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Prussian blue analogs (PBAs) are promising insertion‐type cathode materials for different types of aqueous batteries, capable of accommodating metal or non‐metal ions. However, their practical application is hindered by their susceptibility to dissolution, which leads to a shortened lifespan. Herein, we have revealed that the dissolution of PBAs primarily originates from the locally elevated pH of electrolytes, which is caused by the proton co‐insertion during discharge. To address this issue, the water‐locking strategy has been implemented, which interrupts the generation and Grotthuss diffusion of protons by breaking the well‐connected hydrogen bonding network in aqueous electrolytes. As a result, the hybrid electrolyte enables the iron hexacyanoferrate to endure over 1000 cycles at a 1 C rate and supports a high‐voltage pH‐decoupled cell with an average voltage of 1.95 V. These findings provide insights for mitigating the dissolution of electrode materials, thereby enhancing the viability and performance of aqueous batteries. [ABSTRACT FROM AUTHOR]

In the pursuit of next‐generation ultrahigh‐energy‐density Li−O2 batteries, it is imperative to develop an electrolyte with stability against the strong oxidation environments. N,N‐dimethylacetamide (DMA) is a recognized solvent known for its robust resistance to the highly reactive reduced oxygen species, yet its application in Li−O2 batteries has been constrained due to its poor compatibility with the Li metal anode. In this study, a rationally selected hydrofluoroether diluent, methyl nonafluorobutyl ether (M3), has been introduced into the DMA‐based electrolyte to construct a localized high concentration electrolyte. The stable −CH3 and C−F bonds within the M3 structure could not only augment the fundamental properties of the electrolyte but also fortify its resilience against attacks from O2− and 1O2. Additionally, the strong electron‐withdrawing groups (−F) presented in the M3 diluent could facilitate coordination with the electron‐donating groups (−CH3) in the DMA solvent. This intermolecular interaction promotes more alignments of Li+‐anions with a small amount of M3 addition, leading to the construction of an anion‐derived inorganic‐rich SEI that enhances the stability of the Li anode. As a result, the Li−O2 batteries with the DMA/M3 electrolyte exhibit superior cycling performance at both 30 °C (359th) and −10 °C (120th). [ABSTRACT FROM AUTHOR]

Lithium–oxygen batteries (LOBs) have been regarded as a promising energy storage system for applications in electric vehicles and aviation. However, the development of high-performance LOBs has been hindered by the challenges associated with insulating discharge products, such as low energy efficiency and poor rate performance. Here, we report that insulating lithium peroxide (Li2O2) can deposit with a carbon nanotube (CNT) additive during the discharge process and eventually be woven into a conductive network. The constructed network enhances the conductivity of Li2O2 and accelerates the kinetics of electrode reactions. As a result, the battery containing 1.0 mg mL−1 CNTs in the electrolyte exhibits a high areal capacity of 5.7 mA h cm−2 and superior rate performance at 1.41 A gCNT−1. Furthermore, the introduction of ruthenium nanoparticles to the CNTs results in stable cycling for 550 hours. This research opens up a new avenue for addressing the issues caused by insulating discharge products in LOBs. [ABSTRACT FROM AUTHOR]

In this work, experiment results of CH4 hydrate formation pressure in four imidazole ionic liquid solutions have been determined. Hydrogen bond interaction between ionic liquids and water molecules has been simulated by conductor like screening model for real solvents model (COSMO‐RS). Hydrogen bond energy has been calculated. Variation of hydrogen bond energy between ionic liquid and water molecules was obtained by COSMO‐RS simulation. The inhibition effect of four ionic liquids on water activity was listed from strong to weak in order: [BMIm]Br > [BMIm]BF4 > [BMIm]PF6 > [OMIm]BF4. Compared with experimental results of CH4 hydrate formation pressure in ionic liquid aqueous solution, hydrogen bond interaction between ionic liquid and water molecules obtained by COSMO‐RS is basically consistent with experimental results of hydrate formation pressure in ionic liquid. The study could provide better theoretical basis for ionic liquid selection on gas hydrate study. The simulation would be better as one method to chose admirable ionic liquid in the area of hydrate additives usage. [ABSTRACT FROM AUTHOR]

