In Situ Probing of Ion Ordering at an Electrified Ionic Liquid/Au Interface

Sitaputra, Wattaka; Stacchiola, Dario; Wishart, James F.; Wang, Feng; Sadowski, Jerzy T.

doi:10.1002/adma.201606357

Title: In Situ Probing of Ion Ordering at an Electrified Ionic Liquid/Au Interface

Abstract

Charge transport at the interface of electrodes and ionic liquids is critical for the use of the latter as electrolytes. In this study, a room-temperature ionic liquid, 1-ethyl-2,3-dimethylimidazolium bis(trifluoromethanesulfonyl)imide (EMMIM TFSI), is investigated in situ under applied bias voltage with a novel method using low-energy electron and photoemission electron microscopy. Changes in photoelectron yield as a function of bias applied to electrodes provide a direct measure of the dynamics of ion reconfiguration and electrostatic responses of the EMMIM TFSI. Finally, long-range and correlated ionic reconfigurations that occur near the electrodes are found to be a function of temperature and thickness, which, in turn, relate to ionic mobility and different configurations for out-of-plane ordering near the electrode interfaces, with a critical transition in ion mobility for films thicker than three monolayers.

Authors:

Sitaputra, Wattaka ^[1]; Stacchiola, Dario ^[1]; Wishart, James F. ^[2]; Wang, Feng ^[3];

^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
Brookhaven National Lab. (BNL), Upton, NY (United States). Sustainable Energy Technologies Department

Publication Date:: Fri May 12 00:00:00 EDT 2017

Research Org.:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

OSTI Identifier:: 1376095

Alternate Identifier(s):: OSTI ID: 1401792

Report Number(s):: BNL-113908-2017-JA
Journal ID: ISSN 0935-9648; R&D Project: 16083/16083; KC0403020

Grant/Contract Number:: SC0012704; DE‐SC0012704

Resource Type:: Accepted Manuscript

Journal Name:: Advanced Materials

Additional Journal Information:: Journal Volume: 29; Journal Issue: 27; Journal ID: ISSN 0935-9648

Publisher:: Wiley

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electric double layers; ionic liquids; photoemission electron microscopy

Citation Formats


                    Sitaputra, Wattaka, Stacchiola, Dario, Wishart, James F., Wang, Feng, and Sadowski, Jerzy T. In Situ Probing of Ion Ordering at an Electrified Ionic Liquid/Au Interface.  United States: N. p., 2017. 
Web.  doi:10.1002/adma.201606357.

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                    Sitaputra, Wattaka, Stacchiola, Dario, Wishart, James F., Wang, Feng, & Sadowski, Jerzy T. In Situ Probing of Ion Ordering at an Electrified Ionic Liquid/Au Interface.  United States.  https://doi.org/10.1002/adma.201606357

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                    Sitaputra, Wattaka, Stacchiola, Dario, Wishart, James F., Wang, Feng, and Sadowski, Jerzy T. Fri .  
"In Situ Probing of Ion Ordering at an Electrified Ionic Liquid/Au Interface".  United States.  https://doi.org/10.1002/adma.201606357.  https://www.osti.gov/servlets/purl/1376095.

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@article{osti_1376095,

  title        = {In Situ Probing of Ion Ordering at an Electrified Ionic Liquid/Au Interface},

  author       = {Sitaputra, Wattaka and Stacchiola, Dario and Wishart, James F. and Wang, Feng and Sadowski, Jerzy T.},

  abstractNote = {Charge transport at the interface of electrodes and ionic liquids is critical for the use of the latter as electrolytes. In this study, a room-temperature ionic liquid, 1-ethyl-2,3-dimethylimidazolium bis(trifluoromethanesulfonyl)imide (EMMIM TFSI), is investigated in situ under applied bias voltage with a novel method using low-energy electron and photoemission electron microscopy. Changes in photoelectron yield as a function of bias applied to electrodes provide a direct measure of the dynamics of ion reconfiguration and electrostatic responses of the EMMIM TFSI. Finally, long-range and correlated ionic reconfigurations that occur near the electrodes are found to be a function of temperature and thickness, which, in turn, relate to ionic mobility and different configurations for out-of-plane ordering near the electrode interfaces, with a critical transition in ion mobility for films thicker than three monolayers.},

  doi          = {10.1002/adma.201606357},

  journal      = {Advanced Materials},

  number       = 27,

  volume       = 29,

  place        = {United States},

  year         = {Fri May 12 00:00:00 EDT 2017},

  month        = {Fri May 12 00:00:00 EDT 2017}

}

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Works referencing / citing this record:

Selectively tuning gas transport through ionic liquid filled graphene oxide nanoslits using an electric field
journal, January 2019

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Charge reduction in ions in the ionic liquid 1-ethy-2,3-dimethylimidazolium bis(trifluoromethanesulfonyl)imide on the Au(111) surface
journal, January 2020

Liu, Mingjie; Shao, Yihan; Wu, Qin
Theoretical Chemistry Accounts, Vol. 139, Issue 2
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Title: In Situ Probing of Ion Ordering at an Electrified Ionic Liquid/Au Interface

