Aqueous zinc-metal batteries offer safe, low-cost grid storage but suffer from nonuniform Zn plating and parasitic water reduction. Adsorption-type additives offer interfacial regulation but often lose functionality due to protonation under practical aqueous conditions. Here, we propose a protonation-tolerant molecular design integrating electronic modulation with a planar, zincophilic adsorption scaffold. By introducing an electron-withdrawing cyano substituent into an aromatic amine, the basicity is reduced while preserving the NH2 lone-pair anchoring, enabling 4-aminobenzonitrile (ABN) to maintain stable horizontal adsorption and high surface coverage. The resulting molecular layer reconstructs the electric double layer, suppresses water-induced side reactions, and promotes uniform (002)-oriented Zn plating/stripping through facet-selective interactions. With 3.3 mM ABN, symmetric Zn//Zn cells cycle for >700 h at 4 mAh cm(-2). Zn//beta-MnO2 cells deliver 4.4 mAh cm(-2) after 250 cycles at 0.25 A g(-1) with zinc utilization ratio of 21.4% and retain 4.28 mAh cm(-2) for 150 cycles at ZUR of 46.2%.

Aqueous zinc-ion batteries (AZIBs) are gaining attention due to their safety and cost-effectiveness. However, zinc (Zn) anodes face persistent issues such as dendrite growth, side reactions, and the accumulation of inactive Zn, particularly when Zn powder is used due to its high surface area and corrosion susceptibility. In this work, we demonstrate a conformal SnO2 surface engineering strategy that enables slurry casted Zn powder anodes to operate stably under high depth of discharge (DOD) conditions in aqueous Zn-ion batteries. Electrochemical testing revealed enhanced cycling stability and plating/stripping reversibility in SnO2 coated Zn powder, accompanied by suppressed side reactions and reduced inactive Zn formation. Coulombic efficiency (CE) and DOD were significantly improved, while electrochemical impedance spectroscopy (EIS) confirmed reduced charge transfer resistance and improved interfacial characteristics. The coated Zn powder anodes also exhibited strong compatibility with zinc vanadium oxide (ZVO) and manganese dioxide (beta-MnO2) cathodes, demonstrating their versatility. Their performance in pouch cell configurations suggests practical scalability. Overall, this study highlights SnO2 surface coating as an effective strategy for improving Zn powder anode reversibility and durability, offering a feasible path toward high-performance and long-lasting AZIBs.

Aqueous Zn-I2 batteries are gaining attention as next-generation energy storage systems due to their safety, low cost, and high energy density. However, their practicality is limited by interfacial instabilities at the anode, such as hydrogen evolution, corrosion, and dendritic Zn growth, as well as slow I2/I- conversion and polyiodide shuttling at the cathode. Here, 4-aminobutyric acid (AB), a commercially available amino acid derivative, is utilized as a functional electrolyte additive possessing a push-pull dipolar structure. Unlike conventional additives that adopt folded or congested structures, AB maintains an extended conformation that maximizes its dipole moment and polarizability. This extended structure strongly binds Zn2+ ions, promoting rapid desolvation, inducing (002) directional Zn deposition and suppressing parasitic reactions. Simultaneously, AB selectively interacts with iodine species, inhibiting the formation and migration of polyiodides while accelerating redox reaction rates. Consequently, the Zn||Zn symmetric cell operates stably for over 1000 h at 3 mA cm-2 and 3 mAh cm-2, while the Zn-I2 full cell with a high-capacity cathode (5 mAh cm-2) retains 95.8% capacity after 900 cycles. This study demonstrates that controlling the molecular structure to implement extended dipolar structures is a universal strategy for achieving interfacial stabilization and enhanced kinetics in aqueous Zn-I2 batteries.

Aqueous zinc metal batteries (AZMBs) suffer from Zn surface degradation caused by dendrite growth, corrosion, and electrolyte side reactions. Zn powder is an essential component for flexible electrodes, enhanced electrolyte accessibility, and precise control of areal capacity. However, its application is severely limited by pronounced surface failure. Here, a graphene coating is applied to Zn powder via a shear-stress-driven dry process, forming a basal plane-dominated protective layer. This coating suppresses the surface degradation by simultaneously passivating the surface, regulating the interfacial Zn2+ solvation structure, and establishing epitaxial Zn metal deposition toward the (002) crystallographic orientation. The resulting graphene-coated Zn powder (Gr_Zn) exhibits stable cycling with a low voltage hysteresis of 16.1 mV over 640 h at 1 mA cm-2, outperforming zinc foil and bare Zn powder electrodes. Moreover, Gr_Zn delivers high-rate capability and exceptional high areal capacity (>20 mAh cm-2) in full-cell and pouch-cell configuration.

