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The glassy state of zeolitic imidazolate frameworks (ZIFs) has shown great potential for energy-related applications, including solid electrolytes. However, their thermal conductivity (κ), an essential parameter influencing thermal dissipation, remains largely unexplored. In this work, using a combination of experiments, atomistic simulations, and lattice dynamics calculations, we investigate κ and the underlying heat conduction mechanism in ZIF glasses with varying ratios of imidazolate (Im) to benzimidazolate (bIm) linkers. The substitution of bIm for Im tunes the node–linker couplings but exhibits only a minor impact on the average diffusivity of low-frequency lattice modes. On the other hand, the linker substitution induces significant volume expansion, which, in turn, suppresses the contributions from lattice vibrations to κ, leading to decreased total heat conduction. Furthermore, spatial localization of internal high-frequency linker vibrations is promoted upon substitution, reducing their mode diffusivities. This is ascribed to structural deformations of the bIm units in the glasses. Our work unveils the detailed influences of linker substitution on the dual heat conduction characteristics of ZIF glasses and guides the κ regulation of related hybrid materials in practical applications. [ABSTRACT FROM AUTHOR]

The global demand for high energy density batteries, mostly for application in electric vehicles, offering increased durability, safety, and sustainability is growing rapidly. In the past, this demand has been met primarily by the development and/or improvement of new/established battery materials and technologies. The high-entropy design concept—aiming at increasing chemical complexity/occupational disorder—has recently been introduced into the field of electrochemical energy storage. Various high-entropy battery materials that are seemingly capable of outperforming low-entropy counterparts by offering desirable properties have been reported. However, future studies are required to explore if the concept is broadly applicable and can be extended to all types of battery materials, especially those that are of industrial relevance. Herein, we provide a brief overview of the existing high-entropy anodes, cathodes, and solid/liquid electrolytes for use in rechargeable Li- or Na-ion batteries and discuss potential research directions and opportunities. [ABSTRACT FROM AUTHOR]

Glutaronitrile (GN) doped with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) at concentrations below and above the room-temperature conductivity optimum near 1M of Li salt is investigated using dielectric spectroscopy and shear rheology. The experiments are carried out from ambient down to the glass transition temperature Tg, which increases considerably as LiTFSI is admixed to GN. As the temperature is lowered, the conductivity optimum shifts to lower salt concentrations, while the power-law exponents connecting resistivity and molecular reorientation time remain smallest for the 1M composition. By contrast, the rheologically detected time constants, as well as those obtained using dielectric spectroscopy, increase monotonically with increasing Li salt concentration for all temperatures. It is demonstrated that the shear mechanical measurements are, nevertheless, sensitive to the 1M conductivity optimum, thus elucidating the interplay of the dinitrile matrix with the mobile species. The data for the Li doped GN and other nitrile solvents all follow about the same Walden line, in harmony with their highly conductive character. The composition dependent relation between the ionic and the reorientational dynamics is also elucidated. [ABSTRACT FROM AUTHOR]

Numerical simulations of the evolution of mobile and immobile dislocations in ceramics under applied pressure in dry pressing at a relatively low temperature are performed in order to study the possibility of production of all-dislocation-ceramics of solid electrolytes, which are expected to have extremely high ionic conductivity without dendrite formation because the diameter of a dislocation pipe is considerably larger than the distance between neighboring dislocations. The present numerical simulations are only for the densification process by plastic deformation of grains under high pressure under the assumption that the compaction of particles by their rearrangement is completed beforehand. By the plastic deformation, new dislocations are generated inside the grains. The required total dislocation density of about 1017 m−2 seems to be achievable under some conditions of dry pressing according to the present numerical simulations. Very short ultrasound irradiation at the beginning of the dry pressing sometimes considerably increases the dislocation density, while for other cases, it even considerably decreases the dislocation density due to enhanced annihilation of mobile dislocations by ultrasound. [ABSTRACT FROM AUTHOR]

Since the 1980s, the paddlewheel effect has been suggested as a mechanism to boost lithium-ion diffusion in inorganic materials via the rotation of rotor-like anion groups. However, it remains unclear whether the paddlewheel effect, defined as large-angle anion group rotations assisting Li hopping, indeed exists; furthermore, the physical mechanism by which the anion-group dynamics affect lithium-ion diffusion has not yet been established. In this work, we differentiate various types of rotational motions of anion groups and develop quaternion-based algorithms to detect, quantify, and relate them to lithium-ion motion in ab initio molecular dynamics simulations. Our analysis demonstrates that, in fact, the paddlewheel effect, where an anion group makes a large angle rotation to assist a lithium-ion hop, does not exist and thus is not responsible for the fast lithium-ion diffusion in superionic conductors, as historically claimed. Instead, we find that materials with topologically isolated anion groups can enhance lithium-ion diffusivity via a more classic nondynamic soft-cradle mechanism, where the anion groups tilt to provide optimal coordination to a lithium ion throughout the hopping process to lower the migration barrier. This anion-group disorder is static in nature, rather than dynamic and can explain most of the experimental observations. Our work substantiates the nonexistence of the long-debated paddlewheel effect and clarifies any correlation that may exist between anion-group rotations and fast ionic diffusion in inorganic materials.

The study explored the effect of incorporating niobia (Nb 2 O 5) at 1, 3, and 5 wt percent into 8 mol% yttria-stabilized zirconia (8YSZ), made through a mechanochemical process. Niobia-doped 8YSZ samples were synthesized by a mechanochemical process and analyzed with methods including XRD, XPS, UV–Visible spectroscopy, particle size analysis, BET surface area analysis, FESEM-EDX, and EIS. Sintering was achieved at a reduced temperature of 1373 K , and all niobia-doped samples predominantly exhibited a tetragonal phase. Electrochemical impedance spectroscopy indicated that niobia doping inversely affected oxide ion conductivity-higher dopant concentrations resulted in lower conductivity. Nb-doped 8YSZ also displayed lower activation energy for conductivity compared to high-temperature (1473 K) sintered undoped 8YSZ, demonstrating equivalent performance. The combined benefits of lower sintering temperatures and enhanced ionic conductivities highlight crucial progress in developing cost-effective and energy-efficient electrolytes for clean energy applications. • Niobium pentoxide stabilizes the 8YSZ matrix, enhances densification and grain growth. • Intragranular conductivity affected by niobia doping, not grain boundary conductivity. • Nb 2 O 3 -doped 8YSZ performs similar to undoped at higher sinter temperatures, suggesting efficient lower temperature sintering. • The role of Nb5+ suggested to involve lattice distortion and phase alterations. • Optimal balance between low sintering temperatures and high ionic conductivity hard to achieve, with less than 1 % niobia doping aiding in converting 8YSZ to a cubic phase. This study assesses how niobia (Nb 2 O 5) affects the ionic conductivity of 8 mol% yttria-stabilized zirconia (8YSZ) when added at 1, 3, and 5 wt%. Despite niobia's ability to lower the sintering temperature to 1373 K , it inversely impacts ionic conductivity, with greater doping resulting in reduced conductivity. However, niobia-doped 8YSZ shows lower activation energy for conductivity compared to undoped 8YSZ sintered at temperatures of 1473 K. This suggests that lower sintering temperatures can be used without undermining performance. Yet, the challenge remains to balance the improved sinterability with achieving optimal ionic conductivity, a critical factor for solid electrolytes in clean energy technologies. [ABSTRACT FROM AUTHOR]

Polyethylene oxide (PEO)‐based solid polymer electrolytes are regarded as promising electrolyte materials because of their safety and flexibility. However, low ionic conductivity at ambient temperature and poor mechanical properties have been a hindrance to its development. In this work, we thermally compressed the PEO‐based electrolytes and explored the ionic conductivity, mechanical performance, free volume, and thermal properties of the electrolyte under different thermal pre‐compressing strains (TPC‐strains). The results show that TPC‐strain can significantly improve the ionic conductivity, in‐plane strength, stiffness, and cell specific capacity as well as the mechanical integrity of solid polymer electrolytes within the battery environment. However, it also results in a reduction in the modulus and stiffness of the SPEs in the through‐plane. In particular, applying a TPC‐strain of 10%–20% to the SPEs by thermal compressing may be a suitable option, which can increase the ionic conductivity of the through‐plane to a factor of 3.4 compared with the uncompressed electrolyte, and increase the in‐plane strength by up to 141%, resulting in better mechanical integrity during charging/discharging processes. At the same time, the compression modulus can be maintained at 80% or higher. [ABSTRACT FROM AUTHOR]

