In-situ strategies for melamine-functionalized graphene oxide nanosheets-based nanocomposite proton exchange membranes in wide-temperature range applications.

The traditional preparation of nanocomposite proton exchange membranes (PEM) is hindered by poor organic-inorganic interface compatibility, insufficient proton-conducting sites, easy aggregation of nanoparticles, and difficulty in leveraging nanoscale advantages. In this study, a novel method involving electrochemical anodic oxidation exfoliation was employed to prepare melamine-coated graphene oxide (Me@GO), which was subsequently subjected to in-situ polymerization with poly(2,5-benzimidazole) (ABPBI) to prepare a Me@GO/ABPBI composite proton exchange membrane. Benefiting from the strong hydrogen bonding and large π stacking interactions, melamine (Me) tightly bound to graphene oxide (GO), effectively preventing the secondary aggregation of GO after exfoliation. Moreover, the abundant alkaline functional groups of melamine enhanced the enhancement of phosphoric acid (PA) retention in the Me@GO/ABPBI membranes, thereby increasing the number of proton-conducting sites. The experimental results indicated that the introduction of Me@GO enhanced membrane properties. For Me@GO at a concentration of 1 wt%, the tensile strength of the 1Me@GO/ABPBI composite membrane reached 207 MPa, nearly 2.52 times that of the pure membrane. The proton conductivity of the 1Me@GO/ABPBI composite membrane reached 0.01 S cm-1 across a wide temperature range (40-180 °C), peaking at 0.087 S cm-1 at 180 °C. Additionally, a single-cell incorporating the 1Me@GO/ABPBI composite membrane achieved a peak power density of 0.304 W cm-2 at 160 °C, nearly 1.46 times that of the pure membrane. Benefiting from the well-dispersed and PA-enriched proton channels provided by Me@GO, the Me@GO/ABPBI composite membrane exhibits excellent prospects for wide-temperature range (40-180 °C) applications.

"Bowling Collision Effect" of CoMo6 Polyoxometalate Units Enables Wide Temperature Range from -20 to 60 °C and Dendrite Mitigation Li-S Batteries.

To improve the performance of Lithium-Sulfur (Li-S) batteries, the reaction catalysts of lithium polysulfides (LiPSs) reactions should have the characteristics of large surface area, efficient atomic utilization, high conductivity, small size, good stability, and strong adjustability. Herein, Anderson-type polyoxometalate ([TMMo6O24]n-, TM = Co, Ni, Fe, represented by TMMo6 POMs) are used as the modified materials for Li-S battery separator. By customizing the central metal atoms, this work gains insights into the layer-by-layer electron transfer mechanism between TMMo6 units and LiPSs, similar to the collision effect of a bowling ball. Theoretical analysis and in situ experimental characterization show that the changes of CoMo6 units with moderate binding energy and lowest Gibbs free energy result in the formation of robust polar bonds and prolonged S─S bonds after adsorption. Hence, the representative Li-S battery with CoMo6 and graphene composite modified separator has a high initial capacity of 1588.6 mA h g-1 at 0.2 C, excellent cycle performance of more than 3000 cycles at 5 C, and uniform Li+ transport over 1900 h. More importantly, this work has revealed the inherent contradiction between the kinetics and thermodynamics, achieving a stable cycle in the temperature range of -20 to 60 °C.

Aqueous Electrolyte With Weak Hydrogen Bonds for Four-Electron Zinc-Iodine Battery Operates in a Wide Temperature Range.

