bluuebunny/crossref_metadata_2025_split huggingface dataset:
Detailed Investigation on LiNbO3-Coated Layer of Different Thicknesses on LiNi0.5Co0.2Mn0.3O2 Cathode Material for All-Solid-State Lithium Batteries
Authors: Bong Willy Shun kai , Kuzuhara Minoru , Kawamoto Koji 
Published: December 2024

All-solid-state batteries (ASSBs) are very promising for next-generation energy storage technologies owing to several key advantages including higher power density, better thermal and electrochemical stability, and improved safety for electric vehicles [1, 2]. In this work, bulk-type ASSB cells were prepared with LiNbO3 coatings of different thicknesses, and their electrochemical behaviors at different upper cutoff voltages (upper cutoff potential ≥ 4.40 V) were first systematically compared by using Bulk-type ASSB cells. To eliminate the influence of additives, charge-discharge curves were recorded without conductive carbon or binders in the composite cathodes.
A thicker coating caused three unfavorable electrochemical behaviors in the first three cycles: (1) a higher overpotential, (2) sluggish discharge kinetics, and (3) capacity fading. The measured electronic conductivity decreased drastically with increasing coating thickness, suggesting that this may have caused behaviors (1–3). To overcome this, a carbon additive was used to improve electronic transport in the composite cathode and successfully suppressed the aforementioned behaviors. Our findings indicate that the combination of a thick LiNbO3 coating on NCM523 and carbon additive can achieve synergistic effects to improve both the electrochemical properties and durability of ASSB cells.
To further verify the cycle performance of the NCM523 cathode material with LiNbO3 layers of different thicknesses and uniformity, full-cell ASSBs consisted of a positive electrode and a graphite negative electrode separated by an SE has been fabricated. As a result, the cycle performance was greatly enhanced by increasing the thickness and uniformity of the LiNbO3 coated layer [3]. Our findings further demonstrate that a thick (more than 9 nm) and uniform coated layer (surface without uncoated area) displays outstanding electrochemical performance, especially cycle stability (capacity retention of 85.1% after 300 cycles at 60 ℃), indicating that this strategy is very effective for constructing high-performance NCM cathodes for sulfide-based ASSBs.

【
Acknowledgments
】

This study was supported by the SOLiD-NEXT project (JPNP23005) commissioned by the New Energy and Industrial Technology Development Organization (NEDO).

【
References
】

[1] Y. Kato, S. Hori, T. Saito, K. Suzuki, M. Hirayama, A. Mitsui, M. Yonemura, H. Iba, R. Kanno, Nat. Energy, 1 (2016), 16030.
[2] M. M. Thackeray, C. Wolverton, E. D. Isaacs, Energy Environ. Sci., 5 (2012), 7854−7863.
[3] W. S. K. Bong, A. Shiota, T. Miwa, Y. Morino, S. Kanada and K. Kawamoto, J. Power Sources, 577, 233259 (2023).
Synthesis and Densification of Na1+XZr2SixP3-XO12 Nasicon Solid Electrolyte for Solid-State Na Batteries
Authors: Fung Kuan-Zong , Tsai Shu-Yi , Liu I-Chun , Fung Kenneth 
Published: December 2024

Solid-state batteries using Na+ ion conductors recently tend to receive much attention because the abundance of Na in earth's crust. When the liquid electrolyte is replaced by ceramic solid electrolytes (SE), the fire incidents observed in conventional rechargeable batteries may be effectively suppressed.
Furthermore, solid-state batteries (SSBs) need to reduce the high interface polarization between electrode and SE. For better Na+ conductivity, Na1+XZr2SiXP3-XO12. With NASICON (Na super ionic conductor) structure is selected for this study. Through solid-state reaction method, it is believed the selection of precursors may be critical for better crystallization and densification of Na1+xZr2SixP3-xO12. For instance, adequate amount of Na2CO3 or Na2SiO3 may be used as the Na source as well as flux for densification. Thus, the objectives of this study is to (1) to investigate the importance of precursors such as Na2CO3 or Na2SiO3 for conduction/densification of NASICON, (2) to search the appropriate temperature for synthesis/crystallization of NASICON, (3) to investigate the factors, such as crystallinity/density, affecting the ionic conductivity. With variation in the stages of processing, the structural, microstructural and electrical properties od decomposed precursors and resultant NASICON will be examined using XRD,SEM and DC/AC impedance measurements.
The Dual Role of Thiophosphate Solid Electrolytes as Catholytes and Active Material Precursors in Lithium/Sulfur Solid-State Batteries
Authors: Münch Konrad , Janek Jürgen 
Published: December 2024