Abstract

Citation Formats

Ionic-liquid materials for the electrochemical challenges of the future journal, July 2009

The Electrode/Ionic Liquid Interface: Electric Double Layer and Metal Electrodeposition journal, August 2010

Electronic Structure of the Surface of the Ionic Liquid [EMIM][Tf 2 N] Studied by Metastable Impact Electron Spectroscopy (MIES), UPS, and XPS journal, August 2006

High-mobility, low-power, and fast-switching organic field-effect transistors with ionic liquids journal, March 2008

Thermal properties of imidazolium ionic liquids journal, August 2000

Charge Trapping in Imidazolium Ionic Liquids journal, April 2009

Molecular Beam Deposition of Nanoscale Ionic Liquids in Ultrahigh Vacuum journal, September 2010

Surface Microscopy with Low Energy Electrons book, January 2014

Hydrophobic, Highly Conductive Ambient-Temperature Molten Salts † journal, January 1996

Ordered ionic liquid structure observed at terraced graphite interfaces journal, January 2016

Exploring Electrochemical Windows of Room-Temperature Ionic Liquids: A Computational Study journal, September 2012

Molecular Dynamics Simulations of Ionic Liquids: Cation and Anion Dependence of Self-Diffusion Coefficients of Ions journal, August 2009

Energy applications of ionic liquids journal, January 2009

Lithium-air batteries using hydrophobic room temperature ionic liquid electrolyte journal, August 2005

Adsorption of the ionic liquid [BMP][TFSA] on Au(111) and Ag(111): substrate effects on the structure formation investigated by STM journal, January 2013

Restructuring of the electrical double layer in ionic liquids upon charging journal, February 2015

Electrochemical Windows of Room-Temperature Ionic Liquids book, January 2005

Physical Vapor Deposition of [EMIM][Tf 2 N]: A New Approach to the Modification of Surface Properties with Ultrathin Ionic Liquid Films journal, October 2008

Surface Layering in Liquid Gallium: An X-Ray Reflectivity Study journal, September 1995

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Pronounced Structure in Confined Aprotic Room-Temperature Ionic Liquids journal, May 2009

Safe, high-energy supercapacitors based on solvent-free ionic liquid electrolytes journal, December 2008

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Complementary Molecular Dynamics and X-ray Reflectivity Study of an Imidazolium-Based Ionic Liquid at a Neutral Sapphire Interface journal, January 2015

Liquid-Gated High Mobility and Quantum Oscillation of the Two-Dimensional Electron Gas at an Oxide Interface journal, March 2016

Electrochemical Reactivity in Room-Temperature Ionic Liquids journal, July 2008

Volatile times for ionic liquids journal, February 2006

Direct Measurements of Ionic Mobility of Ionic Liquids Using the Electric Field Applying Pulsed Gradient Spin−Echo NMR journal, June 2009

At the ionic liquid|metal interface: structure formation and temperature dependent behavior of an ionic liquid adlayer on Au(111) journal, January 2013

Thermophysical Properties of Imidazolium-Based Ionic Liquids journal, July 2004

Structure and dynamics of the interfacial layer between ionic liquids and electrode materials journal, April 2014

Slow and fast capacitive process taking place at the ionic liquid/electrode interface journal, January 2012

Ionic liquids as electrolytes for Li-ion batteries—An overview of electrochemical studies journal, December 2009

Mono- and multi-layer adsorption of an ionic liquid on Au(110) journal, January 2012

Suppression of Ionic Liquid Gate-Induced Metallization of SrTiO 3 (001) by Oxygen journal, September 2013

Energy applications of ionic liquids journal, January 2014

Double Layer of Au(100)/Ionic Liquid Interface and Its Stability in Imidazolium-Based Ionic Liquids journal, June 2009

Double Layer in Ionic Liquids: Overscreening versus Crowding journal, January 2011

Hysteresis of Potential-Dependent Changes in Ion Density and Structure of an Ionic Liquid on a Gold Electrode: In Situ Observation by Surface-Enhanced Infrared Absorption Spectroscopy journal, September 2013

At the interface: solvation and designing ionic liquids journal, January 2010

Study of the interface Pt(111)/ [Emmim][NTf2] using laser-induced temperature jump experiments journal, June 2015

Selectively tuning gas transport through ionic liquid filled graphene oxide nanoslits using an electric field journal, January 2019

Electrical field facilitates selective transport of CO 2 through a laminated MoS 2 supported ionic liquid membrane journal, January 2019

Boronic ester-based dynamic covalent ionic liquid gels for self-healable, recyclable and malleable optical devices journal, January 2018

Charge reduction in ions in the ionic liquid 1-ethy-2,3-dimethylimidazolium bis(trifluoromethanesulfonyl)imide on the Au(111) surface journal, January 2020

Ionic-liquid materials for the electrochemical challenges of the future
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The Electrode/Ionic Liquid Interface: Electric Double Layer and Metal Electrodeposition
journal, August 2010

