up new opportunities to study such systems at the single-ion level. 2021-10-27T19:52:58Z 2021-10-27T19:52:58Z 2020 2021-06-07T17:41:01Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/133460 en 10.1021/ACS.NANOLETT.0C02669 Nano Letters Creative Commons Attribution-Noncommercial-Share Alike http://creativecommons.org/licenses/by-nc-sa/4.0/ application/pdf American Chemical Society (ACS) MIT web domain
spellingShingle Li, Hao-Kun
Pedro de Souza, J
Zhang, Ze
Martis, Joel
Sendgikoski, Kyle
Cumings, John
Bazant, Martin Z
Majumdar, Arun
Imaging Arrangements of Discrete Ions at Liquid–Solid Interfaces
title Imaging Arrangements of Discrete Ions at Liquid–Solid Interfaces
title_full Imaging Arrangements of Discrete Ions at Liquid–Solid Interfaces
title_fullStr Imaging Arrangements of Discrete Ions at Liquid–Solid Interfaces
title_full_unstemmed Imaging Arrangements of Discrete Ions at Liquid–Solid Interfaces
title_short Imaging Arrangements of Discrete Ions at Liquid–Solid Interfaces
title_sort imaging arrangements of discrete ions at liquid solid interfaces
url https://hdl.handle.net/1721.1/133460
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