Lithium Transport in Amorphous Al2O3 and AlF3 for Discovery of Battery Coatings

Hao, Shiqiang; Wolverton, Christopher

doi:10.1021/jp311982d

Cited by 106 publications

(105 citation statements)

References 36 publications

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“…Instead, the diffusion was directly modeled by applying periodic boundary conditions to the simulation cell where the Cs interstitial sites were identified by the DFT calculations. A similar approach in a finite cell with periodic boundary conditions successfully modeled the Li diffusion in amorphous (a-) materials, e.g., a-Si 51 , a-Al2O3 52 , and a-AlF3 52 , where they generally showed good agreements with experimental diffusion rates when the comparison was possible.…”

Section: Kinetic Monte Carlo Modelmentioning

confidence: 93%

Cs diffusion in SiC high-energy grain boundaries

Szlufarska

Morgan

2017

Journal of Applied Physics

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Cesium (Cs) is a radioactive fission product whose release is of concern for Tristructural-Isotropic (TRISO) fuel particles. In this work, Cs diffusion through high energy grain boundaries (HEGBs) of cubic-SiC is studied using an ab-initio based kinetic Monte Carlo (kMC) model. The HEGB environment was modeled as an amorphous SiC (a-SiC), and Cs defect energies were calculated using density functional theory (DFT). From defect energies, it was suggested that the fastest diffusion mechanism as Cs interstitial in an amorphous SiC. The diffusion of Cs interstitial was simulated using a kMC, based on the site and transition state energies sampled from the DFT. The Cs HEGB diffusion exhibited an Arrhenius type diffusion in the range of 1200-1600°C. The comparison between HEGB results and the other studies suggests not only that the GB diffusion dominates the bulk diffusion, but also that the HEGB is one of the fastest grain boundary paths for the Cs diffusion. The diffusion coefficients in HEGB are clearly a few orders of magnitude lower than the reported diffusion coefficients from in-and out-of-pile samples, suggesting that other contributions are responsible, such as a radiation enhanced diffusion.

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Section: Kinetic Monte Carlo Modelmentioning

confidence: 93%

Cs diffusion in SiC high-energy grain boundaries

Szlufarska

Morgan

2017

Journal of Applied Physics

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“…The Li diffusivity in the layered-structured Li x MO 2 material is relatively low, in the range of 10 -8 to 10 -13 cm 2 /s. [23][24][25][26] In the solid electrolyte "blue" materials Li 10 GeP 2 S 12 and Li 7 P 3 S 11 , the diffusivity is faster, in the range of about 10 -6 -10 -7 cm 2 /s, which is ≥2 orders of magnitude faster than that in the "red" Li x MO 2 . This heterostructured cathode material could be intercalated primarily through the fast "blue" material, requiring Li migration through only a few nanometers in the "red" high-voltage material.…”

Section: Utilization Of Multiple-redox Transition Metal Atoms With a mentioning

confidence: 98%

“…Some possible specific pairs of the "red" and "blue" materials could be Li x NiO 2 as the high-voltage "red" material and a solid electrolyte material (e.g. Li 10 GeP 2 S 12 or Li 7 P 3 S 11 ) as the low-voltage "blue" material. The Li diffusivity in the layered-structured Li x MO 2 material is relatively low, in the range of 10 -8 to 10 -13 cm 2 /s.…”

Section: Utilization Of Multiple-redox Transition Metal Atoms With a mentioning

confidence: 99%

“…Moreover, interfaces inevitably occur for cathode particles at their surface, either with a solid electrolyte interphase (SEI) or frequently a protective coating layer, the latter of which is typically comprised of insulating metal oxides or fluorides [7][8][9][10][11][12][13][14][15] or sometimes an electrochemically active material (e.g., Li-Ni-PO 4 coating layer) 16 .…”

Section: Introductionmentioning

confidence: 99%

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Nanoscale Voltage Enhancement at Cathode Interfaces in Li-Ion Batteries

Xu¹,

Jacobs²,

Wolverton

et al. 2017

Chem. Mater.

