纤维状锌空气电池是锂离子电池之外前景广阔的柔性可充电储能器件. 然而, 电池的半开放结构导致空气中水分侵入, 从而引发阳极不稳定, 出现析氢副反应和锌枝晶. 因此, 本文利用无监督机器学习确定乙酰胺作为功能性电解质添加剂. 理论和实验表明乙酰胺分子能够调节准固态电解质的Zn2+溶剂化和凝聚态结构, 优先吸附在锌表面, 从而减轻自由水腐蚀, 并引导Zn2+沿着(002)晶面沉积, 抑制枝晶形成. 这些特性使得纤维锌空气电池的可逆性超过1500次循环(500 h), 并且可集成到自供电电子纺织品中.

High-voltage lithium metal batteries require electrolytes that simultaneously combine oxidative stability with Li metal compatibility, posing a major challenge for conventional ether-based systems, which are typically limited to voltages below 4.0 V. Although conventional electrolyte engineering has been widely employed to enhance oxidative stability, they often compromise ionic conductivity or require complex synthetic routes. Herein, we propose a strategy based on dihydrogen-bonding interactions by introducing 0.05 M LiBH₄ into conventional ether-based electrolytes to construct a dihydrogen-bonded electrolyte. The hydridic H- in BH₄- interacts with the active Hδ⁺ atoms of 1,2-dimethoxyethane to form dihydrogen bonds, thereby weakening the Li⁺-solvent interaction, accelerating Li⁺ de-solvation, and promoting uniform Li deposition. Simultaneously, these dihydrogen-bonding interactions shield the active Hδ⁺ sites of the solvent within the positive electrode interface, thereby significantly suppressing the oxidative decomposition of 1,2-dimethoxyethane. As a result, the oxidative stability of the electrolyte is extended to 5.54 V without compromising ionic conductivity (>16 mS cm-1/30 °C). Lithium metal full cells using this electrolyte exhibit stable cycling at 4.5 V. This study provides a promising pathway for the design of high-voltage ether-based electrolytes.

Solid‐state lithium metal batteries (SSLMBs) are widely recognized as next‐generation energy storage devices with great potential. However, their commercialization has been hindered by bottleneck issues related to solid electrolytes (SEs), including poor mechanical strength, inadequate thermal management capabilities, poor interface stability, and limited room‐temperature ionic conductivity. Boron nitride (BN), with its diverse crystal structures and excellent performance, has been widely used in electrolytes for SSLMBs. Herein, we provide a comprehensive review of research progress on BN‐based materials applied in solid‐state electrolytes (SSEs) for SSLMBs. First, the relationships of the basic structure, properties, and synthesis of BN are briefly elucidated. Subsequently, the application strategies and mechanisms of raw/modified BN in polymer‐based and inorganic solid electrolytes are systematically elaborated and discussed, emphasizing its role in enhancing mechanical strength, inhibiting lithium dendrites’ growth, optimizing ion transport, and stabilizing the interfaces. Representative research results demonstrate that SSEs incorporated with BN‐based materials can significantly enhance the cycling stability, ionic conductivity, and rate performance of SSLMBs. Finally, the challenges and future development directions of BN‐based materials in SSEs were proposed, aiming to provide useful references for the design of high‐performance SSEs and their practical applications.

Conventional amine-based electrolytes exhibit superior compatibility with Mg metal anodes, but their practical application is fundamentally constrained by both a restricted electrochemical stability window (<2.0 V on Al foils) and non-negligible high cation desolvation energy barriers. Herein, we first focus on enhancing cation-solvent interaction through a rational high-concentration Li/Mg dual-salt strategy, effectively suppressing free amine solvent molecules and thereby expanding the electrochemical window to exceed 3.0 V. This widened electrochemical window ensures direct compatibility with the industrial Li-ion cathode. Furthermore, to address the high cation desolvation energy barriers and low conductivity in this electrolyte, the ether solvent with a lower coordination ability is introduced into the electrolyte, where part of the ether can participate in the Li+ solvation structure to alleviate overly strong amine coordination, while the rest can serve as a pseudo-diluent, promoting a reduced cathode desolvation energy barrier and enhanced ion transport. Finally, the Mg//LiFePO4 battery delivers a stable plateau of 2.7 V and a high energy density at the electrode level. This work proposes an efficient electrolyte design paradigm that simultaneously balances Mg anode reversibility, high-voltage cathode compatibility, and a facile preparation method in Mg batteries for the first time, revealing a comprehensive exploration process for high-voltage Mg batteries.