In the pursuit of high-performance energy storage systems, four-electron zinc-iodine aqueous batteries (4eZIBs) with successive I-/I2/I+ redox couples are appealing for their potential to deliver high energy density and resource abundance. However, susceptibility of positive valence I+ to hydrolysis and instability of Zn plating/stripping in conventional aqueous electrolyte pose significant challenges. In response, polyethylene glycol (PEG 200) is introduced as co-solvent in 2 m ZnCl2 aqueous solution to design a wide temperature electrolyte. Through a comprehensive investigation combining spectroscopic characterizations and theoretical simulations, it is elucidated that PEG disrupts the intrinsic strong H-bonds of water by global weak PEG-H2O interaction, which strengthens the O─H covalent bond of water and intensifies the coordination with Zn2+. This synergistic effect substantially reduces water activity to restrain the I+ hydrolysis, facilitating I-/I2/I+ redox kinetics, mitigating I3 - formation and smoothening Zn deposition. The 4eZIBs in the optimized hybrid electrolyte not only deliver superior cyclability with a low fading rate of 0.0009% per cycle over 20 000 cycles and a close-to-unit coulombic efficiency but also exhibit stable performance in a wide temperature range from 40 °C to -40 °C. This study offers valuable insights into the rational design of electrolytes for 4eZIBs.

Elevating Discharge Voltage of Li2CO3-Routine Li-CO2 Battery over 2.9†V at an Ultra-Wide Temperature Window.

The Li-CO2 batteries utilizing greenhouse gas CO2 possess advantages of high energy density and environmental friendliness. However, these batteries following Li2CO3-product route typically exhibit low work voltage (<2.5 V) and energy efficiency. Herein, we have demonstrated for the first time that cobalt phthalocyanine (CoPc) as homogeneous catalyst can elevate the work plateau towards 2.98 V, which is higher than its theoretical discharge voltage without changing the Li2CO3-product route. This unprecedented discharge voltage is illustrated by mass spectrum and electrochemical analyses that CoPc has powerful adsorption capability with CO2 (-7.484 kJ mol-1) and forms discharge intermediate of C33H16CoN8O2. Besides high discharge capacity of 18724 mAh g-1 and robust cyclability over 1600 hours (1000 mAh g-1 cut-off) at a current density of 100 mA g-1, the batteries show high temperature adaptability (-30-80 °C). Our work is paving a promising avenue for the progress of high-efficiency Li-CO2 batteries.

Accelerating the Rate-Determining Steps of Sulfur Conversion Reaction for Lithium-Sulfur Batteries Working at an Ultrawide Temperature Range.

Wide operation temperature is the crucial objective for an energy storage system that can be applied under harsh environmental conditions. For lithium-sulfur batteries, the "shuttle effect" of polysulfide intermediates will aggravate with the temperature increasing, while the reaction kinetics decreases sharply as the temperature decreasing. In particular, sulfur reaction mechanism at low temperatures seems to be quite different from that at room temperature. Here, through in situ Raman and electrochemical impedance spectroscopy studies, the newly emerged platform at cryogenic temperature corresponds to the reduction process of Li2S8 to Li2S4, which will be another rate-determining step of sulfur conversion reaction, in addition to the solid-phase conversion process of Li2S4 to Li2S2/Li2S at low temperatures. Porous bismuth vanadate (BiVO4) spheres are designed as sulfur host material, which achieve the rapid snap-transfer-catalytic process by shortening lithium-ion transport pathway and accelerating the targeted rate-determining steps. Such promoting effect greatly inhibits severe "shuttle effect" at high temperatures and simultaneously improves sulfur conversion efficiency in the cryogenic environment. The cell with the porous BiVO4 spheres as the host exhibits excellent rate capability and cycle performance under wide working temperatures.

Air-Stable and Low-Cost High-Voltage Hydrated Eutectic Electrolyte for High-Performance Aqueous Aluminum-Ion Rechargeable Battery with Wide-Temperature Range.

