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The thermal and electrochemical properties of several succinonitrile (SN)-based organic ionic plastic crystals (OIPCs) containing lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), lithium bis(oxalate) borate (LiBOB) or mixtures of the two salts, were investigated with the goal of determining which is most promising for use as a catholyte in solid-state lithium batteries. The best combination of properties for this use was found for the mixture containing 3 mol% LiTFSI and 2 mol% LiBOB in SN. Based on these observations, several solid-state cells containing Al-substituted Li7La3Zr2O12 separators with composite cathodes consisting of LiNi0.33Mn0.33Co0.33O2 (NMC111), carbon black, and the succinonitrile-salt mixtures were assembled and cycled at room temperature, without exogenous pressure, using a simple design.

The transition toward electrification of transportation has resulted in a rapid increase in the demand for battery cells. While this demand is currently being met through the use of lithium‐ion batteries (LIBs), alternative batteries like sodium‐ion batteries (SIBs) and solid‐state batteries (SSBs) are emerging as relevant alternatives. In this study, we analyze, based on current electric vehicle electrode stack designs, the environmental impact of LIB cells, SIB cells, and SSB cells. The life cycle assessment results from this cradle‐to‐gate study show that for LIB cell production today, ∼58–92 kgCO2‐eq are emitted per kWhcell and ∼296–624 kWhCED/kWhcell of primary energy is required. In SIB cell production, ∼75–87 kgCO2‐eq/kWhcell is emitted, and in SSB cell production, ∼88–130 kgCO2‐eq/kWhcell, depending on their specific electrode stack configuration. The results demonstrate that LFP (lithium–iron–phosphate) cells require the least energy for production across all battery types under analysis. Furthermore, the findings indicate that, in terms of global warming potential (GWP), LFP and NMC900 (nickel–manganese–cobalt) cells are the most sustainable battery types, at least when focusing solely on battery cell production and neglecting subsequent use phases. Furthermore, it is demonstrated that by optimizing the cell designs and their production, the environmental impact of battery cell production can be reduced in the short term by up to −38%. This allows the production of LFP battery cells with a low GWP of ∼37 kgCO2‐eq/kWhcell and NMC900 cells with ∼44 kgCO2‐eq/kWhcell. Moreover, there is considerable room for improvement in other major LIB cell types. This article met the requirements for a gold‐gold JIE data openness badge described at http://jie.click/badges. [ABSTRACT FROM AUTHOR]

Pyrite (FeS2), as a transition metal sulfide, has a promise application in the field of secondary batteries due to its abundant reserves, high theoretical capacity, safety, and non‐toxicity. However, serious volume expansion and shuttle effect of FeS2 in liquid secondary batteries limit its further development. Solid‐state batteries offer effective solutions to these challenges. In this review, the synthesis methods of FeS2 and recent progress in FeS2‐based solid‐state lithium/sodium batteries are presented, and the effects of FeS2 size and morphology, solid electrolyte type, and battery structure design on the electrochemical performance of solid‐state batteries are discussed. By analyzing and summarizing the problems in applying FeS2 in solid‐state batteries, the remaining challenges in this field are discussed and future directions are proposed. This review aims to guide research on high‐performance solid‐state batteries based on FeS2 and promote further development of FeS2 in electrochemical energy storage. [ABSTRACT FROM AUTHOR]

Anode‐free manufacturing of solid‐state batteries (SSBs) shows promise to maximize energy density by eliminating excess lithium (Li) and simplifying battery production. However, high reversibility during discharge (stripping of Li) is necessary for long‐lifetime SSBs with a limited Li reservoir. Further, the plastic flow of Li changes depending on the Li thickness, leading to possible differences in discharge performance under stack pressure. This work investigates the pressure‐dependent discharge performance of anode‐free manufactured SSBs with in situ plated Li and compares the performance to that of conventional thick Li foil cells. Distinct stripping behavior is observed at low pressures (0–1 MPa), where Li diffusivity and initial interfacial contact may control accessible capacity, compared to high pressures (3–10 MPa) where mechanical deformation of Li likely governs stripping behavior. Analysis of impedance spectra collected during stripping shows that additional stack pressure delays the formation of deep, as opposed to lateral, voids in the Li anode. These results provide insights to guide the transition from thick Li foil anodes to anode‐free manufactured SSBs. [ABSTRACT FROM AUTHOR]

Solid inorganics, known for kinetically inhibiting polymer crystallization and enhancing ionic conductivity, have attracted significant attention in solid polymer electrolytes. However, current composite polymer electrolytes (CPEs) are still facing challenges in Li metal batteries, falling short of inhibiting severe dendritic growth and resulting in very limited cycling life. This study introduces Ga62.5In21.5Sn16 (Galinstan) liquid metal (LM) as an active liquid alternative to conventional passive solid fillers, aiming at realizing self‐healing protection against dendrite problems. Compared to solid inorganics, for example silica, LM droplets could more significantly reduce polymer crystallinity and enhance Li‐ion conductivity due to their liquid nature, especially at temperatures below the polymer melting point. More importantly, LMs are unraveled as dynamic chemical traps, which are capable of blocking and consuming lithium dendrites upon contact via in situ alloying during battery operation and further inhibiting dendritic growth due to the lower deposition energy barrier of the formed Li‐LM alloy. As a proof of concept, by strategically designing an asymmetric CPE with the active LM filling, a solid‐state Li/LiFePO4 battery achieves promising full‐cell functionality with notable rate performance and stable cycle life. This active filler‐mediated self‐healing approach could bring new insights into the battery design in versatile solid‐state systems. [ABSTRACT FROM AUTHOR]