[Display omitted] • Papermaking nanofibers-derived N -doped carbon aerogels were constructed with Cd crosslinking and volatilization. • Fe-SAC@N/CA-Cd with single-atom Fe-N 4 structure was developed via a CVD strategy. • The Fe-SAC@N/CA-Cd exhibited superb ORR activity due to plentiful active species, ultra-high S BET and hierarchical pore architecture. • The assembled LES-ZAB and ASS-ZAB provided encouraging performances. Single-atom catalysts (SACs), with precisely controlled metal atom distribution and adjustable coordination architecture, have gained intensive concerns as efficient oxygen reduction reaction (ORR) electrocatalysts in Zn-air batteries (ZAB). The attainment of a monodispersed state for metallic atoms anchored on the carbonaceous substrate remains the foremost research priority; however, the persistent challenges lie in the relatively weak metal-support interactions and the instability of captured single atom active sites. Furthermore, in order to achieve rapid transport of O 2 and other reactive substances within the carbon matrix, manufacturing SACs based on multi-stage porous carbon substrates is highly anticipated. Here, we propose a methodology for the fabrication of carbon aerogels (CA)-supported SACs utilizing papermaking nanofibers, which incorporates advanced strategies for N -atom self-doping, defect/vacancy introduction, and single-atom interface engineering. Specifically, taking advantages of using green and energy-efficient feedstocks, combining with a direct pore-forming template volatilization and chemical vapor deposition approach, we successfully developed N -doped carbon aerogels immobilized with separated iron sites (Fe-SAC@N/CA-Cd). The obtained Fe-SAC@N/CA-Cd exhibited substantially large specific surface area (S BET = 1173 m2/g) and a multi-level pore structure, which can effectively mitigate the random aggregation of Fe atoms during pyrolysis. As a result, it demonstrated appreciable activity and stability in catalyzing the ORR progress (E 1/2 = 0.88 V, E onset = 0.96 V). Furthermore, the assembled liquid electrolyte-state Zn-air batteries (LES-ZAB) and all-solid-state Zn-air battery (ASS-ZAB) also provides encouraging performance, with a peak power density of 169 mW cm−2 for LES-ZAB and a maximum power density of 124 mW cm−2 for ASS-ZAB. [ABSTRACT FROM AUTHOR]

[Display omitted] • The H 2 under organic acid regulates the reaction rate and protects the (0 0 2) crystal planes, initiating ultrathin SEI within 1 min. • The exposed (0 0 2) planes induce uniform deposition and enhance corrosion-resistance. • This SEI with organic groups exhibits excellent compatibility, low resistance and isolation of electrolyte/anode. • The ZAC1@Zn possesses practical application value due to the rapid preparation within 1 min and resistance to high current shock. Organic acid treatment can facilitate the in-situ formation of a solid electrolyte interface (SEI) on Zn foil protecting the anode from corrosion. However, the generation of hydrogen (H 2) during this process is inevitable, which is often considered detrimental to getting compact SEI. Herein, a H 2 film-assisted method is proposed under concentrated Amino-Trimethylene-Phosphonic-Acid to construct ultrathin and dense SEI within 1 min. Specifically, the (0 0 2) crystal planes survive from the etching process of 1 min due to the adhered H 2 , inducing uniform deposition and enhanced corrosion-resistance. Moreover, the H 2 can effectively regulate the reaction rate, leading to ultrathin SEI and initiating a morphology preservation behavior, which has been neglected by the previous reports. The quick-formed SEI has excellent compatibility, low resistance and effective isolation of electrolyte/anode, whose advantages work together with exposed (0 0 2) planes to get accustomed to high-current surge, leading to the ZAC1@Zn//ZAC1@Zn consistently cycling over 800 h at 15 mA cm−2 and 15 mAh cm−2, the ZAC1@Zn//Cu preserves high reversibility (CE 99.7 %), and the ZAC1@Zn//MVO exhibits notable capacity retention at 191.7 mAh/g after 1000 cycles. [ABSTRACT FROM AUTHOR]

The demand for electronic devices that utilize lithium is steadily increasing in this rapidly advancing technological world. Obtaining high‐purity lithium in an environmentally friendly way is challenging by using commercialized methods. Herein, we propose the first fuel cell system for continuous lithium‐ion extraction using a lithium superionic conductor membrane and advanced electrode. The fuel cell system for extracting lithium‐ion has demonstrated a twofold increase in the selectivity of Li+/Na+ while producing electricity. Our data show that the fuel cell with a titania‐coated electrode achieves 95% lithium‐ion purity while generating 10.23 Wh of energy per gram of lithium. Our investigation revealed that using atomic layer deposition improved the electrode's uniformity, stability, and electrocatalytic activity. After 2000 cycles determined by cyclic voltammetry, the electrode preserved its stability. [ABSTRACT FROM AUTHOR]

All‐solid‐state lithium batteries (ASSLBs) are expected to revolutionize large‐scale energy storage and electric vehicles due to their exceptional safety and high energy density. Central to this technology is the development of solid electrolytes, with halide electrolytes emerging as highly promising candidates, offering high ionic conductivity, robust electrochemical stability and excellent mechanical properties. Since the breakthrough discovery of Li3YCl6 in 2018, research on halide electrolytes has entered a new era. However, despite continuous research efforts, practical challenges persist in their application, including the need to further enhance ionic conductivity, improve moisture resistance, and achieve better compatibility with electrode materials. This review provides a comprehensive overview of recent progress and ongoing challenges in halide electrolytes, examining crystal structures, conduction mechanisms, and scalable synthesis techniques. Various modification strategies are also explored aimed at boosting ionic conductivity and electrochemical stability, with a particular focus on improving interface stability. Finally, future perspectives are outlined for designing high‐performance halide electrolyte materials, offering guidance for ongoing research efforts toward their commercial application in ASSLBs. [ABSTRACT FROM AUTHOR]

Lithium tantalum phosphate LiTa 2 PO 8 ceramics have attracted significant attention as solid electrolytes in oxide-based all-solid-state batteries owing to their superior bulk conductivity of more than 1 mS cm−1 at room temperature. However, high-temperature sintering at 1050 °C, which is required to achieve a dense morphology, results in a high interfacial resistance at the grain boundaries. In this study, dense LiTa 2 PO 8 ceramics were successfully synthesized via a conventional solid-state method at a low sintering temperature of 900 °C using Bi 2 O 3 as the additive. A total lithium-ion conductivity of 1.41 × 10−3 S cm−1 at 25 °C was achieved. The microstructures of the sintered LiTa 2 PO 8 ceramics were analyzed by X-ray diffraction and scanning electron microscopy with energy-dispersive X-ray spectroscopy. Large LiTa 2 PO 8 grains grew in the dense solid-electrolyte body together with the interfacial BiPO 4 phase, which acted as a sintering flux material, at a low sintering temperature of 900 °C. Thus, these LiTa 2 PO 8 ceramics can serve as oxide solid electrolytes for all-solid-state lithium batteries owing to their high total Li-ion conductivity. [ABSTRACT FROM AUTHOR]

