Spiers Memorial Lecture: From cold to hot, the structure and structural dynamics of dense ionic fluids

Emerson, Matthew S.; Ogbodo, Raphael; Margulis, Claudio J.

doi:10.1039/D4FD00086B

Title: Spiers Memorial Lecture: From cold to hot, the structure and structural dynamics of dense ionic fluids

Journal Article · 25 October 2024 · Faraday Discussions

DOI: https://doi.org/10.1039/D4FD00086B · OSTI ID:2406274

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Department of Chemistry, The University of Iowa, Iowa City, IA 52242, USA

This article presents a perspective on what we think are key topics related to the structure and structural dynamics of ILs and to some extent high-temperature molten salts.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0012704; AC02-05CH11231

OSTI ID:: 2406274

Journal Information:: Faraday Discussions, Journal Name: Faraday Discussions Vol. 253; ISSN FDISE6; ISSN 1359-6640

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United Kingdom

Language:: English

References (68)

Understanding Battery Interfaces by Combined Characterization and Simulation Approaches: Challenges and Perspectives Atkins, Duncan; Ayerbe, Elixabete; Benayad, Anass Advanced Energy Materials, Vol. 12, Issue 17 https://doi.org/10.1002/aenm.202102687	journal	December 2021
Including many-body effects in models for ionic liquids Salanne, Mathieu; Rotenberg, Benjamin; Jahn, Sandro Theoretical Chemistry Accounts, Vol. 131, Issue 3 https://doi.org/10.1007/s00214-012-1143-9	journal	February 2012
Ether tails make a large difference for the structural dynamics of imidazolium-based ionic liquids Amith, Weththasinghage D.; Araque, Juan C.; Margulis, Claudio J. Journal of Ionic Liquids, Vol. 2, Issue 1 https://doi.org/10.1016/j.jil.2021.100012	journal	June 2022
The role of local structure in dynamical arrest Royall, C. Patrick; Williams, Stephen R. Physics Reports, Vol. 560 https://doi.org/10.1016/j.physrep.2014.11.004	journal	February 2015
Advances in central receivers for concentrating solar applications Ho, Clifford K. Solar Energy, Vol. 152 https://doi.org/10.1016/j.solener.2017.03.048	journal	August 2017
Extension of the CL&Pol Polarizable Force Field to Electrolytes, Protic Ionic Liquids, and Deep Eutectic Solvents Goloviznina, Kateryna; Gong, Zheng; Costa Gomes, Margarida F. Journal of Chemical Theory and Computation, Vol. 17, Issue 3 https://doi.org/10.1021/acs.jctc.0c01002	journal	February 2021
Transferable, Polarizable Force Field for Ionic Liquids Goloviznina, Kateryna; Canongia Lopes, José N.; Costa Gomes, Margarida Journal of Chemical Theory and Computation, Vol. 15, Issue 11 https://doi.org/10.1021/acs.jctc.9b00689	journal	September 2019
SEM-Drude Model for the Accurate and Efficient Simulation of MgCl ₂ –KCl Mixtures in the Condensed Phase Sharma, Shobha; Emerson, Matthew S.; Wu, Fei The Journal of Physical Chemistry A, Vol. 124, Issue 38 https://doi.org/10.1021/acs.jpca.0c06721	journal	August 2020
Temperature Dependence of Short and Intermediate Range Order in Molten MgCl ₂ and Its Mixture with KCl Wu, Fei; Sharma, Shobha; Roy, Santanu The Journal of Physical Chemistry B, Vol. 124, Issue 14 https://doi.org/10.1021/acs.jpcb.0c00745	journal	March 2020
A Brief Guide to the Structure of High-Temperature Molten Salts and Key Aspects Making Them Different from Their Low-Temperature Relatives, the Ionic Liquids Sharma, Shobha; Ivanov, Alexander S.; Margulis, Claudio J. The Journal of Physical Chemistry B, Vol. 125, Issue 24 https://doi.org/10.1021/acs.jpcb.1c01065	journal	May 2021
Relationship between the Relaxation of Ionic Liquid Structural Motifs and That of the Shear Viscosity Amith, Weththasinghage D.; Araque, Juan C.; Margulis, Claudio J. The Journal of Physical Chemistry B, Vol. 125, Issue 23 https://doi.org/10.1021/acs.jpcb.1c03105	journal	June 2021
