Cathode electrolyte interface enabling stable Li–S batteries

Xing, Xing; Li, Yejing; Wang, Xuefeng; Petrova, Victoria; Liu, Haodong; Liu, Ping

doi:10.1016/j.ensm.2019.06.022

Cited by 69 publications

(74 citation statements)

References 25 publications

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“…In order to demonstrate the low temperature performance of the 1 M LiFSI DEE system, a SPAN cathode was selected as the basis of eventual full cell construction due to its high capacity, low cost, and modest voltage, which satisfies the oxidative stability range of most ether electrolytes. [ 43 – 45 ] The full cells were comprised of a SPAN cathode with the high mass loading of 3.5 mAh cm −2 paired with a 40 μm Li metal anode, which corresponds to one-fold excess capacity ( Figure 6a ). Due to the inherent solubility of lithium polysulfides in typical ether solvents, the SPAN cathode is generally discouraged from use.…”

Section: Full Cell Behaviormentioning

confidence: 99%

Tailoring electrolyte solvation for Li metal batteries cycled at ultra-low temperature

et al. 2021

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Lithium metal batteries (LMBs) hold the promise to pushing cell level energy densities beyond 300 Wh kg −1 while operating at ultra-low temperatures (< −30°C). Batteries capable of both charging and discharging at these temperature extremes are highly desirable due to their inherent reduction of external warming requirements. Here we demonstrate that the local solvation structure of the electrolyte defines the charge-transfer behavior at ultra-low temperature, which is crucial for achieving high Li metal coulombic efficiency (CE) and avoiding dendritic growth. These insights were applied to Li metal full cells, where a high-loading 3.5 mAh cm −2 sulfurized polyacrylonitrile (SPAN) cathode was paired with a one-fold excess Li metal anode. The cell retained 84 % and 76 % of its room temperature capacity when cycled at −40 and −60 °C, respectively, which presented stable performance over 50 cycles. This work provides design criteria for ultra-low temperature LMB electrolytes, and represents a defining step for the performance of low-temperature batteries.

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Section: Full Cell Behaviormentioning

confidence: 99%

Tailoring electrolyte solvation for Li metal batteries cycled at ultra-low temperature

et al. 2021

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“…As depicted in Figure 3 b, the doublet peaks of S2p 3/2 and S2p 1/2 at around 164.1 eV and 165.2 eV, respectively, can be assigned to thioether sulfur bonded to carbon (C–S–C) species on the narrow XPS spectra of S2p of FG-CYS, and confirmed the successful attachment of the thiol groups from the thiol precursor via thiol-ene click reaction on the surface of the graphene [ 18 , 19 ]. Meanwhile, S2p 3/2 and S2p 1/2 peaks with lower intensities deconvoluted at 164.8 eV and 166.1 eV, respectively, could be ascribed to C–S or S–S species on the surface of graphene [ 20 ]. Note that S2p peak, associated with highly oxidized S species (>166 eV), was absent from the high-resolution S2p spectrum of FG-CYS, which implied good stability of the sulfur species formed on the surface of graphene sheets, despite the exposure of functionalized graphene material to the readily oxidized condition [ 21 ].…”

Section: Resultsmentioning

confidence: 99%

Highly Water Dispersible Functionalized Graphene by Thermal Thiol-Ene Click Chemistry

et al. 2021

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Functionalization of pristine graphene to achieve high water dispersibility remains as a key obstacle owing to the high hydrophobicity and absence of reactive functional groups on the graphene surface. Herein, a green and simple modification approach to prepare highly dispersible functionalized graphene via thermal thiol-ene click reaction was successfully demonstrated on pristine graphene. Specific chemical functionalities (–COO, –NH2 and –S) on the thiol precursor (L-cysteine ethyl ester) were clicked directly on the sp2 carbon of graphene framework with grafting density of 1 unit L-cysteine per 113 carbon atoms on graphene. This functionalized graphene was confirmed with high atomic content of S (4.79 at % S) as well as the presence of C–S–C and N–H species on the L-cysteine functionalized graphene (FG-CYS). Raman spectroscopy evidently corroborated the modification of graphene to FG-CYS with an increased intensity ratio of D and G band, ID/IG ratio (0.3 to 0.7), full-width at half-maximum of G band, FWHM [G] (20.3 to 35.5) and FWHM [2D] (64.8 to 90.1). The use of ethanol as the reaction solvent instead of common organic solvents minimizes the chemical hazards exposure to humans and the environment. This direct attachment of multifunctional groups on the surface of pristine graphene is highly demanded for graphene ink formulations, coatings, adsorbents, sensors and supercapacitor applications.

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“…Liu and co‐workers discovered that the sulfurized polyacrylonitrile (SPAN) cathode in Li–S battery could form a CEI on the surface in a high‐concentration ether‐based electrolyte with LiTFSI and LiNO 3 as co‐salts. [ 54 ] A crystalline CEI of SPAN with LiF and LiNO 2 was first observed by cryo‐TEM (Figure 8c), explaining the stable cycling of SPAN in ether‐based electrolytes derived by the protection of crystalline CEI to avoid the exposure of discharge products of SPAN to large amounts of electrolyte and suppress the formation of soluble polysulfide species.…”

Section: High‐resolution Characterization By Cryo‐temmentioning

confidence: 96%

“…[ 28a ] After that, the CEI in Li–S batteries was characterized by cryo‐TEM in 2019. [ 54 ] Cryo‐SEM/FIB was also employed to characterize the energy materials in recent years, such as the battery slurry [ 60 ] and Li metal anode [ 61 ] in 2015 and 2019, respectively. The significant discoveries of cryo‐EM in analyzing energy materials are mushrooming and great breakthroughs in the development of battery will come by the accurate diagnosis and feedback of cryo‐EM.…”

Section: Introductionmentioning

confidence: 99%

Analyzing Energy Materials by Cryogenic Electron Microscopy

Ren

Zhang

et al. 2020

Advanced Materials

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Safe and high‐energy‐density rechargeable batteries are increasingly indispensable in the pursuit of a wireless and fossil‐free society. Advancements in present battery technologies and the investigation of next‐generation batteries highly depend on the ever‐deepening fundamental understanding and the rational designs of working electrodes, electrolytes, and interfaces. However, accurately analyzing energy materials and interfaces is severely hindered by their intrinsic limitations of air and electron‐beam sensitivity, which restrains the research of energy materials in a low‐efficiency trial‐and‐error paradigm. The emergence of cryogenic electron microscopy (cryo‐EM) has enabled the nondestructive characterization of air‐ and electron‐beam sensitive energy materials in the microscale and nanoscale, and even at atomic resolutions, affording closer insights into the primary chemistry and physics of working batteries. Herein, the development of cryo‐EM and the applications in detecting energy materials are reviewed and analyzed from its overwhelming advantages in disclosing the underlying mystery of energy materials. Critical sample preparation methods as the precondition for cryo‐EM are compared, which strongly affect the characterization accuracy. Furthermore, new developments in the analysis of energy materials, especially bulk electrodes and interfaces in lithium metal batteries, are presented according to different functions of cryo‐EM. Finally, future directions of cryo‐EM for analyzing energy materials are prospected.

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Cathode electrolyte interface enabling stable Li–S batteries

Cited by 69 publications

References 25 publications

Tailoring electrolyte solvation for Li metal batteries cycled at ultra-low temperature

Tailoring electrolyte solvation for Li metal batteries cycled at ultra-low temperature

Highly Water Dispersible Functionalized Graphene by Thermal Thiol-Ene Click Chemistry

Analyzing Energy Materials by Cryogenic Electron Microscopy

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