Molecular design for electrolyte solvents enabling energy-dense and long-cycling lithium metal batteries

Yu, Zhiao; Wang, Hansen; Kong, Xian; Huang, William; Tsao, Yuchi; Mackanic, David G.; Wang, Kecheng; Wang, Xinchang; Huang, Wenxiao; Choudhury, Snehashis; Zheng, Yu; Amanchukwu, Chibueze V.; Hung, Samantha T.; Ma, Yuting; Lomeli, Eder G.; Qin, Jian; Cui, Yi; Bao, Zhenan

doi:10.1038/s41560-020-0634-5

Cited by 849 publications

(858 citation statements)

References 61 publications

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“…In response to these challenges, various strategies, such as the use of different solvents, [ 10–12 ] the optimization of Li salt concentrations, [ 13–15 ] the addition of functionalized additives, [ 16–18 ] and the design of electrolyte nanostructures, [ 19–21 ] have been proposed to construct a stable SEI film on the surface of Li metal anodes. These modifications of the in‐situ formed SEI films could enable uniform Li deposition and suppress Li dendrite growth in initial cycles.…”

Section: Introductionmentioning

confidence: 99%

Robust Artificial Solid‐Electrolyte Interfaces with Biomimetic Ionic Channels for Dendrite‐Free Li Metal Anodes

Jiang

et al. 2020

Advanced Energy Materials

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A robust artificial solid electrolyte interphase (SEI) film with biomimetic ionic channels and high stability is rationally designed and fabricated by combining the ClO4−‐decorated metal‐organic framework (UiO‐66‐ClO4) and flexible lithiated Nafion binder (Li‐Nafion). The high electronegativity and lithiophilicity of ClO4− groups chemically anchored into the UiO‐66 channels endow the SEI film with an excellent single‐ion conducting pathway, high Li+ transference number, and outstanding ionic conductivity, which can effectively prohibit undesirable reactions of the Li metal with the electrolyte and regulate fast and uniform Li+ flux. With further assistance of the flexible Li‐Nafion binder, the resulting UiO‐66‐ClO4/Li‐Nafion (UCLN) composite film exhibits an excellent mechanical strength to suppress the growth of Li dendrites and maintain the integral stability of the Li metal anodes during cycling. Consequently, the UCLN coated Li metal anodes (Li@UCLN) deliver remarkable cycling stabilities even under a high current density of up to 20 mA cm−2 and large areal capacity of up to 30 mAh cm−2, as well as enhanced rate capacities and cycle lifespans in the full cells even under the harsh conditions for high‐energy density applications.

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Section: Introductionmentioning

confidence: 99%

Robust Artificial Solid‐Electrolyte Interfaces with Biomimetic Ionic Channels for Dendrite‐Free Li Metal Anodes

Jiang

et al. 2020

Advanced Energy Materials

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“…Very recently, Bao's group reported a new solvent, 1,4‐dimethoxy‐2,2,3,3‐tetrafluorobutane or fluorinated 1,4‐dimethoxylbutane (Figure 4c), which can be combined with LiFSI to make a single‐salt single‐solvent electrolyte at 1 m concentration for LMBs. [ 49 ] The SEI formed in this electrolyte is ultrathin (≈6 nm), uniform, amorphous, and rich in F, S, and O species. Such an SEI could effectively protect Li metal anode and enable high Li CE of about 99.5% and long cycling stability of Li||NMC cells.…”

Section: Factors Affecting the Properties Of Solid Electrolyte Interpmentioning

confidence: 99%

Recent Progress in Understanding Solid Electrolyte Interphase on Lithium Metal Anodes

Jia

Wang

et al. 2020

Advanced Energy Materials

373

339

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Lithium metal batteries (LMBs) are one of the most promising candidates for next‐generation high‐energy‐density rechargeable batteries. Solid electrolyte interphase (SEI) on Li metal anodes plays a significant role in influencing the Li deposition morphology and the cycle life of LMBs. However, a thorough understanding on the mechanisms of SEI formation and evolution is still inadequate. In this review, the progress in understanding structures, properties, and influencing factors of SEI, as well as efficient strategies of tailoring SEI are focused upon. First, the compositions, models, and recent progress in characterizing atomic structures of SEI are summarized. Second, the properties of SEI, including electronic conduction, ionic conduction, stability, and mechanical properties are elucidated. Structures and properties of SEI are greatly affected by multiple factors, thus interactions between these factors and SEI are systematically discussed. Correlations of SEI with Li deposition morphology, rate capability, and cycle life are further summarized. Moreover, efficient strategies of tailoring SEI with desired properties, including in situ SEI and ex situ SEI, are also reviewed. Finally, future directions, including in‐operando techniques, multi‐modality approaches for characterization of SEI, and artificial intelligence assisted understanding of correlations between electrolyte components and SEI properties are proposed.

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“…The high E s values of the Al-O(OTF À ) tend to impede its dissociation process and promote the co-intercalation. [23,24] Moreover, the lowest unoccupied molecular orbital (LUMO) of (Al 3+ -OTF À ) is higher than the Fermi energy of the PZ, indicating its stability in PZ cathode during the intercalation process. (Figure 4 d) These phenomena coincide well with the experimental results of reversible (Al 3+ -OTF À ) co-intercalation in PZ cathodes.…”

Section: Angewandte Chemiementioning

confidence: 99%

Rechargeable Aqueous Aluminum Organic Batteries

et al. 2021

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Aqueous aluminum‐ion batteries (AABs) are regarded as promising next‐generation energy storage devices, and the current reported cathodes for AABs mainly focused on inorganic materials which usually implement a typical Al3+ ions (de)insertion mechanism. However, the strong electrostatic forces between Al3+ and the host materials usually lead to sluggish kinetics, poor reversibility and inferior cycling stability. Herein, we employ an organic compound with redox‐active moieties, phenazine (PZ), as the cathode material in AABs. Different from conventional inorganic materials confined by limited lattice spacing and rigid structure, the flexible organic molecules allow a large‐size Al‐complex co‐intercalation through reversible redox active centers (‐C=N‐) of PZ. This co‐intercalation behavior can effectively reduce desolvation penalty, and substantially lower the Coulombic repulsion during the ion (de)insertion process. Consequently, this organic cathode exhibits a high capacity and excellent cyclability, which exceeds those of most reported electrode materials for AABs. This work highlights the anion co‐intercalation chemistry of redox‐active organic materials, which is expected to boost the development of high‐performance multivalent‐ion battery systems.

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Molecular design for electrolyte solvents enabling energy-dense and long-cycling lithium metal batteries

Cited by 849 publications

References 61 publications

Robust Artificial Solid‐Electrolyte Interfaces with Biomimetic Ionic Channels for Dendrite‐Free Li Metal Anodes

Robust Artificial Solid‐Electrolyte Interfaces with Biomimetic Ionic Channels for Dendrite‐Free Li Metal Anodes

Recent Progress in Understanding Solid Electrolyte Interphase on Lithium Metal Anodes

Rechargeable Aqueous Aluminum Organic Batteries

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