High-efficiency, anode-free lithium–metal batteries with a close-packed homogeneous lithium morphology

Su, Laisuo; Charalambous, Harry; Cui, Zehao; Manthiram, Arumugam

doi:10.1039/d1ee03103a

Cited by 66 publications

(49 citation statements)

References 34 publications

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“…To understand this phenomenon, Li plating morphologies were investigated in Li|Cu cells. [ 22 ] Figure S12 (Supporting Information) shows that LSE(FEC/EMC) and LSE(EC/EMC) help form a relatively dense Li morphology, while LSE(DME) and LP57 promote the formation of a porous Li morphology during Li plating. The dense Li morphologies not only reduce the side reactions between Li and electrolytes but also provide better structural electronic connections, which is beneficial to the cycling stability of LMBs.…”

Section: Resultsmentioning

confidence: 99%

Uncovering the Solvation Structure of LiPF₆‐Based Localized Saturated Electrolytes and Their Effect on LiNiO₂‐Based Lithium‐Metal Batteries

Zhao

et al. 2022

Advanced Energy Materials

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Electrolytes play a critical role in stabilizing highly reactive lithium‐metal anodes (LMAs) and high‐voltage cathodes for rechargeable lithium‐metal batteries (LMBs). Localized high concentration electrolytes (LHCEs) have achieved remarkable success in the context of LMBs. However, the state‐of‐the‐art LHCEs are based on LiFSI salt, which is prohibitively expensive. Here, the utility of low‐cost LiPF6 salt in localized saturated electrolytes (LSEs) with a series of solvents and diluents in LMBs with cobalt‐free LiNiO2 cathode is systematically explored. Experimental and theoretical analyses reveal that the unique solvation structure formed not only changes the distribution of solvents and anions but also alters the atom–atom distances within them, leading to different reduction and oxidation stabilities compared to low‐concentration electrolytes. In addition, LSEs help form LiF‐rich interphase layers on the LMA and LiNiO2 cathode, protecting the electrodes from degradation during cycling. Different LSEs also lead to differences in lithium plating morphology and impedance buildup during cycling, impacting the performance of LMBs. The solvent and diluent must be carefully selected for compatibility with a lithium salt when developing LHCEs and LSEs for LMBs.

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Section: Resultsmentioning

confidence: 99%

Uncovering the Solvation Structure of LiPF₆‐Based Localized Saturated Electrolytes and Their Effect on LiNiO₂‐Based Lithium‐Metal Batteries

Zhao

et al. 2022

Advanced Energy Materials

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“…The Li morphology resulting from the plating and stripping process significantly depends on the electrolytes. 32 Figure S16a,b shows the cross-section SEM images of cycled Li-metal anodes from cells with LP57 electrolyte and LSE. In the LP57 electrolyte, the cycled Li on the surface of the Li metal anode is thick (Figure S16a-i) and porous (Figure S16a-ii).…”

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confidence: 99%

Protection of Cobalt-Free LiNiO₂ from Degradation with Localized Saturated Electrolytes in Lithium-Metal Batteries

Manthiram

2022

ACS Energy Lett.

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High-nickel layered oxide cathode materials are the most promising candidates for developing lithium-metal batteries (LMBs) because of their high energy density and low cost. Herein, we present a localized saturated electrolyte (LSE) based on readily available, low-cost LiPF6 salt with limited solubility in carbonate solvents for developing LiNiO2 cathodes. Compared to the conventional electrolyte that retains only 55% of the initial capacity after 200 cycles, the LSE retains a record 81% of the initial capacity after 600 deep cycles at 4.4 V (versus Li/Li+). The LSE protects the LiNiO2 surface from degrading into rock-salt and spinel phases during cycling and helps form a robust Li morphology on the Li-metal anode that is covered by an inorganic-rich solid-electrolyte interphase. The drastically enhanced cycling stability with LSE demonstrates the importance of developing robust electrolytes compatible with both high-Ni cathodes and Li-metal anodes.

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“…The choice of electrolyte determines Li plating morphology and thus the Li dendrite formation and growth. [ 69 ] The currently used commercial carbonate electrolyte cannot prevent Li dendrite growth and thus is not compatible with LMBs. [ 70 ] Tremendous effort has been contributed to developing new electrolyte formula to suppress Li dendrite formation in LMBs.…”

Section: Strategies To Suppress LI Dendrite Formationmentioning

confidence: 99%

Lithium‐Metal Batteries via Suppressing Li Dendrite Growth and Improving Coulombic Efficiency

Manthiram

2022

Small Structures

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Lithium‐metal batteries (LMB) are recognized as one of the most promising candidates for the next generation of batteries due to their high energy density. Extensive studies have been refocused on the field in the past decade to make the technology commercially viable. Despite exciting progress that has been made, the practical application of LMBs is still hampered by the uncontrollable Li plating morphology and inferior Coulombic efficiency (CE) during cycling. Herein, first, the relevant research that has been carried out in the past decade (2010–2021) is briefly summarized and then the Li plating behaviors, mechanistic understanding of these behaviors, and strategies to suppress Li dendrite growth are discussed. Finally, the methods and techniques to improve Coulombic efficiency (CE) is discussed, especially the design of liquid electrolytes, and possible research directions for the future development of LMBs.

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High-efficiency, anode-free lithium–metal batteries with a close-packed homogeneous lithium morphology

Abstract: Anode-free lithium-metal batteries (LMBs) are ideal candidates for high-capacity energy storage as they eliminate the need of a conventional graphite electrode or excess lithium-metal anode. Current anode-free LMBs suffer from...

Cited by 66 publications

References 34 publications

Uncovering the Solvation Structure of LiPF₆‐Based Localized Saturated Electrolytes and Their Effect on LiNiO₂‐Based Lithium‐Metal Batteries

Uncovering the Solvation Structure of LiPF₆‐Based Localized Saturated Electrolytes and Their Effect on LiNiO₂‐Based Lithium‐Metal Batteries

Protection of Cobalt-Free LiNiO₂ from Degradation with Localized Saturated Electrolytes in Lithium-Metal Batteries

Lithium‐Metal Batteries via Suppressing Li Dendrite Growth and Improving Coulombic Efficiency

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High-efficiency, anode-free lithium–metal batteries with a close-packed homogeneous lithium morphology

Abstract: Anode-free lithium-metal batteries (LMBs) are ideal candidates for high-capacity energy storage as they eliminate the need of a conventional graphite electrode or excess lithium-metal anode. Current anode-free LMBs suffer from...

Cited by 66 publications

References 34 publications

Uncovering the Solvation Structure of LiPF6‐Based Localized Saturated Electrolytes and Their Effect on LiNiO2‐Based Lithium‐Metal Batteries

Uncovering the Solvation Structure of LiPF6‐Based Localized Saturated Electrolytes and Their Effect on LiNiO2‐Based Lithium‐Metal Batteries

Protection of Cobalt-Free LiNiO2 from Degradation with Localized Saturated Electrolytes in Lithium-Metal Batteries

Lithium‐Metal Batteries via Suppressing Li Dendrite Growth and Improving Coulombic Efficiency

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Uncovering the Solvation Structure of LiPF₆‐Based Localized Saturated Electrolytes and Their Effect on LiNiO₂‐Based Lithium‐Metal Batteries

Uncovering the Solvation Structure of LiPF₆‐Based Localized Saturated Electrolytes and Their Effect on LiNiO₂‐Based Lithium‐Metal Batteries

Protection of Cobalt-Free LiNiO₂ from Degradation with Localized Saturated Electrolytes in Lithium-Metal Batteries