Unraveling Local Structure of Molten Salts via X-ray Scattering, Raman Spectroscopy, and Ab Initio Molecular Dynamics Roy, Santanu; Brehm, Martin; Sharma, Shobha The Journal of Physical Chemistry B https://doi.org/10.1021/acs.jpcb.1c03786	journal	May 2021
Structural Origins of Viscosity in Imidazolium and Pyrrolidinium Ionic Liquids Coupled with the NTf₂^– Anion Ogbodo, Raphael; Karunaratne, Waruni V.; Acharya, Gobin Raj The Journal of Physical Chemistry B, Vol. 127, Issue 28 https://doi.org/10.1021/acs.jpcb.3c02604	journal	July 2023
Heterogeneous Structure, Mechanisms of Counterion Exchange, and the Spacer Salt Effect in Complex Molten Salt Mixtures Including LaCl₃ Emerson, Matthew S.; Ivanov, Alexander S.; Gallington, Leighanne C. The Journal of Physical Chemistry B, Vol. 128, Issue 16 https://doi.org/10.1021/acs.jpcb.4c01429	journal	April 2024
Modern Room Temperature Ionic Liquids, a Simple Guide to Understanding Their Structure and How It May Relate to Dynamics Araque, Juan C.; Hettige, Jeevapani J.; Margulis, Claudio J. The Journal of Physical Chemistry B, Vol. 119, Issue 40 https://doi.org/10.1021/acs.jpcb.5b05506	journal	August 2015
Structure of Molten Alkali Chlorides at Charged Interfaces and the Prediction and Interpretation of Their X-ray Reflectivity Karunaratne, Waruni V.; Sharma, Shobha; Ocko, Benjamin M. The Journal of Physical Chemistry C, Vol. 125, Issue 45 https://doi.org/10.1021/acs.jpcc.1c07135	journal	November 2021
Vacuum Interfacial Structure and X-ray Reflectivity of Imidazolium-Based Ionic Liquids with Perfluorinated Anions from a Theory and Simulations Perspective Karunaratne, Waruni V.; Zhao, Man; Castner, Edward W. The Journal of Physical Chemistry C, Vol. 126, Issue 32 https://doi.org/10.1021/acs.jpcc.2c03311	journal	August 2022
Nanotribology of Ionic Liquids as Lubricant Additives for Alumina Surfaces Cowie, Stephen; Cooper, Peter K.; Atkin, Rob The Journal of Physical Chemistry C, Vol. 121, Issue 51 https://doi.org/10.1021/acs.jpcc.7b09879	journal	December 2017
Ionic Liquid Mixture at the Vacuum Interface and the Peaks and Antipeaks Analysis of X-ray Reflectivity Wu, Fei; Karunaratne, Waruni V.; Margulis, Claudio J. The Journal of Physical Chemistry C, Vol. 123, Issue 8 https://doi.org/10.1021/acs.jpcc.8b11958	journal	January 2019
Structure and Dynamics of an Ionic Liquid Mixture Film Confined by Mica Karunaratne, Waruni V.; Margulis, Claudio J. The Journal of Physical Chemistry C, Vol. 123, Issue 34 https://doi.org/10.1021/acs.jpcc.9b05510	journal	August 2019
A Pictorial View of Viscosity in Ionic Liquids and the Link to Nanostructural Heterogeneity Amith, Weththasinghage D.; Araque, Juan C.; Margulis, Claudio J. The Journal of Physical Chemistry Letters, Vol. 11, Issue 6 https://doi.org/10.1021/acs.jpclett.0c00170	journal	February 2020
Structures of Ionic Liquids Having Both Anionic and Cationic Octyl Tails: Lamellar Vacuum Interface vs Sponge-Like Bulk Order Amith, Weththasinghage Don; Hettige, Jeevapani J.; Castner, Edward W. The Journal of Physical Chemistry Letters, Vol. 7, Issue 19 https://doi.org/10.1021/acs.jpclett.6b01763	journal	September 2016
Elucidating Ionic Correlations Beyond Simple Charge Alternation in Molten MgCl ₂ –KCl Mixtures Wu, Fei; Roy, Santanu; Ivanov, Alexander S. The Journal of Physical Chemistry Letters, Vol. 10, Issue 24 https://doi.org/10.1021/acs.jpclett.9b02845	journal	November 2019
Self-Assembled Nanostructures in Aprotic Ionic Liquids Facilitate Charge Transport at Elevated Pressure Yao, Beibei; Paluch, Marian; Paturej, Jaroslaw ACS Applied Materials & Interfaces, Vol. 15, Issue 33 https://doi.org/10.1021/acsami.3c08606	journal	August 2023
