Probing Electric Fields at the Ionic Liquid−Electrode Interface Using Sum Frequency Generation Spectroscopy and Electrochemistry

Baldelli, Steven

doi:10.1021/jp052913r

Cited by 171 publications

(206 citation statements)

References 44 publications

(71 reference statements)

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“…69 Negative temperat dence was observed for similar ILs and an Hg elec well as for molten salt electrolytes. 71 While Mo simulations, [72][73][74] modified MSA theory, 75 and DF have revealed that the DC can have both negative a temperature dependence for the restricted primitiv negative temperature dependence is expected for t and temperature of our simulations. that the use of single-frequency measurements could lead to misleading results [98][99][100] .…”

Section: B Capacitancementioning

confidence: 55%

Computer simulations of ionic liquids at electrochemical interfaces

Merlet¹,

Rotenberg²,

Madden³

et al. 2013

Phys. Chem. Chem. Phys.

155

188

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Ionic liquids are widely used as electrolytes in electrochemical devices. In this context, many experimental and theoretical approaches have been recently developed for characterizing their interface with electrodes. In this perspective article, we review the most recent advances in the field of computer simulations (mainly molecular dynamics). A methodology for simulating electrodes at constant electrical potential is presented. Several types of electrode geometries have been investigated by many groups, in order to model planar, corrugated and porous materials and we summarize the results obtained in terms of the structure of the liquids. This structure governs the quantity of charge which can be stored at the surface of the electrode for a given applied potential, which is the relevant quantity for the highly topical use of ionic liquids in supercapacitors (also known as electrochemical double-layer capacitors). A key feature, which was also shown by atomic force microscopy and surface force apparatus experiments, is the formation of a layered structure for all ionic liquids at the surface of planar electrodes. This organization cannot take place inside nanoporous electrodes, which results in a much better performance for the latter in supercapacitors. The agreement between simulations and electrochemical experiments remains qualitative only though, and we outline future directions which should enhance the predictive power of computer simulations. In the longer term, atomistic simulations will also be applied to the case of electron transfer reactions at the interface, enabling the application to a broader area of problems in electrochemistry, and the few recent works in this field are also commented upon.

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Section: B Capacitancementioning

confidence: 55%

Computer simulations of ionic liquids at electrochemical interfaces

Merlet¹,

Rotenberg²,

Madden³

et al. 2013

Phys. Chem. Chem. Phys.

155

188

View full text Add to dashboard Cite

show abstract

“…A study using imidazolium bistriflamide, (F 3 CSO 2 ) 2 N − and BF 4 − salts suggested that a model of alternating anion and cation layers may be applicable to the data [29,30]. Baldelli [31,32] concluded that the double layer is one ion layer thick using sum frequency generation spectroscopy and electrochemistry to probe the electric field at the ionic liquid/electrode interface. The double layer capacitance in an ionic liquid is considerably smaller than in an aqueous solution and less than that predicted by having a perfect Helmholtz layer at the interface, which could result from the presence of ion pairs at the electrode surface at all potentials.…”

Section: Why Use Ionic Liquids For Electrodeposition?mentioning

confidence: 99%

Why Use Ionic Liquids for Electrodeposition?

Abbott

Endres

MacFarlane

2017

Electrodeposition From Ionic Liquids

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With any great voyage of discovery the explorer should always be asked at the outset "Why are you doing this?" To answer the question "Why use ionic liquids for electrodeposition?" it is first necessary to look at current best practice and find its limitations.It is widely recognised that in 1805 Italian chemist, Luigi Brugnatelli made the first experiments in what we now know as electroplating. Brugnatelli used the newly discovered Voltaic Pile to deposit gold "I have lately gilt in a complete manner two large silver medals, by bringing them into communication by means of a steel wire, with a negative pole of a voltaic pile, and keeping them one after the other immersed in ammoniuret of gold newly made and well saturated" [1]. The process was later improved by John Wright who found that potassium cyanide was a beneficial electrolyte to add for silver and gold plating as it allowed thick adherent deposits to be obtained. Until the middle of the 19th century the production of jewellery and the gilding of decorative items were the main uses of electrodeposition.With an increased understanding of electrochemistry, the practice of metal deposition spread to non-decorative metals such as nickel, brass, tin, and zinc by the 1850s. Even though electroplated goods entered many aspects of manufacturing industry very little changed about the physical processes involved in electrodeposition for about 100 years. It was only with the advent of the electronics industry in the middle of the 20th century that significant changes occurred in the hardware and chemistry of the plating solutions. The post-war period saw an increase in gold plating for electronic components and the use of less hazardous plating solutions. This trend has continued with increased control of hazardous materials to the environment. Improved solution composition and power supply technology has allowed the development of fast and continuous plating of wire, metal strips, semiconductors and complex substrate geometries.Many of the technological developments seen in the electronics industry depend upon sophisticated electroplating including the use of exotic metals and this is one of the drivers for new technology within the electroplating sector. The other Electrodeposition from Ionic Liquids. Edited

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“…Despite the difficulties in precise alignment of the two incident beams through the solution phase and the very expensive and sophisticated equipment, successful application of SFG spectroscopy in studies of the electrode/ionic liquid interface has been performed. [30,47,[83][84][85][86][87] …”

Section: In Situ Characterizationmentioning

confidence: 99%

The Electrode/Ionic Liquid Interface: Electric Double Layer and Metal Electrodeposition

Wei

et al. 2010

ChemPhysChem

145

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The last decade has witnessed remarkable advances in interfacial electrochemistry in room‐temperature ionic liquids. Although the wide electrochemical window of ionic liquids is of primary concern in this new type of solvent for electrochemistry, the unusual bulk and interfacial properties brought about by the intrinsic strong interactions in the ionic liquid system also substantially influence the structure and processes at electrode/ionic liquid interfaces. Theoretical modeling and experimental characterizations have been indispensable in reaching a microscopic understanding of electrode/ionic liquid interfaces and in elucidating the physics behind new phenomena in ionic liquids. This Minireview describes the status of some aspects of interfacial electrochemistry in ionic liquids. Emphasis is placed on high‐resolution and molecular‐level characterization by scanning tunneling microscopy and vibrational spectroscopies of interfacial structures, and the initial stage of metal electrodeposition with application in surface nanostructuring.

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Probing Electric Fields at the Ionic Liquid−Electrode Interface Using Sum Frequency Generation Spectroscopy and Electrochemistry

Cited by 171 publications

References 44 publications

Computer simulations of ionic liquids at electrochemical interfaces

Computer simulations of ionic liquids at electrochemical interfaces

Why Use Ionic Liquids for Electrodeposition?

The Electrode/Ionic Liquid Interface: Electric Double Layer and Metal Electrodeposition

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