All‐solid‐state Li batteries are desired for better safety and energy density than Li‐ion batteries. However, the lack of a penetrating liquid electrolyte requires a much different approach to the design of cathodes. The solid catholyte must enable good Li+ conduction, form good interfaces with active material particles, and have the strength to bind the cathode together during repeated volume changes. Catholyte formulation is often simply adapted from Li‐ion design principles, adding a Li salt to the PVDF binder. Here we show that such a PVDF binder at 10 wt % loading is a starved catholyte condition that compromises cell performance. By substituting a 70 : 30 blend of PVDF:PEO, performance is improved while maintaining nearly the same areal loading of LFP active material. Increasing the catholyte fraction to 16 % can also improve performance, but in this case the benefit of including PEO is lessened, with PVDF alone being an adequate catholyte. EIS analysis shows that PEO helps to form charge transfer interfaces at 10 % catholyte, but that its inclusion can degrade interfaces when there is ample catholyte at 16 %. It is also shown that catholyte agglomeration can impede bulk Li conduction, indicating that microstructural factors are of critical importance. [ABSTRACT FROM AUTHOR]

The development of battery technology has made great advances in recent years. However, the increasing demand for electric mobility also highlights the limitations of conventional lithium-ion battery (LIB) technology, such as limited range and fast charging capability, as well as challenges related to battery safety. Among all the technology alternatives, the solid-state battery technology shows great potential to enable higher safety due to the use of non-flammable solid electrolytes instead of liquid electrolytes as well as higher energy densities by replacing the graphite anode with a lithium metal anode. In addition to the trend towards improved battery cell performance, there is also a growing need for the production of application-specific cell geometries. At the Institute of Production Science (wbk), the approach of agile cell production for conventional lithium-ion batteries is currently being investigated. In order to extend the scope of this material and format flexible approach, manufacturing processes for solid-state batteries (SSB) are being considered and further investigated. As a first objective, this work presents a concept for the evaluation of the handling processes of polyethylene oxide (PEO)-based composite cathodes with a special focus on the pick-and-place process. PEO-based composite cathodes are mechanically sensitive, with adhesive and limp characteristics. Therefore, the design of a semi-automated test rig is presented, which allows reproducible gripping, moving and placing of PEO-based composite cathode single sheets and thus stacking on pre-defined platforms. A camera system is integrated to monitor and quantify the process quality. An image processing tool is developed to determine the positioning accuracy and to detect possible damages on the electrode surface from handling. Furthermore, a concept for performing the handling tests is presented. [ABSTRACT FROM AUTHOR]

Sulfide‐based inorganic solid electrolytes are promising materials for high‐performance safe solid‐state batteries. The high ion conductivity, mechanical characteristics, and good processability of sulfide‐based inorganic solid electrolytes are desirable properties for realizing high‐performance safe solid‐state batteries by replacing conventional liquid electrolytes. However, the low chemical and electrochemical stability of sulfide‐based inorganic solid electrolytes hinder the commercialization of sulfide‐based safe solid‐state batteries. Particularly, the instability of sulfide‐based inorganic solid electrolytes is intensified in the cathode, comprising various materials. In this study, carbonate‐based ionic conductive polymers are introduced to the cathode to protect cathode materials and suppress the reactivity of sulfide electrolytes. Several instruments, including electrochemical spectroscopy, X‐ray photoelectron spectroscopy, and scanning electron microscopy, confirm the chemical and electrochemical stability of the polymer electrolytes in contact with sulfide‐based inorganic solid electrolytes. Sulfide‐based solid‐state cells show stable electrochemical performance over 100 cycles when the ionic conductive polymers were applied to the cathode. [ABSTRACT FROM AUTHOR]

The intense research of lithium‐ion batteries has been motivated by their successful applications in mobile devices and electronic vehicles. The emerging of intelligent control in kinds of devices brings new requirements for battery systems. The high‐energy lithium batteries are expected to respond or react under different environmental conditions. In this work, a tri‐salt composite electrolyte is designed with a temperature switch function for intelligently temperature‐controlled lithium batteries. Specifically, the halide Li3YBr6 together with LiTFSI and LiNO3 works as active fillers in a low‐melting‐point polymer matrix (polyethyleneglycol dimethyl ether (PEGDME) and polyethylene oxide (PEO)), which is further filled into the pre‐lithiated alumina fiber skeleton. Above 60 °C, the composite electrolyte exists in the liquid state and fully contacts with the working electrodes on the liquid–solid interface, effectively minimizing the interfacial resistance and leading to high discharge capacity in the cell. The electrolyte is changed into a solid state below 30 °C so that the ionic conductivity is significantly reduced and the interface resistance is increased dramatically on the solid–solid interface. Therefore, by simply adjusting the temperature, the cell can be turned "ON" or "OFF" intentionally. This novel function of the composite electrolyte has enlightening significance in developing intelligently temperature‐controlled lithium batteries. [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]

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]

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]

A novel approach is presented to model delamination and recontacting at internal interfaces of three-dimensional resolved microstructures of solid-state batteries. To resolve the effect of delaminations, we incorporate the consistent enforcement of contact constraints at those interfaces using Nitsche's method. The model incorporates charge, mass, and momentum conservation to consider electrochemistry, solid mechanics, and their interaction. After introducing and verifying the model, we examine various scenarios to quantify the effect of delaminations at the electrode-solid electrolyte interface on cell performance. The simulations show that increased mechanical stack pressure during cycling mitigates delamination tendencies at the electrode-solid electrolyte interface. Consistent with existing literature, the simulations demonstrate that delaminations increase the internal resistance and reduce the amount of transferred charge. In contrast to experimental analyses, the presented model allows quantitative and in-depth investigations of delamination effects. Furthermore, our analysis of two cell concepts—one assembled in the discharged state and another assembled in the charged state—indicates that half-cells assembled in an initial state from which the active material shrinks in volume upon first charge or discharge show a higher delamination risk at the electrode-solid electrolyte interface. The study highlights the critical relationship between solid mechanics and electrochemistry in consideration of delamination phenomena in solid-state batteries, offering valuable insights for optimizing battery design and performance. [ABSTRACT FROM AUTHOR]

Sodium-ion batteries offer an attractive alternative to lithium-based chemistries due to the lower cost and abundance of sodium compared to lithium. Using solid electrolytes instead of liquid ones in such batteries may help improve safety and energy density, but they need to combine easy processing with high stability toward the electrodes. Herein, we describe a new class of solid electrolytes that are accessible by room-temperature, aqueous synthesis. The materials exhibit a garnet-type zinc hexacyanoferrate framework with large diffusion channels for alkaline ions. Specifically, they show superionic behavior and allow for facile processing into pellets. We compare the structure, stability, and transport properties of lithium-, sodium-, and potassium-containing zinc hexacyanoferrates and find that Na2Zn3[Fe(CN)6]2 achieves the highest ionic conductivity of up to 0.21 mS/cm at room temperature. In addition, the electrochemical performance and stability of the latter solid electrolyte are examined in solid-state sodium-ion batteries. [ABSTRACT FROM AUTHOR]

