<i>In situ</i>non-linear spectroscopic approaches to understanding adsorption at mineral–water interfaces

Schrödle, Simon; Richmond, Geraldine L.

doi:10.1088/0022-3727/41/3/033001

Cited by 34 publications

(39 citation statements)

References 106 publications

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“…We have also highlighted the synergy between lithium ion battery modeling and theoretical studies of water-material interfaces. [48][49][50] Exchange of knowledge between these disciplines will accelerate progress in modeling battery processes where more fundamental modeling studies are necessary.…”

Section: Discussionmentioning

confidence: 99%

Electronic Structure Modeling of Electrochemical Reactions at Electrode/Electrolyte Interfaces in Lithium Ion Batteries

2012

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We review recent ab initio molecular dynamics studies of electrode/electrolyte interfaces in lithium ion batteries. Our goals are to introduce experimentalists to simulation techniques applicable to models which are arguably most faithful to experimental conditions so far, and to emphasize to theorists that the inherently interdisciplinary nature of this subject requires bridging the gap between solid and liquid state perspectives. We consider liquid ethylene carbonate (EC) decomposition on lithium intercalated graphite, lithium metal, oxide-coated graphite, and spinel manganese oxide surfaces. These calculations are put in the context of more widely studied watersolid interfaces. Our main themes include kinetically controlled two-electron-induced reactions, the breaking of a previously much neglected chemical bond in EC, and electron tunneling. Future work on modeling batteries at atomic lengthscales requires capabilities beyond state-of-the-art, which emphasizes that applied battery research can and should drive fundamental science development. keywords: solid electrolyte interphase; ab initio molecular dynamics; lithium manganese oxide; ethylene carbonate; electron transfer 1 I. INTRODUCTION: BACKGROUND AND CONTEXT Lithium ion batteries (LIB) are currently the devices being implemented or considered for large scale static and transportation energy storage. They carry high energy density and have the potential of dramatically reducing green house gas emission because they operate within a high voltage window. 1 Today's commercial LIBs (Fig. 1a) consist of graphitic carbon anodes, transition metal oxide cathodes, and organic solvent-based electrolyte. Other crucial LIB components include passivating "solid electrolyte interphase" (SEI) films formed from excess electron-induced electrolyte decomposition products on anode surfaces. 2-4 SEI films are heterogeneous in structure and consist of Li 2 CO 3 , ethylene dicarbonate (EDC), oligomeric/polymeric compounds, salt decomposition fragments, and other products. 2-4They prevent continuous electron injection into the electrolyte, averting further loss of Li + and electrolyte molecules. Li + transport through SEI films remains adequately fast. Oxidation products are also often found on cathode surfaces. New concepts of electrodes being pursued, such as Si-based anodes and "air" cathodes in metal-air batteries, share many solid-liquid interface features shown in Fig. 1a. LIBs are pragmatic devices. They combine our best electrochemical, solid, and liquid state expertise to deliver high volumetric and gravimetric energy/power densities. While all-solid batteries have received much attention for niche applications and all-liquid flow-cell batteries have significant potential for static storage, batteries featuring both liquid and solid components will undoubtedly dominate for the foreseeable future.It has been widely acknowledged that interfaces are critical for good performance and long lifetime in batteries. 5 To some extent, interfaces dictate the choice of electrode ...

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Section: Discussionmentioning

confidence: 99%

Electronic Structure Modeling of Electrochemical Reactions at Electrode/Electrolyte Interfaces in Lithium Ion Batteries

2012

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“…The principle is that two incident laser beams (IR beam and visible beam) of frequencies ω IR and ω vis , respectively, overlap at a surface of a material. An output beam is generated with a frequency ω SF , that equals the sum of the two input beams (Nickolov et al, 2004;Schrödle and Richmond, 2008;Van Loon and Allen, 2004;Van Loon et al, 2007).…”

Section: Sum Frequency Vibrational Spectroscopy (Sfvs)mentioning

confidence: 99%

Surface chemistry aspects of bastnaesite flotation with octyl hydroxamate

Zhang

Wang

et al. 2014

International Journal of Mineral Processing

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Surface chemistry features of bastnaesite were investigated with respect to octyl hydroxamate adsorption and the wetting characteristics at different levels of hydroxamate adsorption. The wetting characteristics of bastnaesite in the absence of collector adsorption were examined using both contact angle measurements and MD simulations. As expected, it was found that bastnaesite is naturally hydrophilic. Surface chemistry studies included octyl hydroxamate adsorption by the solution depletion method. The surface state was described by sum-frequency vibrational spectroscopy (SFVS) and molecular dynamic simulations (MDS). The adsorption isotherm at low levels of hydroxamate adsorption was established and the hydrophobic surface state described from contact angle measurements. The relationship between hydrophobicity and adsorption density was examined for the first time by MD simulations. The SFVS spectra indicate that a well-ordered monolayer was formed at a hydroxamate concentration of about 1 ×10-4 M.

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“…The ability to selectively probe interfacial molecules and provide molecular-level information makes techniques such as VSFG powerful tools for the study of interfacial processes. As such, studies utilizing VSFG, along with accompanying theoretical work, have provided much insight into the behavior of molecules at interfaces (10,(12)(13)(14)(15)(16)(17)(18)(19)(20)(21)(22)(23)(24)(25).…”

Section: Introductionmentioning

confidence: 99%

Environmental Chemistry at Vapor/Water Interfaces: Insights from Vibrational Sum Frequency Generation Spectroscopy

Jubb

Wei

Allen

2012

Annu. Rev. Phys. Chem.

149

263

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The chemistry that occurs at surfaces has been an intense area of study for many years owing to its complexity and importance in describing a wide range of physical phenomena. The vapor/water interface is particularly interesting from an environmental chemistry perspective as this surface plays host to a wide range of chemistries that influence atmospheric and geochemical interactions. The application of vibrational sum frequency generation (VSFG), an inherently surface-specific, even-order nonlinear optical spectroscopy, enables the direct interrogation of various vapor/aqueous interfaces to elucidate the behavior and reaction of chemical species within the surface regime. In this review we discuss the application of VSFG to the study of a variety of atmospherically important systems at the vapor/aqueous interface. Chemical systems presented include inorganic ionic solutions prevalent in aqueous marine aerosols, small molecular solutes, and long-chain fatty acids relevant to fat-coated aerosols. The ability of VSFG to probe both the organization and reactions that may occur for these systems is highlighted. A future perspective toward the application of VSFG to the study of environmental interfaces is also provided.

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In situnon-linear spectroscopic approaches to understanding adsorption at mineral–water interfaces

Cited by 34 publications

References 106 publications

Electronic Structure Modeling of Electrochemical Reactions at Electrode/Electrolyte Interfaces in Lithium Ion Batteries

Electronic Structure Modeling of Electrochemical Reactions at Electrode/Electrolyte Interfaces in Lithium Ion Batteries

Surface chemistry aspects of bastnaesite flotation with octyl hydroxamate

Environmental Chemistry at Vapor/Water Interfaces: Insights from Vibrational Sum Frequency Generation Spectroscopy

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