The advancement of high-performance and cost-effective electrocatalysts facilitating oxygen generation utilizing transition metals is pivotal for enabling the widespread implementation of generation of hydrogen through water electrolysis. Here, we designed a heterostructure engineering and Fe incorporation strategy to prepare Fe-NiS/ NiS2 catalyst via one-pot hydrothermal way.Fe doping significantly enhances catalytic performance through a dual regulation mechanism- inducing the phase transformation from NiS to NiS2 and forming NiS/NiS2 heterostructure with optimized electronic structure.Fe-NiS/NiS2 heterostructure demonstrates superior alkaline oxygen evolution activity, attaining ti10 = 264 mV in 1 M KOH electrolyte with accelerated kinetics (Tafel slope = 61.4 mV/dec). Additionally, this catalyst exhibits no significant performance degradation after 24 h of continuous operation. This work demonstrates the feasibility of a strategy with good regulation of the catalyst's electronic structure to improve the catalytic performance of low-cost electrocatalysts for water oxidation.

Sodium superionic conductor (NASICON)-type solid-state electrolytes (SSEs) are promising candidates for solid-state sodium batteries (SSSBs) due to their high room-temperature ionic conductivity and excellent chemical stability. However, their interphascial incompatibility with sodium metal anodes leads to poor contact, slow ion transport, and dendrite growth. In this work, we demonstrate a dual-component interphase with both sodiophilicity and electron-insulating capability to prolong the cyclability of SSSBs. SbF3 was spin-coated onto Na3.4Zn0.2Zr1.8Si2.2P0.8O12 (NZZP) electrolyte surface and then converted to the Na3Sb/NaF (NSF) composite interlayer via the reaction with Na. Na3Sb exhibits high sodiophilicity, enhancing interphascial wettability. Meanwhile, NaF possesses a wide bandgap of 6.17 eV and high mechanical strength, blocking electron leakage and suppressing dendrite propagation. As a result, Na|NSF-NZZP-NSF|Na symmetric cells demonstrate ultra-low interphascial resistance of 4.7 Ω cm2, high critical current density of 2.2 mA cm-2 at 25°C and stable cycles over 2400 h at 0.5 mA cm-2. Using Na3V2(PO4)3 (NVP) cathode, the solid-state full cell displays an impressive capacity retention of 94.5% after 600 cycles at 2 C. This work provides a simple, effective, and scalable approach for constructing stable SSSBs.

The relatively low room-temperature ionic conductivity and terrible lithium dendrite growth of polycarbonate-based solid polymer electrolytes (SPEs) seriously restrict their further development for solid-state lithium metal batteries (SSLMBs). Herein, a polycarbonate-based SPE is innovatively designed through facile in situ polymerization of ferroelectric poly(vinylidene fluoride-trifluoroethylene-chlorotrifluoroethylene) (PVTC) and vinyl ethylene carbonate (VEC) monomer (PVTC-g-PVEC). This in situ polymerized PVTC-g-PVEC SPE with polar & horbar;CF2 group and C & boxH;O/C & horbar;O groups greatly promotes the dissociation of Li salts and enhances the transport of Li+. Moreover, the ferroelectric PVTC-g-PVEC SPE can produce spontaneous polarization under external electric fields, which promotes uniform deposition of Li+ and suppresses lithium dendrite growth. In addition, the fabricated PVTC-g-PVEC SPE facilitates the formation of a stable solid electrolyte interface and cathode electrolyte interface, effectively reducing side reactions at the electrode/electrolyte interfaces. Specifically, the Li|PVTC-g-PVEC|Li symmetric cell can exhibit ultra-long cycle stability for more than 10 000 h (>416 days). The assembled LiFePO4|PVTC-g-PVEC|Li cell and high-voltage LiNi0.8Co0.1Mo0.1O2|PVTC-g-PVEC|Li cell exhibit outstanding cycling stability for 1000 cycles at 2C and 500 cycles at 1C, respectively. The pouch batteries also depict high safety against abusive conditions. This in situ polymerized ferroelectric engineering strategy establishes a new pathway for designing high-performance solid-state lithium batteries.

