Balancing interfacial reactions to achieve long cycle life in high-energy lithium metal batteries

Niu, Chaojiang; Liu, Dianying; Lochala, Joshua; Anderson, Christopher R.; Cao, Xia; Gross, M.; Xu, Wu; Zhang, Ji‐Guang; Whittingham, M. Stanley; Xiao, Jie; Li, Jun

doi:10.1038/s41560-021-00852-3

Cited by 356 publications

(309 citation statements)

References 39 publications

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“…12 Differing from the case of Si, Li metal anode suffers from a dendritic metal growth during Li metal plating, where Li ions travel from cathodes and nucleate on the bare current collector or pre-existing Li metal surface. Due to the hardly controllable mass transfer in a mixed liquid system, 13 Li metal deposits tend to grow as dendrites, which may penetrate through the polymer separator to cause shortcircuiting of battery and raise safety concerns. 14 In contrast, SEI is regarded as the most complex yet least understood components within a battery.…”

Section: Progress and Potentialmentioning

confidence: 99%

Leveraging cryogenic electron microscopy for advancing battery design

Cheng

Raghavendran

et al. 2022

Matter

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Section: Progress and Potentialmentioning

confidence: 99%

Leveraging cryogenic electron microscopy for advancing battery design

Cheng

Raghavendran

et al. 2022

Matter

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“…To the best of our knowledge, this is the first demonstration that long-term stability of LMB with DME-based ether electrolyte at such low concentration can be obtained under a cutoff voltage of 4.3 V. Admittedly, the reported test conditions still fall short of the stringent requirements of practical LMBs (lean electrolyte, thin Li, and > 3 mAh cm -2 cathode loading). 6,24 . Nevertheless, the effectiveness of our proposed anion-adsorption strategy for increasing the high-voltage tolerance of dilute ether electrolytes is clear from the electrochemical measurements.…”

Section: Cell Performances Of Lmbs With No 3 --Containing Ether Elect...mentioning

confidence: 99%

“…19 The early entry of ether electrolytes for high-voltage LMBs adopted the high-concentration formulations (e.g., triglyme and tetraglyme solvents with equimolar Li salt). 20 Although the oxidation stability can be improved to ~5 V on the platinum electrode, only limited cycling stability (200 cycles) was achieved on the LiCoO2 cathode with a cutoff voltage of 4.2 V. Until now, the high-concentration ether electrolytes 14,21,22 and localized high-concentration ether electrolytes 23,24 effectively developed for 4.3/4.4 V NMC cathodes have all followed the same design concept, namely, high salt/solvent molar ratio. 16 Meanwhile, elimination of unbound (free) solvents of electrolyte 16,22 and formation of stable cathode-electrolyte interphase (CEI) 13,14,21,23 have become generally accepted views on the improved oxidation stability.…”

Section: Introductionmentioning

confidence: 99%

“…In particular, the high-concentration ether electrolytes usually suffer from the economic effectiveness, high viscosity and slow dynamics. 15,16 Even for the localized highconcentration electrolyte formulation evaluated for practical applications, 23,24 the usage of hydrofluoroether diluents still results in possible environmental hazards. 25 Hence, compared with these salt-concentrated solutions, dilute ether electrolytes are thus long required to have high-voltage tolerance; however, limited by their intrinsic poor oxidation stability, 8 such achievements are rarely reported.…”

Section: Introductionmentioning

confidence: 99%

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High-voltage dilute ether electrolytes enabled by regulating interfacial structure

Wang

Zhang

et al. 2022

Preprint

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Poor oxidation stability of ether solvents at the cathode restricts the use of dilute ether electrolytes with conventional concentrations around 1 M in high-voltage lithium metal batteries. Here we develop an anion-adsorption approach to altering the ether solvent environment within the electrical double layer (EDL) at the cathode, by adding a small amount of nitrate, so that the oxidation tolerance of nitrate-containing dilute ether electrolytes is enhanced up to 4.4 V (versus Li/Li+), leading to complete compatibility with high-voltage cathodes and exhibiting superior cycling stability. Constant-potential molecular dynamics simulations reveal that ether molecules are mostly excluded from the cathode because of nitrate occupation in the inner layer of the EDL, thus suppressing ether oxidative decomposition. This work highlights that regulating the interfacial structure by adding surface adsorbates, rather than passivating cathode-electrolyte interphase or changing ion solvation, can help to enhance the oxidation stability of ether solvents. It also provides design criteria for adsorption-type additives to achieve high-voltage dilute ether electrolytes.

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“…Developing high-energy-density secondary batteries to appease the increasing consumption of electronic apparatuses and electric vehicles is the responsibility of battery researchers [1,2]. In the last two decades, Li-rich Mn-based solid-solution cathode materials of nLi 2 MnO 3 •(1−n)LiTMO 2 (0 < n < 1, TM = Mn, Ni, Co, Mn 0.5 Ni 0.5 , Mn 0.333 Ni 0.333 Co 0.333 , etc.)…”

Section: Introductionmentioning

confidence: 99%

Exploring the Effect of a MnO2 Coating on the Electrochemical Performance of a Li1.2Mn0.54Ni0.13Co0.13O2 Cathode Material

Yang

Zheng

et al. 2021

Micromachines

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The effect of electrochemically active MnO2 as a coating material on the electrochemical properties of a Li1.2Mn0.54Ni0.13Co0.13O2 (LTMO) cathode material is explored in this article. The structural analysis indicated that the layered structure of the LTMO was unchanged after the modification with MnO2. The morphology inspection demonstrated that the rod-like LTMO particles were encapsulated by a compact coating layer. The MnO2 layer was able to hinder the electrolyte solution from corroding the LTMO particles and optimized the formation of a solid electrolyte interface (SEI). Meanwhile, lithium ions were reversibly inserted into and extracted from MnO2, which afforded an additional capacity. Compared with the bare LTMO, the MnO2-coated sample exhibited enhanced electrochemical performance. After the MnO2 coating, the first discharge capacity rose from 224.2 to 239.1 mAh/g, and the initial irreversible capacity loss declined from 78.2 to 46.0 mAh/g. Meanwhile, the cyclic retention climbed up to 88.2% after 100 cycles at 0.5 C, which was more competitive than that of the bare LTMO with a value of 71.1%. When discharging at a high current density of 2 C, the capacity increased from 100.5 to 136.9 mAh/g after the modification. These investigations may be conducive to the practical application of LTMO in prospective automotive Li-ion batteries.

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Balancing interfacial reactions to achieve long cycle life in high-energy lithium metal batteries

Cited by 356 publications

References 39 publications

Leveraging cryogenic electron microscopy for advancing battery design

Leveraging cryogenic electron microscopy for advancing battery design

High-voltage dilute ether electrolytes enabled by regulating interfacial structure

Exploring the Effect of a MnO2 Coating on the Electrochemical Performance of a Li1.2Mn0.54Ni0.13Co0.13O2 Cathode Material

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