Electrolyte Structure of Lithium Polysulfides with Anti‐Reductive Solvent Shells for Practical Lithium–Sulfur Batteries

Zhang, Xueqiang; Jin, Qi; Nan, Yiling; Hou, Li‐Peng; Li, Bo‐Quan; Chen, Xiang; Zhang, Xitian; Huang, Jia‐Qi; Zhang, Qiang

doi:10.1002/anie.202103470

Cited by 137 publications

(42 citation statements)

References 54 publications

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“…Despite this, they can play a role in the second solvation shell. As proposed by Zhang and co-workers, di-isopropyl ether (DIPE) and di-isopropyl sulfide (DIPS) serve as cosolvents to encapsulate the first solvation shell of lithium-polysulfides, which significantly suppresses the parasitic reactions between encapsulated polysulfides and the Li metal anode. , …”

Section: Electrolyte Microstructuresmentioning

confidence: 99%

Applying Classical, Ab Initio, and Machine-Learning Molecular Dynamics Simulations to the Liquid Electrolyte for Rechargeable Batteries

et al. 2022

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Rechargeable batteries have become indispensable implements in our daily life and are considered a promising technology to construct sustainable energy systems in the future. The liquid electrolyte is one of the most important parts of a battery and is extremely critical in stabilizing the electrode–electrolyte interfaces and constructing safe and long-life-span batteries. Tremendous efforts have been devoted to developing new electrolyte solvents, salts, additives, and recipes, where molecular dynamics (MD) simulations play an increasingly important role in exploring electrolyte structures, physicochemical properties such as ionic conductivity, and interfacial reaction mechanisms. This review affords an overview of applying MD simulations in the study of liquid electrolytes for rechargeable batteries. First, the fundamentals and recent theoretical progress in three-class MD simulations are summarized, including classical, ab initio, and machine-learning MD simulations (section 2). Next, the application of MD simulations to the exploration of liquid electrolytes, including probing bulk and interfacial structures (section 3), deriving macroscopic properties such as ionic conductivity and dielectric constant of electrolytes (section 4), and revealing the electrode–electrolyte interfacial reaction mechanisms (section 5), are sequentially presented. Finally, a general conclusion and an insightful perspective on current challenges and future directions in applying MD simulations to liquid electrolytes are provided. Machine-learning technologies are highlighted to figure out these challenging issues facing MD simulations and electrolyte research and promote the rational design of advanced electrolytes for next-generation rechargeable batteries.

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Section: Electrolyte Microstructuresmentioning

confidence: 99%

Applying Classical, Ab Initio, and Machine-Learning Molecular Dynamics Simulations to the Liquid Electrolyte for Rechargeable Batteries

et al. 2022

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“…In the regular aqueous solution, zinc ions are primarily coordinated with solvent water molecules. [ 24 ] The fact that the water molecules either corrupt zinc metal or participate in dissolving cathode species are unpopularized for bilateral interfaces. Many scheduling strategies of electrolytes, especially the concentrated electrolytes such as “water‐in‐salt” electrolyte and molecular crowding electrolyte, have been reported to exert restriction of water to the utmost.…”

Section: Introductionmentioning

confidence: 99%

Hydrogen Bond‐Functionalized Massive Solvation Modules Stabilizing Bilateral Interfaces

Chen

Guo

Qin

et al. 2022

Adv Funct Materials

114

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Although mild aqueous electrolytes endow zinc‐ion batteries with intrinsic security surpassing that of lithium‐ion batteries, whether irreversible zinc deposition and related corrosion on the anode or cathode species dissolution severely circumscribes their cyclic stability, especially at low current density. Here, hydrogen bond‐functionalized massive solvation modules in a maltose‐based hybrid electrolyte are constructed, which is crucial for the stability of bilateral interfaces in the cycling process, to address this infamous issue. The intensive solvated interactions and diffusion hindrance effect yield uniform deposition of zinc at the anode interface, while the hydrogen bond confinement to free water interdicts derived parasitic reactions. As for the cathode interface, the massive solvation modules avoid structural framework collapse from vanadium dissolution and preserve low interfacial activation energy during cycling. The above bilateral interface regulation enables resultant full batteries to unprecedentedly maintain 84.2% of its initial specific capacity after 400 continuous cycles even at a very low current density of 50 mA g–1. This work provides a new perspective toward economical and eco‐friendly electrolytes for stable aqueous batteries.

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“…They store energy via insertion/extraction of Li ions, which highly depends on the crystal structure and limits their capacities and energy densities (<300 mAh⋅g −1 with energy density of <1,000 Wh⋅kg −1 ). Some new battery systems with conversion reaction cathodes, such as Li-S (2,600 Wh⋅kg −1 ) and Li-O 2 (3,450 Wh⋅kg −1 ) batteries ( 13 – 19 ), have been extensively investigated due to their high theoretical energy densities. However, they suffer from serious dissolution, interfacial stability, and/or side reaction issues, and the practical energy densities are much lower than their theoretical values.…”

mentioning

confidence: 99%

A nitroaromatic cathode with an ultrahigh energy density based on six-electron reaction per nitro group for lithium batteries

Chen

Sun

et al. 2022

Proc. Natl. Acad. Sci. U.S.A.

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Organic electrode materials have emerged as promising alternatives to conventional inorganic materials because of their structural diversity and environmental friendliness feature. However, their low energy densities, limited by the single-electron reaction per active group, have plagued the practical applications. Here, we report a nitroaromatic cathode that performs a six-electron reaction per nitro group, drastically improving the specific capacity and energy density compared with the organic electrodes based on single-electron reactions. Based on such a reaction mechanism, the organic cathode of 1,5-dinitronaphthalene demonstrates an ultrahigh specific capacity of 1,338 mAh⋅g−1 and energy density of 3,273 Wh⋅kg−1, which surpass all existing organic cathodes. The reaction path was verified as a conversion from nitro to amino groups. Our findings open up a pathway, in terms of battery chemistry, for ultrahigh-energy-density Li-organic batteries.

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Electrolyte Structure of Lithium Polysulfides with Anti‐Reductive Solvent Shells for Practical Lithium–Sulfur Batteries

Cited by 137 publications

References 54 publications

Applying Classical, Ab Initio, and Machine-Learning Molecular Dynamics Simulations to the Liquid Electrolyte for Rechargeable Batteries

Applying Classical, Ab Initio, and Machine-Learning Molecular Dynamics Simulations to the Liquid Electrolyte for Rechargeable Batteries

Hydrogen Bond‐Functionalized Massive Solvation Modules Stabilizing Bilateral Interfaces

A nitroaromatic cathode with an ultrahigh energy density based on six-electron reaction per nitro group for lithium batteries

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