Lithium/sulfur cell chemistry combines low material cost and high availability of sulfur with high specific energies. However, liquid electrolyte cells are plagued by the parasitic polysulfide shuttle effect between the electrodes, which reduces reversible capacity and efficiency and passivates the negative electrode. Inorganic solid electrolytes (SE) are single-ion conductors and can therefore block the parasitic electrode crosstalk by blocking polysulphide dissolution and transport. In particular, the combination of sulfur battery chemistry with thiophosphate-based SEs is considered obvious due to their high ionic conductivities and their electrochemical stability window corresponding to the usual voltage ranges used in lithium/sulfur battery chemistry.
Lithium/sulfur solid-state batteries (SSLSBs) based on thiophosphate SE are generally reported to have higher capacities, based on the mass of active material, than their liquid counterparts. These can reach up to the theoretical capacity of sulphur (1672 mAh g-1) and even beyond, implying a capacity contribution from the SE and its degradation products. As the degradation products potentially block ionic conduction pathways, this is often considered undesirable. However, other work has reported stable cycling of carbon/SE composites without the addition of additional active material, postulating in situ formation of active material by degradation of the SE.
In this work we show the capacity contribution of the SE by introducing a balance of charge and discharge capacity in SSLSBs. By comparing positive electrode composites with and without additional sulfur as an active material, we show the importance of the storage capacity contribution of the thiophosphate SE in state-of-the-art electrode composites. Using electrochemical and instrumental analysis (XPS, ToF-SIMS), we investigate the formation of degradation products during the first cycles and their reversible redox during cycling. Based on this, we postulate that a controlled amount of degradation may be useful in SSLSBs and that this additional role of SE as a contributor of charge storage capacity may be a design principle for the development of high capacity positive electrode composites.
Phase-Structure-Property Relationships of Halide Coating Materials for Solid Composite Electrodes
Authors: Lee Yeo Kyung , Yun Jonghyeok , Kang Junhee , Lee Jong-Won 
Published: December 2024

Lithium-ion batteries (LIBs) have played a pivotal role in advancing energy storage technologies, enabling high-demand applications such as electric vehicles and renewable energy storage systems. Despite their widespread use, LIBs face significant challenges in terms of energy density and intrinsic safety issues. These challenges have spurred interest in all-solid-state batteries (ASSBs), which utilize solid electrolytes (SEs) to offer safe alternatives to conventional liquid electrolyte-based LIBs. Among the various types of SEs explored to date, halide SEs exhibit improved compatibility with high-voltage oxide cathodes, as compared with sulfide-based SEs. Thus, halide SEs may be utilized as cathode coating materials for ASSBs using sulfide SEs with high ionic conductivity. However, the specific material properties that determine the chemical/electrochemical characteristics of halide coatings have not been clearly studied yet.
In this study, we synthesize lithium yttrium chloride (Li3YCl6, LYC) SEs using different methods (solid-state synthesis and ammonium-assisted liquid-phase synthesis) at various heat-treatment temperatures to control phase compositions and crystal structures. These allow us to systematically explore the phase-structure-property relationship of LYC SEs and their roles as coating materials for LiNi0.90Co0.05Mn0.05O2 (NCM). Our experimental findings reveal that the phase, crystal structure and crystallinity of LYC significantly influence the microstructure, ionic conductivity, interfacial compatibility, and thermal stability of LYC-coated NCM (NCM@LYC). The crystal structure and crystallinity of synthesized LYC SEs are explored by Rietveld refinement of X-ray diffraction patterns. Notably, LYC SEs prepared via wet synthesis under optimal heat-treatment conditions exhibit superior Li-ion transport kinetics due to the enhanced crystallinity of phase-pure LYC. This leads to the improved interfacial resistances of NCM@LYC, as evidenced by impedance analyses of NCM composite electrodes. Therefore, the NCM@LYC composite electrodes with the optimized LYC SE show significant improvement in rate capability and cycle lifetimes. This research elucidates the critical role of the synthesis conditions in controlling the properties of halide coating materials and thus in improving the interfacial kinetics and stability of composite cathodes of ASSBs. The insights gained from the phase-structure-property relationships provide valuable guidelines for the development of highly conductive and stable SEs for next-generation batteries.
Effect of Dopant Concentration in Li7La3Zr2O12(LLZO) on Performance of Thermal Battery
Authors: Ahn Tae-Young , Roh Heesook , Kang Hyungu , Kim Jiyoun , Lee Jongseo , Choi Yusong 
Published: December 2024

