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All-solid-state batteries with inorganic solid electrolytes are recognized as an ultimate goal of rechargeable batteries because of their high safety, versatile geometry and good cycle life. Compared to thin-film batteries, increasing the reversible capacity of bulk-type all-solid-state batteries using electrode active material particles is difficu...
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Although solid-state lithium (Li) batteries theoretically have higher energy density and better safety than organic solvent-based Li-ion batteries, they currently suffer from problems such as poor power density and rapid performance degradation, hindering their wide applications. The cause of these problems can be largely related to the electrode m...
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... All-solid-state lithium batteries are promising energy storage solutions, offering high safety standards, impressive output capabilities, and enhanced energy densities [1,2]. Despite these advantages, challenges specific to solid electrolytes, absent in liquid counterparts, have emerged. ...
All-solid-state batteries are typically manufactured under high pressure to decrease the resistance of the solid interface. However, until now, there has been a lack of research concerning changes in the structure of solid electrolytes owing to pressurization. Our study addresses this gap by exploring the structural modifications of the sulfide solid electrolyte Li3PS4 under high-pressure conditions. We observed a tendency for PS4 molecules to converge upon each other in both β-Li3PS4 and g-Li3PS4 crystals when subjected to a pressure of 100 MPa. In g-Li3PS4, X-ray scattering and pair distribution function analyses following pressure application and subsequent return to ambient conditions remained consistent with pre-compression measurements. Conversely, in β-Li3PS4 crystals, post-pressure X-ray scattering differed from pre-compression measurements, suggesting pressure-induced atomic rearrangement within the crystal lattice. This underscores the importance of accounting for pressure-induced structural changes, especially in computational simulation studies where crystal structures are often assumed to remain static pre- and post-pressurization. Our findings demonstrate that under high pressure, the crystal structure of Li3PS4 slightly changes by approximately 1~2%, rendering it a viable candidate for utilization as a solid electrolyte in all-solid-state batteries.
... Additionally, Na2S is a necessary precursor for solid-state electrolytes, which might make using a sodium-metal anode safe. Na2S is also a handy reagent for making a variety of specialized chemicals, such as metal-sulfide compounds and polymers incorporating sulfides [12]. Finally, Na2S has drawn interest as a "rapid-release" donor of H2S in aqueous solutions, a vital gasotransmitter that may be used to treat a variety of illnesses, including neurological and cardiovascular conditions. ...
This study was conducted to check the possibility of hydrogen sulfide as a material to produce sodium sulphide. It is a harmful substance that is released during production in many industrial production processes. In laboratory and semi-industrial conditions, the possibility of producing hydrogen sulfide using associated acid gases from hydrocarbon production as raw materials has been established. The resulting purified hydrogen sulfide, absorbed by a solution of sodium hydroxide, is a promising raw material in the production of sodium sulfide. The experiments on the production of sodium sulfide from natural gas processing waste, which contains hydrogen sulfide, showed the promise of using the proposed method. A new method and technology for the production of sodium sulfide has been developed, while the cost of the resulting product has been reduced due to the available local cheap raw materials, widely used in the chemical and mining industries and the simplification of the technological scheme and equipment used. Due to the developed method for the production of Na2S, it is possible to utilize a large number of waste gases from hydrocarbon production, as a result of which both environmental problems of the regions are solved, and it is also possible to obtain a product with great economic profitability.
... 1 In particular, all-solid-state Li batteries are a promising next-generation technology because of their high energy density and safety. [2][3][4][5] Solid electrolytes (SEs) play an important role in this system. Sulfide-based SEs that have been actively researched and developed, such as Li 10 GeP 2 S 12 and Li 6 PS5X (X = Cl, Br), have a high Li-ion conductivity equivalent to or superior to that of organic electrolytes, along with excellent formability. ...
The Li-ion conductivities of Li3InCl6 (LIC), which is a promising chloride solid electrolyte, and its compositional derivatives, Nb5+- and Zr4+-doped LIC, i.e., Li3−2xIn1−xNbxCl6 and Li3−yIn1−yZryCl6, respectively, were experimentally and computationally investigated. An increase in the ionic conductivity caused by Nb5+ or Zr4+ doping, which was due to the increase in Li vacancies, was observed in both the experimental and computational results. Nb5+ doping yielded a larger increase in conductivity at 60 °C. First-principles molecular dynamics studies indicated two factors affecting the Li-ion conductivity under doping with higher-valent ions: (1) the vacancy trapping effect and (2) the reduction in the phase-transition temperature from a Li/vacancy ordered structure to a disordered structure. In particular, in factor (2), the effect of Nb5+ doping is larger than that of Zr4+ doping, which supports the improvement in ionic conductivity at 333 K in the experiment.
... Alternatively, the sol-gel method can be employed to prepare oxide solid-state electrolytes with higher density and improved composition uniformity [85][86][87]. For sulfide solid-state electrolytes, the production process is similar to that of oxide solid-state electrolytes, but the controlled inert atmosphere is typically required due to their sensitivity to air [88]. Additionally, thin-film processing techniques such as pulsed laser deposition [89], atomic layer deposition [90], and sputter deposition [91] can also be employed to manufacture sulfide solid-state electrolyte with crystallization. ...