Cubic phase Li 7 La 3 Zr 2 O 12 (LLZO) is a promising electrolyte material for all-solid-state rechargeable lithium-ion batteries. The homogeneous densification of the garnet solid electrolyte ceramic material is crucial for enhancing its ionic conductivity performance. Herein, an Al/Ta co-doped strategy is employed to stabilize the cubic phase structure of LLZO and is combined with a two-step sintering method to enhance densification, in order to investigate its effect on microstructure, ionic conductivity, and electrochemical properties. During the formation process, amorphous Li 2 O reacts with doped Al 2 O 3 to create a Li–Al–O liquid phase at the grain boundaries. Combined with two-step sintering to ensure that the desired material transformation is achieved, resulting in a dense microstructure and better mechanical properties. The solid electrolyte Li 6.4 Al 0.1 La 3 Zr 1.7 Ta 0.3 O 12 under two-step sintering (LLZATO-2) is successfully synthesized, delivering an ionic conductivity up to 7.33 × 10−4 S cm−1 at room temperature and an activation energy of 0.22 eV. This work also highlights the critical role of co-doping combined with two-step sintering in preparing well-performing solid-state electrolytes and all-solid-state lithium-ion batteries. LLZO solid electrolyte with lithium ion conductivity is prepared by Al/Ta co-doped combined with two-step sintering. The experimental and theoretical results indicate that amorphous Li 2 O reacts with Al 2 O 3 to form a Li–Al–O liquid phase at the grain boundaries, filling the pores generated at the grain boundaries. The two-step sintering further suppresses grain growth and promotes densification growth. [Display omitted] [ABSTRACT FROM AUTHOR]

All‐solid‐state sulfur batteries (ASBs) suffer from electrical and ionic conduction problems due to the insulating sulfur. By comparing three host materials with different structural characteristics, herein, carbon nanotubes (CNTs) decorated with a conductive metal sulfide (CoMoS2@CNT) is demonstrated, designed to host sulfur and exchange both Li‐ions and electrons, effectively. In this hierarchical wire structure, porous CoMoS2 nanosheets form close interfaces with sulfur, and the CNT core directly transfers electrons to the sulfur‐impregnated CoMoS2. Simultaneously, the solid electrolyte positioned on the outer region of the nanowire material ensures facile Li‐ion conduction to the sulfur‐impregnated CoMoS2. An ASB featuring a CoMoS2@CNT host material with a sulfur loading of 3 mg cm−2 exhibits a high‐areal‐capacity of 4.5 mAh cm−2 at a current density of 2.5 mA cm−2, while retaining 79.4% of its initial capacity after 300 cycles. When sulfur is replaced with SeS2 to further reinforce the charge conduction properties, all‐solid‐state SeS2 batteries (ASeS2Bs) with an extremely high‐areal‐capacity of 16.3 mAh cm−2 retain 99.3% of their initial capacities after 60 cycles at 60 °C. This study provides guidelines for the design principles of cathode composites for the ASBs and ASeS2Bs through multiangle comparative analysis. [ABSTRACT FROM AUTHOR]

Lithium cobalt oxide (LiCoO2) is considered an indispensable cathode material in the realm of consumer electronic batteries due to its high volumetric energy density. However, at a charging cut‐off voltage as high as 4.6 V, significant interfacial side reactions between LiCoO2 and the electrolyte occur, which adversely impact the battery's cycle performance. The surface‐related issues of LiCoO2 at high charge voltages not only constrain its utilization in conventional lithium‐ion batteries with liquid electrolytes but also limit its application in solid‐state batteries. Although traditional coating methods using inert inorganic compounds can partially alleviate this issue, their point‐like coatings fail to completely prevent the surface of LiCoO2 from direct contact with the electrolyte. The exploration of novel surface protection strategies for LiCoO2 remains imperative to address the associated challenges. Herein, introducing a sulfone‐based polymer electrolyte interface is proposed on the surface of LiCoO2 using methyl vinyl sulfone (MVS) through in situ polymerization. Remarkably, LiCoO2 with sulfone‐based polymer electrolyte interface exhibits a capacity retention rate of 83% after 500 cycles when employing a carbonate electrolyte without additives at a charge cut‐off voltage of 4.6 V. Furthermore, the LiCoO2 and polymer electrolyte interface exhibits exceptional cycle stability when paired with polyether solid electrolytes that do not possess high voltage tolerance. Moreover, the incorporation of a polymer electrolyte interface not only enhances the cycle stability of LiCoO2 but also improves its thermal stability. This work presents novel research perspectives for exploring high‐voltage stable LiCoO2. [ABSTRACT FROM AUTHOR]

In the development of lithium‐ion batteries (LIBs), cheaper and safer solid polymer electrolytes are expected to replace combustible organic liquid electrolytes to meet the larger market demand. However, low ionic conductivity and inadequate cycling stability impede their commercial viability. Herein, a novel flexible conducting solid polymer electrolytes (CSPEs) based on polyvinyl alcohol (PVA) and ion‐polarized diethylenetriaminepentaacetic acid (P‐DETP) is developed for the first time and applied in LIBs. PVA and P‐DETP form a compact polymer network through hydrogen bonding, enhancing the thermomechanical stability of CSPE while restricting the migration of larger anions. Furthermore, density functional theory calculations confirm that P‐DETP can facilitate the dissociation of Li+‐TFSI‐ via electrostatic attraction, resulting in increased mobility of lithium ions. Additionally, P‐DETP contributes to the formation of a stable electrode‐electrolyte interface layer, effectively suppressing the growth of lithium dendrites and improving antioxidant capacity. These synergistic effects enable CSPE to exhibit remarkable properties including high ionic conductivity (2.8 × 10−4 S cm−1), elevated electrochemical potential (5.1 V), and excellent lithium transference number (0.869). Notably, the P‐DETP/LiTFSI CSPE demonstrates stable performance not only in LiFePO4 batteries but also adapts to high‐nickel ternary LiNi0.88Co0.06Mn0.06O2 cathode, highlighting its immense potential for application in high energy density LIBs. [ABSTRACT FROM AUTHOR]

The lifespan of lithium (Li) metal batteries (LMBs) can be greatly improved by the formation of inorganic‐rich electrode‐electrolyte interphases (EEIs) (including solid‐electrolyte interphase on anode and cathode‐electrolyte interphase on cathode). In this work, a localized high‐concentration electrolyte containing lithium bis(fluorosulfonyl)imide (LiFSI) salt, 1,2‐dimethoxyethane (DME) solvent and 1,2‐bis(1,1,2,2‐tetrafluoroethoxy)ethane (BTFEE) diluent is optimized. BTFEE is a fluorinated ether with weakly‐solvating ability for LiFSI so it also acts as a co‐solvent in this electrolyte. It can facilitate anion decomposition at electrode surfaces and promote the formation of more inorganic‐rich EEI layers. With an optimized molar ratio of LiFSI:DME:BTFEE = 1:1.15:3, LMBs with a high loading (4 mAh cm−2) lithium nickel manganese cobalt oxide (LiNi0.8 Mn0.1 Co0.1) cathode can retain 80% capacity in 470 cycles when cycled in a voltage range of 2.8–4.4 V. The fundamental understanding on the functionality of BTFEE revealed in this work provides new perspectives on the design of practical high‐energy density battery systems. [ABSTRACT FROM AUTHOR]

Solid polymer electrolytes offer a safer alternative to organic liquid electrolytes in high‐voltage lithium metal batteries, yet challenges remain in achieving adequate cyclability, energy density, scalability, and safety. This study presents the cycling performance of 1 Ah high‐voltage lithium polymer batteries featuring a hybrid ceramic polymer electrolyte (HCPE), a lithium metal anode, and a LiNi0.8Mn0.1Co0.1O2 (NMC‐811)‐based positive electrode. The HCPE stands out for its remarkable mechanical properties, with a Young's modulus exceeding 200 MPa at room temperature, providing robust resistance against dendrite formation. The Li||Li symmetric cells exhibited outstanding performance, cycling for over 1000 hours at a capacity of 2 mAh cm−2, highlighting the exceptional attributes of HCPE. Full cell testing is conducted under practical conditions, utilizing various cell configurations, from coin cells to large pouch cells with a 1 Ah capacity, achieving an energy density of nearly 250 Wh kg−1 and promising cyclability with 80% capacity retention after 110 cycles. The study also investigated thermal runaway characteristics, showing comparability with commercial lithium‐ion batteries. This research underscores the scalability and performance of high‐voltage lithium metal polymer batteries, advancing their potential for commercial viability. [ABSTRACT FROM AUTHOR]