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Abstract:Interfaces are ubiquitous in Li-ion battery electrodes, occurring across compositional gradients, regions of multiphase intergrowths, and between electrodes and solid electrolyte interphases or protective coatings. However, the impact of these interfaces on Li energetics remains largely unknown. In this work, we calculated Li intercalation-site energetics across cathode interfaces and demonstrated the physics governing these energetics on both sides of the interface. We studied the olivine/olivine-structured

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“…Atomic-layer deposition of Al 2 O 3 has been used to provide ultrathin (a few nm) and uniform coatings. Using DFT methods, Hao et al 155 showed that Li diffusion in Al 2 O 3 through the interstitial mechanism is slow. Jung et al 156 studied Al 2 O 3 lithiation to form amorphous Li-Al 2 O 3 coating layers using AIMD and found that the Li diffusion is significantly enhanced at the lithiated state.…”

Section: Silicon and Other Anodesmentioning

confidence: 99%

Computational studies of solid-state alkali conduction in rechargeable alkali-ion batteries

Deng

Ong

2016

NPG Asia Mater

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The facile conduction of alkali ions in a crystal host is of crucial importance in rechargeable alkali-ion batteries, the dominant form of energy storage today. In this review, we provide a comprehensive survey of computational approaches to study solid-state alkali diffusion. We demonstrate how these methods have provided useful insights into the design of materials that form the main components of a rechargeable alkali-ion battery, namely the electrodes, superionic conductor solid electrolytes and interfaces. We will also provide a perspective on future challenges and directions. The scope of this review includes the monovalent lithium-and sodium-ion chemistries that are currently of the most commercial interest. NPG Asia Materials (2016) 8, e254; doi:10.1038/am.2016.7; published online 25 March 2016 INTRODUCTIONThe facile conduction of alkali ions in a crystal is of critical importance in energy storage. Today, the dominant form of energy storage in consumer electronics is the rechargeable lithium-ion (Li-ion) battery, 1-5 a device that functions entirely on the basis of the reversible transport of Li + ions. With one of the highest energy densities of known energy storage technologies, Li-ion batteries are finding increasingly large-scale applications in electrified transportation and grid storage. In recent years, there has also been a resurgence of interest in rechargeable sodium-ion (Na-ion) batteries, 6-12 which function on the same basic principle but with Na + instead of Li + because of concerns regarding the abundance and cost of lithium. Figure 1 shows a representation of a rechargeable alkali-ion battery. The typical electrode in an alkali-ion battery is an intercalation compound, which, as the name implies, stores alkali ions by inserting them into its crystal structure in a topotactic manner. During discharge, A + ions are transported from the anode, through the electrolyte and into the cathode. The reverse happens during charge. Throughout this review, we will adopt the customary terminology of defining the 'cathode' as the positive electrode during discharge, even though the formal definition of the cathode changes depending on whether the charging or discharging process is being referred to. Current cathodes are typically transition metal oxides, and the insertion/removal of each A + in the cathode is accompanied by the concomitant reduction/oxidation of a transition metal ion to accommodate the compensating insertion/removal of an electron. Graphitic carbon is the most common anode.The performance of a rechargeable alkali-ion battery depends crucially on the ease with which alkali ions move in the host crystal of the cathode and anode, in the electrolyte, and in the electrodeelectrolyte interface. Poor alkali transport in any part of the battery

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Lithium Transport in Amorphous Al₂O₃ and AlF₃ for Discovery of Battery Coatings

Cited by 106 publications

References 36 publications

Cs diffusion in SiC high-energy grain boundaries

Cs diffusion in SiC high-energy grain boundaries

Nanoscale Voltage Enhancement at Cathode Interfaces in Li-Ion Batteries

Computational studies of solid-state alkali conduction in rechargeable alkali-ion batteries

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