High-capacity Li-rich oxide materials have received extensive attention due to their unique anion–cation charge compensation involvement. However, the high operating voltage, poor cycling performance, unsafe oxygen evolution, and voltage decay limit their industrial application. The emergence and development of solid-state batteries offer a great opportunity to solve these issues by replacing flammable and unstable liquid electrolytes with solid electrolytes. Meanwhile, utilization of high-capacity Li-rich oxide cathodes enables to establish high-energy-density solid-state batteries with wide voltage ranges, light weight, and high mechanical properties. This review summarizes the recent progress of Li-rich oxide materials and solid electrolytes, emphasizing their major advantages, interface challenges, and modification approaches in the development of Li-rich solid-state batteries. We also propose possible characterization strategies for effective interfacial observation and analyses. It is hoped that this review should inspire the rational design and development of better solid-state batteries for application in portable devices, electric vehicles, as well as power grids.
... Among all the types of solid electrolytes, sulfide solid electrolytes meet the demand of high conductivity and excellent surface contacts because of the presence of sulfide-based anion groups and softness. [1][2][3][4] The early low-temperature phase of Na 3 PS 4 with a conductivity of 10 −6 S cm −1 was announced in 1992. 5 In 2012, Hayashi et al. improved the cubic Na 3 PS 4 crystal glassceramic electrolyte with the conductivity of 0.2 mS cm −1 . ...
Solid Na‐ion‐conducting sulfides exhibited potential applications for commercial solid‐state rechargeable batteries because of their low cost and good contact with the electrode. In the present work, a sulfide sodium‐ion conductor 2Na3SbS4·Na2WS4 with a conductivity of 1.55 mS cm⁻¹ was obtained, which was identified as superior to the 2Na3SbS4·Na4XS4 (X = Si, Ge, Sn) systems. Further exploration of the heat treatment to improve the crystallinity of the glass resulted in a high conductivity of 1.9 mS cm⁻¹ and low activation energy of 0.24 eV for the 2Na3SbS4·Na2WS4 glass–ceramic electrolyte. The high crystallinity after heat treatment at 380°C facilitated the migration of Na⁺ together with large sodium vacancies formed by doping with W⁶⁺ in 2Na3SbS4·Na2WS4 glass–ceramic electrolyte, resulting in the improved electrochemical performance. In addition, the air stability of the 2Na3SbS4·Na2WS4 glass–ceramic electrolyte decreased monotonically with increase of the annealing temperature, and heat application at 380°C effectively improved the electrolyte tolerance to the air compared with pure Na3PS4 electrolyte. The origins of aliovalent ion doping and thermal effect on the electrochemical performance were discussed in detail.
... [4][5][6][7][8][9] For sulfide-based Na-ion SEs, exceptional ionic conductivity ranging from 2 x 10 -4 S cm -1 to 3 x 10 -2 S cm -1 has been achieved in Na 3 PnX 4 -type (Pn = P, Sb, W; X = S, Se) and Na 11 Sn 2 PnX 12 -type (Pn = P, Sb; X = S, Se) structures. [10][11][12][13][14][15][16] Nevertheless, unlike their Li-ion counterparts, the absence of effective Na-ion coatings hinders the formation of favorable interfaces between sulfide SEs and typical layered oxide or polyanion-type cathodes in ASSNIBs, thus limiting their practical applications. [17][18][19] In comparison, while halide-based Na-ion solid electrolytes (SEs) offer favorable mechanical flexibility and a broad electrochemical stability window, their limited Na-ion migration hampers the practical utilization. ...
... Powder pressing is classified into two types: (i) cold pressing and (ii) hot pressing [51]. Cold pressing techniques are broadly used that unambiguously influence the porosity of the materials [52]. J. M Doux et al. studied the pressure impacts on the sulfide-based electrodes and reported that high pressure about 370 MPa greatly improved overall cell performance whereas stack pressure does not expose key bearing on the cyclability [53]. ...
Conventional design of all-solid-state battery limits the portable device fabrication due to sluggish interfacial contact, safety, and high manufacturing cost. Additionally, unfavorable Li-dendrite formation and low coulombic efficiency hinder the further use. This will lead to low energy density that cannot satisfy current energy demand for the potential applications. Geometry evolution is one choice to address these challenges where we switch one dimensional to different dimensional, based on our demand. New full cell geometry will play vital role in achieving great contact between the electrode and electrolyte. Recently, the full cell geometry has shown great attraction starting from thin-film design to 3D geometry. In this chapter, we centered the conventional batteries merits and demerits. Also, we described the materials compatibility, electrode–electrolyte interface, and conventional battery design strategies. Followed, this chapter summarized the recent advances and critical challenges on the full cell geometry design which are presented with discussion with respect to interfacial interactions and ionic conductivity improvements for all-solid-state batteries.
... All-solid-state lithium-ion batteries (ASSLIBs) have attracted considerable attention as next-generation batteries owing to their excellent properties, such as high energy and high power densities, as well as high safety [1,2,3]. In ASSLIBs, a non-flammable solid electrolyte (SE) is used instead of the flammable liquid electrolyte of conventional lithium-ion batteries, resulting in a much lower risk of accidents like electrolyte leakage and explosion [4,5,6]. ...