Solid‐state batteries (SSBs) with high‐voltage cathodes and Li‐anodes offer promising energy density and safety for next‐generation batteries. However, poor contact and electrochemical instability of solid electrolyte interfaces hinder their long‐term performance. Traditional rigid solidification interlayers possess restricted capability to address these issues. Herein, a composite buffer interlayer (CBI) with localized high‐concentration electrolytes (LHCEs) in a flexible polymer scaffold, tackling contact and stability problems and ensuring a perfect interface is developed. The extended electrochemical window provides it with synergistic antioxidation and antireduction capabilities, making it compatible with high‐voltage cathodes and Li anodes, while an in situ formed LiF‐Li3N rich inorganic interface ensures uniform lithium deposition and prevents dendrite formation. This CBI enables lithium symmetric cells to achieve a super high critical current density of 7.2 mA cm−2. Most impressively, coupled with a high‐voltage LiNi0.83Co0.12Mn0.05O2 cathode (NCM83), the full cell achieves 94.1% capacity retention after 125 cycles (coulombic efficiency >99.8%) at a mass loading of 14.6 mg cm−2 and a high voltage of 4.45 V. Additionally, a pouch cell with 17.2 mg cm−2 NCM83 achieves an initial discharge capacity of 3.82 mAh cm−2 an superior cycling stability (75 cycles, 89% capacity retention), showcasing the practical potential of LHCE‐CBI enabled SSBs. [ABSTRACT FROM AUTHOR]

The double skeleton interpenetrating network fixed the quaternary ammonium salt, and various internal conduction modes cooperated to promote the transport of hydroxide ions. [Display omitted] The alkaline solid-state electrolytes have received widespread attention for their good safety and electrochemical stability. However, they still suffer from low conductivity and poor mechanical properties. Herein, we report the synthesis of double-network featured hydroxide-conductive membranes fabricated by polyvinyl alcohol (PVA) and chitosan (CS) as the double-skeletons. Then, we implanted quaternary ammonium salt guar hydroxypropyltrimonium chloride (GG) as the OH− conductor for high-performance electrochemical devices. By virtue of the unique stripe-like structure shared from the double skeleton with a high degree of compatibility and stronger hydrogen bond interactions, the polyvinyl alcohol/chitosan-guar hydroxypropyltrimonium chloride (PCG) solid-state electrolytes achieved optimal thermal stability (> 300 °C), mechanical property (∼ 34.15 MPa), dimensional stability (at any bending angle), and high ionic conductivity (13 mS cm−1) and ion mobility number (t ion ∼ 0.90) compared with chitosan-guar hydroxypropyltrimonium chloride (CG) and polyvinyl alcohol-guar hydroxypropyltrimonium chloride (PG) electrolyte membrane. As a proof-of-concept application, the "sandwich"-type zinc-air battery (ZAB) assembled using PCG membrane as the electrolyte realized a high open-circuit voltage (1.39 V) and an excellent power density (128 mW cm−2). Notably, in addition to its long-term cycle life (30 h, 2 mA cm−2) and stable discharge plateau (12 h, 5 mA cm−2), it could even enable a flexible ZAB (F-ZAB) to readily power light-emitting diodes (LED) at any bending angle. These merits afford the PCG membrane a promising electrolyte for improving the performance of solid-state batteries. [ABSTRACT FROM AUTHOR]

Solid‐state lithium metal batteries incorporating LiNixCoyMnzO2 (NCM) as cathodes are developed to meet the high‐energy‐density requirements of energy storage systems. Nevertheless, the process of plating and stripping of Li‐ions on lithium metal electrodes causes significant volume changes, in which ultimately degrade battery performance. In this study, an elastomeric electrolyte with special latitude‐longitude interwoven structure is designed and synthesized successfully, which is composed of a crosslinked phase as filler and a polymeric phase as skeleton. With the increase of polymeric phase, the electrolyte changes from an irregular wrinkle structure to latitude‐longitude interwoven structure. The optimal electrolyte ATPE‐1 with a predominant latitude feature demonstrates remarkable resilience of 800% stretchability and high room temperature ionic conductivity (1.72 mS cm−1). Therefore, the close contact and excellent compatibility with lithium metal anode enable the lithium symmetric cell with ATPE‐1 as electrolyte to maintain a stable and extended cycle life for over 2000 h. Additionally, the existence of the supramolecular interaction between the polymeric phase and crosslinked phase effectively increases the decomposition voltage of the electrolyte. A Li/ATPE‐1/NCM622 cell delivers superior rate performance under ambient conditions. This innovative elastomeric electrolyte offers a promising potential for the practical application in high‐performance solid‐state lithium metal batteries. [ABSTRACT FROM AUTHOR]

The advancement of conventional lithium–sulfur batteries (LSBs) is hindered by the shuttle effect and corresponding safety issues. All‐solid‐state lithium–sulfur batteries (ASSLSBs) substitute the liquid electrolytes with solid‐state electrolytes (SEs) to completely isolate the cathode and anode, thereby effectively suppressing polysulfide migration and growth while significantly enhancing energy density and safety. However, the development of ASSLSBs is accompanied by several challenges such as the formation of Li dendrites, electrode degradation, poor interfacial wettability, and sluggish reaction kinetics, etc. This review systematically summarizes the recent advancements made in ASSLSBs. First, a comprehensive overview of the research conducted on advanced cathodes utilizing sulfur (S) and lithium sulfide (Li2S) is displayed. Subsequently, the SEs are classified and discussed that have been implemented in ASSLSBs. Furthermore, the issues of interfaces and anodes in ASSLSBs are analyzed. Finally, based on current laboratory advancements, rational design guidelines are proposed for each component of ASSLSBs while also presenting four practical recommendations for facilitating early commercialization. [ABSTRACT FROM AUTHOR]

The inorganic solid‐state electrolytes play a crucial role in all‐solid‐state batteries. The entropy of solid‐state electrolytes has a significant impact on ion transport. It has been reported that ionic conductivity can be enhanced by increasing the entropy by adding multiple atoms to the materials. However, there is a lack of understanding regarding the potential mechanism between entropy and ion transport in the atomic‐level microstructure of materials. Herein, a new point of view is brought up to understand the influence of entropy on lithium ionic conductivity at an atomic level only by adding one element at a time inspired by the diagonal relationship. A series of materials is designed, including Li1.75Zr0.75Ta0.25Cl6, Li1.75Zr0.75Nb0.25Cl6, Li1.75Zr0.75Mo0.25Cl6, and Li1.75Zr0.75W0.25Cl6, with various mixed entropy, directed by diagonal relationship. It reveals that the substitution increases the mixed entropy, alters the disorder degree of cations around lithium ions, and improves ionic conductivity. Highlighting the importance of mixed entropy in ion migration and establishing the close connection between mixed entropy and ion conduction could provide new insights into the design and development of solid‐state electrolytes. [ABSTRACT FROM AUTHOR]

Solid‐state electrolytes (SSEs) are promising future power sources for electronic vehicles (EVs) and devices due to their enhanced safety features, high energy density, and nonflammability. The NASICON structure has emerged as a frontrunner in oxide‐based electrolytes, boasting high Li‐ion conductivity and air stability. Nevertheless, developing high‐performance oxide‐based electrolytes remains challenging due to their inherently hard and brittle nature, presenting obstacles to achieving an optimal interface between the cathode and anode. In this study, to overcome this issue and enhance electrochemical stability and Li‐ion conductivity, a new approach employing a hybrid solid electrolyte amalgamating polymer electrolytes with inorganic Li1.3+xAl0.3−xMgxTi1.7(PO4)3 powder (x = 0, 0.015, 0.030, 0.045, and 0.060) was investigated. Notably, employing nanosized Li1.3Al0.3Ti1.7(PO4)3 (LATP) synthesized via the sol–gel method led to a remarkable increase in ionic conductivity to 7.29 × 10–4 S cm–1, which was attributed to enhanced pellet density. Electrochemical analysis revealed that Li1.345Al0.255Mg0.045Ti1.7(PO4)3 exhibited superior specific capacity, stable high current density performance, and capacity recoverability compared to LATP. This pioneering study highlights the potential of hybrid solid electrolytes incorporating Mg‐doped LATP as a promising material for practical solid‐state lithium batteries. [ABSTRACT FROM AUTHOR]

