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All-solid-state batteries show great promise as next-generation batteries with high safety, high power, and long life. In addition to high-performance active electrode materials and solid electrolytes, the properties of the electrode–electrolyte interface and the morphology of the electrode layer are important for the development of high-performanc...
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... 8)10) Thin-film batteries consist of a positive elec- trode, a negative electrode, and solid electrolyte films. The composite electrodes used in bulk-type batteries consist of an active material and solid electrolyte particles, with a solid electrolyte separator layer sandwiched between the positive and negative composite electrodes as shown in Fig. 2. Solid electrolyte particles are blended into the electrode layer to form lithium-ion conducting pathways and increase the contact area between the electrode and electrolyte. 9) The incorporation of particles of the active electrode material particles in the electrode layer can increase the battery capacity. Thus, bulk-type batteries ...
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... batteries are roughly classified into two categories: thin film batteries 4)?7) and bulk-type batter- ies. 8)?10) Thin-film batteries consist of a positive elec- trode, a negative electrode, and solid electrolyte films. The composite electrodes used in bulk-type batteries consist of an active material and solid electrolyte particles, with a solid electrolyte separator layer sandwiched between the positive and negative composite electrodes as shown in Fig. 2. Solid electrolyte particles are blended into the electrode layer to form lithium-ion conducting pathways and increase the contact area between the electrode and electrolyte. 9) The incorporation of particles of the active electrode material particles in the electrode layer can increase the battery capacity. Thus, bulk-type batteries are more suitable for large-scale ...
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... [14][15][16] In an ideal cathode, the porosity is minimized, the CAM content is maximized (it is the only constituent storing charge), and the ISE is distributed homogeneously forming low resistance charge transport pathways. 12,13,17 This means that the cathode microstructure must conduct ions and electrons and provide a large interfacial contact area between ISE and CAM to ensure rapid transfer of lithium during charging and discharging. 12 However, charge transport pathways are often tortuous and charge carriers must travel longer distances than one might initially assume based on the geometric dimensions. ...
The kinetics of composite cathodes for solid-state batteries (SSBs) relies heavily on their microstructure. Spatial distribution of the different phases, porosity, interface areas, and tortuosity factors are important descriptors that need accurate quantification for models to predict the electrochemistry and mechanics of SSBs. In this study, high-resolution focused ion beam-scanning electron microscopy tomography was used to investigate the microstructure of cathodes composed of a nickel-rich cathode active material (NCM) and a thiophosphate-based inorganic solid electrolyte (ISE). The influence of the ISE particle size on the microstructure of the cathode was visualized by 3D reconstruction and charge transport simulation. By comparison of experimentally determined and simulated conductivities of composite cathodes with different ISE particle sizes, the electrode charge transport kinetics is evaluated. Porosity is shown to have a major influence on the cell kinetics and the evaluation of the active mass of electrochemically active particles reveals a higher fraction of connected NCM particles in electrode composites utilizing smaller ISE particles. The results highlight the importance of homogeneous and optimized microstructures for high performance SSBs, securing fast ion and electron transport.
... Moreover, in contrast to conventional LIBs multilayer pouch cells in bipolar order could be realized for SSBs under the achievement of an enhanced energy density and a reduction of necessary contacting of the current collectors. [145,146] According to Jung et al., the current collector acts both as positive and negative pole, unit cells do not have to be packed and sealed individually and cell modules can be achieved by sequentially stacking or laminating of the cathode, current collector, anode and separator without external wiring. [146] While this publication is limited to sulfidic SEs and focuses on the process engineering implementation of the steps from synthesis to calendering, the works of Schnell et al., [1] Duffner et al. [147] and Tan et al. [148] are recommended for the study of alternative SSB concepts, as well as economic perspectives. ...
Solid‐state batteries possess the potential to combine increased energy densities, high voltages, as well as safe operation and therefore are considered the future technology for electrical energy storage. In particular, sulfides as solid electrolyte are promising candidates due to their high ionic conductivities and the possibility of a scalable production. This review aims to demonstrate ways to manufacture suspension‐based sulfidic solid‐state batteries both on a laboratory scale and on an industrial level, focusing on the assessment of current knowledge and its discussion from a process engineering point of view. In addition to the influence of process parameters during mechanochemical synthesis of the solid electrolyte, formulation strategies for electrodes and separators are presented. The process chain from dispersion to cell assembly is evaluated. Scale‐up technologies are considered in comparison to established techniques in the field of conventional lithium‐ion batteries with liquid electrolyte summarizing the current status of sulfidic solid‐state battery production.