A comprehensive sketch of the study logic is listed. The origin of our investigation is based on the ideational attempt that replacing traditional sulfide interlayer in halide-based all solid-state electrolyte to realize the independent application or flexible collocation of halide solid-state electrolyte. For this purpose, we find Li 3 Y(BrCl) 3 is the potential answer via screening the chemical system by thermodynamical stability, cost, ionic conductivity. Then, the electrochemical behavior of Li 3 Y(BrCl) 3 is completely investigated. [Display omitted] Halide-type solid-state electrolytes (SEs) are regarded as promising candidates for the commercialization of all solid-state lithium metal batteries (ASLMBs). However, the poor reduction stability of their central structural metal cations complicates the direct contact with lithium metal, thus conventionally requiring a sulfide interlayer between the lithium metal anode and halide SE. Concerning this issue, we developed a systematic approach to identify the SE in the halide family with thermodynamic stability, cost-effectiveness, and ionic conductivity to substitute the sulfide buffer layer and support the operation of ASLMBs utilizing solely halide-type SEs. The initial screen results indicate that Li 3 Y(BrCl) 3 (LYBC) is a promising candidate. Our theoretical calculations confirmed its lower reduction potential of 0.58 V. The lithium symmetrical cell using LYBC was able to cycle for over 1000 h at a current density of 0.255 mA cm−2 and an areal capacity of 0.255mAh cm−2. The performance of ASLMBs also notarized the feasibility of our strategy. In addition, according to our experiment, we deduce that the reduced LYBC can still conduct lithium-ion rapidly, which may be the key to supporting the normal operation of the electrochemical system. Combined with our cost analysis, LYBC is identified as one of the most suitable commercial materials for realizing the self-liberation of halide SEs. Our research proposes a novel pathway for the future development of halide SEs. [ABSTRACT FROM AUTHOR]

Sodium‐based batteries are gaining momentum due to the abundance and lower cost of sodium compared to lithium. Solid‐state sodium batteries can also provide further safety advantages. However, sodium‐based solid‐state electrolytes (SSEs) that meet all the rigorous requirements, such as high ionic conductivity, oxidative stability with the cathode, and ease of processability, are lacking. We present here a new class of sodium‐based oxyhalide electrolytes NaNbCl6‐2xOx with a facile mechanochemical synthesis. The oxyhalide NaNbCl4O exhibits close to two orders of magnitude higher ambient‐temperature sodium‐ion conductivity (1.03×10−4 S cm−1) compared to the halide counterpart NaNbCl6 (3×10−6 S cm−1). Structural motifs unique to the oxygen content in NaNbCl6‐2xOx are identified with 23Na and 93Nb magic angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy and x‐ray diffraction (XRD). Solid‐state sodium batteries assembled with NaNbCl4O electrolyte and the cobalt‐ and nickel‐free layered Na0.70Fe0.3Mn0.65Al0.05O2 cathode exhibit a maximum discharge capacity of 155 mAh g−1 with good cycle life at ambient temperature. [ABSTRACT FROM AUTHOR]

“Anodeless” electrodes for all‐solid‐state batteries (ASSBs) have been attracting attention as a solution for achieving high energy density. Recent studies on anodeless electrodes have shown improvements in cycle life and energy density through the stabilization of plated lithium (Li) using Li‐soluble metals (e.g., Ag, Zn, etc.). In this study, magnesium‐based materials (MgF2@C) are introduced for use as an anodeless electrode. Nanodot magnesium fluoride (MgF2) is synthesized onto a carbon black surface via sonochemical synthesis. MgF2 is converted to a Mg‐Li alloy and LiF during lithiation. The Mg‐Li alloy from the MgF2@C anodeless electrode reduces lithiation overpotential and provides a uniform and dense Li layer between the current collector and the anodeless electrode. The ASSB cell assembled with the MgF2@C anodeless electrode exhibits 81.4% capacity retention after 200 cycles at 30 °C. [ABSTRACT FROM AUTHOR]

Solid polymer electrolytes (SPEs) are crucial in the development of lithium metal batteries. Recently, metal–organic frameworks (MOFs) with open metal sites (OMSs) have shown promise as solid fillers to improve the performance of SPEs. However, the number of OMS‐containing MOFs is quite limited, comprising less than 5% of the total MOFs. When considering yield, cost, and processability, the commonly used OMS‐containing MOFs are no more than 10 types, causing great limitations. Herein, we reported a simple and universal methodology that converted OMS‐free MOFs to OMS‐rich quasi‐MOFs for developing high‐performance SPEs, and explored the underlying mechanism. The “OMS‐polymer” and “OMS‐ion” interactions were investigated in detail to elucidate the role of quasi‐MOFs on battery performance. It was found that quasi‐MOFs, functioning as ion sieves, can effectively regulate ion migration, thus promoting uniform Li deposition and enabling an ultra‐stable interface. As a result, the Li symmetric cell stably ran over 3000 h at 0.3 mA cm−2, while the full cell retained 85 % of its initial capacity after 1500 cycles at 1.0 C. Finally, universal testing was performed using other MOFs, confirming the generalizability and effectiveness of our design concept. [ABSTRACT FROM AUTHOR]