A dual-modification approach was developed to tailor the bulk crystal structure and surface/interface characteristics of LiFePO4 cathodes for high-performance lithium-ion batteries. This approach was based on the idea that intrinsic constraints in lithium-ion transport and electrical conductivity frequently cannot be overcome by single-component modifications. A carbon–fluorine–titanium (C/F/Ti) hybrid surface modification was introduced together with W/B co-doping to modify both bulk and interfacial properties. W-containing species were associated with improved electronic transport characteristics, whereas boron incorporation was supported by enhanced structural stability of the polyanion framework. It is suggested that the Ti/F-containing surface layer provides a modified interfacial region that could protect the electrode surface and help Li+ transit. With a capacity retention of 91.12

Aqueous zinc-ion batteries (AZIBs) are one of the most promising energy storage technologies due to their high safety, low cost, and environmental friendliness. However, challenges such as dendrite growth, hydrogen evolution reactions, and anode-electrolyte side reactions hinder the further development of AZIBs. Herein, we introduce a functional MXene/TiO2 heterojunction artificial coating layer, and the zincophilic properties of TiO2 and the MXene/TiO2 heterojunction of this coating layer provide abundant zincophilic sites, promoting uniform Zn deposition and effectively suppressing dendrite growth on the Zn anode. Additionally, the constructed MXene/TiO2 SEI isolates the aqueous ZnSO4 electrolyte from the zinc anode, protecting it from corrosion. As a result, the MXene/TiO2@Zn anode exhibits enhanced long-term cycling performance, achieving 1200 h at a current density of 0.2 mA cm- 2 and 0.2 mAh cm- 2. The MXene/TiO2@Zn anode also demonstrates excellent plating/stripping behavior over 400 cycles on Cu foil. Moreover, the assembled MXene/TiO2@Zn/MnO2 and MXene/TiO2@Zn/NH4V4O10 full cells show significantly improved long-term cycling stability and high capacity retention. This strategy offers a highly reversible zinc anode, paving the way for the future development of rechargeable AZIBs.

Zinc-air batteries are considered promising candidates for the next generation of batteries due to their significant advantages in theoretical specific capacity, safety, and environmental friendliness. The combination of gel polymer electrolytes and zinc-air batteries further expands future energy storage applications. However, traditional alkaline gel zinc-air batteries are usually constructed by post-stacking methods, and their poor interfacial contact and weakened long-term durability in the ambient air hinders practical applications. Here, we synthesized a non-alkaline gel electrolyte with a liquid-solid phase transition mechanism utilizing agar, and constructed an integrated gel zinc-air battery by direct injection and encapsulation methods. This strategy realizes the integrated assembly of non-alkaline gel zinc-air full batteries, thereby obtaining all-round high stability. The agar gel electrolyte endows the battery with outstanding performance, including a high output specific capacity (706 mAh g Zn-1), a long discharge duration (270 h at 0.1 mA cm(-2)), and a significant operational life (850 h at 0.2 mA cm(-2)). Importantly, the integrated zinc-air pouch battery can achieve a high zinc utilization rate of over 80% in various discharge states and exhibit satisfactory cycling stability (>200 h at 0.1 mA cm(-2)). This technology alleviates the current challenges of gel zinc batteries, and highlights the direction for the development of non-alkaline gel zinc-air full batteries.

Magnesium-oxygen (Mg-O2) batteries are considered promising candidates for next-generation energy storage systems due to their high specific energy, low cost and intrinsic safety. However, poor rechargeability remains a critical barrier, largely due to the lack of suitable electrolytes and undesired irreversible cathode reactions. Here we report a rechargeable non-aqueous Mg-O2 battery enabled by a tailored electrolyte featuring a cage-like Mg2+ solvation environment. We find that varying ether solvent chain lengths, alongside a tridentate chelating agent, can act coordinately to form a dynamic solvation microreactor. This solvation environment is consistent with the reversible formation of nanocrystalline magnesium peroxide at the cathode and remains compatible with reversible magnesium plating/stripping. The resulting Mg-O2 batteries achieve a high initial discharge voltage approaching 2.0 V, an ultralow overpotential of 0.35 V, a remarkable round-trip energy efficiency of 80% and over 450 stable cycles. These results highlight a solvation-structure-guided strategy for enabling rechargeable Mg-O2 batteries and potentially other multivalent metal-air systems.