A thermal battery is a type of reserved battery that operates by melting a mixture of electrolytes to form the battery's functioning components. Due to its ability to function at high temperatures (500°C), it is primarily used as a power source for high-performance equipment, with much higher ionic conductivity than lithium-ion batteries. Furthermore, at room temperature, the molten salt exists in a solid state with little to no ionic conductivity, making it ideal for use in guided weapons that require activation when necessary without self-discharge. However, in order to be used in weapons that operate in a rotating environment such as projectiles, improvements are needed as the molten salt exists in a liquid state at operating high temperatures. Additionally, ceramic binders such as MgO are used to prevent leakage of the molten salt, but this factor increases the resistance of the battery. A LLZO as solid electrolyte, being excellent in thermal stability and remaining solid at the operating temperatures of thermal battery, could improve stability. LLZO is known to exist two kinds of crystal structures, with the cubic crystal structure known to have high ionic conductivity. It has been reported that the cubic crystal structure can be obtained through doping.
A lot of research group has been studied within the temperature range used for lithium ion batteries; therefore, we aimed to select the optimal dopant concentration at high temperatures to improve the discharge performance of thermal batteries. The cubic structure LLZO was synthesized by using Ta, known for its excellent ion conductivity, as a dopant for solid-state transformation. As the amount of Ta dopant increased(Li7−xLa3Zr2−xTaxO12, x = 0.0–0.6), all X-ray diffraction (XRD) results of the obtained LLZO confirmed a cubic crystal structure. The discharge test results confirm that Ta dopant exhibits the best discharge performance when x=0.5, as shown in the figure 1. Although FeS2 is commonly used as a cathode material in thermal batteries, its performance is limited by its low operating voltage. In this study, the performance of solid-state electrolytes was evaluated using FeF3 as a cathode material, known as promising candidates for high voltage. We also present findings to elucidate the performance variation of thermal batteries, which results from the addition of eutectic salts, while utilizing FeF3 as the cathode material and Ta-doped LLZO as the electrolyte.

Figure 1
Solid State Gradients: One Step Aqueous Spray Deposition of Novel Graduated Cathode/Solid Electrolyte Interfaces for Improved Solid State Batteries.
Authors: Tudball Matthew , Miller Thomas Samuel 
Published: December 2024