A duplex electrode architecture (double-layer electrode, DLE) is constructed to alleviate concentration polarization during the lithiation of the negative electrode. A smaller local voltage deviation in the electrode after lithiation and a reduced probability of Li plating on the top surface of the electrode during high-current-density applications are benefits of the modulated tortuosity and porosity of the upper electrode layer. By reducing the Li-ion concentration polarization in the DLE, the delivered capacity at the C-rate charging step is significantly increased; consequently, the quick charge cycleability is improved. The electrode thickness after cycling and the degree of failure of the electrode due to Li plating and polarization growth were reduced by the uniform utilization of the active materials in the DLE. Given the alleviated concentration polarization after lithiation, the DLE structure exhibited promising electrochemical characteristics that significantly improved its quick-charging performance.

Bulk-type all-solid-state Li batteries (ASLBs) employing inorganic solid electrolytes are considered a nextgeneration energy storage system due to their potentials to overcome the limitations of current lithium-ion batteries (LIBs) such as a safety concern and narrow operating temperature. Inorganic solid electrolytes (SEs) with high ionic conductivity, good chemical- and electrochemical stability are crucial for high-performance ASLBs. Among them, halide SEs have gained attention for their high-voltage stability, high ionic conductivity, and potentially lower cost compared to sulfide counterparts. Notably, the recently reported LiNbOCl4 exhibiting high ionic conductivity (>= 10 mS cm-1) can be a promising candidate. However, in the literature, LiNbOCl4 was prepared by the reaction of LiOH and NbCl5, producing caustic HCl as a by-product. This is problematic for largescale production and may hinder potential improvement through compositional modification. In this work, we demonstrate an alternative hydrochloric acid-free synthesis route using NbOCl3 that can yield LiNbOCl4 with the same crystal structure and high ionic conductivity of 8.4 mS cm-1 at 25 degrees C. To confirm its feasibility for the bulktype ASLB application, its electrochemical properties and dry room stability were also investigated.

Aqueous zinc-ion batteries are promising energy storage systems owing to the abundance of zinc resources and the safety of aqueous electrolytes. However, direct Zn-electrolyte contact induces dendritic growth and side reactions, compromising cycle life. Herein, a mixed ionic-electronic conducting interphase is fabricated via a layer-by-layer (LBL) assembly of poly(diallyldimethylammonium chloride) (PDDA) and poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS). This interphase i) directs Zn2⁺ flux, ii) maintains electronic conductivity for uniform field distribution, and iii) mitigates water-induced side reactions. Electrochemical and spectroscopic analyses confirm reduced Zn2⁺ desolvation energy and suppressed hydrogen evolution and corrosion. Consequently, Zn/Zn symmetric cells exhibit stable cycling over 1800 h at 1 mA cm-2, while five bilayers of (PDDA/PEDOT:PSS)-coated Zn/MnO2 full cells retain 3.92 mAh cm-2 after 350 cycles at 0.25 A g-1. This ecofriendly and cost-effective LBL strategy significantly enhances the energy density and cycle life of aqueous zinc-metal batteries, facilitating their industrial application.

Zn ion batteries have suffered from various problems, such as hydrogen gas evolution (HER), passivation of corrosion byproduct, and dendritic growth of Zn metal. Moreover, these critical issues are generally correlated with each other and the sluggish desolvation kinetics of Zn ion is one of the important causes of them. Herein, a concept of heterogeneous nanoparticle-based interphase layer (HeNIL) composed of zincophilic aluminum fluoride and hydrophilic aluminum oxide with nanodomains is firstly introduced for multifunctional protective layer of Zn metal to effectively prevent the parasitic side reactions, facilitated ion desolvation kinetics, and suppressing dendritic growth. HeNIL could enable well-balanced ion transfer process with accelerated desolvation process, ascribed to dynamic interaction between hydrated Zn ion and HeNIL. As a result, HeNIL coated Zn metal symmetric cell exhibits an enhanced lifetime over 1000 h utilizing 2.5 mAh cm-2, and Zn/MnO2 full cell demonstrates splendid capacity retention of 90.1% after 200 cycles using high areal high areal capacity (4.6 mAh cm-2) positive electrode. This work primally provides unique guidance of design utilizing HeNIL for improving ion transfer kinetics and realizing long-life Zn metal batteries.

