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Sulfurized polyacrylonitrile (SPAN) is recognized as a promising organic cathode for long-lifespan lithium metal batteries. Nevertheless, the irreversible cleavage/formation of multiple sulfur-sulfur (S-S) bonds of SPAN within conventional ether-based electrolytes results in loss of active S species, severe capacity fading and shuttle effects. Herein, we propose a new electrolyte based on dipropyl ether (PE) solvent for Li-SPAN batteries. Benefiting from the particular chain-coordination structure and weak dipole interactions with Li+ and active species, the resulting electrolyte not only achieves low desolvation energy barrier and high Li+ transference number, but also displays stable electrolyte-electrode interface (EEI). Consequently, the full cells utilizing this electrolyte exhibit good cyclability, outstanding capacity retention and superior extreme-temperature (-50°C to 50 °C) performance. Furthermore, the Ah-scale pouch cell with lean electrolyte (2.5 g Ah-1) achieves record cycle stability with 96.5% capacity retention after 75 cycles, which deliver an initial specific energy density of 150 Wh kg-1 (based on the weight of the entire cell). Impressively, this strategy demonstrates universality in a series of organic electrodes employing with PE-based electrolytes. This work highlights the strategy for modulating the dipole interaction at EEI for long-lifespan Li-organic batteries at extreme conditions., (© 2024 Wiley‐VCH GmbH.)

The inferior oxidative stability of commercial carbonate electrolytes and overgrowth of the electrode-electrolyte interphase (EEI) have largely hindered the development of high-voltage lithium metal batteries. In this study, these challenges are addressed by designing Li + -solvent chelating solvation structures to inhibit solvent decomposition using cyano-alkyl-phosphate as a demonstration. Theoretical and experimental studies confirm that the -P═O and -C≡N groups within diethyl (2-cyanethyl) phosphonate exhibit a comparable ability to coordinate with Li + , facilitating the formation of seven-membered chelating structures. This unique solvation structure contributes to the formation of anion-derived inorganic-rich EEI with high stability and robustness, hindering the further decomposition of the electrolyte. Additionally, the cyano group has a strong complexation with the transition metal (TM) in the cathode to inhibit TM dissolution, thereby ensuring the structural stability of the cathode particle. Utilizing this special chelating structure, the designed electrolyte demonstrates favorable Li plating/stripping reversibility and promising oxidative stability in high-voltage batteries. Consequently, the LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode exhibits a high capacity retention (90%) after operating 300 cycles. Under harsh testing conditions, the 4.6 V Li||NCM811 pouch cell with a capacity of 1.4 Ah (∼295 Wh kg -1 based on the total mass of the cell) retains 70% capacity after 80 cycles. This work provides new insights into the correlation between the solvation structure and oxidative stability of electrolytes, contributing significantly to the advancement of high-voltage lithium metal batteries.

Electrolytes that can keep liquid state are one of the most important physical metrics to ensure the ions transfer with stable operation of rechargeable lithium-based batteries at a wide temperature window. It is generally accepted that strong polar solvents with high melting points favor the safe operation of batteries above room temperatures but are susceptible to crystallization at low temperatures (≤-40 °C). Here, a crystallization limitation strategy was proposed to handle this issue. We demonstrate that, although the high melting points of ethylene sulfite (ES, -17 °C) and fluoroethylene carbonate (FEC, ≈23 °C), their mixtures can avoid crystallization at low temperatures, which can be attributed to low intermolecular interactions and altered molecular motion dynamics. A suitable ES/FEC ratio (10 % FEC) can balance the bulk and interface transport of ions, enabling LiNi 0.8 Mn 0.1 Co 0.1 O 2 ||lithium (NCM811||Li) full cells to deliver excellent temperature resilience and cycling stability over a wide temperature range from -50 °C to +70 °C. More than 66 % of the capacity retention was achieved at -50 °C compared to room temperature. The NCM811||Li pouch cells exhibit high cycling stability under realistic conditions (electrolyte weight to cathode capacity ratio (E/C)≤3.5 g Ah -1 , negative to positive electrode capacity ratio (N/P)≤1.09) at different temperatures., (© 2023 Wiley-VCH GmbH.)

Quinone compounds, which are capable of accommodating proton (H + ), are emerging electrodes in aqueous batteries. However, the storage mechanism of proton in quinone compounds is less known and the energy/power density of quinone-based proton battery is still limited. Here we design a series of quinone anodes and study their electrochemical properties in acidic electrolyte, in which tetramethylquinone (TMBQ) delivers a high capacity of 300 mAh g -1 with an extremely low polarization of 20 mV at 1 C, and maintains over 50 % theoretical capacity in less than 16 seconds. The fast kinetics of TMBQ is attributed to the continuous H + migration channel, high H + diffusion coefficient (10 -6  cm 2  s -1 ), and low H + migration energy barrier (0.26 eV). When coupling with MnO 2 cathode, the battery shows a long lifespan of 4000 cycles with a capacity retention of 77 % at 5 C. This study reveals the proton transport in quinone-electrodes and offers new insights to design advanced aqueous batteries., (© 2022 Wiley-VCH GmbH.)

Rare multiple fluorescence properties including aggregation-induced emission and polymorphism/shape/size-dependent emission were found coexisting in a class of typical non-steroidal anti-inflammatory analgesic drugs, fenamates, which could provide a new approach toward future drug evaluation. Different from the complexity and biological incompatibility of the traditional AIE molecular design, this work opens new avenues to the development of new AIE systems.