Potentiometric Measurement to Probe Solvation Energy and Its Correlation to Lithium Battery Cyclability

Kim, Sang Cheol; Kong, Xian; Vilá, Rafael A.; Huang, William; Chen, Yuelang; Boyle, David T.; Yu, Zhiao; Wang, Hansen; Bao, Zhenan; Qin, Jian; Cui, Yi

doi:10.1021/jacs.1c03868

Cited by 118 publications

(155 citation statements)

References 42 publications

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“…[7,8] Some researchers have reported that increasing the content of inorganics in the SEI layer is beneficial for improving its stability and mechanical strength. [9][10][11] Different strategies for modulating the Li anode interface were investigated, including the use of electrolyte additives and artificial SEI layers. [12][13][14][15][16][17][18] Among them, regulating the composition of the SEI layers by changing the solvation structure of Li + using electrolyte additives seemed simpler.…”

mentioning

confidence: 99%

Rigid and Flexible SEI Layer Formed Over a Cross‐Linked Polymer for Enhanced Ultrathin Li Metal Anode Performance

Wang

Yang

Huang

et al. 2022

Advanced Energy Materials

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The design of the anode material is considered the core subject in manufacturing a battery system, among which, Li is a commonly used, ideal anode material. Normally, the electrolyte is decomposed on the Li metal anode to form a solid electrolyte interphase (SEI) layer. [4] Owing to this layer, the contact between the electrolyte and Li metal decreases, causing the batteries to be recyclable and efficient. During batteries cycling, however, a large volume expansion of the Li anode may lead to a rupture of the SEI layer, exposing fresh Li that could react with the electrolyte. The rupture of SEI therefore leads to a low coulombic efficiency (CE) and poor cycling stability. [5,6] Generally, the decomposition of Li salts in electrolytes results in the SEI layer that comprises inorganic compounds, while the electrolyte solvents are composed mainly of organic components. [7,8] Some researchers have reported that increasing the content of inorganics in the SEI layer is beneficial for improving its stability and mechanical strength. [9][10][11] Different strategies for modulating the Li anode interface were investigated, including the use of electrolyte additives and artificial SEI layers. [12][13][14][15][16][17][18] Among them, regulating the composition of the SEI layers by changing the solvation structure of Li + using electrolyte additives seemed simpler. [19] During the transfer of Li + through the SEI layer, Li + desolvation causes coordination anions and solvents to decompose and spontaneously form the SEI layer. [20][21][22][23] Unfortunately, most electrolyte additives themselves participate in the formation of the SEI layer. [24][25][26] Moreover, the effect of the additives gradually disappears owing to their continuous decomposition. By contrast, the artificial SEI layers, where extra protective layers are grafted directly onto the surface of Li metal, will not decompose significantly as the batteries cycle. Instead, the artificial SEI layer inhibits the growth of dendrite because of its specific mechanical properties. [27][28][29][30] In addition, it helps disperse Li + after passing through the membrane, homogenize the flux of Li + , and reduce the formation of dendrites. [31][32][33][34] Due to the remarkable effect of artificial layers, previous researches on the nature of the protective layers themselves are intense. [35][36][37][38][39] However, it should be noted that artificial layer has always a certain lifetime, and we suppose Li metal has been attracting considerable attention as the most promising anode material for application in next-generation Li rechargeable batteries. However, the instability of the formed solid electrolyte interphase (SEI) in the Li metal anode leads to a low coulombic efficiency (CE). Here, two kinds of synthesized polymer materials with different molecular configurations (chain and cross-linked), which are grafted as skins on Cu foils (current collectors), are reported. The interaction between the polymers and electrolyte solvent reduces the amount of the solvent used in...

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mentioning

confidence: 99%

Rigid and Flexible SEI Layer Formed Over a Cross‐Linked Polymer for Enhanced Ultrathin Li Metal Anode Performance

Wang

Yang

Huang

et al. 2022

Advanced Energy Materials

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“… 31 However, the weaker solvation may lead to the decrease of inferior ionic conductivity of the electrolyte. 33 As shown in Table S1, † the ionic conductivity ( σ ) of the CDE electrolyte is 2.63 mS cm −1 . As the concentration of LiFSI increased from 0.02 M to 0.12 M, the ionic conductivity decreased from 2.50 to 2.26 mS cm −1 .…”

Section: Resultsmentioning

confidence: 99%

A novel high-energy-density lithium-free anode dual-ion battery and in situ revealing the interface structure evolution

Wang

Dai

et al. 2022

Chem. Sci.

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“…30 The stark difference for FDEE is likely due to the special Li + …F-CH2-interaction between FDEE and Li + , as suggested by the induced chemical shifts of 7 Li-NMR and 19 F-NMR (Figure 1f and Figure S6-8). 23,24,31 Such interaction apparently increases the solvating ability of FDEE (Figure S9) to reduce the anion coordination for more facial ionic conduction. 29,32 As indicated in Figure 1g, the ionic conductivity of FDEE-LHCE (~3.25 mS cm -1 ) is about twice of that in DEE-LHCE (~1.71 mS cm -1 ).…”

Section: Unique Properties Of Fdee and Reduced LI + -Anion Coordinationmentioning

confidence: 99%

Monofluoro-ether electrolyte design with reduced Li+-anion coordination enables fast-charging ultrahigh-voltage lithium metal batteries

Ruan

Tan

Chen

et al. 2022

Preprint

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Ether-based electrolytes are particularly useful for lithium metal batteries (LMBs) and have shown improved anodic stability with the high concentration design. Nevertheless, the vaunted anion-reinforced solvation in concentrated electrolytes has non-negligible adverse effect on ion conduction and battery rate performance. Here, we propose a new solvent design strategy of ether monofluorination to tune the Li+-anion interaction for fast-charging LMBs. With the highly polar monofluoro functional groups, the ether-based electrolyte not only exhibits excellent high oxidation stability due to the strong electron-withdrawing effect of F, but also has a greatly increased ionic conductivity because of reduced anion coordination. The unique solvation structure also enables the formation of robust and highly conductive interphases at both the Li anode and NMC811 surfaces. High Li CEs (~99.4%) and stable long-term cycling with low overpotential under ultrahigh current densities (10 mA cm-2) could be achieved for Li anode. Li||NMC811 cells exhibit outstanding cycling performance under ultrahigh cut-off voltages of 4.6 V and 4.7 V, or at high current densities (5.1 mA cm-2). This work provides critical insights into the ion-solvent interactions in the solvation complex and their profound influence on the battery electrochemical performances.

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Potentiometric Measurement to Probe Solvation Energy and Its Correlation to Lithium Battery Cyclability

Cited by 118 publications

References 42 publications

Rigid and Flexible SEI Layer Formed Over a Cross‐Linked Polymer for Enhanced Ultrathin Li Metal Anode Performance

Rigid and Flexible SEI Layer Formed Over a Cross‐Linked Polymer for Enhanced Ultrathin Li Metal Anode Performance

A novel high-energy-density lithium-free anode dual-ion battery and in situ revealing the interface structure evolution

Monofluoro-ether electrolyte design with reduced Li+-anion coordination enables fast-charging ultrahigh-voltage lithium metal batteries

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