Bulk‐type all‐solid‐Li batteries based on inorganic solid electrolytes (SEs) are considered promising candidates for next‐generation energy storage systems for their potential to overcome the limitations of current lithium‐ion batteries, such as safety concerns, narrow operating temperature. Following the intensive efforts to search for affordable sulfide SEs, recently, chloride SEs are in the spotlight for their better high‐voltage stability and potentially lower cost than the sulfide counterparts. However, many chloride SEs exhibiting appreciable ionic conductivity adopt rare‐earth metals, which arises the motivation to search for new chloride SEs based on earth‐abundant minerals. Herein, Li 6−x Fe 1−x Al x Cl 8 (0 ≤ × ≤ 0.8) SEs exhibiting significantly improved ionic conductivity of 3.9 × 10 −5 S cm −1 at 25°C for Li 5.5 Fe 0.5 Al 0.5 Cl 8 compared to Li 6 FeCl 8 (3.1 × 10 −6 S cm −1 ) are reported. The formation of a metastable spinel‐like phase was observed for Li 5.5 Fe 0.5 Al 0.5 Cl 8 prepared by mechanical ball‐milling. Furthermore, its electrochemical properties as a catholyte were examined, coupled with a LiFePO 4 cathode active material.

Bulk-type all-solid-Li batteries based on inorganic solid electrolytes (SEs) are considered promising candidates for next-generation energy storage systems for their potential to overcome the limitations of current lithium-ion batteries, such as safety concerns, narrow operating temperature. Following the intensive efforts to search for affordable sulfide SEs, recently, chloride SEs are in the spotlight for their better high-voltage stability and potentially lower cost than the sulfide counterparts. However, many chloride SEs exhibiting appreciable ionic conductivity adopt rare-earth metals, which arises the motivation to search for new chloride SEs based on earth-abundant minerals. Herein, Li6-xFe1-xAlxCl8 (0 <= x <= 0.8) SEs exhibiting significantly improved ionic conductivity of 3.9 x 10-5 S cm-1 at 25 degrees C for Li5.5Fe0.5Al0.5Cl8 compared to Li6FeCl8 (3.1 x 10-6 S cm-1) are reported. The formation of a metastable spinel-like phase was observed for Li5.5Fe0.5Al0.5Cl8 prepared by mechanical ball-milling. Furthermore, its electrochemical properties as a catholyte were examined, coupled with a LiFePO4 cathode active material.

Although aqueous zinc ion batteries are promising for grid-scale energy storage because of their low cost, safety, and high capacity, they are still limited by poor reversibility and a short cycle lifetime. The main causes of these problems are the spontaneous side reactions and the inhomogeneous deposition/dissolution behavior of the zinc electrode. In this study, we address these limitations by mitigating the inhomogeneous surface reactions of the zinc electrode, a key factor in achieving long-term cycling stability. By employing appropriate surface modification techniques to eliminate the intrinsic passivation layer and reduce surface roughness, we enable uniform electrochemical reactions on the electrode surface, resulting in homogeneous zinc deposition, accelerated electrochemical kinetics, and enhanced cycling performance. Two distinct surface modification strategies were utilized: chemical treatment and mechanical polishing. The chemical treatment entailed the application of acidic, neutral, or alkaline solutions to the zinc electrode, effectively removing the organic passivation layer, improving electrolyte wettability, rate capability, and enabling uniform zinc deposition. Mechanical polishing not only removed the passivation layer but also smoothed the rough surface of the zinc electrode, reducing local charge concentrations and further promoting uniform deposition, which enhanced long-term stability. Our research indicates that simple surface modification methods can significantly improve the electrochemical performance of zinc electrodes. These strategies may be applicable to other types of energy storage systems using metal foil-based electrode, including lithium, magnesium, and aluminum batteries, as well as zinc-ion batteries.