Complete Description of the LaCl₃–NaCl Melt Structure and the Concept of a Spacer Salt That Causes Structural Heterogeneity Emerson, Matthew S.; Sharma, Shobha; Roy, Santanu Journal of the American Chemical Society, Vol. 144, Issue 47 https://doi.org/10.1021/jacs.2c09987	journal	November 2022
Do Ionic Liquids Slow Down in Stages? Borah, Bichitra; Acharya, Gobin Raj; Grajeda, Diana Journal of the American Chemical Society, Vol. 145, Issue 47 https://doi.org/10.1021/jacs.3c08639	journal	November 2023
Complex Structure of Ionic Liquids. Molecular Dynamics Studies with Different Cation–Anion Combinations Freitas, Adilson A.; Shimizu, Karina; Canongia Lopes, José N. Journal of Chemical & Engineering Data, Vol. 59, Issue 10 https://doi.org/10.1021/je500197x	journal	May 2014
Nanostructural Organization in Ionic Liquids Canongia Lopes, José N. A.; Pádua, Agílio A. H. The Journal of Physical Chemistry B, Vol. 110, Issue 7 https://doi.org/10.1021/jp056006y	journal	February 2006
Calculation of Activities of Ions in Molten Salts with Potential Application to the Pyroprocessing of Nuclear Waste Salanne, Mathieu; Simon, Christian; Turq, Pierre The Journal of Physical Chemistry B, Vol. 112, Issue 4 https://doi.org/10.1021/jp075299n	journal	January 2008
What is the Origin of the Prepeak in the X-ray Scattering of Imidazolium-Based Room-Temperature Ionic Liquids? Annapureddy, Harsha V. R.; Kashyap, Hemant K.; De Biase, Pablo M. The Journal of Physical Chemistry B, Vol. 114, Issue 50 https://doi.org/10.1021/jp108545z	journal	December 2010
How Is Charge Transport Different in Ionic Liquids and Electrolyte Solutions? Kashyap, Hemant K.; Annapureddy, Harsha V. R.; Raineri, Fernando O. The Journal of Physical Chemistry B, Vol. 115, Issue 45 https://doi.org/10.1021/jp204182c	journal	November 2011
Mesoscopic Structural Heterogeneities in Room-Temperature Ionic Liquids Russina, Olga; Triolo, Alessandro; Gontrani, Lorenzo The Journal of Physical Chemistry Letters, Vol. 3, Issue 1 https://doi.org/10.1021/jz201349z	journal	December 2011
Anions, the Reporters of Structure in Ionic Liquids Hettige, Jeevapani J.; Kashyap, Hemant K.; Annapureddy, Harsha V. R. The Journal of Physical Chemistry Letters, Vol. 4, Issue 1 https://doi.org/10.1021/jz301866f	journal	December 2012
Irreversible reorganization in a supercooled liquid originates from localized soft modes Widmer-Cooper, Asaph; Perry, Heidi; Harrowell, Peter Nature Physics, Vol. 4, Issue 9 https://doi.org/10.1038/nphys1025	journal	July 2008
Pressure-induced liquid-liquid transition in a family of ionic materials Wojnarowska, Zaneta; Cheng, Shinian; Yao, Beibei Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-29021-0	journal	March 2022
Self-assembled nanostructures in ionic liquids facilitate charge storage at electrified interfaces Mao, Xianwen; Brown, Paul; Červinka, Ctirad Nature Materials, Vol. 18, Issue 12 https://doi.org/10.1038/s41563-019-0449-6	journal	August 2019
Long range electrostatic forces in ionic liquids Gebbie, Matthew A.; Smith, Alexander M.; Dobbs, Howard A. Chemical Communications, Vol. 53, Issue 7 https://doi.org/10.1039/C6CC08820A	journal	January 2017
Coupling between the mesoscopic dynamics and shear stress of a room-temperature ionic liquid Yamaguchi, Tsuyoshi Physical Chemistry Chemical Physics, Vol. 20, Issue 26 https://doi.org/10.1039/C8CP02814A	journal	January 2018
Structure and dynamics of the molten alkali-chloride salts from an X-ray, simulation, and rate theory perspective Roy, Santanu; Wu, Fei; Wang, Haimeng Physical Chemistry Chemical Physics, Vol. 22, Issue 40 https://doi.org/10.1039/D0CP03672B	journal	January 2020