Electronic Structure of the Surface of the Ionic Liquid [EMIM][Tf ₂ N] Studied by Metastable Impact Electron Spectroscopy (MIES), UPS, and XPS
journal, August 2006

High-mobility, low-power, and fast-switching organic field-effect transistors with ionic liquids
journal, March 2008

Thermal properties of imidazolium ionic liquids
journal, August 2000

Charge Trapping in Imidazolium Ionic Liquids
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Molecular Beam Deposition of Nanoscale Ionic Liquids in Ultrahigh Vacuum
journal, September 2010

Surface Microscopy with Low Energy Electrons
book, January 2014

Hydrophobic, Highly Conductive Ambient-Temperature Molten Salts ^†
journal, January 1996

Ordered ionic liquid structure observed at terraced graphite interfaces
journal, January 2016

Exploring Electrochemical Windows of Room-Temperature Ionic Liquids: A Computational Study
journal, September 2012

Molecular Dynamics Simulations of Ionic Liquids: Cation and Anion Dependence of Self-Diffusion Coefficients of Ions
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Lithium-air batteries using hydrophobic room temperature ionic liquid electrolyte
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Adsorption of the ionic liquid [BMP][TFSA] on Au(111) and Ag(111): substrate effects on the structure formation investigated by STM
journal, January 2013

Restructuring of the electrical double layer in ionic liquids upon charging
journal, February 2015

Electrochemical Windows of Room-Temperature Ionic Liquids
book, January 2005

Physical Vapor Deposition of [EMIM][Tf ₂ N]: A New Approach to the Modification of Surface Properties with Ultrathin Ionic Liquid Films
journal, October 2008

Surface Layering in Liquid Gallium: An X-Ray Reflectivity Study
journal, September 1995

Crowding and Anomalous Capacitance at an Electrode–Ionic Liquid Interface Observed Using Operando X-ray Scattering
journal, March 2016

Pronounced Structure in Confined Aprotic Room-Temperature Ionic Liquids
journal, May 2009

Safe, high-energy supercapacitors based on solvent-free ionic liquid electrolytes
journal, December 2008

XPS enables visualization of electrode potential screening in an ionic liquid medium with temporal- and lateral-resolution
journal, January 2016

Metallization of Epitaxial VO ₂ Films by Ionic Liquid Gating through Initially Insulating TiO ₂ Layers
journal, August 2016

Complementary Molecular Dynamics and X-ray Reflectivity Study of an Imidazolium-Based Ionic Liquid at a Neutral Sapphire Interface
journal, January 2015

Liquid-Gated High Mobility and Quantum Oscillation of the Two-Dimensional Electron Gas at an Oxide Interface
journal, March 2016

Electrochemical Reactivity in Room-Temperature Ionic Liquids
journal, July 2008

Volatile times for ionic liquids
journal, February 2006

Direct Measurements of Ionic Mobility of Ionic Liquids Using the Electric Field Applying Pulsed Gradient Spin−Echo NMR
journal, June 2009

At the ionic liquid|metal interface: structure formation and temperature dependent behavior of an ionic liquid adlayer on Au(111)
journal, January 2013

Thermophysical Properties of Imidazolium-Based Ionic Liquids
journal, July 2004

Structure and dynamics of the interfacial layer between ionic liquids and electrode materials
journal, April 2014

Slow and fast capacitive process taking place at the ionic liquid/electrode interface
journal, January 2012

Ionic liquids as electrolytes for Li-ion batteries—An overview of electrochemical studies
journal, December 2009

Mono- and multi-layer adsorption of an ionic liquid on Au(110)
journal, January 2012

Suppression of Ionic Liquid Gate-Induced Metallization of SrTiO ₃ (001) by Oxygen
journal, September 2013

Energy applications of ionic liquids
journal, January 2014

Double Layer of Au(100)/Ionic Liquid Interface and Its Stability in Imidazolium-Based Ionic Liquids
journal, June 2009

Double Layer in Ionic Liquids: Overscreening versus Crowding
journal, January 2011

Hysteresis of Potential-Dependent Changes in Ion Density and Structure of an Ionic Liquid on a Gold Electrode: In Situ Observation by Surface-Enhanced Infrared Absorption Spectroscopy
journal, September 2013

At the interface: solvation and designing ionic liquids
journal, January 2010

Study of the interface Pt(111)/ [Emmim][NTf2] using laser-induced temperature jump experiments
journal, June 2015

Selectively tuning gas transport through ionic liquid filled graphene oxide nanoslits using an electric field
journal, January 2019

Electrical field facilitates selective transport of CO ₂ through a laminated MoS ₂ supported ionic liquid membrane
journal, January 2019

Boronic ester-based dynamic covalent ionic liquid gels for self-healable, recyclable and malleable optical devices
journal, January 2018

Charge reduction in ions in the ionic liquid 1-ethy-2,3-dimethylimidazolium bis(trifluoromethanesulfonyl)imide on the Au(111) surface
journal, January 2020