Lithium (Li) is a promising anode material for all‐solid‐state Li metal batteries (ASSLMBs) due to its high energy density. However, the interface incompatibility of Li/solid electrolyte and uneven Li deposition induces the penetration of Li dendrites. Herein, a multifunctional rich‐LiF/Mg artificial solid electrolyte interphase (SEI) layer is constructed from a MgF2‐PVDF‐HFP film to passivate the Li anode and achieve effective inhibition of Li dendrites. Notably, the triggered LixMg alloys rivet the Li6PS5Cl (LPSCl) electrolyte and Li anode together well, producing satisfactory interface contact and reducing overpotential. The mechanism of LiF and LixMg alloys to enhance the stability of the Li/LPSCl interface is further elucidated by density functional theory (DFT). Moreover, the synergistic interaction of LiF with high interfacial energy and LixMg alloys with low diffusion barrier promotes uniform deposition of Li during plating/stripping and structural stability. Therefore, the modified Li‐symmetric cell exhibits ultra‐high critical current density (2.0 mA cm−2) and considerable cyclic stability (more than 1000 h at 0.5 mA cm−2). Remarkably, NCM//LPSCl//3% MgF2‐PVDF‐HFP@Li ASSLMBs exhibit considerable long‐term cycle stability (86.9% capacity retention after 100 cycles at 0.2 C). This work highlights the critical role of the intermediate passivating layer in mitigating side reactions and preventing Li penetration. [ABSTRACT FROM AUTHOR]

All‐solid‐state lithium batteries (ASSLBs) incorporating sulfide solid electrolytes capture great attention due to their intrinsic safety features and high energy density. Nevertheless, the implementation of sulfide solid electrolytes faces significant challenges, including moisture sensitivity, narrow intrinsic electrochemical windows, and excessively thick solid electrolyte layers. Here, the substitution of In for P and F for Cl in argyrodite sulfide Li5.7PS4.7Cl1.3 is presented. With appropriate elemental substitutions, the Li symmetric cells exhibit a high critical current density value of 2.5 mA cm−2 and deliver prolonged plating/stripping over 1000 h at 1 mA cm−2 and 25 °C. Further, the Li5.82P0.94In0.06S4.7Cl1.12F0.18 displays high chemical stability toward organic solvents, which is further demonstrated by the density functional theory (DFT) calculations. Using polyisobutylene as a binder, a uniform sulfide film (35 µm) is prepared by slurry casting and hot pressing process, delivering a high ionic conductivity of 1.4 mS cm−1 at 25 °C. Coupled with FeS2 and LiCoO2 cathode, the all‐solid‐state lithium metal cell exhibits a long cycling life and excellent rate performance. This study provides a design strategy and reveals the importance of high‐performance sulfide SEs in the scalable production of sulfide film. [ABSTRACT FROM AUTHOR]

To facilitate the use of solid polymer electrolytes (SPEs) with high‐nickel (Ni) cathodes in high‐voltage lithium (Li) metal batteries (LMBs), it is crucial to address the challenges of low oxidative stability and the formation of vulnerable interphases. In this study, isocyanate groups (−N═C═O) are incorporated to develop an SPE with a bi‐continuous structure, consisting of elastomeric and plastic crystal phases. This rationally designed SPE exhibits high ionic conductivity (0.9 × 10−3 S cm−1 at 25 °C), excellent elasticity (elongation at break of 330%), and enhanced oxidative stability (over 4.8 V vs. Li/Li⁺). A full cell, incorporating this SPE with a thin Li foil of 40 µm, and a high‐Ni LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode operating at 4.7 V vs. Li/Li⁺, demonstrates excellent cyclability, retaining 70% of its initial capacity after 200 cycles under a high C‐rate of 1C at 25 °C. The extended cycling of isocyanate‐containing SPE at 4.7 V vs. Li/Li⁺ is attributed to robust and compact inorganic‐rich interphases enabled by antioxidative −N−C═O components, as well as uniform Li deposition attributed to the bi‐continuous structured SPE. This study suggests that the isocyanate‐containing SPE system is a promising candidate for high‐voltage solid‐state LMBs by constructing stable interphases. [ABSTRACT FROM AUTHOR]

All‐solid‐state lithium‐sulfur batteries (ASSLSBs) are garnering significant interest due to their high energy density and safety. Nevertheless, the interfacial instability, particularly with sulfide‐based solid electrolytes, poses a formidable challenge to their widespread application. Herein, to adjust the p‐band center of the tetrahedron in Li6PS5Cl is proposed to alleviate undesirable reactions at anode and cathode interfaces via facile Sb/O co‐doping. The incorporation of Sb into Li6PS5Cl forms an SbS4 tetrahedron, resulting in the downward shift of the S‐p band center. This benefits the acquisition of electrons from Li to in situ forming stable LixSbySz interphase at the Li/LPSC‐SbO interface. The Li symmetric cell endows a high stability for over 4000 h. Moreover, the lower p‐band center of the S‐p band also strengthens the interaction of the SbS4 tetrahedron with surrounding Li atoms, impeding charge transfer to S8 and mitigating interfacial side reactions on the sulfur cathode. Additionally, O doping enhances the air stability of the electrolyte. The ASSLSBs with LPSC‐SbO achieve a high specific capacity of 932.6 mAh g−1 at 0.1 C with 83.7% capacity retention over 150 cycles. Furthermore, the practical all‐solid‐state pouch cell demonstrates stable cycling performance and anticipated safety. This work provides insights into constructing stable dual solid–solid interfaces for sulfide‐based room‐temperature high‐performance ASSLSBs. [ABSTRACT FROM AUTHOR]

Coulombic efficiency and cycle life require further improvement in an ever-growing practical demand for lithium-ion batteries (LIBs), which are one of the most prevalent electrochemical energy storage systems. In this work, a more stable and highly lithium-ion (Li-ion) conductive artificial solid electrolyte interface (A-SEI) is constructed by coating polythiophene (PTh) on the surface of a graphite anode based on molecular dynamic simulations. Our findings reveal that PTh chains effectively prevent direct contact between the electrolyte and the negative electrode while providing a rapid transport channel for lithium ions (Li-ions), resulting in significantly shorter trapping times for Li-ions—at least two orders of magnitude shorter than those in the predominant component of traditional SEI layers. [ABSTRACT FROM AUTHOR]

Solid‐state lithium metal batteries based on fluorinated solid electrolytes have attracted attention due to their safety and stability advantages. However, the fluoride solid electrolytes face the problem of relatively low Li‐ion conductivity due to the lacking of suitable structural prototypes and their corresponding modulation modes. In this work, a chlorine‐doped fluoride solid electrolyte Li3AlF5.87Cl0.13 is developed with high ionic conductivity by thermal fluorination and weak chlorination of mixed ionic liquids. The Cl anion is doped into the cryolite‐like open framework structure, and the electrolyte particle boundaries are decorated by solidified thin‐layer (≈2 nm) ionic liquid. Both the bulk and interface modifications enable the improvement of Li‐ion conductivity to 2 × 10−4 S cm−1 at 30 °C, which is the highest level among fluoride solid electrolytes. The Li3AlF5.87Cl0.13 with residual solidified ionic liquid shows the excellent stability of interface contact with Li metal, and the corresponding Li symmetric cell exhibits a small overvoltage (≈100 mV) with outstanding cycle life (at least 500 h). For the first time, a conversion‐type solid‐state Li/FeF3 battery is developed based on this fluoride electrolyte, delivering a reversible capacity as high as 430 mAh g−1. The existence of natural F‐rich interface promotes the conversion reaction reversibility of FeF3 cathode. [ABSTRACT FROM AUTHOR]

