A perspective on inverse design of battery interphases using multi-scale modelling, experiments and generative deep learning

Bhowmik, Arghya; Castelli, Ivano E.; Garcı́a-Lastra, J. M.; Jørgensen, Peter Bjørn; Winther, Ole; Vegge, Tejs

doi:10.1016/j.ensm.2019.06.011

Cited by 112 publications

(116 citation statements)

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“…Furthermore, the fundamentals of ASSBs were reviewed by several authors [ 28 , 29 , 30 , 31 , 32 , 33 , 34 , 35 ]. The number of reviews on various aspects of electrolytes, cathodes, mechanical properties, and interface engineering has grown exponentially since 2018 [ 36 , 37 , 38 , 39 , 40 , 41 , 42 , 43 , 44 , 45 , 46 , 47 , 48 , 49 , 50 , 51 , 52 , 53 , 54 , 55 , 56 , 57 , 58 , 59 , 60 , 61 , 62 , 63 , 64 , 65 , 66 , 67 , 68 , 69 , 70 , 71 , 72 , 73 , 74 , 75 , 76 , 77 , 78 ...…”

Section: Introductionmentioning

confidence: 99%

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

et al. 2020

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Energy storage materials are finding increasing applications in our daily lives, for devices such as mobile phones and electric vehicles. Current commercial batteries use flammable liquid electrolytes, which are unsafe, toxic, and environmentally unfriendly with low chemical stability. Recently, solid electrolytes have been extensively studied as alternative electrolytes to address these shortcomings. Herein, we report the early history, synthesis and characterization, mechanical properties, and Li+ ion transport mechanisms of inorganic sulfide and oxide electrolytes. Furthermore, we highlight the importance of the fabrication technology and experimental conditions, such as the effects of pressure and operating parameters, on the electrochemical performance of all-solid-state Li batteries. In particular, we emphasize promising electrolyte systems based on sulfides and argyrodites, such as LiPS5Cl and β-Li3PS4, oxide electrolytes, bare and doped Li7La3Zr2O12 garnet, NASICON-type structures, and perovskite electrolyte materials. Moreover, we discuss the present and future challenges that all-solid-state batteries face for large-scale industrial applications.

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Section: Introductionmentioning

confidence: 99%

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

et al. 2020

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“…The other is the construction of capacitive cathode and battery-type anode. 9,[13][14][15][16] In 2001, Amatucci et al had developed the system which consists of nano-Li 4 Ti 5 O 12 as the battery-type anode and N-doped activated carbon as the capacitor-type cathode. 17 However, on account of the different mechanisms of energy storage, the power and energy densities depends on the faradaic-type anode with sluggish reaction kinetics and the adsorption-type cathode with low capacity, respectively.…”

Section: Introductionmentioning

confidence: 99%

MoS₂/carbon composites prepared by ball-milling and pyrolysis for the high-rate and stable anode of lithium ion capacitors

et al. 2019

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“…36 They found that the initial SEI produced in the presence of K + is enriched in LiF and depleted in other F-containing species. In contrast, 19 F SSNMR measurements performed on our electrodes after extended cycling show that KPF6 addition results in enrichment of other F-containing species (e.g. organofluorides), but the amount of LiF remains either unchanged ( Figure S9) or decreases ( Figure S10).…”

Section: Discussionmentioning

confidence: 79%

“…Higher samples dilutions were used to fill the volume of 3.2 mm o.d. ZrO2 rotors for analysis with 19 F SSNMR. Before loading into the SSNMR probehead, filled rotors were weighed to allow for quantitative comparison of the resulting SSNMR spectra.…”

Section: Solid-state Nmr Measurementsmentioning

confidence: 99%

“…[12][13][14][15][16][17] Among these, altering the solid electrolyte interphase (SEI) that forms on the electrode surface is a simple and scalable approach that can readily produce low-surface area Li deposits and improved Coulombic efficiency in Li metal batteries. 2,11,[18][19][20] Widely used strategies to control the composition and thickness of the SEI include tailoring the anion of the Li salt, 21 increasing the concentration of the electrolyte, [22][23][24][25][26] and using sacrificial organic electrolyte additives. [27][28][29] These strategies lead to increased amounts of LiF, cross-linking polymeric species, and polyene moieties in the SEI that are correlated with improved battery performance.…”

Section: Introductionmentioning

confidence: 99%

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Leveraging Cation Identity to Engineer Solid Electrolyte Interphases for Rechargeable Lithium Metal Anodes

May¹,

Denny²,

Viswanathan³

et al. 2020

Preprint

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Lithium metal anodes enable substantially higher energy density than current technologies for Li batteries. However, rechargeable Li metal anodes suffer from low Coulombic efficiency (loss of electrochemically active Li), leading to poor cycle life and safety. Engineering the electrolyte formulation to form a stable, well-functioning solid electrolyte interphase (SEI) is a promising approach to improving these performance figures of merit. While design rules have been established for selecting electrolyte solvents and salt anions to establish a more robust SEI, the impact of altering cation identity is not well understood. In this work, we demonstrate that alkali metal additives (here, K+) alter SEI composition and thickness. Through post-mortem elemental analyses, we show that K+ ions do not directly participate in metal electrodeposition, but rather modify the chemical and electrochemical reactivity of the electrode-electrolyte interface. Through a combination of quantitative nuclear magnetic resonance (NMR) spectroscopic characterization and density functional theory (DFT) simulations, we show that decomposition of electrolyte solvent molecules, ethylene carbonate (EC) and dimethyl carbonate (DMC), at the lithium metal surface is suppressed in the presence of a K+ additive. We attribute this to K+ being a softer cation compared to Li+, leading to preferred pair formation between K+ and the soft base carbonates, and thus increased salt-solvent coordination. Electrolyte cation engineering is an underexplored strategy to control the SEI, and we believe that the mechanistic understanding and insight developed in this work will spur further investigation of this promising approach.

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A perspective on inverse design of battery interphases using multi-scale modelling, experiments and generative deep learning

Cited by 112 publications

References 113 publications

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

MoS₂/carbon composites prepared by ball-milling and pyrolysis for the high-rate and stable anode of lithium ion capacitors

Leveraging Cation Identity to Engineer Solid Electrolyte Interphases for Rechargeable Lithium Metal Anodes

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A perspective on inverse design of battery interphases using multi-scale modelling, experiments and generative deep learning

Cited by 112 publications

References 113 publications

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

MoS2/carbon composites prepared by ball-milling and pyrolysis for the high-rate and stable anode of lithium ion capacitors

Leveraging Cation Identity to Engineer Solid Electrolyte Interphases for Rechargeable Lithium Metal Anodes

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Product

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MoS₂/carbon composites prepared by ball-milling and pyrolysis for the high-rate and stable anode of lithium ion capacitors