Lithium ion batteries are a necessity of daily life, being used more than ever in increasing size and power for applications like handheld devices, large scale energy storage and transport. They also offer huge potential in our shift towards renewable energy, therefore the production and use of these batteries is set to increase dramatically.
Solid state batteries (SSB’s) replace the liquid electrolyte with a solid. This offers more stability against lithium dendrite formation which is the main cause of battery short-circuiting and failure. Because of this, solid state electrolytes (SSE’s) may be the answer to the challenge of pure lithium anodes, which are the highest theoretical capacity anode, but are hampered by rapid dendrite formation. SSE’s can have higher gravimetric and volumetric capacity due to the reduced electrolyte content and also make for safer batteries, particularly under stress, as the flammable liquid electrolyte has been removed.
This work demonstrates a new manufacturing method for SSB’s, that allows for the formation of a novel design of the electrode/electrolyte interface. Ultrasonic spray coating is the process of spraying a material layer by layer to form thin films. By graduating between two or more different materials a gradient can be manufactured.
Current SSB’s are formed by separately manufacturing a cathode film and a solid electrolyte film, then assembling these on top of each other to make the battery. This can cause interface issues between the cathode and the SSE, particularly, areas of poor contact, poor solid electrolyte interface (SEI) formation and degradation of the cathode. All of these issues lead to higher resistance, lower capacity and higher degradation.
This work shows that a spray deposited graduated combined cathode/SSE removes the interfacial issues seen in the literature to create a battery that has 10x lower resistance, longer cycle life, lower capacity loss and performs substantially better under high rate conditions. All of which are necessary to help solid state batteries become more real world applicable.
This new manufacturing technique is the only known way to produce this structure in a cheap, industrially relevant way, and is easily expandable to a larger scale. On top of this, unlike standard manufacturing methods, the methodology is almost entirely water based, which removes costs of solvent recapture and increases safety.
This layer by layer gradient deposition technique is also applicable to other areas of materials research and has been used on silicon anodes and lithium sulfur batteries, as well as membranes for direct air capture and fuel cells.

Figure 1
Sulfide Solid Electrolyte Coated Cathode in All-Solid-State Batteries
Authors: Kim Jun tae , Shin Hyeon-ji , Jung Hun-Gi 
Published: December 2024

Using a sulfide solid electrolyte, the all-solid-state batteries emerge as a promising candidate for next generation batteries, having significant advantages such as high lithium ionic conductivity and wide electrochemical stability window. These characteristics pave the way for the realization of elevated power and energy densities. Nonetheless, this cutting-edge technology is not without its hurdles; indeed, there are pressing issues that demand attention and refinement.
In contrast to conventional lithium-ion batteries, which rely on organic liquid electrolytes with high wettability having uniform lithium ion transfer pathways within electrodes, the ASSBs encounter constraints in establishing solid-solid interfaces owing to its intrinsic solid nature. This limitation becomes particularly apparent during the cycling, wherein the fluctuating volume of the active material, prompted by the (de)intercalation of lithium ions, precipitates the degradation of the interface between active material and solid electrolyte within the composite electrode. This phenomenon leads up to loss of the lithium ionic pathway, precipitating a deterioration in cell performance
The key point of this study lies in the endeavor to enhance battery performance through the application of a solid electrolyte coating onto the surface of the active material. By doing so, the aim is to preserve a uniform pathway for lithium ion transfer within the composite electrode. It is noteworthy that the solid electrolyte coating layer exerts profound influence on the electrochemical dynamics of the cell, important in adapting the formation of homogeneous lithium ionic pathway and the mitigation of void formation within the composite electrode. Thus, the main thrust of this research is to validate the formation of meticulously uniform solid electrolyte coating layer, depend upon the size of the solid electrolyte particles.
In pursuit of this objective, a multifaceted approach was adopted. Through the utilization of liquid-phase process and a dispersant, the particle size of the solid electrolyte was deliberately manipulated, thereafter subjecting it to a dispersion process for the application of solid electrolyte coating. Intriguingly, it was observed that as the particle size of the solid electrolyte diminished, a more uniform solid electrolyte coating layer ensured, thereby engendering better electrochemical performance. Furthermore, it was corroborated that the lithium ionic pathway persevered even after long cycling, attributable to the presence of the solid electrolyte coating layer. Concomitantly, the incidence of undesirable side reactions was appreciably mitigated, with the homogeneous electrochemical reactions within composite electrode.
Design of Spherical Hard Carbon Secondary Particles for Na-Ion Battery Anode Application
Authors: Hong Seong Ung , Lee Byoung-Sun 
Published: December 2024