[Display omitted] • Composite polymer electrolytes were successfully prepared using solution casting and electrospinning method. • LaFeO 3 increases the amorphous regions of poly(vinylidene fluoride hexafluoropropylene) enhancing the ionic conduction. • Solution casted electrolyte with 5 wt% LaFeO 3 shows very low polarization voltage and excellent electrochemical compatibility against lithium metal. • Solid-state battery using solution casted electrolyte with 5 wt% LaFeO 3 shows superior cycling stability and electrospun electrolyte with 5 wt% LaFeO 3 exhibits better rate performance. Composite polymer electrolytes (CPEs) are a promising alternative to flammable conventional liquid electrolytes for high-safety lithium-ion batteries. Establishing low-cost filler that enhances the amorphous nature of polymer in the CPEs and exhibits efficient Lewis acid-base interaction between fillers and anions of lithium salt, leading to improved dissociation of salts for enhanced conduction, is indispensable. In this work, for the first time, we construct a solid composite polymer electrolyte of poly(vinylidene fluoride hexafluoropropylene) embedded LaFeO 3 (LFO) particles prepared by solution casting and electrospinning methods and study their performances. The 5 wt% LFO filler embedded CPE made by means of solution casting and electrospinning methods exhibited the highest ionic conductivity of 5.9 × 10-4 and 1.49 × 10-3 S cm−1 at room temperature and electrochemical stability window up to 4.6 and 4.45 V, respectively. Further, as-assembled solid-state lithium-ion batteries using electrospun CPE showed an initial discharge capacity of 166 mAh/g at 0.1C-rate and solution-casted CPE showed excellent cycling stability with 98.6 % capacity retention at 0.3C-rate even at 50th cycle. Such excellent performance originated from the introduction of the LFO particles as filler into the polymer matrix to enhance the ionic conductivity, mechanical strength and lithium metal compatibility of the resulting CPEs. [ABSTRACT FROM AUTHOR]

Solid-state batteries (SSBs) have received widespread attention with their high safety and high energy density characteristics. However, solid-solid contacts in the internal electrode material and the electrode material/solid electrolyte (SE) interfaces, as well as the severe electrochemo-mechanical effects caused by the internal stress due to the volume change of the active material, these problems hinder ion/electron transport within the SSBs, which significantly deteriorates the electrochemical performance. Applying fabrication pressures and stack pressures are effective measures to improve solid-solid contact and solve electrochemo-mechanical problems. Herein, the influences of different pressures on cathode material, anode material, SEs, and electrode/SEs interface are briefly summarized from the perspective of interface ion diffusion, transmission of electrons and ions in internal particles, current density and ion diffusion kinetics, and the volume changes of Liþ stripping/plating based on two physical contact models, and point out the direction for the future research direction of SSBs and advancing industrialization by building the relationship between pressures and SSBs electrochemistry. [ABSTRACT FROM AUTHOR]

In the current aera of rapid development in the field of electric vehicles and electrochemical energy storage, solid-state battery technology is attracting much research and attention. Solid-state electrolytes, as the key component of next-generation battery technology, are favored for their high safety, high energy density, and long life. However, finding high-performance solid-state electrolytes is the primary challenge for solid-state battery applications. Focusing on inorganic solid-state electrolytes, this work highlights the need for ideal solid-state electrolytes to have low electronic conductivity, good thermal stability, and structural and phase stability. Traditional experimental and theoretical computational methods suffer from inefficiency, thus machine learning methods become a novel path to intelligently predict material properties by analyzing a large number of inorganic structural properties and characteristics. Through the gradient descent-based XGBoost algorithm, we successfully predicted the energy band structure and stability of the materials, and screened out only 194 ideal solid-state electrolyte structures from more than 6000 structures that satisfy the requirements of low electronic conductivity and stability simultaneously, which greatly accelerated the development of solid-state batteries. [ABSTRACT FROM AUTHOR]

Li1.3Al0.3Ti1.7(PO4)3 (LATP) electrolyte has a great potential for application in solid‐state lithium metal batteries. However, due to the poor interfacial contact and thermodynamic instability between LATP and Li metal, a series of interfacial problems, such as high interfacial resistance, undesirable interfacial reaction and dendrite growth are deeply criticized. Herein, a hybrid LiCl/LixSn conductive interlayer is constructed through an in situ electrochemical reaction of SnCl4 with Li metal to effectively improve the compatibility and stability of the Li/LATP interface. LiCl with both electronic insulation and high ionic conductivity can provide fast Li+ diffusion channel, block electron injection, avoid side reactions, and effectively inhibit dendrite growth. LixSn can reduce interfacial impedance, eliminate local electric field concentration, and significantly improve interfacial wettability. Under the protection of LiCl/LixSn hybrid interlayer, the initial resistance of the symmetric battery is reduced from 1066.3 to 133.6 Ω cm−2, achieving a high critical current density of 1.4 mA cm−2. At 0.1 mA cm−2/0.1 mAh cm−2 and 0.2 mA cm−2/0.2 mAh cm−2, the symmetric battery can cycle stably for more than 4000 h at 25 °C. Moreover, the full battery displays a high capacity retention ratio of 90.4% after 420 cycles at 0.5 C. [ABSTRACT FROM AUTHOR]

This study investigates the performance and cycling fading of a solid-state fluoride-ion battery (FIB) based on the CuF2 electrode. The cathode and solid electrolyte of CuF2 composite and La0.9Ba0.1F2.9 are prepared by ballmilling. Meanwhile, the anode materials are used as Sn and Pb. All FIB cells with sandwich structures are fabricated by compressing under a pressure of 4.5 tons/cm². Electrochemical measurements of discharge/charge are performed at 423 K and under 40 μA/cm². The resultant cycling stability of the cell with the Pb anode is higher than that of the cell with the Sn anode. Concerning the cell with Pb anode, the first and tenth discharge capacities of 150 and 90 mAh/g are obtained. X-ray photoelectron analysis demonstrates that the cycling fading of the cell with the Sn (or Pb) anode may be attributed to the irreversible formation of materials (e.g., SnF4 or PbF4) during the electrochemical reaction. [ABSTRACT FROM AUTHOR]