Aqueous aluminum-ion batteries (AAIBs) are considered as a promising alternative to lithium-ion batteries due to their large theoretical capacity, high safety, and low cost. However, the uneven deposition, hydrogen evolution reaction (HER), and corrosion during cycling impede the development of AAIBs, especially under a harsh environment. Here, a hydrated eutectic electrolyte (AATH40) composed of Al(OTf)3, acetonitrile (AN), triethyl phosphate (TEP), and H2O was designed to improve the electrochemical performance of AAIBs in a wide temperature range. The combination of molecular dynamics simulations and spectroscopy analysis reveals that AATH40 has a less-water-solvated structure [Al(AN)2(TEP)(OTf)2(H2O)]3+, which effectively inhibits side reactions, decreases the freezing point, and extends the electrochemical window of the electrolyte. Furthermore, the formation of a solid electrolyte interface, which effectively inhibits HER and corrosion, has been demonstrated by X-ray photoelectron spectroscopy, X-ray diffraction tests, and in situ differential electrochemical mass spectrometry. Additionally, operando synchrotron Fourier transform infrared spectroscopy and electrochemical quartz crystal microbalance with dissipation monitoring reveal a three-electron storage mechanism for the Al//polyaniline full cells. Consequently, AAIBs with this electrolyte exhibit improved cycling stability within the temperature range of -10-50 °C. This present study introduces a promising methodology for designing electrolytes suitable for low-cost, safe, and stable AAIBs over a wide temperature range.

Synergistic Strain Suppressing and Interface Engineering in Na4MnV(PO4)3/C for Wide-Temperature and Long-Calendar-Life Sodium-Ion Storage.

A Na4MnV(PO4)3 (NMVP) cathode is regarded as a promising cathode candidate for sodium-ion batteries (SIBs). However, issues such as low electronic conductivity and partial cation dissolution contribute to high polarization and structure distortion. Herein, we engineered the local electron density and reaction kinetic properties of NMVP cathodes with varying oxygen vacancies by introducing varying amounts of Zr doping and carbon coating. The optimized sample exhibited a high-rate capacity of 71.8 mAh g-1 at 30 C (83.1% capacity retention after 1000 cycles) and excellent performance over a wide temperature range (84.1 mAh g-1 at 60 °C and 61.4 mAh g-1 at -30 °C). In situ X-ray diffraction technology confirmed a redox solid solution and a two-phase reaction mechanism, revealing minor changes in cell volume and slight strain variations after Zr doping, effectively suppressing the structural distortion. Theoretical calculations illustrated that Zr doping largely shrinks the band gap of NMVP, enriches local electron density, and slightly alters the local element distribution and bond lengths. Moreover, full-cells have shown high energy density (259.9 Wh kg-1) and outstanding cycling stability (200 cycles). The work provides fresh insights into the synergistic effect of strain suppressing and interface engineering in promoting the development of wide temperature range and long-calendar-life SIBs.

A Hydrogel Electrolyte with High Adaptability over a Wide Temperature Range and Mechanical Stress for Long-Life Flexible Zinc-Ion Batteries.

Flexible zinc-ion batteries have garnered significant attention in the realm of wearable technology. However, the instability of hydrogel electrolytes in a wide-temperature range and uncontrollable side reactions of the Zn electrode have become the main problems for practical applications. Herein, N,N-dimethylformamide (DMF) to design a binary solvent (H2O-DMF) is introduced and combined it with polyacrylamide (PAM) and ZnSO4 to synthesize a hydrogel electrolyte (denoted as PZD). The synergistic effect of DMF and PAM not only guides Zn2+ deposition on Zn(002) crystal plane and isolates H2O from the Zn anode, but also breaks the hydrogen bonding network between water to improve the wide-temperature range stability of hydrogel electrolytes. Consequently, the symmetric cell utilizing PZD can stably cycle over 5600 h at 0.5 mA cm- 2@0.5 mAh cm-2. Furthermore, the Zn//PZD//MnO2 full cell exhibits favorable wide-temperature range adaptability (for 16000 cycles at 3 A g-1 under 25 °C, 750 cycles with 98 mAh g-1 at 0.1 A g-1 under -20 °C) and outstanding mechanical properties (for lighting up the LEDs under conditions of pressure, bending, cutting, and puncture). This work proposes a useful modification for designing a high-performance hydrogel electrolyte, which provides a reference for investigating the practical flexible aqueous batteries.

Nano-Interfacial Supramolecular Adhesion of Metal-Organic Framework-Based Separator Enables High-Safety and Wide-Temperature-Range Lithium Batteries.