Charge transfer and polarisability in ionic liquids: a case study Philippi, Frederik; Goloviznina, Kateryna; Gong, Zheng Physical Chemistry Chemical Physics, Vol. 24, Issue 5 https://doi.org/10.1039/D1CP04592J	journal	January 2022
Force field refinement for reproducing experimental infrared spectra of ionic liquids Szabadi, András; Doknic, Aleksandar; Netsch, Jonathan Physical Chemistry Chemical Physics, Vol. 25, Issue 29 https://doi.org/10.1039/D3CP00932G	journal	January 2023
Wave mechanics in an ionic liquid mixture Groves, Timothy S.; Perkin, Susan Faraday Discussions https://doi.org/10.1039/D4FD00040D	journal	January 2024
SAXS anti-peaks reveal the length-scales of dual positive–negative and polar–apolar ordering in room-temperature ionic liquids Kashyap, Hemant K.; Hettige, Jeevapani J.; Annapureddy, Harsha V. R. Chemical Communications, Vol. 48, Issue 42 https://doi.org/10.1039/c2cc30609c	journal	January 2012
Ionic liquids in confined geometries Perkin, Susan Physical Chemistry Chemical Physics, Vol. 14, Issue 15 https://doi.org/10.1039/c2cp23814d	journal	January 2012
Ionic liquid lubrication: influence of ion structure, surface potential and sliding velocity Li, Hua; Rutland, Mark W.; Atkin, Rob Physical Chemistry Chemical Physics, Vol. 15, Issue 35 https://doi.org/10.1039/c3cp52638k	journal	January 2013
An ionic liquid lubricant enables superlubricity to be “switched on” in situ using an electrical potential Li, Hua; Wood, Ross J.; Rutland, Mark W. Chemical Communications, Vol. 50, Issue 33 https://doi.org/10.1039/c4cc00979g	journal	January 2014
Ewald summation of electrostatic multipole interactions up to the quadrupolar level Aguado, Andrés; Madden, Paul A. The Journal of Chemical Physics, Vol. 119, Issue 14 https://doi.org/10.1063/1.1605941	journal	October 2003
On the study of collective dynamics in supercooled liquids through the statistics of the isoconfigurational ensemble Widmer-Cooper, Asaph; Harrowell, Peter The Journal of Chemical Physics, Vol. 126, Issue 15 https://doi.org/10.1063/1.2719192	journal	April 2007
Calculations of the thermal conductivities of ionic materials by simulation with polarizable interaction potentials Ohtori, Norikazu; Salanne, Mathieu; Madden, Paul A. The Journal of Chemical Physics, Vol. 130, Issue 10 https://doi.org/10.1063/1.3086856	journal	March 2009
Relationship between mesoscale dynamics and shear relaxation of ionic liquids with long alkyl chain Yamaguchi, Tsuyoshi; Mikawa, Ken-ichi; Koda, Shinobu The Journal of Chemical Physics, Vol. 137, Issue 10 https://doi.org/10.1063/1.4751547	journal	September 2012
Structure of molten MCl3 systems from a polarizable ion simulation model Hutchinson, Francis; Rowley, Adrian J.; Walters, Malcolm K. The Journal of Chemical Physics, Vol. 111, Issue 5 https://doi.org/10.1063/1.479471	journal	August 1999
Communication: Anomalous temperature dependence of the intermediate range order in phosphonium ionic liquids Hettige, Jeevapani J.; Kashyap, Hemant K.; Margulis, Claudio J. The Journal of Chemical Physics, Vol. 140, Issue 11 https://doi.org/10.1063/1.4867900	journal	March 2014
Ionic liquids—Conventional solvent mixtures, structurally different but dynamically similar Araque, Juan C.; Hettige, Jeevapani J.; Margulis, Claudio J. The Journal of Chemical Physics, Vol. 143, Issue 13 https://doi.org/10.1063/1.4932331	journal	October 2015
Communication: Nanoscale structure of tetradecyltrihexylphosphonium based ionic liquids Hettige, Jeevapani J.; Araque, Juan C.; Kashyap, Hemant K. The Journal of Chemical Physics, Vol. 144, Issue 12 https://doi.org/10.1063/1.4944678	journal	March 2016