We report on the use of an atmospheric pressure, open-air plasma treatment to remove Li2CO3 species from the surface of garnet-type tantalum-doped lithium lanthanum zirconium oxide (Li6.4La3Zr1.4Ta0.6O12, LLZTO) solid-state electrolyte pellets. The Li2CO3 layer, which we show forms on the surface of garnets within 3 min of exposure to ambient moisture and CO2, increases the interface (surface) resistance of LLZTO. The plasma treatment is carried out entirely in ambient and is enabled by use of a custom-built metal shroud that is placed around the plasma nozzle to prevent moisture and CO2 from reacting with the sample. After the plasma treatment, N2 compressed gas is flowed through the shroud to cool the sample and prevent atmospheric species from reacting with the LLZTO. We demonstrate that this approach is effective for removing the Li2CO3 from the surface of LLZTO. The surface chemistry is characterized with X-ray photoelectron spectroscopy to evaluate the effect of process parameters (plasma exposure time and shroud gas chemistry) on removal of the surface species. We also show that the open-air plasma treatment can significantly reduce the interface resistance. This platform demonstrates a path towards open-air processed solid-state batteries. [ABSTRACT FROM AUTHOR]

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Liquid electrolytes are currently state-of-the-art for commercial Li-ion batteries. However, their use implicates inherent challenges, including safety concerns associated with flammability, limited thermal stability, and susceptibility to dendrite formation on the lithium metal anode, that can compromise the battery lifespan. Solid-state polymer electrolytes offer an alternative to conventional liquid electrolytes, aiming to mitigate safety, stability, and performance drawbacks. This study investigates the preparation and the comprehensive characterization of polyethylene oxide (PEO) and polycarbonate (PC) blends obtained through extrusion process. The process is solvent-free and easily scalable at the industrial level; it grants the efficient dispersion and mixing of PEO and PC. Blends at different ratios of PEO (Mw of 4 × 105 and 4 × 106 g mol˗1) and two types of PCs (namely, polyethylene and polypropylene carbonate) including lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) are prepared. Optimization and investigation of the relative effects between the application of different PCs and the variable ratios of PEO/PCs on the mechanical, morphologic and electrochemical properties of the final polymeric membranes is carried out for future applications of these systems, as efficient electrolytes in all-solid-state lithium batteries.

Abstract All‐solid‐state Li batteries are desired for better safety and energy density than Li‐ion batteries. However, the lack of a penetrating liquid electrolyte requires a much different approach to the design of cathodes. The solid catholyte must enable good Li+ conduction, form good interfaces with active material particles, and have the strength to bind the cathode together during repeated volume changes. Catholyte formulation is often simply adapted from Li‐ion design principles, adding a Li salt to the PVDF binder. Here we show that such a PVDF binder at 10 wt % loading is a starved catholyte condition that compromises cell performance. By substituting a 70 : 30 blend of PVDF:PEO, performance is improved while maintaining nearly the same areal loading of LFP active material. Increasing the catholyte fraction to 16 % can also improve performance, but in this case the benefit of including PEO is lessened, with PVDF alone being an adequate catholyte. EIS analysis shows that PEO helps to form charge transfer interfaces at 10 % catholyte, but that its inclusion can degrade interfaces when there is ample catholyte at 16 %. It is also shown that catholyte agglomeration can impede bulk Li conduction, indicating that microstructural factors are of critical importance.

The solid-state battery is crucial for achieving the next-generation batteries that possess high energy density, high safety, long service life, and low cost. Major countries and regions are rapidly advancing the research and industrial application of solid-state batteries. This study reviews the development status of key material systems for solid-state batteries worldwide from the aspects of technological, industrial, and supporting systems. It analyzes the technical development paths, industrial scales, and supporting systems of solid-state batteries in countries and regions including the United States, Europe, Japan, and Republic of Korea, and summarizes the development status and goals of the key material system for solid-state batteries in China. Our study reveals that the solid-state batteries are currently in a promotion stage in China, facing challenges in terms of key raw materials, breakthroughs in critical scientific and technological bottlenecks, mass production, and industrial application. To promote the development of solid-state batteries in China, we propose the following suggestions: (1) adhering to an overall staged-development strategy for solid-state batteries, (2) establishing national-level development programs and major scientific and technological projects for solid-state batteries, (3) promoting the construction of technology research and development institutions for solid-state batteries, (4) encouraging the market application and industrial transformation of solid-state batteries, and (5) optimizing the solid-state battery ecosystem.

The desirable characteristics of an energy storage system (ESS) to fulfill the energy requirement in electric vehicles (EVs) are high specific energy, significant storage capacity, longer life cycles, high operating efficiency, and low cost. In order to advance electric transportation, it is important to identify the significant characteristics, pros and cons, new scientific developments, potential barriers, and imminent prospects of various energy storage technology. The objective of current research is to analyse and find out the optimal storage technology among different electro-chemical, chemical, electrical, mechanical, and hybrid storage system. Different batteries including lead-acid, nickel-based, lithium-ion, flow, metal-air, solid state, and ZEBRA along with their operating parameters are reviewed. The potential roles of fuel cell, ultracapacitor, flywheel and hybrid storage system technology in EVs are explored. Performance parameters of various battery system are analysed through radar based specified technique to conclude the best storage medium in electric mobility. Additionally, the current study compiles a critical analysis of 264 publications from various sources.

Microstructure of argyrodite solid‐state electrolyte (SSE) critically affects lithium metal electrodeposition/dissolution. While the stability of unmodified SSE is mediocre, once optimized state‐of‐the‐art electrochemical performance is achieved (symmetric cells, full cells with NMC811) without secondary interlayers or functionalized current collectors. Planetary mechanical milling in wet media (m‐xylene) is employed to alter commercial Li6PS5Cl (LPSCl) powder. Quantitative stereology demonstrates how milling progressively refines grain and pore size/distribution in the SSE compact, increases its density, and geometrically smoothens the SSE‐Li interface. Mechanical indentation demonstrates that these changes lead to reduced site‐to‐site variation in the compact's hardness. Milled microstructures promote uniform early‐stage electrodeposition on foil collectors and stabilize solid electrolyte interphase (SEI) reactivity. Analysis of half‐cells with bilayer electrolytes demonstrates the importance of microstructure directly contacting current collector, with interface roughness due to pore and grain size distribution being key. For the first time, short‐circuiting Li metal dendrite is directly identified, employing 1.5 mm diameter "mini" symmetrical cell and cryogenic focused ion beam (cryo‐FIB) electron microscopy. The branching sheet‐like dendrite traverses intergranularly, filling the interparticle voids and forming an SEI around it. Mesoscale modeling reveals the relationship between Li‐SSE interface morphology and the onset of electrochemical instability, based on underlying reaction current distribution. [ABSTRACT FROM AUTHOR]

