High-throughput computational design of cathode coatings for Li-ion batteries

Aykol, Muratahan; Kim, Soo Jeong; Hegde, V.; Snydacker, David H.; Lü, Zhi; Hao, Shiqiang; Kirklin, Scott; Morgan, Dane; Wolverton, Christopher

doi:10.1038/ncomms13779

Cited by 173 publications

(156 citation statements)

References 77 publications

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“…High-throughput calculations and computational screening are therefore needed to guide the discovery of the most promising candidates. [212][213][214] Reactive gas treatment (N 2 , O 2 , CO 2 , F 2 , and SO 2 ) on lithium metal can create a passivation layer with controlled structural, electronic, and elastic properties of the electrode surface. 215 Among the gases investigated by DFT and MD calculations, Koch et al 215 revealed that N 2 -treated adlayer is the most elastic compliant passivation layer for the interface between lithium and adsorbate, minimizing the possibility of crack formation and lithium dendrite growth.…”

Section: In Vitro Design Of the Seimentioning

confidence: 99%

Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries

et al. 2018

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A passivation layer called the solid electrolyte interphase (SEI) is formed on electrode surfaces from decomposition products of electrolytes. The SEI allows Li + transport and blocks electrons in order to prevent further electrolyte decomposition and ensure continued electrochemical reactions. The formation and growth mechanism of the nanometer thick SEI films are yet to be completely understood owing to their complex structure and lack of reliable in situ experimental techniques. Significant advances in computational methods have made it possible to predictively model the fundamentals of SEI. This review aims to give an overview of state-of-the-art modeling progress in the investigation of SEI films on the anodes, ranging from electronic structure calculations to mesoscale modeling, covering the thermodynamics and kinetics of electrolyte reduction reactions, SEI formation, modification through electrolyte design, correlation of SEI properties with battery performance, and the artificial SEI design. Multiscale simulations have been summarized and compared with each other as well as with experiments. Computational details of the fundamental properties of SEI, such as electron tunneling, Li-ion transport, chemical/mechanical stability of the bulk SEI and electrode/(SEI/) electrolyte interfaces have been discussed. This review shows the potential of computational approaches in the deconvolution of SEI properties and design of artificial SEI. We believe that computational modeling can be integrated with experiments to complement each other and lead to a better understanding of the complex SEI for the development of a highly efficient battery in the future.

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Section: In Vitro Design Of the Seimentioning

confidence: 99%

Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries

et al. 2018

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“…Hence, target strategies to enhance oxygen retention such as surface doping or coatings are of interest. Coating procedures, either by atomic layer deposition or chemical processes, are known as an efficient procedure to protect surfaces from various degradation processes including hydrofluoric acid attack and metal dissolution 9,10 ; however, surface coatings may also impede Li mobility 11 . On the other hand, it is reported that surface doping can minimize phase segregation or separation at interfaces during the cycling process 12 .…”

Section: Introductionmentioning

confidence: 99%

Alleviating oxygen evolution from Li-excess oxide materials through theory-guided surface protection

et al. 2018

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Li-excess cathodes comprise one of the most promising avenues for increasing the energy density of current Li-ion technology. However, the first-cycle surface oxygen release in these materials causes cation densification and structural reconstruction of the surface region, leading to encumbered ionic transport and increased impedance. In this work, we use the first principles Density Functional Theory to systematically screen for optimal cation dopants to improve oxygen-retention at the surface. The initial dopant set includes all transition metal, post-transition metal, and metalloid elements. Our screening identifies Os, Sb, Ru, Ir, or Ta as high-ranking dopants considering the combined criteria, and rationalization based on the electronic structure of the top candidates are presented. To validate the theoretical screening, a Ta-doped Li1.3Nb0.3Mn0.4O2 cathode was synthesized and shown to present initial improved electrochemical performance as well as significantly reduced oxygen evolution, as compared with the pristine, un-doped, system.

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“…Energy storage devices, such as Li‐ and Na‐ion batteries have been studied intensively by the first principles calculations and numerous papers have been published in the last two decades, providing useful insights about voltage dependence from charge carrier concentrations, phase transitions upon charge/discharge cycling, materials stability, charge carrier migration pathways and many other aspects. In these studies, the reliability of employed ab initio methodology is one of the key prerequisites, required for adequate description of studied phenomena, providing qualitative and, when required, quantitative agreement with experimental observations.…”

Section: Introductionmentioning

confidence: 99%

Theoretical Analysis of Materials, used in Energy Storage Applications: the Quest for Robust and Accurate Computational Methodologies

Shishkin

Sato

2018

The Chemical Record

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Study of materials, used as constituents for energy storage devices (e. g. Li‐ or Na‐ion batteries) has been greatly enhanced by the first principles theoretical modeling. As a prerequisite, accurate computational framework should be employed in order to provide adequate description of studied materials in close agreement with available experimental data. In this account we present our approach to formulation of a suite of computational techniques, that can be used for accurate evaluation of key materials properties with a moderate computational cost. Using the results of our calculations, we show that Hubbard corrected DFT+U method with self‐consistent evaluation of U parameters employing linear response approach can be used for accurate evaluation of redox potentials of cathode materials, although in some cases (e. g. Fe sulfates), addition of other corrections may be required. Moreover, we also provide examples of applications of developed techniques for construction of phase diagrams of cathode materials and analysis of the effects of doping of NaMnO2 cathodes. Finally, we discuss possible directions for future development of computational methodologies and propose new avenues for their applications in battery research.

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High-throughput computational design of cathode coatings for Li-ion batteries

Cited by 173 publications

References 77 publications

Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries

Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries

Alleviating oxygen evolution from Li-excess oxide materials through theory-guided surface protection

Theoretical Analysis of Materials, used in Energy Storage Applications: the Quest for Robust and Accurate Computational Methodologies

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