FSI-inspired solvent and “full fluorosulfonyl” electrolyte for 4 V class lithium-metal batteries

Xue, Weimin; Shi, Zhe; Huang, Mingjun; Feng, Shuting; Wang, Chao; Wang, Fei; Lopez, Jeffrey; Qiao, Bo; Xu, Guiyin; Zhang, Wenxu; Dong, Yanhao; Gao, Rui; Shao‐Horn, Yang; Johnson, Jeremiah A.; Li, Ju

doi:10.1039/c9ee02538c

Cited by 234 publications

(183 citation statements)

References 61 publications

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“…The XPS spectra of F 1s and P 2p are considered to be the representative of the inorganic-rich CEI (Fig. 5f-j, g-k) 26,50 , derived from the LiPF 6 salt. A small amount of LiF exists in the CEI (organic-rich) formed in 1 M (Fig.…”

Section: Characterization Of Lnfmomentioning

confidence: 99%

Inhibition of transition metals dissolution in cobalt-free cathode with ultrathin robust interphase in concentrated electrolyte

et al. 2020

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The low Coulombic efficiency during cycling hinders the application of Cobalt-free lithiumrich materials in lithium-ion batteries. Here we demonstrated that the dissolution of iron, rather than traditionally acknowledged manganese, is mainly responsible for the low Coulombic efficiency of the iron-substituted cobalt-free lithium-rich material. Besides, we presented an approach to inhibit the dissolution of transition metal ions by using concentrated electrolytes. We found that the cathode electrolyte interphase (CEI) layer formed in the concentrated electrolyte is a uniform and robust LiF-rich CEI, which is a sharp contrast with the uneven and fragile organic-rich CEI formed in the dilute electrolyte. The LiF-rich CEI not only effectively inhibits the dissolution of TMs but also stabilizes the cathode structure. The Coulombic efficiency, cycling stability, rate performance, and safety of the Fe-substituted cobalt-free lithium-rich cathode material in the concentrated electrolyte have been improved tremendously.

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Section: Characterization Of Lnfmomentioning

confidence: 99%

Inhibition of transition metals dissolution in cobalt-free cathode with ultrathin robust interphase in concentrated electrolyte

et al. 2020

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“…It has been recently proposed that highly concentrated electrolytes (HCEs) induce highly reversible Li plating/stripping because the modified Li + solvation structure results in the reduced activity of solvent molecules, fluorinated SEI derived from anion and average concentration gradients near the electrode surface. [ 7c,9,10 ] However, HCEs are typically of high cost, high density, narrow liquid range, poor viscosity, and poor wettability, which present great challenges for their practical applications. [ 10,11 ] To address such shortcomings without sacrificing their superiority in cycling performance, researchers developed diluted high concentration electrolytes (DHCE) by introducing a cosolvent (also a diluent).…”

Section: Introductionmentioning

confidence: 99%

Fluorobenzene, A Low‐Density, Economical, and Bifunctional Hydrocarbon Cosolvent for Practical Lithium Metal Batteries

Jiang

Zeng

Liang

et al. 2020

Adv Funct Materials

160

137

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Highly concentrated electrolytes (HCEs) significantly improve the stability of lithium metal anodes, but applications are often impeded by their limitation of density, viscosity, and cost. Here, fluorobenzene (FB), an economical hydrocarbon with low density and low viscosity, is demonstrated as a bifunctional cosolvent to obtain a novel FB diluted highly concentrated electrolyte (FB‐DHCE). First, the addition of FB suppresses the decomposition of dimethoxyethane (DME) on the Li metal by strengthening the interactions of DME and FSI− around Li+. Second, FB efficiently elevates the content of LiF in the solid electrolyte interphase (SEI) based on its electrochemical reduction reaction. The unique solvation and interfacial chemistry of FB‐DHCE enable dendrite‐free deposition of lithium with high Coulombic efficiency (up to 99.3%) and prolong cycling life (over 500 cycles at 1 mA cm−2). The performance of FB‐DHCE is further demonstrated in full cells under practical conditions, including ambient to low temperature (–20 °C), high areal capacity (7.6 mAh cm−2), high current density (3 mA cm−2), limited excess Li (20 µm Li), and lean electrolyte (3 g Ah−1). Employing FB as a cosolvent not only opens a novel pathway to stabilize Li metal anodes, but also could greatly advance the development of Li metal batteries.

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“…SEI derived from the decomposition products of the solvation sheath plays a significant role in regulating Li + desolvation and transport, further profoundly affecting the deposition/stripping electrokinetics and morphologies. [ 23–25 ] Tuning the SEI chemistry by designing special solvation structure (e.g., fluorinated solvents, [ 26 ] fluorinated anions, [ 27 ] sulfite solvents [ 28 ] ) or increasing the salt/solvent molar ratio [ 29 ] can alleviate the formation of “dead Li,” but the correlation between SEI nanostructure and the battery performance has not been well‐established.…”

Section: Introductionmentioning

confidence: 99%

Engineering Wavy‐Nanostructured Anode Interphases with Fast Ion Transfer Kinetics: Toward Practical Li‐Metal Full Batteries

Zhang

Shen

Liu

et al. 2020

Adv Funct Materials

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Fast Li-metal depletion and severe anode pulverization are the most critical obstacles for the energy-dense Li-metal full batteries using thin Li-metal anodes (<50 µm). Here, a wavy-nanostructured solid electrolyte interphase (SEI) with fast ion transfer kinetics is reported, which can promote highefficiency Li-metal plating/stripping (>98% at 4 mAh cm −2) in conventional carbonate electrolyte. Cryogenic transmission electron microscopy (cryo-TEM) further reveals the fundamental relationship between wavy-nanostructured SEI, function, and the electrochemical performance. The wavy SEI with greatly decreased surface diffusion resistance can realize grain coarsening of Li-metal deposition and exhaustive dissolution of active Li-metal during the stripping process, which can effectively alleviate "dead Li" accumulation and anode pulverization problems in practical full cells. Under highly challenging conditions (45 µm Li-metal anodes, 4.3 mAh cm −2 high capacity LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathodes), full cells exhibit significantly improved cycling lifespan (170 cycles; 20 cycles for control cells) via the application of wavy SEI.

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FSI-inspired solvent and “full fluorosulfonyl” electrolyte for 4 V class lithium-metal batteries

Abstract: A new “full fluorosulfonyl” (FFS) electrolyte is developed for highly reversible 4 V class lithium-metal batteries (LMBs).

Cited by 234 publications

References 61 publications

Inhibition of transition metals dissolution in cobalt-free cathode with ultrathin robust interphase in concentrated electrolyte

Inhibition of transition metals dissolution in cobalt-free cathode with ultrathin robust interphase in concentrated electrolyte

Fluorobenzene, A Low‐Density, Economical, and Bifunctional Hydrocarbon Cosolvent for Practical Lithium Metal Batteries

Engineering Wavy‐Nanostructured Anode Interphases with Fast Ion Transfer Kinetics: Toward Practical Li‐Metal Full Batteries

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