Sulfide solid electrolytes (SSEs) with high ionic conductivity and mechanical flexibility are considered promising Li+ transport media for all-solid-state batteries (ASSBs). However, susceptibility to moisture originating from their crystal structures degrades their inherent superior properties. In this study, we synthesized core-shell structured SSEs by inducing the growth of compounds with moisture-stable SnS44- units on the surface of Li6PS5Cl (LPSC). This Li10SnP2S12 (LSPS)@LPSC showed > 30 times higher Li+ conductivity than LPSC after exposure to dry room environment for 2 h. Additionally, the hydrolysis reaction was effectively inhibited in LSPS@LPSC, resulting in not only significant reduction of hydrogen sulfide (H2S) gas release, but the onset of its generation was also more delayed than in LPSC. Also, in LSPS@LPSC, the inhibition of P-O bond formation after moisture exposure contributes to retention of mechanical properties, as demonstrated by nano-indentation measurements: hardness changes from 1.42 GPa to 1.50 GPa for LSPS@LPSC versus from 1.21 GPa to 1.62 GPa for LPSC (dew point of -7.5 degrees C, 5 min). Furthermore, the Li(Ni0.8Co0.1Mn0.1)O-2 cell with LSPS@LPSC exhibited excellent cycling stability comparable to that of LPSC under typical external pressure (30 MPa), and more remarkably, it showed superior cycle retention than LPSC cell under ultra-low external pressure (similar to 0.3 MPa).

Though lithium-ion batteries (LIBs) have seen a meteoric rise in worldwide deployment over the last decade, they should be further advanced in constant demand of higher rate capability and wider temperature adaptability. A solid electrolyte interphase (SEI) is the essential part of LIBs, determining the charge-discharge performance and degradation behavior. Herein, improvement of the SEI properties is achieved by regulating the electrochemical double layer structure with a nonsacrificial electrolyte additive, that is, lithium nonafluoro-1-butanesulfonate. The anion adsorption of the additive affects the decomposition behavior of other additive and solvent species, and the generated SEI at the graphite electrode becomes thinner and more uniform, leading to decreased impedance and finally resulting in improved energy efficiency, power capability, and fast charging performance of the graphite/NCM811 cell. Furthermore, the low-temperature cycleability at -20 °C is considerably enhanced with no dendritic Li metal deposition at the negative electrode surface. A mechanistic study on the interfacial phenomena and the effect is carried out by using various theoretical and experimental methods, such as density functional theory calculations, electrochemical quartz crystal microbalance, and transmission electron microscopy. Consequently, the approach of SEI modification with the nonsacrificial electrolyte additive can be one of the effective ways to advance LIB technology in future.

Li-metal anode (LMA) is considered promising for overcoming the energy density limit of current Li-ion batteries. However, LMAs in large-scale cells are limited by uneven and excessive anode swelling, owing to the notorious buildup of a highly porous passivation (“dead” Li) layer. To demonstrate the impact of the pressure environment on the LMA swelling behavior and cycling stability, the distribution of the actual stack pressure was visualized in pouch cell platforms using pressure-sensitive films. If the stack pressure is not uniform, pouch cell failure occurs regardless of how high the applied pressure is. Conformal stack pressure assisted by the modified pressure setup with force redistributing pads enabled stable cycling even at a lower external pressure. By correlating with the thickness distribution of the “dead” Li layer over the LMA surfaces after cycling, it is suggested that a uniform stack pressure is crucial for mitigating anode swelling and the stable cycling of Li metal pouch cells.

Magnesium ion batteries (MIBs) are attracting attention as promising alternatives to next-generation energy storage systems owing to their high safety, high volumetric capacity, low reduction potential, abundant raw materials, and economic efficiency. However, developing highly reversible and kinetically fast MIB cathode materials is very challenging owing to the sluggish Mg2+ ion diffusion and low reversible capacity typical of bivalent magnesium ions, as well as the strong electrostatic interactions with the host cathode material. Herein, we designed a charge transfer interaction of a bilayered V2O5/PEDOT (VOP) complex with involving the phase transition of PEDOT from a quinoid to a benzoid structure which could be realized because of reversible and fast Mg2+ ion storage through an enlarged interlayer spacing of 19.02A. Furthermore, the effect of water activation on the enhancement of the kinetics was confirmed by conducting electrochemical and in-situ/ex-situ charac-terizations. Consequently, the as-designed VOP electrodes delivered a high specific capacity of 339.7 mAh/g at 100 mA g-1, high-rate capacity of 256.3 mAh/g at 500 mA g-1, and long-term cyclic stability with a 0.065 % decay rate and high capacity of 172.5 mAh/g after 500 cycles.