Solid polymer electrolytes have been considered as promising candidates for solid-state batteries (SSBs), owing to their excellent interfacial compatibility and high mechanical toughness; however, they suffer from intrinsic low ionic conductivity (lower than 10−6 S/cm) and large thickness (usually surpassed over 100 μm or even 500 μm), which has a negative influence on the interface resistance and ionic migration. In this work, ceria quantum dot (CQD)-modified composite polymer electrolyte (CPE) membranes with a thickness of 20 μm were successfully manufactured via 3D printing technology. The CQD fillers can reduce the crystallinity of the polymer, and the oxygen vacancies on CQDs can facilitate the dissociation of ion pairs in the NaTFSI salt to release more free Na+, improving the ionic conductivity. Meanwhile, tailoring the thickness of the CPE-CQDs membrane via 3D printing can further promote the migration and transport of Na+. Furthermore, the printed NNM//CPE-CQDs//Na SSB exhibited outstanding rate capability and cycling stability. The combination of CQD modification and thickness tailoring through 3D printing paves a new avenue for achieving high performance solid electrolyte membranes for practical application in Na SSBs. [ABSTRACT FROM AUTHOR]

[Display omitted] SnO 2 layer between Li 1.5 Al 0.5 Ge 1.5 (PO 4) 3 (LAGP) and lithium anode was prepared through simple scratch-coating process to improve interface properties. The physical phase, morphology, and electrochemical properties of Li/SnO 2 /LAGP structure were characterized by X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, and electrochemical analytical methods. It was found that SnO 2 layer effectively improved the interface stability of LAGP and lithium anode. The prepared Li/SnO 2 /LAGP/SnO 2 /Li symmetric cell exhibited a large critical current density of 1.8 mA cm−2 and demonstrated excellent cycling characteristics. The polarization voltages of symmetric cell were 0.1 V and 0.8 V after 1000 h of cycling at current densities of 0.04 mA cm−2 and 0.5 mA cm−2, respectively. Li/SnO 2 @LAGP/LiFePO 4 solid-state full cells were also assembled, exhibiting a discharge specific capacity of 150 mAh g−1 after 200 cycles at 0.1C with capacity retention rate of 96 %. The good interface properties of Li/SnO 2 /LAGP structure are attributed to the transformation of SnO 2 layer into a buffer layer containing Li 2 O, Sn0, and Li x Sn y alloy during cycling process, which effectively inhibits the reduction reaction between LAGP and lithium anode. [ABSTRACT FROM AUTHOR]

Na3Zr2Si2PO12(NZSP)‐based NASICON solid‐state electrolytes (SSEs) show not only competitive ionic conductivity but also high chemical stability in air, holding a great promise for enabling the use of sodium metal anode in solid‐state sodium batteries. However, sodium (Na) metal dendrite growth inside SSE always leads to undesirable short‐circuiting in battery even no obvious changes in interfacial contact loss and interfacial decomposition during cycling. How to control Na metal dendrite growth and in situ observe the effect of SSE/Na interface change on dendrite growth is quite challenging. Herein, an in situ synchrotron‐based X‐ray imaging method is developed to systematically investigate the dendrite origin in NZSP‐based SSEs. It is find that the dendrite growth intrinsically depends on the grain boundaries (GBs) in NZSP and the NZSP/Na interfacial properties. It is confirmed that Na dendrite infiltration kinetic evolution in NZSP is strongly associated with Na ion/electron conductivity and Young's modulus of GBs. Moreover, the electro‐chemo‐mechanical phase‐field model evaluation demonstrates that the basic reason for Na metal dendrite intrusion into the GBs of SSE is a combination of local polarization potential and the presence of stress formed at GBs. [ABSTRACT FROM AUTHOR]

Garnet solid state electrolytes (SSEs) have emerged as propitious candidates for solid‐state batteries (SSBs) with exceptional ionic conductivity and excellent (electro)chemical stability. However, the Li|garnet interface contact deterioration still remains a major challenge resulting in Li dendrite propagation. Herein, a method is proposed to strengthen the adhesion of garnet SSE and Li by incorporating Sr3N2 into the Li metal. Density functional theory (DFT) calculations reveal that the interfacial formation energy of Li|garnet is decreased by the obtained Li‐Sr‐N (LSN) composite, which can enable a shift from poor contact to intimate bonding at the Li|garnet interface and a homogenous Li+ flux as well as electric field distribution. Simultaneously, the produced Li3N and LiSrN, which are known for their strong Li adsorption affinity and rapid Li+ transfer kinetics, actively govern the Li plating process. Thereby this rational design brings a notable reduction in interfacial impedance (4.5 Ω cm2), along with the increased critical current density (1.3 mA cm−2) and enhanced cycle stability (1200 h at 0.3 mA cm−2). Furthermore, The LFP|garnet|LSN full cell has demonstrated remarkable cycling performance (95.9% capacity retention after 200 cycles at 1 C) and favorable rate capability (150.2 mAh g−1 at 0.1 C and 134.9 mAh g−1 at 1 C). The research provides a new sight into lithium modification that can restrain Li|garnet interface deterioration and lay the groundwork for future advancements in high‐performance garnet‐ based SSBs. [ABSTRACT FROM AUTHOR]

