Thermodynamic Aspects of Cathode Coatings for Lithium‐Ion Batteries

Aykol, Muratahan; Kirklin, Scott; Wolverton, Christopher

doi:10.1002/aenm.201400690

Cited by 102 publications

(112 citation statements)

References 90 publications

(231 reference statements)

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“…We stress, however, that the techniques are directly transferable to other battery components, such as anode materials, [20][21][22][23] solid electrolytes, 12,13,24 and electrode surface coatings. 25 …”

Section: Introductionmentioning

confidence: 99%

Computational understanding of Li-ion batteries

2016

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Over the last two decades, computational methods have made tremendous advances, and today many key properties of lithium-ion batteries can be accurately predicted by first principles calculations. For this reason, computations have become a cornerstone of battery-related research by providing insight into fundamental processes that are not otherwise accessible, such as ionic diffusion mechanisms and electronic structure effects, as well as a quantitative comparison with experimental results. The aim of this review is to provide an overview of state-of-the-art ab initio approaches for the modelling of battery materials. We consider techniques for the computation of equilibrium cell voltages, 0-Kelvin and finite-temperature voltage profiles, ionic mobility and thermal and electrolyte stability. The strengths and weaknesses of different electronic structure methods, such as DFT+U and hybrid functionals, are discussed in the context of voltage and phase diagram predictions, and we review the merits of lattice models for the evaluation of finite-temperature thermodynamics and kinetics. With such a complete set of methods at hand, first principles calculations of ordered, crystalline solids, i.e., of most electrode materials and solid electrolytes, have become reliable and quantitative. However, the description of molecular materials and disordered or amorphous phases remains an important challenge. We highlight recent exciting progress in this area, especially regarding the modelling of organic electrolytes and solid-electrolyte interfaces.

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Section: Introductionmentioning

confidence: 99%

Computational understanding of Li-ion batteries

2016

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“…[4,5] The coating materials investigated to date include various carbons, [6] metal oxides, [7] metal phosphates, [8] metal fluorides, [9] etc. Many coating materials on the one hand may suppress metal dissolution or provide anti-corrosion properties [10,11] successfully, however on the other hand, they often introduce other problems such as decreasing Li mobility [12] or discontinuity of volume [13] and hence design and choice of coating materials are difficult, but critical to help improve overall performance.…”

Section: Introductionmentioning

confidence: 99%

Quaternary phase diagrams of spinelLiy□1−yMnxNi2−xO4
Hao
¹
,
Lü
²
,
Wolverton
³

2016
Phys. Rev. B
6
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“…For instance, reactivity between coatings and HF in the electrolyte has been studied by Aykol et al 24 These authors provided a thermodynamic framework for determining coatings that can react with (or scavenge) HF, as well as those that can provide a stable barrier to HF.…”

Section: -9mentioning

confidence: 99%

“…[13][14][15][16][17][18][19] Surface coatings can perform a variety of functions for different cathode materials. [20][21][22][23][24][25][26][27][28][29][30][31][32] In this work, we evaluate the ability of coating materials to contain TMs in the cathode and thereby prevent TM dissolution into the electrolyte.To evaluate a coating material for TM containment, we use two criteria: 1) A coating material should exhibit low TM solubility. If a coating exhibits high TM solubility, then TMs can be present in the coating near the particle surface, where they are susceptible to dissolution into the electrolyte.…”

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Lithium-Ion Cathode/Coating Pairs for Transition Metal Containment

Snydacker

Aykol

Kirklin

et al. 2016

J. Electrochem. Soc.

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For many lithium-ion cathode materials, transition metal (TM) dissolution into the electrolyte contributes to cell degradation. Cathode coatings can limit TM dissolution by containing TMs in cathode materials. We perform density functional theory calculations to evaluate cathode/coating pairs for TM containment, specifically focusing on reactive stability of coating/cathode pairs as well as TM solubility in the coating materials. We consider stability and containment of materials at both synthesis and operating conditions. We find that many cathode/coating pairs are reactive when lithiated, while other cathode-coating pairs are stable when lithiated but become reactive following delithiation. Of all the coatings that we considered, Li 3 PO 4 occupies a unique chemical position, in that its coatings on oxide cathode materials maintained equilibrium under both lithiated and delithiated conditions. Furthermore, for oxide cathode materials, the Li 3 PO 4 coatings exhibit low TM solubilities across all cathode states of charge. Our results demonstrate that Li 3 PO 4 is a promising candidate for stable coatings on oxide cathode materials to limit TM dissolution into the electrolyte. Li-ion batteries are the dominant power sources in consumer electronics, and they are emerging as cost-competitive players in lowcarbon electricity systems and vehicles. However, many technologies are encumbered by the limited durability of today's Li-ion cells. For these applications, battery manufacturers have an incentive to improve cell durability. Transition metal (TM) dissolution from the cathode is a major contributor to cell degradation during cycling and aging.1 TM dissolution from the cathode contributes directly to capacity loss by decreasing the amount of cathode material. Furthermore, TMs that dissolve from the cathode material can migrate through the electrolyte to the anode, where they can cause changes to the anode Solid Electrolyte Interphase (SEI).2,3 These changes to the SEI increase impedance, decrease cell capacity, and decrease lifespan.A variety of strategies have been used to limit degradation by TMs. Electrolyte additives have been used to control SEI formation and limit the impact of TMs in the electrolyte. 4,5 Molecules have been attached to the polymer separator to sequester TMs from the electrolyte before they reach the anode. 6 In this work, we consider upstream strategies that limit TM dissolution from the cathode into the electrolyte. These upstream strategies are complementary to other strategies, including SEI formation and TM sequestration. There are several distinct categories of strategies for limiting TM dissolution from the cathode. Electrolytes can be tailored to reduce reactivity with the cathode. 7-9Cathode materials can be doped to control the oxidation states of transition metals. 10,11 This doping can be applied to the entire cathode particle or just near the surface.12 Cathode materials can also be covered with surface coatings to limit TM dissolution. [13][14][15][16][17][18][19] Surface coati...

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Thermodynamic Aspects of Cathode Coatings for Lithium‐Ion Batteries

Cited by 102 publications

References 90 publications

Computational understanding of Li-ion batteries

Computational understanding of Li-ion batteries

Quaternary phase diagrams of spinelLiy□1−yMnxNi2−xO4
Hao
¹
,
Lü
²
,
Wolverton
³

2016
Phys. Rev. B
6
1
4
0
View full text Add to dashboard Cite

Lithium-Ion Cathode/Coating Pairs for Transition Metal Containment

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Thermodynamic Aspects of Cathode Coatings for Lithium‐Ion Batteries

Cited by 102 publications

References 90 publications

Computational understanding of Li-ion batteries

Computational understanding of Li-ion batteries

Quaternary phase diagrams of spinelLiy□1−yMnxNi2−xO4Hao1, Lü2, Wolverton3 2016Phys. Rev. B6140View full textAdd to dashboardCite

Lithium-Ion Cathode/Coating Pairs for Transition Metal Containment

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About

Quaternary phase diagrams of spinelLiy□1−yMnxNi2−xO4
Hao
¹
,
Lü
²
,
Wolverton
³

2016
Phys. Rev. B
6
1
4
0
View full text Add to dashboard Cite