... [1] Among basic routes of ASSBs, sulfide solid electrolyte (SE) is widely recognized as the most promising one due to its high ionic conductivity [2][3][4] and favorable deformability. [5] Aiming to bridge the great gap between lab-scale fabrication and industrial large-scale production of sulfide-based ASSBs, the mass production of sulfide solid electrolytes is one of the most overwhelming issues. High-temperature solid state reaction [2][3][4] and mechanochemical method [6][7][8] are typical conventional solidphase synthesis methods of sulfide solid electrolytes with relatively high-energy cost in high-temperature heat treatment process [2][3][4][9][10][11] and high-energy ball milling process. ...
Sulfide solid electrolytes are widely regarded as one of the most promising technical routes to realize all-solid-state batteries (ASSBs) due to their high ionic conductivity and favorable deformability. However, the relatively high price of the crucial starting material, Li 2 S, results in high costs of sulfide solid electrolytes, limiting their practical application in ASSBs. To solve this problem, we develop a new synthesis route of Li 2 S via liquid-phase synthesis method, employing lithium and biphenyl in 1, 2-dimethoxyethane (DME) ether solvent to form a lithium solution as the lithium precursor. Because of the comparatively strong reducibility of the lithium solution, its reaction with sulfur proceeds effectively even at room temperature. This new synthesis route of Li 2 S starts with cheap precursors of lithium, sulfur, biphenyl and DME solvent, and the only remaining byproduct (DME solution of biphenyl) after the collection of Li 2 S product can be recycled and reused. Besides, the reaction can proceed effectively at room temperature with mild condition, reducing energy cost to a great extent. The as-synthesized Li 2 S owns uniform and extremely small particle size, proved to be feasible in synthesizing sulfide solid electrolytes (such as the solid-state synthesis of Li 6 PS 5 Cl). Spontaneously, this lithium solution can be directly employed in the synthesis of Li 3 PS 4 solid electrolytes via liquid-phase synthesis method, in which the centrifugation and heat treatment processes of Li 2 S are not necessary, providing simplified production process. The as-synthesized Li 3 PS 4 exhibits typical Li ⁺ conductivity of 1.85×10 ⁻⁴ S⋅cm ⁻¹ at 30 °C.
... However, by replacing electrolyte solutions with a solid superionic conductor, an all-solid-state battery that does not exhibit the problems associated with liquid electrolytes can be obtained. Improved safety, wide operating temperature ranges, and high energy density are the advantages of solid electrolytes [1,2]. ...
The formation phenomena of silver carbonate (Ag2CO3)–silver iodide (AgI) solid solutions were investigated by X-ray diffraction, thermogravimetry-differential thermal analysis, and electrical conductivity measurement. Results revealed that AgI and Ag2CO3 reacted with each other when mixed at room temperature. The reaction products were classified into three types: (1) AgI-based solid solutions in the AgI-rich region for x = 10% or less in x Ag2CO3–(1 − x) AgI; (2) Ag2CO3-based solid solutions in the Ag2CO3-rich region for x = 60% or more; and (3) silver carbonate iodides in the intermediate range for x between 10% and 60%. For the AgI-based solid solutions, the incorporation of Ag2CO3 into the AgI lattice expanded the unit cell and enhanced electrical conductivity. The solubility limit of Ag2CO3 into the AgI lattice estimated from the differential thermal analysis was x ≈ 5%.
... As an example, the sulfide glass electrolyte 0.75Li 2 S-0.25P 2 S 5 (LPS) has a porosity of about 8% after room-temperature pressing at 360 MPa [9] . Secondly, manufacturing a homogeneous composite electrode with favorable Li-ion pathways is a technological challenge [15] . Thirdly, ensuring the mechanical integrity of the fabricated cell and preserving it during operation where active materials can and will change their volume [ 16 , 17 ] is probably the most serious issue. ...
