• Ceramist
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• v.22 no.2
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• pp.170-181
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• 2019

All-solid-state batteries have received increasing attention because of their high safety aspect and high energy and power densities. However, the inferior solid-solid interfaces between solid electrolyte and active materials in electrode, which cause high interfacial resistance, reduce ion and electron transfer rate and limit battery performance. Recently, spark plasma sintering is emerging as a promising technique for fabricating solid electrolytes and composite-electrodes. Herein, this paper focuses on the overview of spark plasma sintering to fabricate solid electrolytes and composite-electrodes for all-solid-state batteries. In the end, future opportunities and challenges associated with SPS technique for all-solid-state batteries are described.

• Journal of the Korean Electrochemical Society
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• v.22 no.3
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• pp.87-103
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• 2019

Nonaqueous organic electrolyte solution in commercially available lithium-ion batteries, due to its flammability, corrosiveness, high volatility, and thermal instability, is demanding to be substituted by safer solid electrolyte with higher cycle stability, which will be utilized effectively in large-scale power sources such as electric vehicles and energy storage system. Of various types of solid electrolytes, composite solid electrolytes with polymer matrix and active inorganic fillers are now most promising in achieving higher ionic conductivity and excellent interface contact. In this review, some kinds and brief history of solid electrolyte are at first introduced and consequent explanations of polymer solid electrolytes and inorganic solid electrolytes (including active and inactive fillers) are comprehensively carried out. Composite solid electrolytes including these polymer and inorganic materials are also described with their electrochemical properties in terms of filler shapes, such as particle (0D), fiber (1D), plane (2D), and solid body (3D). In particular, in all-solid-state lithium batteries using lithium metal anode, the interface characteristics are discussed in terms of cathode-electrolyte interface, anode-electrolyte interface, and interparticle interface. Finally, current requisites and future perspectives for the composite solid electrolytes are suggested by help of some decent reviews recently reported.

• Korean Journal of Materials Research
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• v.18 no.9
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• pp.470-474
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• 2008

Composites of gadolinium-doped ceria/magnesia(CGO/MgO) were synthesized and characterized for the electrolytes of intermediate temperature solid oxide fuel cells. XRD and SEM results revealed that composite electrolytes consisted of their own phases after sintering at $1400^{\circ}C$ without noticeable solid solution of Mg into CGO. As the MgO content increased, the total electrical conductivity decreased, which might be attributed to the decrease of grain boundary conductivity, possibly due to the lowering of the continuity of the CGO grains and blocking effects of the insulating MgO phase. The space charge effect may not be a significant factor to affect the electrical conductivity of the CGO/MgO composites.

• ETRI Journal
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• v.42 no.1
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• pp.129-137
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• 2020

All-solid-state batteries are promising energy storage devices in which high-energy-density and superior safety can be obtained by efficient cell design and the use of nonflammable solid electrolytes, respectively. This paper presents a systematic study of experimental factors that affect the electrochemical performance of all-solid-state batteries. The morphological changes in composite electrodes fabricated using different mixing speeds are carefully observed, and the corresponding electrochemical performances are evaluated in symmetric cell and half-cell configurations. We also investigate the effect of the composite electrode thickness at different charge/discharge rates for the realization of all-solid-state batteries with high-energy-density. The results of this investigation confirm a consistent relationship between the cell capacity and the ionic resistance within the composite electrodes. Finally, a concentration-gradient composite electrode design is presented for enhanced power density in thick composite electrodes; it provides a promising route to improving the cell performance simply by composite electrode design.

• Electronics and Telecommunications Trends
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• v.36 no.3
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• pp.76-86
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• 2021

Technologies for lithium secondary batteries are now increasingly expanding to simultaneously improve the safety and higher energy and power densities of large-scale battery systems, such as electric vehicles and smart-grid energy storage systems. Next-generation lithium batteries, such as lithium-sulfur (Li-S) and lithium-air (Li-O₂) batteries by adopting solid electrolytes and lithium metal anode, can be a solution for the requirements. In this analysis of battery technology trends, solid electrolytes, including polymer (organic), inorganic (oxides and sulfides), and their hybrid (composite) are focused to describe the electrochemical performance achievable by adopting optimal components and discussing the interfacial behaviors that occurred by the contact of different ingredients for safe and high-energy lithium secondary battery systems. As next-generation rechargeable lithium batteries, Li-S and Li-O₂ battery systems are briefly discussed coupling with the possible use of solid electrolytes. In addition, Electronics and Telecommunications Research Institutes achievements in the field of solid electrolytes for lithium rechargeable batteries are finally introduced.

• Korean Journal of Materials Research
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• v.32 no.10
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• pp.429-434
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• 2022

There is ongoing research to develop lithium ion batteries as sustainable energy sources. Because of safety problems, solid state batteries, where electrolytes are replaced with solids, are attracting attention. Sulfide electrolytes, with a high ion conductivity of 10^-3 S/cm or more, have the highest potential performance, but the price of the main materials is high. This study investigated lithium hydride materials, which offer economic advantages and low density. To analyze the change in ion conductivity in polymer electrolyte composites, PVDF, a representative polymer substance was used at a certain mass ratio. XRD, SEM, and BET were performed for metallurgical analyses of the materials, and ion conductivity was calculated through the EIS method. In addition, thermal conductivity was measured to analyze thermal stability, which is a major parameter of lithium ion batteries. As a result, the ion conductivity of LiH was found to be 10^-6 S/cm, and the ion conductivity further decreased as the PVDF ratio increased when the composite was formed.