Polyolefin separators are the most commonly used separators for lithium batteries; however, they tend to shrink when heated, and their Li+ transference number (t Li +) is low. Metal-organic frameworks (MOFs) are expected to solve the above problems due to their high thermal stability, abundant pore structure, and open metal sites. However, it is difficult to prepare high-porosity MOF-based membranes by conventional membrane preparation methods. In this study, a high-porosity free-standing MOF-based safety separator, denoted the BCM separator, is prepared through a nano-interfacial supramolecular adhesion strategy. The BCM separator has a large specific surface area (450.22 m2 g-1) and porosity (62.0%), a high electrolyte uptake (475 wt%), and can maintain its morphology at 200 °C. The ionic conductivity and t Li + of the BCM separator are 1.97 and 0.72 mS cm-1, respectively. Li//LiFePO4 cells with BCM separators have a capacity retention rate of 95.07% after 1100 cycles at 5  C, a stable high-temperature cycling performance of 300 cycles at 80 °C, and good capacity retention at -40 °C. Li//NCM811 cells with BCM separators exhibit significantly improved rate performance and cycling performance. Pouch cells with BCM separators can work at 120 °C and have good safety at high temperature.

Interphase Engineering via Solvent Molecule Chemistry for Stable Lithium Metal Batteries.

Lithium metal battery has been regarded as promising next-generation battery system aiming for higher energy density. However, the lithium metal anode suffers severe side-reaction and dendrite issues. Its electrochemical performance is significantly dependant on the electrolyte components and solvation structure. Herein, a series of fluorinated ethers are synthesized with weak-solvation ability owing to the duple steric effect derived from the designed longer carbon chain and methine group. The electrolyte solvation structure rich in AGGs (97.96 %) enables remarkable CE of 99.71 % (25 °C) as well as high CE of 98.56 % even at -20 °C. Moreover, the lithium-sulfur battery exhibits excellent performance in a wide temperature range (-20 to 50 °C) ascribed to the modified interphase rich in LiF/LiO2. Furthermore, the pouch cell delivers superior energy density of 344.4 Wh kg-1 and maintains 80 % capacity retention after 50 cycles. The novel solvent design via molecule chemistry provides alternative strategy to adjust solvation structure and thus favors high-energy density lithium metal batteries.

Enabling All-Solid-State Lithium-Carbon Dioxide Battery Operation in a Wide Temperature Range.

Flexible all-solid-state lithium-carbon dioxide batteries (FASSLCBs) are recognized as a next-generation energy storage technology by solving safety and shuttle effect problems. However, the present FASSLCBs rely heavily on high-temperature operation due to sluggish solid-solid-gas multiphase mass transfer and unclear capacity degradation mechanism. Herein, we designed bicontinuous hierarchical porous structures (BCHPSs) for both solid polymer electrolyte and cathode for FASSLCBs to facilitate the mass transfer in all connected directions. The formed large Lewis acidic surface effectively promotes the lithium salt dissociation and the CO2 conversion. Furthermore, it is unraveled that the battery capacity degradation originates from the "dead Li2CO3" formation, which is inhibited by the fast decomposition of Li2CO3. Accordingly, the assembled FASSLCBs exhibit an excellent cycling stability of 133 cycles at 60 °C, which is 2.7 times longer than that without BCHPSs, and the FASSLCBs can be operated repeatedly even at room temperature. This BCHPS method and fundamental deactivation mechanism provide a perspective for designing FASSLCBs with long cycling life.

Enhanced Thermal Stability and Broad Temperature Range in High-Entropy (La0.2Ce0.2Nd0.2Sm0.2Eu0.2)NbO4 Ceramics.

