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

Journal Article · · Advanced Materials
 [1];  [1];  [2];  [3]; ORCiD logo [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Sustainable Energy Technologies Department

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.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0012704
OSTI ID:
1376095
Report Number(s):
BNL--113908-2017-JA; KC0403020
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 27 Vol. 29; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (42)

Electrochemical Windows of Room-Temperature Ionic Liquids book January 2005
Double Layer of Au(100)/Ionic Liquid Interface and Its Stability in Imidazolium-Based Ionic Liquids journal June 2009
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
The Electrode/Ionic Liquid Interface: Electric Double Layer and Metal Electrodeposition journal August 2010
Surface Microscopy with Low Energy Electrons book January 2014
Thermal properties of imidazolium ionic liquids journal August 2000
Study of the interface Pt(111)/ [Emmim][NTf2] using laser-induced temperature jump experiments journal June 2015
Lithium-air batteries using hydrophobic room temperature ionic liquid electrolyte journal August 2005
Safe, high-energy supercapacitors based on solvent-free ionic liquid electrolytes journal December 2008
Ionic liquids as electrolytes for Li-ion batteries—An overview of electrochemical studies journal December 2009
Structure and dynamics of the interfacial layer between ionic liquids and electrode materials journal April 2014
Metallization of Epitaxial VO 2 Films by Ionic Liquid Gating through Initially Insulating TiO 2 Layers journal August 2016
Crowding and Anomalous Capacitance at an Electrode–Ionic Liquid Interface Observed Using Operando X-ray Scattering journal March 2016
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
Hydrophobic, Highly Conductive Ambient-Temperature Molten Salts journal January 1996
Thermophysical Properties of Imidazolium-Based Ionic Liquids journal July 2004
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
Charge Trapping in Imidazolium Ionic Liquids journal April 2009
Pronounced Structure in Confined Aprotic Room-Temperature Ionic Liquids journal May 2009
Direct Measurements of Ionic Mobility of Ionic Liquids Using the Electric Field Applying Pulsed Gradient Spin−Echo NMR journal June 2009
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
Complementary Molecular Dynamics and X-ray Reflectivity Study of an Imidazolium-Based Ionic Liquid at a Neutral Sapphire Interface journal January 2015
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
Suppression of Ionic Liquid Gate-Induced Metallization of SrTiO 3 (001) by Oxygen journal September 2013
Molecular Beam Deposition of Nanoscale Ionic Liquids in Ultrahigh Vacuum journal September 2010
Volatile times for ionic liquids journal February 2006
Ionic-liquid materials for the electrochemical challenges of the future journal July 2009
Slow and fast capacitive process taking place at the ionic liquid/electrode interface journal January 2012
Energy applications of ionic liquids journal January 2014
Ordered ionic liquid structure observed at terraced graphite interfaces journal January 2016
XPS enables visualization of electrode potential screening in an ionic liquid medium with temporal- and lateral-resolution journal January 2016
Energy applications of ionic liquids journal January 2009
At the interface: solvation and designing ionic liquids journal January 2010
Mono- and multi-layer adsorption of an ionic liquid on Au(110) journal January 2012
At the ionic liquid|metal interface: structure formation and temperature dependent behavior of an ionic liquid adlayer on Au(111) journal January 2013
High-mobility, low-power, and fast-switching organic field-effect transistors with ionic liquids journal March 2008
Restructuring of the electrical double layer in ionic liquids upon charging journal February 2015
Double Layer in Ionic Liquids: Overscreening versus Crowding journal January 2011
Surface Layering in Liquid Gallium: An X-Ray Reflectivity Study journal September 1995
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

Cited By (4)

Charge reduction in ions in the ionic liquid 1-ethy-2,3-dimethylimidazolium bis(trifluoromethanesulfonyl)imide on the Au(111) surface journal January 2020
Boronic ester-based dynamic covalent ionic liquid gels for self-healable, recyclable and malleable optical devices journal January 2018
Electrical field facilitates selective transport of CO 2 through a laminated MoS 2 supported ionic liquid membrane journal January 2019
Selectively tuning gas transport through ionic liquid filled graphene oxide nanoslits using an electric field journal January 2019