• Journal of Electrochemical Science and Technology
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• v.12 no.2
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• pp.217-224
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• 2021

In this study, Monte Carlo (MC) simulation is conducted with recurrence relation to study the effect of SiO₂ with different particle size and their roles in enhancing the ionic conductivity and lithium transference number of PMMA composite polymer electrolytes (CPEs). The MC simulated ionic conductivity is verified with the measurements from Electrochemical Impedance Spectroscopy (EIS). Then, the lithium transference number of CPEs is calculated using recurrence relation with the MC simulated current density and the reference transference number obtained. Incorporation of micron-size SiO₂ (≤10 ㎛) fillers into the mixture improves the ionic conductivity from 8.60×10^-5 S/cm to 2.35×10^-4 S/cm. The improvement is also observed on the lithium transference number, where it increases from 0.088 to 0.3757. Furthermore, the addition of nano-sized SiO₂ (≤12 nm) fillers further increases the ionic conductivity up towards 3.79×10^-4 S/cm and lithium transference number of 0.4105. The large effective surface area of SiO₂ fillers is responsible for the improvement in ionic conductivity and the transference number in PMMA composite polymer electrolytes.

• Journal of Ceramic Processing Research
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• v.19 no.5
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• pp.413-418
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• 2018

All-solid-state lithium batteries (ASSBs) using inorganic sulfide-based solid electrolytes are considered prospective alternatives to existing liquid electrolyte-based batteries owing to benefits such as non-flammability. However, it is difficult to form a favorable solid-solid interface among electrode constituents because all the constituents are solid particles. It is important to form an effective electron conduction network in composite cathode while increasing utilization of active materials and not blocking the lithium ion path, resulting in excellent cell performance. In this study, a mixture of fibrous VGCF and spherical nano-sized Super P was used to improve rate performance by fabricating valid conduction paths in composite cathodes. Then, composite cathodes of ASSBs containing 70% and 80% active materials ($LiNi_{0.6}Co_{0.2}Mn_{0.2}O_2$) were prepared by a solution-based process to achieve uniform dispersion of the electrode components in the slurry. We investigated the influence of binary carbon additives in the cathode of all-solid-state batteries to improve rate performance by constructing an effective electron conduction network.

• Journal of Electrochemical Science and Technology
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• v.13 no.2
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• pp.199-207
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• 2022

Lithium-sulfur batteries (LSBs) have emerged as a promising alternative to lithium-ion batteries (LIBs) owing to their high energy density and economic viability. In addition, all-solid-state LSBs, which use solid-state electrolytes, have been proposed to overcome the polysulfide shuttle effect while improving safety. However, the high interfacial resistance and poor ionic conductivity exhibited by the electrode and solid-state electrolytes, respectively, are significant challenges in the development of these LSBs. Herein, we apply a poly (ethylene oxide) (PEO)-based composite solid-state electrolyte with oxide Li₇La₃Zr₂O₁₂ (LLZO) solid-state electrolyte in an all-solid-state LSB to overcome these challenges. We use an electrochemical method to evaluate the degradation of the all-solid-state LSB in accordance with the carbon content and loading weight within the cathode. The all-solid-state LSB, with sulfur-carbon content in a ratio of 3:3, exhibited a high initial discharge capacity (1386 mAh g^-1), poor C-rate performance, and capacity retention of less than 50%. The all-solid-state LSB with a high loading weight exhibited a poor overall electrochemical performance. The factors influencing the electrochemical performance degradation were revealed through systematic analysis.

• Journal of the Korean Ceramic Society
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• v.36 no.4
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• pp.391-402
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• 1999

Characteristics of composite electrolytes which were prepared by coating a thin film of YSZ (yttria sta-bilized zirconia : (ZrO2)0.92 (Y2O3)0.08) on YDC (yttria doped ceria : Ce0.8Y0.2O1.9) with mixed conductivity have been investigated in order to develop the low-temperature solid oxide fuel cell. The thickness (t) of spin-coated YSZ thin films after the heat-treatment at 600$^{\circ}C$ was increased proportionally to the sol con-centrations (C) while the decrease in its thickness with the spin rate ($\omega$) could be expressed in the e-quation of ln t=9.49-0.53 ln $\omega$(0.99mol//s sol conc.) When the sol concentration and the spin rate being less than 0.99 mol/l and higher than 1000 rpm respectively reliable YSZ/YDC composite electrolytes could be obtained by multi-coating although several micro-cracks were observed in singly coated YSZ film surfaces. The dense YSZ film with a 1$\mu\textrm{m}$ thickness was prepared by coating of 0.99 mol/l YSZ sol five-times at 2000 rpm followed by heat-treatment at 1400$^{\circ}C$ for 2h, The adhesion between YSZ film and YDC substrate was found to be very good. The open circuit voltages of H2/O2 single cell with YSZ/YDC composite electrolytes were 0.79∼0.82 V at 800$^{\circ}C$ and 0.75∼0.77V at 900$^{\circ}C$ The open circuit voltage was inversely proportioned to the thickness ratio of YSZ thin film (1$\mu\textrm{m}$) to YDC substrate(0.28-2.22 mm)