Growing market demands on portable electronics, electric vehicles, and energy storage system calls for the development of high‐energy density lithium (Li) batteries. Li metal is considered as a promising anode material owing to their high capacity and low electrochemical potential. However, high reactivity of Li metal with conventional flammable liquid electrolytes easily forms Li dendrites, which may cause short‐circuit and even catching fire, obstructing the wide application of Li metal batteries. Although non−/less‐flammable solid electrolytes have replaced the conventional liquid electrolytes, solid‐state Li metal batteries (SSLMBs) suffer from lower Li+ conductivities, chemical/electrochemical incompatibilities toward Li metal, and inhomogeneous Li+ flux at the interfaces. Therefore, many researchers have devoted themselves to solve these problems. For a better understanding on the current issues and recent advances, this article provides (1) a review on various solid electrolytes with high Li+ conductivity and their interfacial issues in SSLMBs, and (2) recent progress in stabilization of the interface between the Li node and solid electrolytes, including an electrolyte modification (e.g., composition, additives) and introduction of an interlayer. [ABSTRACT FROM AUTHOR]

Poly(ethylene oxide) (PEO)‐based solid polymer electrolytes (SPEs) are widely utilized in all‐solid‐state sodium metal batteries (ASSSMBs) due to their excellent flexibility and safety. However, poor ionic conductivity and mechanical strength limit its development. In this work, an emerging solvent‐free hot‐pressing method is used to prepare mechanically robust PEO‐based SPE, while sodium superionic conductors Na3Zr2Si2PO12 (NZSP) and NaClO4 are introduced to improve ionic conductivity. The as‐prepared electrolyte exhibits a high ionic conductivity of 4.42 × 10−4 S cm−1 and a suitable electrochemical stability window (4.5 V vs Na/Na+). Furthermore, the SPE enables intimate contact with the electrode. The Na||Na3V2(PO4)3@C ASSSMB delivers a high‐capacity retention of 97.1% after 100 cycles at 0.5 C and 60 °C, and exhibits excellent Coulombic efficiency (CE) (close to 100%). The ASSSMB with the 20 µm thick electrolyte also demonstrates excellent cyclic stability. This study provides a promising strategy for designing stable polymer‐ceramic composite electrolyte membranes through hot‐pressing to realize high‐energy‐density sodium metal batteries. [ABSTRACT FROM AUTHOR]

Solid-state electrolytes have received widespread attention for solving the problem of the leakage of liquid electrolytes and effectively improving the overall performance of supercapacitors. However, the electrochemical performance and environmental friendliness of solid-state electrolytes still need to be further improved. Here, a binary biomass-based solid electrolyte film (LSE) was successfully synthesized through the incorporation of lignin nanoparticles (LNPs) with sodium alginate (SA). The impact of the mass ratio of SA to LNPs on the microstructure, porosity, electrolyte absorption capacity, ionic conductivity, and electrochemical properties of the LSE was thoroughly investigated. The results indicated that as the proportion of SA increased from 5% to 15% of LNPs, the pore structure of the LSE became increasingly uniform and abundant. Consequently, enhancements were observed in porosity, liquid absorption capacity, ionic conductivity, and overall electrochemical performance. Notably, at an SA amount of 15% of LNPs, the ionic conductivity of the resultant LSE-15 was recorded at 14.10 mS cm−1, with the porosity and liquid absorption capacity reaching 58.4% and 308%, respectively. LSE-15 was employed as a solid electrolyte, while LNP-based carbon aerogel (LCA) served as the two electrodes in the construction of a symmetric all-solid-state supercapacitor (SSC). The SSC device demonstrated exceptional electrochemical storage capacity, achieving a specific capacitance of 197 F g−1 at 0.5 A g−1, along with a maximum energy and power density of 27.33 W h kg−1 and 4998 W kg−1, respectively. Furthermore, the SSC device exhibited highly stable electrochemical performance under extreme conditions, including compression, bending, and both series and parallel connections. Therefore, the development and application of binary biomass-based solid electrolyte films in supercapacitors represent a promising strategy for harnessing high-value biomass resources in the field of energy storage. [ABSTRACT FROM AUTHOR]

Solid-state batteries (SSBs) have been widely studied as next-generation lithium-ion batteries (LiBs) for many electronic devices due to their high energy density, stability, nonflammability, and chemical stability compared to LiBs which consist of liquid electrolytes. However, solid electrolytes exhibit poor electrochemical characteristics due to their interfacial properties, and the sintering process, which necessitates high temperatures, is an obstacle to the commercialization of SSBs. Hence, the aim of this study was to improve the interfacial properties of the lithium tantalum phosphate (LTPO) solid electrolyte by adding succinonitrile (SN) on the interface of the LTPO particle to enhance ionic conductivity without the sintering process. Electrochemical impedance spectroscopy (EIS), the Li symmetric cell test, and the galvanostatic cycle test were performed to verify the performance of the SN-containing LTPO composite electrolyte. The LTPO composite solid electrolyte exhibited a high ionic conductivity of 1.93 × 10−4 S/cm at room temperature (RT) compared to the conventional LTPO. Also, it showed good cycle stability, and low interfacial resistance with Li metal, ensuring electrochemical stability. On the basis of our experimental results, the performance of solid electrolytes could be improved by adding SN and lithium salt. In addition, the SN can be used to fabricate the solid electrolytes without the sintering process at high temperatures. [ABSTRACT FROM AUTHOR]

All‐solid‐state batteries have drawn a lot of concern owing to their distinct advantages in energy density and safety. However, the interfacial issues between the solid electrolyte and electrodes are still roadblocks to large scale application of rechargeable solid‐state batteries. In this work, it reveals that promoting the Na‐O affinity in Na3Zr2Si2PO12 electrolyte can effectively boost its air stability. Specifically, a two‐step sintering approach is employed to actively regulate the microstructure evolution of Na3Zr2Si2PO12 electrolyte. Apart from the enhanced strength of the Na‐O bond, the mechanical performance and ionic conductivity are also apparently improved in comparison with the traditional one‐step sintering. Moreover, a low resistance of 68 Ω cm2 is achieved with the Na/Na3Zr2Si2PO12 interface, demonstrating long cycling stability of 1000 cycles at 0.1 mA cm−2. The designed Na3Zr2Si2PO12 ceramic electrolyte paired with Na3.5V0.5Mn0.5Fe0.5Ti0.5(PO4)3 cathode and metallic Na anode manifests outstanding cycling stability with a high reversible discharge capacity of 136 mAh g−1 after nearly 400 cycles at 1 C, and 25 °C. Therefore, it is believed that the delicate modulation of solid electrolyte microstructure is of great importance for accelerating the application of solid‐state batteries. [ABSTRACT FROM AUTHOR]

Despite their potential as next-generation energy storage devices, all-solid-state batteries (ASSBs) have not been widely developed because of the low ionic conductivity of solid electrolytes and the high interfacial impedance with electrodes. This study addressed these issues by enhancing the electrochemical properties through composition control. A composite solid electrolyte (CSE) was fabricated using Li6.5Ga0.2La2.95Rb0.05Zr2O12 (Ga–Rb-doped LLZO) and poly(ethylene oxide) (PEO) with various compositions. The results demonstrated high ionic conductivity and electrochemical stability when the weight ratio of Ga–Rb-doped LLZO to PEO was 6:4. These characteristics effectively mitigated Li dendrite formation and ensured excellent interfacial stability. Notably, LiFePO4/CSEs/Li full cells retained 92.3% of their initial capacity after 100 cycles at a 0.3 C rate. This study will promote the research and development of practical ASSBs incorporating LLZO solid electrolytes. [ABSTRACT FROM AUTHOR]

