Featured with the highest possible energy density, anode-free lithium-metal batteries (AFBs) are still challenged by the fast capacity decay, especially for the ones operated in commercial carbonate electrolytes, which can be ascribed to the poor stability and continual broken/formation of the solid-electrolyte interface (SEI) formed on the anode side. Here, sacrificial additives, which have low solubility in carbonate electrolytes and can be continuously released, are proposed for AFBs. The sacrificial and continuously-releasing feature gifts the additives the capability to form and heal the SEI during the long-term cycling process, thus minimizing the loss of active Li and enabling the AFLMBs with high loading LiNiCoMnO (21.
View Article and Find Full Text PDFThe utilization of thin zinc (Zn) anodes with a high depth of discharge is an effective strategy to increase the energy density of aqueous Zn metal batteries (ZMBs), but challenged by the poor reversibility of Zn electrode due to the serious Zn-consuming side reactions at the Zn||electrolyte interface. Here, we introduce 2-bromomethyl-1,3-dioxolane (BDOL) and methanol (MeOH) as electrolyte additive into aqueous ZnSO electrolyte. In the as-formulated electrolyte, BDOL with a strong electron-withdrawing group (-CHBr) tends to pair with the HO-Zn-MeOH complex, leading to the formation of organobromine-partnered HO-Zn-MeOH cluster ions.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Lithium (Li) metal electrodes show significantly different reversibility in the electrolytes with different salts. However, the understanding on how the salts impact on the Li loss remains unclear. Herein, using the electrolytes with different salts (e.
View Article and Find Full Text PDFRestricted by the available energy storage modes, currently rechargeable aluminum-ion batteries (RABs) can only provide a very limited experimental capacity, regardless of the very high gravimetric capacity of Al (2980 mAh g ). Here, a novel complexation mechanism is reported for energy storage in RABs by utilizing 0D fullerene C as the cathode. This mechanism enables remarkable discharge voltage (≈1.
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2023
Stable zinc (Zn)/electrolyte interface is critical for developing rechargeable aqueous Zn-metal batteries with long-term stability, which requires the dense and stable Zn electrodeposition. Herein, an interfacial lattice locking (ILL) layer is constructed via the electro-codeposition of Zn and Cu onto the Zn electrodes. The ILL layer shows a low lattice misfit (δ = 0.
View Article and Find Full Text PDFAqueous zinc-ion batteries (ZIBs) are promising energy storage solutions with low cost and superior safety, but they suffer from chemical and electrochemical degradations closely related to the electrolyte. Here, a new zinc salt design and a drop-in solution for long cycle-life aqueous ZIBs are reported. The salt Zn(BBI) with a rationally designed anion group, N-(benzenesulfonyl)benzenesulfonamide (BBI ), has a special amphiphilic molecular structure, which combines the benefits of hydrophilic and hydrophobic groups to properly tune the solubility and interfacial condition.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2023
The use of non-solvating, or as-called sparingly-solvating, electrolytes (NSEs), is regarded as one of the most promising solutions to the obstacles to the practical applications of Li-S batteries. However, it remains a puzzle that long-life Li-S batteries have rarely, if not never, been reported with NSEs, despite their good compatibility with Li anode. Here, we find the capacity decay of Li-S batteries in NSEs is mainly due to the accumulation of the dead Li S at the cathode side, rather than the degradation of the anodes or electrolytes.
View Article and Find Full Text PDFACS Appl Mater Interfaces
October 2022
Due to the poor electronic conductivity of solid sulfur and sulfides, the dissolution of S (α = 0, 2/8, 2/6, 2/4) into a liquid electrolyte and the vehicular diffusion of S to carbon black are necessary for the electrochemical activity of a sulfur cathode in lithium-sulfur (Li-S) batteries. However, exactly how much dissolution and diffusion are required for high sulfur utilization and how this may control the minimum electrolyte/sulfur ratio, (E/S), have not been quantitatively settled. In this work, we show experimentally that a dissolved polysulfide concentration which is too high (>10-20 MS) may gel the liquid electrolyte, leading to catastrophic loss of S mobility, a failure mode that is especially susceptible in a high-donor-number (DN) electrolyte under a lean condition (low E/S), similar to a traffic jam, resulting in high electrochemical polarization and low sulfur utilization.
View Article and Find Full Text PDFLean electrolyte (small E/S ratio) is urgently needed to achieve high practical energy densities in Li-S batteries, but there is a distinction between the cathode's absorbed electrolyte (AE) which is cathode-intrinsic and total added electrolyte (E) which depends on cell geometry. While total pore volume in sulfur cathodes affects AE/S and performance, it is shown here that pore morphology, size, connectivity, and fill factor all matter. Compared to conventional thermally dried sulfur cathodes that usually render "open lakes" and closed pores, a freeze-dried and compressed (FDS-C) sulfur cathode is developed with a canal-capillary pore structure, which exhibits high mean performance and greatly reduces cell-to-cell variation, even at high sulfur loading (14.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
August 2020
For Li-Se batteries, ether- and carbonate-based electrolytes are commonly used. However, because of the "shuttle effect" of the highly dissoluble long-chain lithium polyselenides (LPSes, Li Se , 4≤n≤8) in the ether electrolytes and the sluggish one-step solid-solid conversion between Se and Li Se in the carbonate electrolytes, a large amount of porous carbon (>40 wt % in the electrode) is always needed for the Se cathodes, which seriously counteracts the advantage of Se electrodes in terms of volumetric capacity. Herein an acetonitrile-based electrolyte is introduced for the Li-Se system, and a two-plateau conversion mechanism is proposed.
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