All solid‐state lithium–sulfur batteries (ASSLSBs) have attracted significant attention due to their enhanced safety and superior energy density. However, the considerable volume change during cycling poses a challenge, resulting in electrochemical‐mechanical degradation. To address this issue, polypyrrole (PPy) is coated on a nitrogen‐doped carbon nanotube (NCNT) network to exhibit suitable conductivity and compatibility with sulfide electrolyte. Functionally, PPy@NCNT provides a continuous and conductive pathway, reducing the tortuosity of charge transport. Mechanically, operando pressure measurements and atomic force microscopy (AFM) tests are conducted, demonstrating that the flexible and viscoelastic structure of PPy@NCNT can alleviate local stress. The axial pressure on the cathode can be reduced by 11% with a sulfur area capacity of 3 mg cm−2 at 30 °C. At a high areal mass loading of 4.5 mg cm−2, a high areal capacity of 6 mAh cm−2 (1348 mAh g−1, 1C = 1675 mA g−1) is achieved at 0.1C, maintaining stability over 300 cycles at 0.2C. Remarkably, it can achieve an areal capacity of over 8.8 mAh cm−2 and stable cycling even at 60 °C. This study, being the first to regulate mechano‐electrochemical action in ASSLSBs with flexible conducting polymer, highlights the significance of integrating a continuous and elastic network into solid‐state conversion‐type cathodes. [ABSTRACT FROM AUTHOR]

Superionic sulfide solid electrolytes (SEs) are of considerable interest for application in solid‐state batteries, but suffer from limited stability. When in combination with state‐of‐the‐art cathode active materials (CAMs), severe degradation at the CAM/SE interface occurs during electrochemical cycling. To improve upon the interfacial stability, inert coatings can be applied to the CAM particles, with the goal of preventing direct contact to the SE. In this study, different methods of depositing coatings, including hexagonal boron nitride, tungsten sulfide and exfoliated ((CH3(CH2)3)4N)4Nb6O17, in the form of nanosheets onto the free surface of a Ni‐rich LiNixCoyMnzO2 (NCM) CAM are examined and compared with one another. While dry coating is shown to produce relatively uniform coatings (good surface coverage), the secondary particle morphology of the NCM makes ball milling as a mechanical deposition method less attractive. In contrast, deposition from dispersions in organic solvents yields protective coatings with a lower degree of surface coverage. The different materials are electrochemically tested in liquid‐ and solid‐electrolyte‐based lithium‐ion batteries. A stabilizing effect from nanosheet coating is only observed for the cells with lithium thiophosphate SE. [ABSTRACT FROM AUTHOR]

The high theoretical energy density (1274 Wh kg−1) and high safety enable the all‐solid‐state Na−S batteries with great promise for stationary energy storage system. However, the uncontrollable solid–liquid‐solid multiphase conversion and its associated sluggish polysulfides redox kinetics pose a great challenge in tunning the sulfur speciation pathway for practical Na−S electrochemistry. Herein, we propose a new design methodology for matrix featuring separated bi‐catalytic sites that control the multi‐step polysulfide transformation in tandem and direct quasi‐solid reversible sulfur conversion during battery cycling. It is revealed that the N, P heteroatom hotspots are more favorable for catalyzing the long‐chain polysulfides reduction, while PtNi nanocrystals manipulate the direct and full Na2S4 to Na2S low‐kinetic conversion during discharging. The electrodeposited Na2S on strongly coupled PtNi and N, P‐codoped carbon host is extremely electroreactive and can be readily recovered back to S8 without passivation of active species during battery recharging, which delivers a true tandem electrocatalytic quasi‐solid sulfur conversion mechanism. Accordingly, stable cycling of the all‐solid‐state soft‐package Na−S pouch cells with an attractive specific capacity of 876 mAh gS−1 and a high energy of 608 Wh kgcathode−1 (172 Wh kg−1, based on the total mass of cathode and anode) at 60 °C are demonstrated. [ABSTRACT FROM AUTHOR]

This study aims to predict the commercialization of lithium-based solid-state battery (LSSB) technology and identify the solid electrolyte type that will dominate the market. This study analyzed LSSB patents filed from 2000 to 2020 to determine the current stage of the technology life cycle, and examined the patent quality and competitiveness of three types of solid electrolytes (oxide-, sulfide-, and polymer-based) to identify the most promising. We found that LSSB technology is moving from the emerging to the growth phase, while the oxide-based solid electrolyte is the most promising technology, followed by sulfide- and polymer-based electrolyte technology. [ABSTRACT FROM AUTHOR]

The incomplete sulfur reduction and high ZnS re-oxidation energy barrier along with severe side reactions during the battery cycling compromise the practical application of Zn–S electrochemistry. Herein, a bifunctional electrocatalytic sulfur matrix that simultaneously accelerates the sulfur reduction and ZnS oxidation is proposed to realize a highly-efficient Zn–S cell. It is revealed that the N-heteroatom hotspots are more favorable for facilitating the conversion of S to ZnS while the CoO nanocrystal substantially lowers the ZnS activation energy barrier thereby suppressing the formation of disproportionation species (e.g., SO 4 2 − ) and accumulation of inactive ZnS. Accordingly, the CoO anchored on the N-doped carbon-supported sulfur cathode delivers a high Zn2+ storage capacity of 1,172 mAh g−1 and outstanding cycling stability with a capacity retention of 71.6% after 500 cycles with a high average Coulombic efficiency of 97.8%. Simultaneously, the stable cycling of solid-state Zn–S pouch cells with an energy density of 585 Wh kg − 1 sulfur is also demonstrated. Moreover, the postmortem analysis reveals that the degradation of Zn–S cells is mainly attributed to the limited reversibility of Zn anodes rather than the ZnS decomposition and/or accumulation. The approach to the bidirectional catalysis manipulated the sulfur redox provides a new perspective to realize the theoretical potentials of Zn–S cells. [ABSTRACT FROM AUTHOR]

With the in-depth study of solid-state batteries (SSBs), various in situ and ex situ characterization technologies have been widely used to study them. The performance and reliability of SSBs are limited by the formation and evolution of lithium dendrites at the interfaces between solid electrodes and solid electrolytes. We propose a new method based on optical coherence tomography (OCT) for in situ characterization of the internal state of solid-state batteries. OCT is a low-loss, high-resolution, non-invasive imaging technique that can provide real-time monitoring of cross-sectional images of internal structures of SSBs. The morphology, growth, and evolution of lithium dendrites at different stages of cycling under various conditions can be visualized and quantified by OCT. Furthermore, we validate and correlate the OCT results with scanning electron microscopy (SEM) and XPS, proving the accuracy and effectiveness of the OCT characterization method. We reveal the interfacial phenomena and challenges in SSBs and demonstrate the feasibility and advantages of OCT as a powerful tool for in situ and operando imaging of battery interfaces. This study provides new insights into the mechanisms and factors that affect SSB performance, safety, and lifetime, and suggests possible solutions for improvement and application in the field of applied energy. [ABSTRACT FROM AUTHOR]

Highlights Thermally stable catholyte buffer layer was fabricated via incorporating a multi-functional flame-retardant triphenyl phosphate additive into poly(ethylene oxide). The optimized catholyte buffer layer enabled thermal and electrochemical stability at interface level, delivering comparable cycling stability of garnet-based all solid-state lithium battery, i.e., capacity retention of 98.5% after 100 cycles at 60 °C, and 89.6% after 50 cycles at 80 °C. Exceptional safety performances were demonstrated, i.e., safely cycling behavior at temperature up to 100 °C and spontaneous fire-extinguishing ability.