Next-generation high-temperature applications increasingly rely heavily on advanced thermistor materials with enhanced thermal stability and electrical performance. However, thus far, the great challenge of realizing high thermal stability and precision in a wide temperature range has become a key bottleneck restricting the high-temperature application. Here, we propose a high-entropy strategy to design novel high-temperature thermistor ceramics (La0.2Ce0.2Nd0.2Sm0.2Eu0.2)NbO4. Differences in atomic size, mass, and electronegativity in this high-entropy system cause high lattice distortion, substantial grain boundaries, and high dislocation density. These enhance the charge carrier transport and reduce the grain boundary resistance, thus synergistically broadening the temperature range. Our samples maintain high precision and thermal stability over a wide temperature range from room temperature to 1523 K (ΔT = 1250 K) with an aging value as low as 0.42% after 1000 h at 1173 K, showing breakthrough progress in high-temperature thermistor ceramics. This study establishes an effective approach to enhancing the performance of high-temperature thermistor materials through high-entropy strategies.

Locally Concentrated Ionic Liquid Electrolytes for Wide-Temperature-Range Aluminum-Sulfur Batteries.

Aluminum-sulfur (Al-S) batteries are promising energy storage devices due to their high theoretical capacity, low cost, and high safety. However, the high viscosity and inferior ion transport of conventionally used ionic liquid electrolytes (ILEs) limit the kinetics of Al-S batteries, especially at sub-zero temperatures. Herein, locally concentrated ionic liquid electrolytes (LCILE) formed via diluting the ILEs with non-solvating 1,2-difluorobenzene (dFBn) co-solvent are proposed for wide-temperature-range Al-S batteries. The addition of dFBn effectively promotes the fluidity and ionic conductivity without affecting the AlCl4 - /Al2 Cl7 - equilibrium, which preserves the reversible stripping/plating of aluminum and further promotes the overall kinetics of Al-S batteries. As a result, Al-S cells employing the LCILE exhibit higher specific capacity, better cyclability, and lower polarization with respect to the neat ILE in a wide temperature range from -20 to 40 °C. For instance, Al-S batteries employing the LCILE sustain a remarkable capacity of 507 mAh g-1 after 300 cycles at 20 °C, while only 229 mAh g-1 is delivered with the dFBn-free electrolyte under the same condition. This work demonstrates the favorable use of LCILEs for wide-temperature Al-S batteries.

An All-Climate Nonaqueous Hydrogen Gas-Proton Battery.

Rechargeable hydrogen gas batteries, driven by hydrogen evolution and oxidation reactions (HER/HOR), are emerging grid-scale energy storage technologies owing to their low cost and superb cycle life. However, compared with aqueous electrolytes, the HER/HOR activities in nonaqueous electrolytes have rarely been studied. Here, for the first time, we develop a nonaqueous proton electrolyte (NAPE) for a high-performance hydrogen gas-proton battery for all-climate energy storage applications. The advanced nonaqueous hydrogen gas-proton battery (NAHPB) assembled with a representative V2(PO4)3 cathode and H2 anode in a NAPE exhibits a high discharge capacity of 165 mAh g-1 at 1 C at room temperature. It also efficiently operates under all-climate conditions (from -30 to +70 °C) with an excellent electrochemical performance. Our findings offer a new direction for designing nonaqueous proton batteries in a wide temperature range.

Hydrated Eutectic Electrolyte Induced Bilayer Interphase for High-Performance Aqueous Zn-Ion Batteries with 100 °C Wide-Temperature Range.

The practical implementation of aqueous zinc-ion batteries (AZIBs) encounters challenges such as dendrite growth, parasitic reactions, and severe decay in battery performance under harsh environments. Here, a novel hydrated eutectic electrolyte (HEE) composed of Zn(ClO4 )2 ·6H2 O, ethylene glycol (EG), and InCl3 solution is introduced to effectively extend the lifespan of AZIBs over a wide temperature range from -50 to 50 °C. Molecular dynamics simulations and spectroscopy analysis demonstrate that the H2 O molecules are confined within the liquid eutectic network through dual-interaction, involving coordination with Zn2+ and hydrogen bonding with EG, thus weakening the activity of free water and extending the electrochemical window. Importantly, cryo-transmission electron microscopy and spectroscopy techniques reveal that HEE in situ forms a zincophobic/zincophilic bilayer interphase by the dissociation-reduction of eutectic molecules. Specifically, the zincophilic interphase reduces the energy barrier for Zn nucleation, promoting uniform Zn deposition, while the zincophobic interphase prevents active water from contacting the Zn surface, thus inhibiting the side reactions. Furthermore, the relationships between the structural evolution of the liquid eutectic network and interfacial chemistry at electrode/electrolyte interphase are further discussed in this work. The scalability of this design strategy can bring benefits to AZIBs operating over a wide temperature range.