All-solid-state lithium-ion batteries (ASSLIBs) are promising candidates for next-generation batteries because of their various attractive properties. The uniform mixing of active materials (AMs) and solid electrolytes (SEs) is important for high-performance ASSLIBs. However, most AMs and SEs have poor flowability owing to their small particle size, which makes it difficult to uniformly mix the AM and SE particles. This study is focused on a high-shear mixer (HSM) as a scalable method to uniformly mix the AM and SE particles. The objective of this study is to determine the optimal operating conditions for HSM and its effectiveness in AM-SE mixing. The higher rotating speed of the chopper caused uniform SE dispersion by deagglomerating the SE particles and improving the adhesion of SE onto the AM particles, affording an electrode with well-balanced electrical/ionic conductivity and lower internal resistance. The ASSLIB with this electrode exhibited lower electrode polarization and excellent rate and cycle performance. Additionally, it has been demonstrated that the HSM could lead to a more uniform SE dispersion than conventional lab-scale mixing methods, resulting in significantly improved battery performance. Moreover, insights into the process-homogeneity-performance relations have been obtained.
... r e s u m e n En el presente trabajo, el electrolito sólido de sulfuro argirodita Li 6 PS 5 Cl se prepara mediante un proceso en fase líquida, que consta de 2 pasos: 1) suspensión-reacción bajo radiación ultrasónica de los precursores de Li 2 S, P 2 S 5 y LiCl en acetonitrilo, y 2) disoluciónprecipitación que involucra la adición de etanol/acetonitrilo y eliminación de disolventes a 180 • C. También se estudia el efecto de la adición de un surfactante no iónico sobre las propiedades del electrolito sólido de sulfuro. El proceso de síntesis permite obtener electrolito sólido Li 6 PS 5 Cl con alta conductividad iónica de 2,0 × 10 -4 S cm -1 , baja energía Introduction All-solid-state batteries based on sulfide solid electrolytes are actively investigated because sulfide solid electrolytes have high ionic conductivity (10 −2 -10 −4 S cm −1 ) and form low interfacial electrode-electrolyte resistance by simple cold pressure procedure [1,2]. The sulfide solid electrolytes have been commonly prepared by mechanical milling and high-temperature solid-state synthesis [2]. ...
... El proceso de síntesis permite obtener electrolito sólido Li 6 PS 5 Cl con alta conductividad iónica de 2,0 × 10 -4 S cm -1 , baja energía Introduction All-solid-state batteries based on sulfide solid electrolytes are actively investigated because sulfide solid electrolytes have high ionic conductivity (10 −2 -10 −4 S cm −1 ) and form low interfacial electrode-electrolyte resistance by simple cold pressure procedure [1,2]. The sulfide solid electrolytes have been commonly prepared by mechanical milling and high-temperature solid-state synthesis [2]. Recently, the liquid phase syntheses [3,4] have attracted much attention as a versatile chemical route to prepare sulfide solid electrolytes since this is considered more practical from a mass-produce point of view through reducing processing time and thermal treatments. ...
In the present work, argyrodite Li6PS5Cl sulfide solid electrolyte is prepared by a liquid phase process, consisting of two steps: (1) suspension-reaction under the ultrasonication of Li2S, P2S5, and LiCl precursors in acetonitrile and, (2) dissolution-precipitation involving the addition of ethanol/acetonitrile and solvents removal by heating at 180 °C. The effect of the addition of a nonionic surfactant on the properties of the sulfide solid electrolyte is also studied. The synthesis process allows to obtain Li6PS5Cl argyrodite solid electrolyte with high ionic conductivity of 2.0 × 10⁻⁴ S cm⁻¹, the low activation energy of 0.22 eV, and electrochemical stability up to 5 V (vs. Li). A regular particle distribution with a size smaller than 1 μm is obtained by the addition of the surfactant.
... Due to the inherently narrow electrochemical stability window, many sulfide SSEs decompose spontaneously simply by contacting a Li-metal anode [19]. Several efforts have been made to evaluate Li-metal/sulfide-SSE interfaces both theoretically and experimentally [18,50,[56][57][58][59][60][61][62][63][64][65][66][67]. The interfaces formed between Li metal and the SSE can be classified into the following three types [68]. ...
All-solid-state batteries have emerged as promising alternatives to conventional Li-ion batteries owing to their higher energy density and safety, which stem from their use of inorganic solid-state electrolytes instead of flammable organic liquid electrolytes. Among various candidates, sulfide solid-state electrolytes are particularly promising for the development of high-energy all-solid-state Li metal batteries because of their high ionic conductivity and deformability. However, a significant challenge remains as their inherent instability in contact with electrodes forms unstable interfaces and interphases, leading to degradation of the battery performance. In this review article, we provide an overview of the key issues for the interfaces and interphases of sulfide solid-state electrolyte systems as well as recent progress in understanding such interface and interphase formation and potential solutions to stabilize them. In addition, we provide perspectives on future research directions in this field.