Recently, Na-ion rechargeable batteries have been successfully developed and launched as the main power sources of a few novel electric vehicles in China. An energy density of the mass-produced Farasis Energy Na-ion batteries have been announced as between 140 Wh/kg and 160 Wh/kg with the layered oxide cathode and hard carbon anode combination. Though the commercialization of the Na-ion batteries is highly remarkable owing to the cost-effectiveness and long lifespan, the energy density of the Na-ion batteries needs to be improved even further considering the current state-of-art advanced practical Li-ion batteries of ca. 300 Wh/kg.
Development of a novel anode material can contribute to the energy density improvement. Hard carbons with random shapes, which have been employed as the main anode materials in the commercial Na-ion batteries, have demonstrated the specific capacity of 200 to 300 mAh/g based on the carbonized biomasses. To improve energy density, shape and microstructure of the hard carbons need to be carefully designed. On the one hand, random shapes are not highly desired to achieve high tap density. Instead, spherical shapes with uniform particle sizes are beneficial to increase tap density as well as the energy density [1]. On the other hand, the carbonaceous microstructure needs to be optimized because the Na is stored through various mechanisms with combinations of i) adsorption at the surface of open pores, ii) adsorption at defect sites of graphene sheets, iii) insertion between graphene layers, and iv) pore filling [2]. As such, design of spherical hard carbon with well-established microstructure can provide high energy density. In this work, spherical hard carbon in Figure 1 was prepared using carbon precursor material (polyacrylonitrile) and sacrificial polymer (poly(styrene-co-acrylonitrile)) dissolved in the cosolvent (N,N-dimethylformamide). Carbonaceous microstructures were modified using the chemical and physical approaches. The morphological, structural, and electrochemical characterizations will be presented at the conference.
[1] Oh, H. J. et al., Chem. Eng. J. 454, 140252 (2023)
[2] Chen, C. et al., Carbon Energy 4, 1133-1150 (2022)
Figure 1. SEM image of spherical hard carbon

Figure 1
Hybrid Electrolyte Strategies for High-Energy Sodium-Based Batteries
Authors: Lee Wang-Geun 
Published: December 2024

Sodium-based batteries are emerging as a promising and crucial technology for sustainable energy storage due to the abundance and cost-effectiveness of sodium compared to lithium. While these batteries offer an attractive option for large-scale applications, they face challenges such as lower voltage and energy density. To overcome these limitations and enhance high-energy sodium-based battery performance, researchers are exploring innovative hybrid electrolyte strategies. Hybrid electrolytes, which combine solid and liquid systems, provide improvements in safety, efficiency, and performance.
This study explores various hybrid approaches, including organic-solid-aqueous hybrids, quasi-solid anolytes, and over-saturated catholytes. These methods aim to address the limitations of sodium-ion batteries and pave the way for high-performance energy storage solutions. For instance, an organic-solid-aqueous hybrid system lets different non-aqueous and aqueous materials adapt, which leads to wider voltage ranges. Additionally, using non-aqueous sodium metal anodes and aqueous ferrocyanide redox cathodes in these hybrid electrolyte systems demonstrates viable voltage ranges and reversible performance. Research on quasi-solid electrolytes showed potential in developing thicker anodes, while over-saturated catholyte research explored the use of solid cathode materials.The diverse hybrid electrolyte approaches have revealed promising possibilities for both aqueous and non-aqueous sodium-based batteries. These advancements enhance battery stability and durability, leading to higher voltage and energy density across various applications. Recent advancements in sodium anode and aqueous cathode designs have enabled the application of sodium-based batteries in different types, including seawater and sodium-flow batteries. One significant innovation is the use of NASICON ceramic electrolytes, which offer improved ionic conductivity and stability, allowing for further material adaptations and optimization of battery performance.
In conclusion, the exploration of hybrid electrolyte strategies for sodium-based batteries represents a novel approach towards realizing the full potential of this technology. As research and development progress, sodium-based batteries with hybrid electrolytes could become foundational for sustainable energy storage, contributing to a cleaner and more efficient energy future.