Endowing the Operability of Supercapacitors at High Temperatures by Regulating the Solvation Structure in Dilute Hybrid Electrolyte with Trimethyl Phosphate Cosolvent.

The redox stabilities of different oxygen donor solvents (C═O, P═O and S═O) and lithium salt anions for supercapacitors (SCs) electrolytes have been compared by calculating the frontier molecular orbital energy. Among six lithium difluoro(oxalate)borate (LiDFOB)-based mono-solvent electrolytes, the dilute LiDFOB-1,4-butyrolactone (GBL) electrolyte exhibits the highest operating voltage but suffers from electrolyte breakdown at elevated temperatures. Trimethyl phosphate (TMP) exhibits the highest redox stability and a strongly negative electrostatic potential (ESP), making it suitable for promoting the dissolution of LiDFOB as expected. Therefore, TMP is selected as a co-solvent into LiDFOB-GBL electrolyte to regulate Li+ solvation structure and improve the operability of electrolytes at high temperatures. The electrochemical stable potential window (ESPW) of 0.5 m LiDFOB-G/T(5/5) hybrid electrolyte can reach 5.230 V. The activated carbon (AC)-based symmetric SC using 0.5 m LiDFOB-G/T(5/5) hybrid electrolyte achieves a high energy density of 54.2 Wh kg-1 at 1.35 kW kg-1 and the capacitance retention reaches 89.2% after 10 000 cycles. The operating voltage of SC can be maintained above 2 V when the temperature rises to 60 °C.

A Non-Flammable and Flexible Aluminum Derived Lithium-Ion Storage Device with a Wide Temperature Range of Operation.

With the rapid development and increasing popularity of electric vehicles and wearables, battery safety has become a leading focus in the field of energy storage research. Specifically, aluminum-ion batteries are gaining increasing attention as low-cost energy-storage systems with high safety levels and theoretical energy density. However, the dense alumina passivation layer on the aluminum anode surface and slow kinetic performance of commonly used ionic liquid electrolytes still render poor performance. This report presents a new type of aluminum-derived lithium-ion battery (ALIB) that maintains a certain discharge performance under damaging conditions, including continuous bending, high- and low-temperature environments, and shearing. This new ALIB effectively meets the current demand for flexible and wearable batteries. The prepared ALIB achieves a stable cycle of 130 mAh g-1 specific capacity and ≈260 Wh kg-1 theoretical energy density at a wide voltage platform of 2 V and a test temperature of 25 °C without undergoing combustion. Additionally, the study analyzes the reaction mechanism of this ALIB based on density functional theory and conducts ex situ XRD and XPS analyses to elucidate the underlying storage mechanism.

Adaptive Ionization-Induced Tunable Electric Double Layer for Practical Zn Metal Batteries over Wide pH and Temperature Ranges.