A suite of bulk and surface analytical techniques was applied to shed light on the factors limiting fast cycling of composite graphite electrodes in all-solid-state cells based on sulfide electrolytes 0.75Li2S-0.25P2S5 (LPS) and 0.3LiI-0.7(0.75Li2S-0.25P2S5). Cracks in the composite electrodes and poor percolation of the ionic conducting particles were identified by both scanning electron microscopy and X-ray tomography and the slow kinetics during lithiation (limiting practical specific charge at rates >C/10, at geometrical current densities >120 μA cm⁻²) was monitored by operando X-ray diffraction and supported by Raman microscopy. Operando X-ray photoelectron spectroscopy and X-ray absorption spectroscopy detected the formation of Li2S and LixP at the interface between LPS and graphite, both compounds increasing the interfacial resistance. Despite the kinetic limitations, excellent long-term cycling performance is demonstrated at C/20 rate (at current density of about 60 μA cm⁻²), revealing slow self-passivation processes at the sulfide/graphite interface which stabilizes after approximately 200 full cycles.
... As another alternative, all-solid-state batteries (ASSBs) with lithium [6][7][8][9][10][11][12][13] or sodium [14][15][16][17] as the guest ion have been proposed. ASSBs include an oxide solid electrolyte with a higher Young's modulus than that of a sulphide solid electrolyte; as a result, it is difficult to reduce the interface resistance by pressure moulding alone 17 . ...
An all-solid-state battery (ASSB) with a new structure based on glass-ceramic that forms Na2FeP2O7 (NFP) crystals, which functions as an active cathode material, is fabricated by integrating it with a β″-alumina solid electrolyte. Two important factors that influence the rate capability of this ASSB were optimised. First, the particle size of the precursor glass powder from which the NFP crystals are formed was decreased. Consequently, the onset temperature of crystallisation shifts to a lower temperature, which enables the softening of NFP crystals and their integration with β″-alumina at a low temperature, without the interdiffusion of different crystal phases or atoms. Second, the interface between the β″-alumina solid electrolyte and cathode active materials which consisted of the NFP-crystallised glass and acetylene black used as a conductive additive, is increased to increase the insertion/release of ions and electrons from the active material during charge/discharge processes. Thus, the internal resistance of the battery is reduced considerably to 120 Ω. Thus, an ASSB capable of rapid charge/discharge that can operate not only at room temperature (30 °C) but also at −20 °C is obtained. This technology is an innovative breakthrough in oxide-based ASSBs, considering that the internal resistance of liquid electrolyte-based Li-ion batteries and sulphide-based ASSBs is ~10 Ω.
... Kanno reported the development of high-power all-solid-state batteries using sulfide-based solid electrolytes [8]. Since his results were reported, research in this area has developed rapidly [121][122][123]. The possibility of realizing high-power, all-solid-state batteries by 2030 has been raised [124]. ...
... The process is performed with a dry mixing and pressing method. Planar Al and Cu foils used in conventional liquid LIBs are used as CCs for cathodes and anodes [121]. On the other hand, to decrease the contact resistance between the CC and cathode or anode active materials, CNT sheets can be fabricated as CCs and placed between the active materials and battery case materials (Figure 14), resulting in a reversible capacity and high-rate discharge performance in the resulting all-solid-state LIBs [129]. ...
Current collectors (CCs) are an important and indispensable constituent of lithium-ion batteries (LIBs) and other batteries. CCs serve a vital bridge function in supporting active materials such as cathode and anode materials, binders, and conductive additives, as well as electrochemically connecting the overall structure of anodes and cathodes with an external circuit. Recently, various factors of CCs such as the thickness, hardness, compositions, coating layers, and structures have been modified to improve aspects of battery performance such as the charge/discharge cyclability, energy density, and the rate performance of a cell. In this paper, the details of interesting and useful attempts of preparing CCs for high battery performance in lithium-ion and post-lithium-ion batteries are reviewed. The advantages and disadvantages of these attempts are discussed.
... Schematic structure of a solid-state battery.(Source:[20]) ...