[Display omitted] • Na 3.4 Mn 0.7 Ti 0.3 Cr(PO 4) 3 /C cathode material is prepared by a simple sol–gel method. • Ti substitution shortens the average bond length of TM-O. • Ti substitution can suppress the Jahn-Teller effect of Na 4 MnCrPO 4 cathode material. • Ti substitution reduces the R ct of cathode and suppress interface side reactions. The sodium superionic conductor Na 4 MnCr(PO 4) 3 gains increasing attention owing to its three-dimensional structure and the three-electron reaction. However, rapid structure degradation during cycling is the major challenge for its practical application. Herein, Ti4+ is utilized to replace a portion of Mn2+ in Na 4 MnCr(PO 4) 3. The low redox voltage and d 0 electronic configuration of the Ti4+ ions are helpful to suppress the structure alteration and improve electronic conduction. Consequently, the as-prepared Na 3.4 Mn 0.7 Ti 0.3 Cr(PO 4) 3 /C cathode exhibits a remarkable good 91.0% capacity retention after 500 cycles at 10C rate, with exceptional rate capacities of 99.5 mAh g−1 and 81.0 mAh g−1 at 5C and 10C rate, respectively. Furthermore, based on ≈2.86-electron reactions involving Mn2+/Mn3+ (3.5 V), Mn3+/Mn4+ (4.1 V), Cr3+/Cr4+ (4.3 V), and Ti3+/Ti4+ (2.1 V), the material can provide an energy density of approximately 541.6 Wh kg−1, slightly surpassing that of Na 4 MnCr(PO 4) 3. Ex-situ XRD investigation further elucidates that throughout the entire charge–discharge process, the Ti-substituted material experiences highly reversible solid-solution and two-phase reactions. Additionally, Ti substitution can greatly promote the interfacial charge transfer of the material and suppress the decomposition of the electrolyte during cycling. This work might open a new insight for designing sodium-ion battery cathode materials with good cycling stability and high energy density. [ABSTRACT FROM AUTHOR]

The development of highly conductive and thermally stable solid electrolytes is crucial for the next generation of intermediate temperature solid oxide fuel cells (IT-SOFCs). This study investigates the influence of copper (Cu) doping on the microstructure and ionic conductivity of 8 mol. % yttria-stabilized zirconia (8YSZ) when sintered at lower temperatures. The mechanochemical synthesized 1, 3, and 5 wt. % Cu-doped 8YSZ compacts were extensively characterized their properties through a suite of analytical techniques like X-ray diffraction, Raman, X-ray photoelectron, UV–Vis diffused reflectance, particle size analyzer, BET surface area, Emission Scanning Electron Microscopy-Energy Dispersive X-Ray, and AC impedance. The results revealed enhanced ionic conductivity and sinterability, at reduced temperature of 1373 K, with the 5 wt. % Cu-doped 8YSZ demonstrating the highest ionic conductivity of 4.18 × 10−3 S cm−1 at 1023 K, alongside reduced activation energy of 1.14 eV. The lower sintering temperatures and consequential benefits in performance metrics suggest Cu-doping as an effective strategy for optimizing 8YSZ-based electrolytes lowering SOFC manufacturing costs without compromising performance for IT-SOFCs. [Display omitted] • 1. Copper -doped 8YSZ synthesized via mechanochemical process results in varied cubic, tetragonal, and monoclinic crystal phases. 2. Copper doping improves 8YSZ's ionic conductivity and sinterability for intermediate -temperature solid oxide fuel cells. 3. 5 wt. % Cu -doped 8YSZ achieves the highest conductivity (4.18 × 10−3 S cm−1 at 1023 K) and lowest activation energy (1.11 eV). 4. Copper doping is suggested to make 8YSZ-based solid oxide fuel cell electrolytes more cost-effective. [ABSTRACT FROM AUTHOR]

Using first-principles density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations, we performed this study on the phase stability, the intrinsic redox stability, and the Li+ conductivity of Li10GexMo1−xP2S12 (x = 0~1) superionic conductors. Molybdenum (Mo) is expected to replace expensive germanium (Ge) to lower tmaterial costs, reduce sensitivity to ambient water and oxygen, and achieve acceptable Li+ conductivity. The ab initio first principle molecular dynamics simulations show that room-temperature Li+ conductivity is 1.12 mS·cm−1 for the Li10Ge0.75Mo0.25P2S12 compound, which is comparable to the theoretical value of 6.81 mS·cm−1 and the experimental measured one of 12 mS·cm−1 of the Li10GeP2S12 (LGPS) structure. For Li10GexMo1−xP2S12 (x = 0, 0.25, 0.5 and 1) compounds, the density of states and the projection fractional wave state density were calculated. It was found that when Ge atoms were partially replaced by Mo atoms, the band gap remained unchanged at 2.5 eV, but deep level defects appeared in Mo-substituted compounds. Fortunately, this deep level defect is difficult to ionize at room temperature, so it has no effect on the electronic conductivity of Mo substitute compounds, making Mo substitution a suitable solution for electrolyte materials. The projection fractional wave state density calculation shows that the covalent bond between Mo and S is stronger than that between Ge and S, which reduces the sensitivity of Mo-substituted compounds to water and oxygen contents in the air. In addition, the partial state density coincidence curve between Li and S elements disappears in the 25% Mo-substituted compound with energies of 4–5 eV, indicating that the Li2S by-product is decreased. [ABSTRACT FROM AUTHOR]

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Sodium superionic conductor (NASICON)‐type cathode materials are considered promising candidates for high‐performance sodium‐ion batteries (SIBs) because of the abundance and low cost of raw materials. However, NASICON‐type cathodes suffer from low capacities. This limitation can be addressed through the activation of sodium‐excess phases, which can enhance capacities up to theoretical values. Thus, this paper proposes the use of transition metal (TM)‐substituted Na3V2(PO4)2F3 (NVPF) to induce sodium‐excess phases. To identify suitable doping elements, an inverse design approach is developed, combining machine learning prediction and density functional theory (DFT) calculations. Graph‐based neural networks are used to predict two crucial properties, i. e., the structural stability and voltage level. Results indicate that the use of TM‐substituted NVPF materials leads to about 150 % capacity enhancement with reduced time and resource requirements compared with the direct design approach. Furthermore, DFT calculations confirm improvements in cyclability, electronic conductivity, and chemical stability. The proposed approach is expected to accelerate the discovery of superior materials for battery electrodes. [ABSTRACT FROM AUTHOR]

In comparison with solid polymer electrolytes, hydrogel polymer electrolytes are now a potentially suitable candidate for aqueous zinc‐ion batteries (ZIBs). Generally, a hydrogel is mainly composed of a hydrophilic polymer network with a high water absorption propensity and the distinctive properties of being soft and wet, becoming a gel and solid polymer electrolyte in terms of ionic conductivity and mechanical properties. All these unique characteristics of electrolytes combine with an appropriate anode and cathode materials to deliver high safety, low cost, environmental friendliness, and excellent electrochemical performance in ZIB. Nevertheless, there is no comprehensive overview on the development of hydrogel electrolytes for ZIBs available. Therefore, this study focuses on the most recent breakthroughs in hydrogel‐based polymer electrolytes for ZIBs. Further, a brief explanation of various types of hydrogel electrolytes as well as the electrochemical performance of different polymer‐based electrolytes arediscussed. Finally, the challenges of hydrogel electrolytes for currently established Zn‐ion batteries and the future research directions towards the high‐performance flexibile ZIBs are explored. [ABSTRACT FROM AUTHOR]

Interfaces within batteries, such as the widely studied solid electrolyte interface (SEI), profoundly influence battery performance. Among these interfaces, the solid–solid interface between electrode materials and current collectors is crucial to battery performance but has received less discussion and attention. This review highlights the latest research advancements on the solid–solid interface between lithium metal (the next-generation anode) and current collectors (typically copper), focusing on factors affecting the Li-current collector interface and improvement strategies from perspectives of current collector substrate (lithiophilicity, crystal facets, mechanical properties, and topological structure), electrolyte chemistry, current density, stacking pressure, SEI, electric field and temperature, and provides a future directions and opportunities on this topic. [ABSTRACT FROM AUTHOR]