The inevitable poor electrochemical stability of transition metal nitrides (TMNs), along with the formation of transition metal oxide layers in electrolytes that undermine their electrochemical activity, has severely hindered the extensive viability of lithium-ion batteries (LIBs) because of the resulting poor stability and low specific capacitance. To tackle these challenges, we have innovatively constructed titanium nitride (TiN) nanoparticles in situ grown on three-dimensional (3D) Ti3C2Tx MXene. The highly conductive TiN nanoparticles were effectively incorporated into the interlayer and surface of 3D ultrathin Ti3C2Tx MXene via a precisely controlled in-situ nitridation method, thereby engineering a distinctive 3D hollow Ti3C2Tx/TiN interfacial heterostructure. The Ti3C2Tx MXene-wrapped structure not only effectively prevents the electrochemical oxidation of the TiN particles but also suppresses the structural collapse defect of the Ti3C2Tx MXene. Consequently, the 3D Ti3C2Tx/TiN-650 composite delivered exceptional Li+ storage performance with outstanding cycle stability, maintaining 400 mA h g- 1 across 1000 cycles even at 1.0 A g- 1. This investigation can potentially serve as a valuable reference for fabricating advanced lithium-ion storage systems.

Achieving both long-term stability and superior rate capability in Na4Fe3(PO4)2P2O7 (NFPP) cathodes remains a major challenge for sodium-ion batteries. Herein, we demonstrate a synergistic bond-defect strategy that circumvents this trade-off. The complementary interaction between Zn and F establishes a synergistic bond-defect environment. The strong bonding of Zn2+ mitigates the charge localization associated with F- doping. Furthermore, the strategy narrows the electronic bandgap to near-metallic values and enhances the degree of graphitization in carbon coatings, resulting in a marked improvement in electronic conductivity. The optimized Na3.95Fe2.95Zn0.05(PO4)2P2O6.95F0.05 (NFZPPF) exhibits outstanding cycling stability with 76.25% retention after 16,000 cycles at 20 C and remarkable rate performance, delivering 68.6 mAh g-1 at 50 C. Coupled with a hard carbon anode, the full cell retains 88.8% capacity after 200 cycles at 2 C, underscoring its viability for practical sodium-ion storage.

Aqueous zinc-metal batteries are promising candidates for sustainable energy storage; but their practical viability is severely limited by poor cryogenic performance caused by kinetic sluggishness and interfacial instability. Here we show a strategy for low-temperature ZMBs based on tailoring the Zn2+ solvation environment by engineering the dielectric constant (ε). By incorporating ethyl acetate, a low-ε co-solvent, into a Zn(ClO4)2 electrolyte, we strategically weaken water's hydrogen-bond network and increase cation-anion pairing. This modified solvation structure accelerates Zn2⁺ transport and desolvation, promotes the formation of a protective solid electrolyte interphase rich in organic and inorganic components, and inhibits parasitic hydrogen evolution. Consequently, the optimized electrolyte enhances Zn plating/stripping stability, with Zn||Zn cells operating at 0.2 mA cm-2 for 10 months (25 °C) and 1 mA cm-2 for 4,000 hours (-50 °C), and Zn||PANI batteries at 1 A g-1 sustaining 10,000 cycles with negligible degradation (-50 °C). This work highlights the critical importance of dielectric constant engineering in electrolyte design and paves the way for high-performance, low-temperature aqueous batteries.

ABSTRACT Alkali metal (Li, Na, and K) batteries (AMBs) have attracted widespread attention in recent years because of their high theoretical specific capacity and attractive energy density. However, they still suffer from uncontrollable dendrite growth and sluggish conductivity during cycling, which lead to security issues and inferior cycling performance. Fortunately, the introduction of high‐entropy electrolytes (HEEs) in AMBs can effectively inhibit dendrites' growth and accelerate the ion diffusion kinetics, resulting in improved electrochemical performance. Considering the rapidly growing research enthusiasm for this topic over the past few years, we have comprehensively and systematically summarized the recent advances in HEEs (including liquid electrolyte, gel polymer electrolytes, and solid‐state electrolytes) and their corresponding mechanisms in AMBs, particularly focusing on their enhancement of ionic conductivity and cycling performance. Finally, rational suggestions and prospects for the future development of HEEs are also proposed.

Multiple-bonded compounds involving heavy group 14 elements (Si, Ge, Sn, Pb) and bismuth (Bi), as heavier analogs of imines, have not previously been isolated as stable entities. In this study, we report the successful isolation of a stannabismuthene (2), a Sn/Bi analog of imines, achieved through the kinetic stabilization provided by a bulky terphenyl substituent. The stannabismuthene was synthesized via a one-pot reduction of BiBr3 and carboranyl distannene (1) using two equivalents of KC8 in THF, and it has been unambiguously characterized through spectroscopic analysis, x-ray diffraction, and DFT calculations. This compound features a Sn═Bi double bond, which acts as a π donor, coordinating with AgNTf2 to form a π complex 3. DFT calculations reveal two significant interactions in 3: the donation from the Bi-Sn π-bonding orbital to the 5s orbital of the Ag atom, and the backdonation from the 4d orbital of Ag to the Bi-Sn π* orbital. These interactions conform to the Dewar-Chatt-Duncanson model for π-complexes, highlighting the unique bonding characteristics of stannabismuthene.

Garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZTO) serves as an active filler in solid-state composite electrolytes for high-performance solid-state batteries because of its excellent conductivity, high chemical stability, and superior shear modulus. Nevertheless, composite electrolytes with LLZTO often exhibit slow Li+ transport and poor interface compatibility because of alkaline impurities (e.g., Li2CO3) formed on the LLZTO's surface, hindering fast Li+ transport. Herein, we report a simple strategy to achieve in situ transformation of the alkaline impurities (Li2CO3) into an ion-conducting layer on the LLTZO's surface via a trifluoromethanesulfonic acid (TfOH) treatment, which not only establishes effective interfacial contact with polyvinylidene fluoride (PVDF) but also facilitates Li+ transport. The resulting LiOTf layer can facilitate the formation of an LiF-enriched solid electrolyte interphase and a cathode-electrolyte interphase, which greatly improve the electrochemical performance of the solid state Li batteries with LiOTf@LLZTO electrolyte. Specifically, the PVDF/LiOTf@LLZTO electrolyte achieved a higher room-temperature ionic conductivity (6.0 x 10-4 S cm-1) and a higher Li+ transference number of 0.45 than the PVDF@LLZTO electrolyte. Moreover, the symmetric battery with the PVDF/LiOTf@LLZTO electrolyte showed a stable cycling for 1200 h at 0.2 mA cm-2, and the assembled Li|LiNi0.8Co0.1Mn0.1O2 full battery exhibited a high capacity retention rate of 88.1 % for 1000 cycles at 2 C.

Alkali metal-chalcogen batteries(AMCBs)are one of the most promising next-generation energy storage systems because of their high energy density and reasonably low cost.However,the practical application of AMCBs is severely hindered by the volume expansion of the chalcogen cathode,the shuttle effect of polychalcogenides,and unstable alkali metal anodes during cycling.Owing to MXene's remarkable chemical stability,rich surface functional groups,outstanding electrical conductivity,and superior mechanical flexibility,MXene(transition metal carbides or nitrides)and its composites have been extensively used in different battery components of AMCBs to resolve these issues.Herein,we summarize the recent advances in the design,fabrication,and application of MXene and its composites for high-performance AMCBs.The advantages and issues of AMCBs and several typical solutions are first introduced.Subsequently,we describe the classification and synthetic methods of MXene,with a comparison of the advantages and disadvantages of these methods.Moreover,the relationships between nano/micro-structures,synthetic methods of MXene-based materials,and the electrochemical performance of MXene-based AMCBs are systematically summarized and discussed.In addition,technologies for the advanced characterization of the reaction mecha-nisms of MXene-based materials in AMCBs are also reviewed.Finally,the remaining challenges and future research directions are proposed and discussed.

MXene materials have emerged as a highly recognized fast-charging anode candidate for lithium-ion batteries (LIBs), owing to their adjustable surface chemistry, ultrathin two-dimensional morphology, and superior electrical conductivity. Nevertheless, their practical applications are severely limited by interlayer self-restacking tendencies and surface oxidation-induced structural instability, which resulted in the inferior rate capability. Designing MXene-based heterostructures has emerged as an effective way to address these issues. Herein, we have innovatively developed a novel one-step solution-based oxidation approach that simultaneously converts MXene into an in-situ grown heterostructure composed of hexagonal Ti(OH)₄ nanosheets and TiO₂ nanoparticles on 2D Ti₃C₂Tₓ MXene. The resulting Ti3C2Tx/Ti(OH)4/TiO2 heterostructure leveraged rapid ion diffusion, elevated electrical conductivity, additional reactive sites derived from the heterogeneous multi-component synergistic effects, and durable interfacial bonding. Consequently, it exhibits exceptional lithium-ion storage properties, delivering a reversible capacity of 325.4 mA h g-1 after 800 cycles at 1.0 A g-1. Beyond presenting a scalable fabrication strategy for fast-kinetics MXene-based anodes, this work elucidates how interfacial engineering contributes to long-term stability in LIBs.