The quick-charging performance of SiO electrodes is evaluated with a focus on solid electrolyte interphase (SEI)-reinforcing effects. The study reveals that the incorporation of fluoroethylene carbonate (FEC) into the SiO electrode significantly reduced the electrode fatigue, which is from the the viscoelastic properties of the FEC-derived SEI film. The impact of FEC is attributed to its ability to minimize the mechanical failure of the electrode caused by additional electrolyte decomposition. This beneficial outcome arises from volumetric stain-tolerant characteristics of the FEC-derived SEI film, which limited exposure of the bare SiO surface during 0.5 C-rate cycling. Notably, FEC greatly improves Li deposition during quick-charge cycles following aging at 0.5 C-rate cycling due to its ability to maintain a strong electrical connection between active materials and the current collector, even after extended cycling. Given these findings, we assert that mitigating SEI layer deterioration, which compromises the electrode structure, is vital. Hence, enhancing the interfacial attributes of the SiO electrode becomes crucial for maintaining kinetic efficiency of battery system.

All-solid-state batteries employing inorganic solid electrolytes are considered a promising next-generation energy storage system. Especially, argyrodite-type Li6PS5Cl (LPSCl) was highlighted for its good ionic conductivity and malleability. In the electrode level, achieving an efficient Li+ pathway even with the maximized active material proportion and electrode mass loading is vital for a high energy density. Therefore, a smaller solid electrolyte particle is highly sought for. Herein, we demonstrated a spiral jet mill process for refining LPSCl particle size. The mean particle size (D50) of LPSCl was reduced from 39.9 to 1.9 mu m where the ionic conductivity was decreased from 2.0 to 0.23 mS cm-1. The post-annealing in a mild-temperature range (T < 250 degrees C) led to the even more decreased ionic conductivity. Although the ionic conductivity was restored when T > 300 degrees C, this high-temperature annealing resulted in severe particle agglomeration. Spectroscopic observations revealed that particle surfaces were damaged during pulverization and irreversible sulfur losses occurred during the mild-temperature annealing.

Silicon oxide (SiOx) has attracted considerable attention as an advanced anode material; however, SiOx becomes extensively pulverized during an electrochemical process, resulting in increased resistances. To address this issue, it is proposed the use of effective electrolyte additives, the combination of lithium bis(fluoromethanesulfonyl)imide (LiFSI) and lithium difluorophosphate (LiPO2F2). LiFSI allowed for the stable cycling of the SiOx anode by forming LiF-based solid-electrolyte interphases. Meanwhile, LiPO2F2 effectively suppressed undesirable LiFSI-induced corrosion reactions at the cathode also by forming stable cathode-electrolyte interphases on the surface of the Al current collector. Consequently, the cell cycled with LiFSI/LiPO2F2-containing electrolyte exhibited improved cycling retention (94.6%).

The failure of the quick rechargeability of SiO-based lithium-ion batteries is examined based on different SOC ranges pre-cycling. In detail, the effect of the SiO electrode during normal C -rate applied cycling on the subsequent quick charge is analyzed. The degradation of the SiO electrode is greatly influenced by the design of cycling SOC range of the SiO/NCM811 cell, and severe mechanical and solid electrolyte interphase degradation of the SiO electrode occurred with highly utilized SiO electrodes, resulting in Li plating on the SiO surface under quick charge conditions due to the low open-circuit voltage of SiO electrode and high charge transfer resistance, which is derived from the Li-trap at SiO and subsequent SEI development and electrode crack. The degraded SiO electrode is vulnerable to Li plating at high C -rate applications; hence, the pre-cycling condition of the SiO electrode influences the quick rechargeability of the SiO/NCM811 cell. Consequently, proper manipulation of the cycling range of SiO-based cells should be conducted to enhance the durability of SiO-based quick rechargeable cells.

The critical mechanism underlying the degradation of the Li metal electrode and the positive electrode caused by operating voltage-dependent LiFSI-DME electrolyte decomposition is revealed.