Solid polymer electrolytes (SPEs) based all-solid-state batteries (ASSBs) have attracted extensive attention as a promising candidate for next-generation energy storage systems. Typical ASSBs require high fabrication pressure to achieve high areal capacity, under which, however, SPEs struggle and risk damage or failure due to their low mechanical strength. There is also a lack of study on complex stress and strain SPEs experience during ASSB cell assembly processes. Here, ceramic solid electrolytes are selected as interlayers to address the stress–strain conditions during assembling. As a result, high areal capacity ASSBs with a LiCoO2 loading of 12 mg·cm−2 were assembled with SPE-based composite electrolytes. Around 200 cycles were carried out for these cells at a current density of 1 mA·cm−2 under room temperature. The capacity decay of the battery at 200 cycles is observed to be as low as 0.06% per cycle. This work identifies a critical issue for application of SPEs in ASSBs and provides a potential strategy for the design of SPE-based ASSBs with high specific energy and long cycle life. [ABSTRACT FROM AUTHOR]

Na metal batteries (NMBs) stand at the forefront of advancing energy storage technologies, but are severely hampered by Na dendrite issues, especially when using carbonate electrolytes. Suppressing the growth of Na dendrites through constructing NaF‐rich solid‐electrolyte‐interphase (SEI) is a commonly‐used strategy to prolong the lifespan of NMBs. In contrast, fluorinated organic SEI components are often underutilized. Inspired by unveiling the adsorption configuration of fluorinated organic compounds on the surface of Na metal, an optimized SEI architecture for stabilizing NMBs is proposed by investigating the C4H9SO2F‐/C4F9SO2F‐treated Na metal anodes. It is revealed that the SEI built on a fluorinated inorganic/organic hybrid layer exhibit favorable Na passivation capability, significantly improving Na deposition behavior. As a result, the NMB with a high‐loading cathode (15 mg cm−2) and a negative/positive capacity ratio (N/P) ratio of 4 shows a long‐term life span over 1000 cycles with 92.8% capacity retention at 2 C. This work opens a new pathway for developing robust and high‐energy‐density NMBs. [ABSTRACT FROM AUTHOR]

Silicon (Si) anodes offer excellent lithium storage capacity for lithium‐ion batteries but face practical limitations due to significant volume expansion and low intrinsic electrical conductivity. These issues lead to side reactions that consume the electrolyte and impede ion‐electron transport, resulting in low areal loading (<2 mg cm⁻²) and restricted energy density. To address this, a scalable method is developed using spray drying of commercial graphite flakes (s‐Gr) and nanosilicon particles (n‐Si), followed by chemical vapor deposition to create microscale Si/C anodes (s‐Gr/n‐Si/VGs). Thin vertical graphene nanosheets (VGs) are grown on the surfaces and within the internal pores, forming a robust, micron‐sized Si/C spherical composite material. The VGs construct the conductive network, allowing the electrodes to operate at high areal loadings without pulverization and promoting LiF‐enriched solid electrolyte interphase for improved cycling stability. The s‐Gr/n‐Si/VGs maintain a capacity of 641.9 mAh g⁻¹ after 1000 cycles at 11.0 mg cm⁻², retaining 95.9% capacity. In pouch cells with NCM811 cathodes, the 5.0 Ah‐level cells achieved 80.0% capacity retention after 510 cycles at 1.0 C. This research provides a feasible pathway for manufacturing high‐performance, low‐cost, and scalable Si/C anodes suitable for high‐energy‐density lithium‐ion batteries. [ABSTRACT FROM AUTHOR]

The Li+ transport kinetics and electrochemical stability of advanced solid‐state Li metal batteries (SLMBs) are seriously limited by the actual electrolyte compositions. Here, a novel polyether‐based electrolyte (PTGDOX) is presented through in situ co‐polymerization by integrating 1,3‐dioxane with a multifunctional 1,3,5‐triglycidyl isocyanurate additive. The isocyanurate group in PTGDOX not only provides abundant coordinating sites for Li+ transfer and restricts the movement of anions, but also prompts a beneficial inorganic‐rich solid electrolyte interface on the Li electrode. As a result, PTGDOX exhibits a remarkably increased ionic conductivity of 0.48 mS cm−1 at 30 °C and a reasonable Li‐ion transference number of 0.68, enabling the Li||Li symmetric cells to stably cycle for over 2000 h at 1 mAh cm−2. Meanwhile, the assembled Li||LiFePO4 exhibit a 97.4% capacity retention after 700 cycles at 3 C with excellent thermal stability. Moreover, PTGDOX also demonstrates excellent interfacial compatibility with high‐voltage LiNi0.8Co0.1Mn0.1O2 cathode. As such, this work provides a facile and accessible strategy for designing interface‐stable polymer electrolytes and achieving practical dendrite‐free SLMBs. [ABSTRACT FROM AUTHOR]

The demand for high-capacity batteries with long cycle life and safety has been increasing owing to the expanding mid-to-large battery market. Li–S batteries are suitable energy-storage devices because of their reversibility, high theoretical capacity, and inexpensive construction materials. However, their performance is limited by various factors, including the shuttle effect and dendrite growth at the anode. Here, an integrated electrode for use in all-solid-state (ASS) Li–S batteries was formed via hot pressing. In detail, S particles dispersed in a functionalized reduced graphite oxide (rGO) cathode with a binder-less polymer electrolyte (PE) and a dual-anion ionic liquid-containing cross-linked poly(ethylene oxide)–Li bis(fluoromethanesulfonyl)imide–N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl) imide-based solid polymer electrolyte (SPE, PEO–LiFSI0.1(Pyr14TFSI)0.4) were hot-pressed into an integrated electrode, which serves as both the cathode and electrolyte. The resulting S/rGO-based solid-state Li–S batteries exhibited more stable performance than Li–S batteries using liquid electrolytes did, indicating that the dual-anion SPE layer effectively suppressed dendritic Li formation and the shuttle effect with high ionic conductivity. At 0.1 C, the battery discharge capacities were 957 and 576 mAh g−1 in the first cycle and after 100 cycles, respectively. At 1 C, the reversible capacity was 590 and 417 mAh g−1 in the first cycle and after 100 cycles, respectively (capacity retention = 71%). Therefore, the proposed S/rGO/PE//LiFSI0.1(Pyr14TFSI)0.4-integrated electrodes are beneficial for ASS Li–S batteries. Sulfur particles disperse in a functionalized reduced graphite oxide (rGO) cathode with a binder-less polymer electrolyte and a dual-anion ionic liquid-containing cross-linked PEO–LiFSI0.1(Pyr14TFSI)0.4 are hot-pressed into an integrated electrode, serving as both the cathode and electrolyte. Dual-anion solid polymer electrolyte and rGO-functional integrated sulfur electrode presents a novel method to improve the electrochemical properties of lithium-sulfur batteries. [ABSTRACT FROM AUTHOR]

Recently, in electric mobilities and stationary energy storage device applications, the development of long‐lasting, low‐cost, and high‐safety lithium‐ion batteries (LIBs) is widely studied. LiFePO4 (LFP) is a core cathode material for LIBs owing to its cost‐effectiveness and high safety. However, it exhibits low electronic conductivity and sluggish Li+ diffusion, hindering the application of LFP cathodes in high‐power battery industries. Herein, a triazole‐motivated electrolyte additive, 1‐(trimethylsilyl)−1H‐benzotriazole (TMSBTA) is presented, for mitigating iron dissolution via HF scavenging, reinforcing the robustness of the solid electrolyte interphase and constructing a cathode–electrolyte interface (CEI) to balance the ion and electron conduction of the CEI on the LFP cathode. Scanning probe microscopy performed in the conductive atomic force microscopy mode indicates that the electronically conductive CEI created by the oxidative decomposition of TMSBTA enables rapid and homogeneous lithiation and delithiation during cycling without morphological changes in the LFP particles. This study elucidates the design principles of the CEI on the LFP cathode and is expected to guide integrated electrolyte additive engineering for LFP‐containing LIBs. [ABSTRACT FROM AUTHOR]