Sodium-ion batteries offer an attractive alternative to lithium-based chemistries due to the lower cost and abundance of sodium compared to lithium. Using solid electrolytes instead of liquid ones in such batteries may help improve safety and energy density, but they need to combine easy processing with high stability toward the electrodes. Herein, we describe a new class of solid electrolytes that are accessible by room-temperature, aqueous synthesis. The materials exhibit a garnet-type zinc hexacyanoferrate framework with large diffusion channels for alkaline ions. Specifically, they show superionic behavior and allow for facile processing into pellets. We compare the structure, stability, and transport properties of lithium-, sodium-, and potassium-containing zinc hexacyanoferrates and find that Na2Zn3[Fe(CN)6]2 achieves the highest ionic conductivity of up to 0.21 mS/cm at room temperature. In addition, the electrochemical performance and stability of the latter solid electrolyte are examined in solid-state sodium-ion batteries.

As the demand for battery technology with enhanced safety and high energy density increases, solid-state batteries are currently attracting attention as a solution to problems such as fire and explosion risks associated with lithium-ion batteries. In this study, experiments were conducted to synthesize and optimize Li7La3Zr2O12 (LLZO), a solid electrolyte that is a key component of lithium-ion batteries with stability and high energy density. Experimental results showed that sintering at a low temperature of 800 °C for 8 h was the optimal synthesis and sintering time. Additionally, the excess lithium-containing bed powder enabled the production of pure cubic-phase LLZO. Through a sintering process that creates a lithium atmosphere on the bottom surface and facilitates lithium replenishment, an additional tunnel was introduced between the specimen and the alumina powder, allowing the bottom surface of the specimen to be exposed to the lithium atmosphere. By manufacturing a uniform cubic electrolyte, the path to manufacturing all-solid-state batteries was opened. These findings provide a new approach to forming cubic-phase LLZO with much higher ionic conductivity than the tetragonal phase at low sintering temperatures. [ABSTRACT FROM AUTHOR]

Despite the variety of solid electrolytes available, no single solid electrolyte has been found that meets all the requirements of the successor technology of lithium-ion batteries in an optimum way. However, composite hybrid electrolytes that combine the desired properties such as high ionic conductivity or stability against lithium are promising. The addition of conductive oxide fillers to sulfide solid electrolytes has been reported to increase ionic conductivity and improve stability relative to the individual electrolytes, but the influence of the mixing process to create composite electrolytes has not been investigated. Here, we investigate Li3PS4 (LPS) and Li7La3Zr2O12 (LLZO) composite electrolytes using electrochemical impedance spectroscopy and distribution of relaxation times. The distinction between sulfide bulk and grain boundary polarization processes is possible with the methods used at temperatures below 10 °C. We propose lithium transport through the space-charge layer within the sulfide electrolyte, which increases the conductivity. With increasing mixing intensities in a high-energy ball mill, we show an overlay of the enhanced lithium-ion transport with the structural change of the sulfide matrix component, which increases the ionic conductivity of LPS from 4.1 × 10−5 S cm−1 to 1.7 × 10−4 S cm−1. [ABSTRACT FROM AUTHOR]

The increasing adoption of additive manufacturing (AM), also known as 3D printing, is revolutionizing the production of wearable electronics and energy storage devices (ESD) such as batteries, supercapacitors, and fuel cells. This surge can be attributed to its outstanding process versatility, precise control over geometrical aspects, and potential to reduce costs and material waste. In this comprehensive review, major AM processes like inkjet printing, direct ink writing, fused deposition modeling, and selective laser sintering/melting along with possible configurations and architectures, are elaborately discussed for each bespoke ESD. The application of 3D‐printed energy storage devices in wearable electronics, Internet of Things (IoT)‐based devices, and electric vehicles are also mentioned in the review. The role of AM in facilitating the production of solid‐state batteries has also revolutionized the electric vehicle (EV) industry. Recent progress in the field of AM of energy systems with solid electrolytes and potential future directions such as 4D printing to incorporate stimuli‐responsive behavior in 3D‐printed materials, biomimetic design optimization, and additive manufacturing of ESD in a micro‐gravity environment have also been highlighted. Extensive research and continuous progress in this field are expected to enhance the longetivity, industrial scalability, and electrochemical performance of 3D‐printed energy storage devices in future. [ABSTRACT FROM AUTHOR]

Solid‐state lithium metal batteries (SSLMBs) offer numerous advantages in terms of safety and theoretical specific energy density. However, their main components namely lithium metal anode, solid‐state electrolyte, and cathode, show chemical instability when exposed to humid air, which results in low capacities and poor cycling stability. Recent studies have shown that bioinspired hydrophobic materials with low specific surface energies can protect battery components from corrosion caused by humid air. Air‐stable inorganic materials that densely cover the surface of battery components can also provide protection, which improves the storage stability of the battery components, broadens their processing conditions, and ultimately decreases their processing costs while enhancing their safety. In this review, the mechanism behind the surface structural degradation of battery components and the resulting consequences are discussed. Subsequently, recent strategies are reviewed to address this issue from the perspectives of lithium metal anodes, solid‐state electrolytes, and cathodes. Finally, a brief conclusion is provided on the current strategies and fabrication suggestions for future safe air‐stable SSLMBs. [ABSTRACT FROM AUTHOR]