Stable cycling and uniform lithium deposition in anode-free lithium-metal batteries enabled by a high-concentration dual-salt electrolyte with high LiNO3 content
“…S3a~f), whereas a homogeneous and silverish Li deposition was observed when LiNO 3 was added (Fig. S3g), which was attributed to the LiNO 3 ability altering the deposited Li shape from dendritic to spherical [39].…”
Section: Resultsmentioning
confidence: 97%
“…7). As mentioned above, LiNO 3 is widely applied as an effective additive in ether-based electrolytes to increase the interfacial stability of Li-metal anode but it shows poor solubility in carbonate-based electrolyte [3,39]. Thus, in order to improve the LiNO 3 solubility, we mixed a trace amount of TEP in the carbonate electrolyte, and dissolved the LiNO 3 in the carbonate and ester mixed solvent.…”
ANODE-free Li-metal batteries (AFLMBs) operating with Li of cathode material have attracted enormous attention due to their exceptional energy density originating from anode-free structure in the confined cell volume. However, uncontrolled dendritic growth of lithium on a copper current collector can limit its practical application as it causes fatal issues for stable cycling such as dead Li formation, unstable solid electrolyte interphase, electrolyte exhaustion, and internal short-circuit. To overcome this limitation, here, we report a novel dual-salt electrolyte comprising of 0.2 M LiPF 6 + 3.8 M lithium bis(fluorosulfonyl)imide in a carbonate/ester co-solvent with 5 wt% fluoroethylene carbonate, 2 wt% vinylene carbonate, and 0.2 wt% LiNO 3 additives. Because the dual-salt electrolyte facilitates uniform/dense Li deposition on the current collector and can form robust/ionic conductive LiF-based SEI layer on the deposited Li, a Li/Li symmetrical cell exhibits improved cycling performance and low polarization for over 200 h operation. Furthermore, the anode-free LiFePO 4 /Cu cells in the carbonate electrolyte shows significantly enhanced cycling stability compared to the counterparts consisting of different salt ratios. This study shows an importance of electrolyte design guiding uniform Li deposition and forming stable SEI layer for AFLMBs.
“…S3a~f), whereas a homogeneous and silverish Li deposition was observed when LiNO 3 was added (Fig. S3g), which was attributed to the LiNO 3 ability altering the deposited Li shape from dendritic to spherical [39].…”
Section: Resultsmentioning
confidence: 97%
“…7). As mentioned above, LiNO 3 is widely applied as an effective additive in ether-based electrolytes to increase the interfacial stability of Li-metal anode but it shows poor solubility in carbonate-based electrolyte [3,39]. Thus, in order to improve the LiNO 3 solubility, we mixed a trace amount of TEP in the carbonate electrolyte, and dissolved the LiNO 3 in the carbonate and ester mixed solvent.…”
ANODE-free Li-metal batteries (AFLMBs) operating with Li of cathode material have attracted enormous attention due to their exceptional energy density originating from anode-free structure in the confined cell volume. However, uncontrolled dendritic growth of lithium on a copper current collector can limit its practical application as it causes fatal issues for stable cycling such as dead Li formation, unstable solid electrolyte interphase, electrolyte exhaustion, and internal short-circuit. To overcome this limitation, here, we report a novel dual-salt electrolyte comprising of 0.2 M LiPF 6 + 3.8 M lithium bis(fluorosulfonyl)imide in a carbonate/ester co-solvent with 5 wt% fluoroethylene carbonate, 2 wt% vinylene carbonate, and 0.2 wt% LiNO 3 additives. Because the dual-salt electrolyte facilitates uniform/dense Li deposition on the current collector and can form robust/ionic conductive LiF-based SEI layer on the deposited Li, a Li/Li symmetrical cell exhibits improved cycling performance and low polarization for over 200 h operation. Furthermore, the anode-free LiFePO 4 /Cu cells in the carbonate electrolyte shows significantly enhanced cycling stability compared to the counterparts consisting of different salt ratios. This study shows an importance of electrolyte design guiding uniform Li deposition and forming stable SEI layer for AFLMBs.
“…While there was no evident morphological change in the SEM and transmission electron microscopy (TEM) images after acid treatment (Figure 2b,c), the X-ray photoelectron spectroscopy (XPS) survey spectra showed that oxygen and nitrogen-containing functional groups were newly formed on the SP carbon (Figure 2d). High-resolution elemental XPS (C 1s and O 1s) and Fourier transform infrared (FT-IR) spectra (Figures S6 and S7, Supporting Information) also revealed that the specific deconvolution peaks are assigned to CO, CO, CH, COH, and NO 2 bonds, [26][27][28][29][30][31] which suggests that the major functional groups are attributed to carboxylic acid (COOH) and nitric acid (NO 3 ). Such acidic pendant groups at the SP carbon can enhance the hydrophilicity, leading to excellent dispersion in the aqueous electrolyte (Figure 2e).…”
“…In the aforementioned AFLMBs, the cathode provides all the active Li + for plating on an untreated Cu substrate (no excess Li is present in the cell). [14][15][16] The absence of an anodic Li + host and the lack of Cu treatment result in lower cell weight, less space, and lower fabrication cost; thus, these batteries provide a higher energy density than do conventional lithium-ion batteries. [15][16][17] However, limited research has been conducted on AFLMBs because of the low cycling efficiency of Li on the untreated Cu substrate, which is caused by the formation of an erratic SEI and dead Li.…”
Anode-free lithium metal batteries (AFLMBs) have high energy density and simple assembly. The major challenge in their production is related to the reversibility of Li deposition, which is governed by...
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