2020
DOI: 10.1073/pnas.2010852117
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Role of inner solvation sheath within salt–solvent complexes in tailoring electrode/electrolyte interphases for lithium metal batteries

Abstract: Functional electrolyte is the key to stabilize the highly reductive lithium (Li) metal anode and the high-voltage cathode for long-life, high-energy-density rechargeable Li metal batteries (LMBs). However, fundamental mechanisms on the interactions between reactive electrodes and electrolytes are still not well understood. Recently localized high-concentration electrolytes (LHCEs) are emerging as a promising electrolyte design strategy for LMBs. Here, we use LHCEs as an ideal platform to investigate the fundam… Show more

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Cited by 260 publications
(215 citation statements)
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“…However, the uncontrollable growth of Li dendrites and collapse of the solid electrolyte interphase (SEI) layer lead to low Coulombic efficiency (CE) and deteriorated cycling performance, which largely restrict the practical application of the Li metal anode (LMA) (7)(8)(9)(10)(11)(12)(13). Considerable efforts have been made to regulate the Li plating/ stripping behaviors for stable Li metal batteries, including developing functional electrolytes (14)(15)(16)(17)(18), constructing well-designed three-dimensional (3D) host structures (19)(20)(21)(22)(23)(24), and using artificial protection layers (25)(26)(27)(28)(29)(30). Despite much progress (31,32), it remains a challenge to explore LMA with stable cycling life over 500 cycles at practical current densities greater than 1 mA cm −2 .…”
Section: Introductionmentioning
confidence: 99%
“…However, the uncontrollable growth of Li dendrites and collapse of the solid electrolyte interphase (SEI) layer lead to low Coulombic efficiency (CE) and deteriorated cycling performance, which largely restrict the practical application of the Li metal anode (LMA) (7)(8)(9)(10)(11)(12)(13). Considerable efforts have been made to regulate the Li plating/ stripping behaviors for stable Li metal batteries, including developing functional electrolytes (14)(15)(16)(17)(18), constructing well-designed three-dimensional (3D) host structures (19)(20)(21)(22)(23)(24), and using artificial protection layers (25)(26)(27)(28)(29)(30). Despite much progress (31,32), it remains a challenge to explore LMA with stable cycling life over 500 cycles at practical current densities greater than 1 mA cm −2 .…”
Section: Introductionmentioning
confidence: 99%
“…They both have high contents of Li and Oa nd low content of C, indicating inorganic-rich SEIs formed on Li-Mg5 and Li-Mg10 anode surfaces.T he atomic ratio is similar to the result of the pure Li metal in our previous study. [22] As indicated by Figure 5h,for C1sspectra, the main difference is that the SEI on Li-Mg5 has more signal of CO 3…”
Section: Resultsmentioning
confidence: 90%
“…Thepure Li metal in the same electrolyte in our previous study showed similar F1sspectra. [22] They all indicate the critical effect of the reduction of LiFSI salt. O1s spectra of Li-Mg10 is similar to that of pure Li metal and they both have the signal of Li 2 O, while Li-Mg5 doesnthave Li 2 O. Li-Mg5 and Li-Mg10 have similar S2pspectra and they have lower amount of Li 2 Sc ompared with pure Li metal.…”
Section: àmentioning
confidence: 95%
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“…[4][5][6][7][8] Unfortunately, the practical application of Li metal anodes (LMAs) has not been realized due to the structural and interfacial instability issues induced by the uncontrollable growth of Li dendrites during repeated electrochemical cycling processes. [9][10][11] Extensive efforts have been recently made to regulate the Li deposition/dissolution properties for stable LMAs, including developing compatible electrolytes, [12][13][14][15][16] engineering rationally designed three-dimensional (3D) scaffolds for Li accom-modation, [17][18][19][20] and constructing artificial solid-electrolyte interphase (SEI) layers. [21][22][23][24] Among these approaches, 3D host nanostructures for LMAs have shown outstanding electrochemical properties because of the largely decreased local current density and accommodated huge volume variation during Li accommodation/extraction.…”
mentioning
confidence: 99%