The violent side reactions of Zn metal in aqueous electrolyte lead to sharp local-pH fluctuations at the interface, which accelerate Zn anode breakdown; thus, the development of an optimization strategy to accommodate a wide pH range is particularly critical for improving aqueous Zn metal batteries. Herein, we report a pH-adaptive electric double layer (EDL) tuned by glycine (Gly) additive with pH-dependent ionization, which exhibits excellent capability to stabilize Zn anodes in wide-pH aqueous electrolytes. It is discovered that a Gly-ionic EDL facilitates the directed migration of charge carriers in both mildly acidic and alkaline electrolytes, leading to the successful suppression of local saturation. It is worth mentioning that the regulation effect of the additive concentration on the inner Helmholtz plane (IHP) structure of Zn electrodes is clarified in depth. It is revealed that the Gly additives without dimerization can develop orderly and dense vertical adsorption within the IHP to effectively reduce the EDL repulsive force of Zn2+ and isolate H2O from the anode surface. Consequently, they Zn anode with tunable EDL exhibits superior electrochemical performance in a wide range of pH and temperature, involving the prodigious cycle reversibility of 7000 h at Zn symmetric cells with ZnSO4-Gly electrolytes and an extended lifespan of 50 times in Zn symmetric cells with KOH-Gly electrolytes. Moreover, acidic Zn powder||MnO2 pouch cells, and alkaline high-voltage Zn||Ni0.8Co0.1Mn0.1O2 cells, and Zn||NiCo-LDH cells also deliver excellent cycling reversibility. The tunable EDL enables the ultrahigh depth of discharge (DOD) of 93%. This work elucidates the design of electrolyte additives compatible in a wide range of pH and temperature, which might cause inspiration in the fields of practical multiapplication scenarios for Zn anodes.

Breaking Barriers to High-Practical Li-S Batteries with Isotropic Binary Sulfiphilic Electrocatalyst: Creating a Virtuous Cycle for Favorable Polysulfides Redox Environments.

Investigations into lithium-sulfur batteries (LSBs) has focused primarily on the initial conversion of lithium polysulfides (LiPSs) to Li2 S2 . However, the subsequent solid-solid reaction from Li2 S2 to Li2 S and the Li2 S decomposition process should be equally prioritized. Creating a virtuous cycle by balancing all three chemical reaction processes is crucial for realizing practical LSBs. Herein, amorphous Ni3 B in synergy with carbon nanotubes (aNi3 B@CNTs) is proposed to implement the consecutive catalysis of S8(solid) → LiPSs(liquid) → Li2 S(solid) →LiPSs(liquid) . Systematic theoretical simulations and experimental analyses reveal that aNi3 B@CNTs with an isotropic structure and abundant active sites can ensure rapid LiPSs adsorption-catalysis as well as uniform Li2 S precipitation. The uniform Li2 S deposition in synergy with catalysis of aNi3 B enables instant/complete oxidation of Li2 S to LiPSs. The produced LiPSs are again rapidly and uniformly adsorbed for the next sulfur evolution process, thus creating a virtuous cycle for sulfur species conversion. Accordingly, the aNi3 B@CNTs-based cell presents remarkable rate capability, long-term cycle life, and superior cyclic stability, even under high sulfur loading and extreme temperature environments. This study proposes the significance of creating a virtuous cycle for sulfur species conversion to realize practical LSBs.

Weak solvent chemistry enables stable aqueous zinc metal batteries over a wide temperature range from -50 to 80 °C.

The development of electrolytes with a wide temperature range, no dendrite growth and corrosion resistance is essential for the practical application of aqueous zinc metal batteries. Herein, γ-valerolactone is developed as the co-solvent to extend the operating temperature range of the aqueous electrolyte and stabilize the zinc metal anode interface. This weak solvent acts as a strong hydrogen bonding ligand and "diluent" to break the hydrogen bonds between free water molecules, thus enhancing the temperature tolerance and chemical stability of the electrolyte. The γ-valerolactone can also be adsorbed on the anode surface to achieve a dendrite-free zinc deposition behavior by promoting zinc nucleation and regulating zinc growth texture. The optimized electrolyte enables the symmetric cell to deliver a cycle/rest life of 2160 h and operate stably over a wide temperature range of -50 to 80 °C. The corresponding Zn||AC and Zn||PANI cells exhibit capacity retention of 92.5% and 85% after 8100 and 1600 cycles, respectively. This mechanism of weak solvent-regulated hydrogen bonding and solvent sheath provides new insights into the design of advanced aqueous electrolytes.