Mode-coupling theoretical study on the roles of heterogeneous structure in rheology of ionic liquids Yamaguchi, Tsuyoshi The Journal of Chemical Physics, Vol. 144, Issue 12 https://doi.org/10.1063/1.4944679	journal	March 2016
A link between structure, diffusion and rotations of hydrogen bonding tracers in ionic liquids Araque, Juan C.; Daly, Ryan P.; Margulis, Claudio J. The Journal of Chemical Physics, Vol. 144, Issue 20 https://doi.org/10.1063/1.4951012	journal	May 2016
Experimental study on the relationship between the frequency-dependent shear viscosity and the intermediate scattering function of representative viscous liquids Yamaguchi, Tsuyoshi The Journal of Chemical Physics, Vol. 145, Issue 19 https://doi.org/10.1063/1.4968208	journal	November 2016
Analysis of shear viscosity and viscoelastic relaxation of liquid methanol based on molecular dynamics simulation and mode-coupling theory Yamaguchi, Tsuyoshi; Faraone, Antonio The Journal of Chemical Physics, Vol. 146, Issue 24 https://doi.org/10.1063/1.4990408	journal	June 2017
Communication: Stiff and soft nano-environments and the “Octopus Effect” are the crux of ionic liquid structural and dynamical heterogeneity Daly, Ryan P.; Araque, Juan C.; Margulis, Claudio J. The Journal of Chemical Physics, Vol. 147, Issue 6 https://doi.org/10.1063/1.4990666	journal	August 2017
Nanoscale organization in the fluorinated room temperature ionic liquid: Tetraethyl ammonium (trifluoromethanesulfonyl)(nonafluorobutylsulfonyl)imide Lo Celso, F.; Appetecchi, G. B.; Jafta, C. J. The Journal of Chemical Physics, Vol. 148, Issue 19 https://doi.org/10.1063/1.5016236	journal	May 2018
In an ionic liquid, high local friction is determined by the proximity to the charge network Araque, Juan C.; Margulis, Claudio J. The Journal of Chemical Physics, Vol. 149, Issue 14 https://doi.org/10.1063/1.5045675	journal	October 2018
Deep eutectic solvents—The vital link between ionic liquids and ionic solutions Abbott, Andrew P.; Edler, Karen J.; Page, Alister J. The Journal of Chemical Physics, Vol. 155, Issue 15 https://doi.org/10.1063/5.0072268	journal	October 2021
Evidence of a liquid–liquid transition in a glass-forming ionic liquid Harris, Matthew A.; Kinsey, Thomas; Wagle, Durgesh V. Proceedings of the National Academy of Sciences, Vol. 118, Issue 11 https://doi.org/10.1073/pnas.2020878118	journal	March 2021
A unified description of MCI₃systems with a polarizable ion simulation model Hutchinson, Francis; Wilson, Mark; Madden, Paul A. Molecular Physics, Vol. 99, Issue 10 https://doi.org/10.1080/00268970010022878	journal	May 2001
Transport coefficients and the Stokes–Einstein relation in molten alkali halides with polarisable ion model Ishii, Yoshiki; Kasai, Satoshi; Salanne, Mathieu Molecular Physics, Vol. 113, Issue 17-18 https://doi.org/10.1080/00268976.2015.1046527	journal	May 2015
(Keynote) Theoretical Deconstruction of the X-ray Structure Function Exposes Polarity Alternations in Room Temperature Ionic Liquids Kashyap, H. K.; Margulis, C. J. ECS Transactions, Vol. 50, Issue 11 https://doi.org/10.1149/05011.0301ecst	journal	March 2013
Separation of Lanthanides and Actinides in a Chloride Melt - Liquid Metal System: The Effect of Phase Composition Volkovich, Vladimir A.; Maltsev, Dmitry S.; Melchakov, Stanislav Yu. ECS Transactions, Vol. 75, Issue 15 https://doi.org/10.1149/07515.0397ecst	journal	August 2016
MetalWalls: A classical molecular dynamics software dedicated to the simulation of electrochemical systems Marin-Laflèche, Abel; Haefele, Matthieu; Scalfi, Laura Journal of Open Source Software, Vol. 5, Issue 53 https://doi.org/10.21105/joss.02373	journal	September 2020

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