Plug-in electric vehicles (PEVs) play a significant role in the development of green cities since they generate less pollution than conventional vehicles. To promote PEV adoption and mitigate range anxiety, charging infrastructure should be deployed at strategic locations that are readily accessible to the public. Nebraska is working on the expansion of charging infrastructure around the state; however, stakeholders face several difficulties in trying to minimize irregular charging behaviors. Most electric vehicle users plug in and leave their vehicles for an extended time at public parking lots designated for PEVs. Some users even leave their vehicles for longer than 24 hours. Prolonged idle time is a concern for other PEV users who need to charge their vehicles to complete their planned trip. This thesis proposes several well-known regression methods to predict the idle time to help policymakers minimize the impact of irregular charging behaviors. In addition, PEV user charging behavior has a significant influence on the distribution network and its reliability. In addition, to increase efficiency in management of the electric grid, this thesis also proposes several well-known regression methods to predict the energy consumption of a charging session. The performance of different regression methods for predicting the idle time as well as energy consumption are characterized using established statistical metrics. Adviser: Mahmoud Alahmad
... Kato et al. have produced a solid state battery with 15.7 mAh cm −2 at room temperature using a cathode layer with a thickness of 600 µm, which is more than twice the maximum thickness in our study [17]. Currently, most solid state battery prototypes use thinner composite electrodes to compensate for the lower ionic conductivity of the electrode material and the absence of electrolytes wetting the electrode [18]. ...
The electrolyte is one of the three essential constituents of a Lithium-Ion battery (LiB) in addition to the anode and cathode. During increasingly high power and high current charging and discharging, the requirement for the electrolyte becomes more strict. Solid State Electrolyte (SSE) sees its niche for high power applications due to its ability to suppress concentration polarization and otherwise stable properties also related to safety. During high power and high current cycling, heat management becomes more important and thermal conductivity measurements are needed. In this work, thermal conductivity was measured for three types of solid state electrolytes: Li 7 La 3 Zr 2 O 12 (LLZO), Li 1 . 5 Al 0 . 5 Ge 1 . 5 (PO 4 ) 3 (LAGP), and Li 1 . 3 Al 0 . 3 Ti 1 . 7 (PO 4 ) 3 (LATP) at different compaction pressures. LAGP and LATP were measured after sintering, and LLZO was measured before and after sintering the sample material. Thermal conductivity for the sintered electrolytes was measured to 0.470 ± 0.009 WK - 1 m - 1 , 0.5 ± 0.2 WK - 1 m - 1 and 0.49 ± 0.02 WK - 1 m - 1 for LLZO, LAGP, and LATP respectively. Before sintering, LLZO showed a thermal conductivity of 0.22 ± 0.02 WK - 1 m - 1 . An analytical temperature distribution model for a battery stack of 24 cells shows temperature differences between battery center and edge of 1–2 K for standard liquid electrolytes and 7–9 K for solid state electrolytes, both at the same C-rate of four.
... Among various SSLBs, inorganic sulfide solid electrolyte-based SSLBs demonstrate strong competitiveness stemming from its high ionic conductivities and favorable mechanical properties [5][6][7][8]. However, constructing homogeneous contacts within the composite electrode and the electrode/electrolyte interface via simple mixing and cold-pressing processes is still challenging [9][10][11]. Inconsistent reactions resulted from the formation of non-uniform contact/ interfaces could cause significant degradation in the cycle performance and energy density [12][13][14][15]. ...
Solid-state lithium batteries (SSLBs) exhibit numerous advantages including high safety, high energy density，and power density, etc., and therefore become the most promising candidate for next-generation batteries. However, constructing an intimate contact within the composite electrode and the electrode/electrolyte interface via simple mixing and cold-pressing processes is still challenging. Herein, a novel fabrication process for homogeneous composite electrodes used in SSLBs is successfully demonstrated. An in-situ liquid-phase approach employing the [Li(triglyme)]+[TFSI]- (LiG3) solvent-salt complex with excellent stability to modify the sulfide-based solid-state electrolyte interfaces, is introduced into the SSLBs system, which enables SSLBs to work efficiently at lower external pressures. The quasi-solid-state prototype cells with Li4Ti5O12 (LTO) active material deliver excellent room-temperature performance, generating a super high capacity of 160 mAh g-1 and high capacity retention of 91.4% for 1500 cycles under 0.25 C. This work gives new insight into the interface engineering, processing and more positive impact on the industrial production of SSLBs.