The surrounding hydrogen bond (H‐bond) interaction around the active sites plays indispensable functions in enabling the organic electrode materials (OEMs) to fulfill their roles as ion reservoirs in aqueous zinc‐organic batteries (ZOBs). Despite important, there are still no works could fully shed its real effects light on. Herein, quinone‐based small molecules with a H‐bond evolution model has been rationally selected to disclose the regulation and equilibration of H‐bond interaction between OEMs, and OEM and the electrolyte. It has been found that only a suitable H‐bond interaction could make the OEMs fully liberate their potential performance. Accordingly, the 2,5‐diaminocyclohexa‐2,5‐diene‐1,4‐dione (DABQ) with elaborately designed H‐bond structure exhibits a capacity of 193.3 mAh g−1 at a record‐high mass loading of 66.2 mg cm−2 and 100 % capacity retention after 1500 cycles at 5 A g−1. In addition, the DABQ//Zn battery also possesses air‐rechargeable ability by utilizing the chemistry redox of proton. Our results put forward a specific pathway to precise utilization of H‐bond to liberate the performance of OEMs. [ABSTRACT FROM AUTHOR]

Garnet solid‐state electrolytes (SSEs) Li6.5La3Zr1.5Ta0.5O12 (LLZTO) suffer from poor air stability, producing Li2CO3 by‐products and causing poor interfacial contact against the Li metal. Obtaining hydrophobic and lithiophilic surface of LLZTO is meaningful for high‐performance solid‐state batteries. Here, a hydrophobic CFx film is firstly introduced on the LLZTO surface (CFx‐LLZTO) by magnetron sputtering the polytetrafluoroethylene (PTFE) target. Benefit from its outstanding hydrophobicity, this CFx film provides the LLZTO a Li2CO3‐free surface. Moreover, the LiC‐LiF mixed conductive interlayer is formed through the reaction between CFx film and Li metal, resulting in a low interfacial resistance of 73.49 Ω/cm2. In addition, the LiC‐LiF mixed conductive interlayer can also homogenize the electric‐field distribution and enable fast Li+ conduction. As a result, the construction of the hydrophobic mixed conductive interlayer makes the CFx‐LLZTO based symmetric Li/Li cell exhibit a high critical current density of 1.2 mA/cm2 and a stable cycling life for over 1200 h at 0.1 mA/cm2. Furthermore, the Li/LiFePO4 cells with the CFx‐LLZTO show improved cycling and rate performance at room temperature. This work provides a practical solution for achieving high‐performance solid‐state lithium batteries. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: The increasing demand for high‐energy storage systems has propelled the development of Li‐air batteries and Li‐O2/CO2 batteries to elucidate the mechanism and extend battery life. However, the high charge voltage of Li2CO3 accelerates the decomposition of traditional sulfone and ether electrolytes, thus adopting high‐voltage electrolytes in Li‐O2/CO2 batteries is vital to achieve a stable battery system. Herein, we adopt a commercial carbonate electrolyte to prove its excellent suitability in Li‐O2/CO2 batteries. The generated superoxide can be captured by CO2 to form less aggressive intermediates, stabilizing the carbonate electrolyte without reactive oxygen species induced decomposition. In addition, this electrolyte permits the Li metal plating/stripping with a significantly improved reversibility, enabling the possibility of using ultra‐thin Li anode. Benefiting from the good rechargeability of Li2CO3, less cathode passivation, and stabilized Li anode in carbonate electrolyte, the Li‐O2/CO2 battery demonstrates a long cycling lifetime of 167 cycles at 0.1 mA·cm–2 and 0.25 mAh·cm–2. This work paves a new avenue for optimizing carbonate‐based electrolytes for Li‐O2 and Li‐O2/CO2 batteries. [ABSTRACT FROM AUTHOR]