bluuebunny/crossref_metadata_2025_split huggingface dataset:
Multifunctional Cyclic Phosphoramidate Solvent for Safe Lithium-Ion Batteries
Authors: Ko Seongjae , Matsuoka Ayaka , Chen Wenting , Iwata Taiga , Otsuka Hiromi , Yamaguchi Shoji , Masuda Takuya , Zheng Qifeng , Shang Rui , Nakamura Eiichi , Yamada Atsuo 
Published: December 2024

To enhance the overall safety of electronic devices and energy storage systems, the development of functional electrolytes that improve the thermal stability of rechargeable batteries is of utmost importance. Here, we report a novel cyclic phosphoramidate, 2-(N,N-dimethylamino)-1,3,2-dioxaphospholane-2-oxide (DMAP), which has been newly designed and synthesized as a multifunctional solvent for safe Li-ion batteries.1 Its unique molecular structure, incorporating an amine moiety into a five-membered cyclic phosphate, provides both high electrochemical and thermal benefits: (i) a stable DMAP-derived passivation film (solid electrolyte interphase, SEI) is formed on the graphite surface, thereby suppressing electrolyte reduction, (ii) exothermic reactions induced by the thermal decomposition of the SEI and direct reactions between a lithiated graphite anode and electrolyte salt, which are known to trigger and accelerate battery temperature rise, are largely mitigated thanks to DMAP's inherently high radicals-/Lewis acids-/HF-scavenging abilities, (iii) the moisture sensitivity is improved with reduced nucleophilic attack at the P atom caused by water contamination in the electrolyte due to the presence of a substituted N atom in the DMAP, thus enhancing storage stability, and (iv) the stable cycling of LiFePO4 cathodes is achieved based on moderate oxidation stabilities and suppressed aluminum current collector dissolution in the DMAP-based electrolytes. Importantly, all these advantages can be obtained with DMAP used as both an electrolyte solvent and additive, regardless of the types of salts (LiFSI or LiPF6) and co-solvents (fluorinated ethyl methyl carbonate or dimethyl carbonate) employed.
We believe that our solvent-design strategies, based on molecular modification and optimization, combined with fine-tuning the elements in the molecular structure, can endow the electrolyte with highly functional physicochemical and electrochemical properties, thus opening new possibilities for developing safe batteries with high energy densities.1,2

S.Ko, A.Matsuoka et al., R.Shang and A.Yamada, ACS Energy Lett., 9, 7, 3628–3635 (2024)

Q.Zheng et al., E.Nakamura and A.Yamada, Nat. Energy, 5, 291-298 (2020)

Figure 1
Ultrasonic Atomization of New Alloys for Powder-Based Anodes in Next-Generation Non-Lithium Batteries
Authors: Ciftci Jakub , Kalicki Bartosz , Choma Tomasz , Morończyk Bartosz , Żrodowski Łukasz 
Published: December 2024

Improved battery performance has led to significant advancements in anode materials, with powder-based anodes emerging as a promising alternative to traditional graphite anodes[1,2]. Next-Generation Non-Lithium Batteries, like potassium and magnesium–ion batteries require anodes tailored to the ion diffusivity and anode-electrolyte-cathode compatibility[3,4]. Candidates like bismuth, magnesium, and antimony-based anodes can maximize specific capacity and cycling stability. Passivation film formed on their surface causes large potential drop and energy loss[5]. The alloys with tailored chemical composition can improve the electrochemical behavior of the anodes and significantly promote film formation influencing the interface with electrolyte[6]. Current powder-based anodes preparation methods involve mechanical milling, which produces irregular particles and distorts the structure obtained by eutectic solidification, which can showcase outstanding electrochemical properties[7,8]. We propose a powder production method based on ultrasonic atomization technology[9]. This technology uses the vibrations to eject the particles from liquid metal. Plasma or induction heating can be used for melting, allowing a wide range of metals to be processed. Powders obtained by ultrasonic atomization possess high sphericity which can stabilize the dissolution rate of the anode during cyclic charging and facilitate obtaining uniform coating thickness. Thanks to vibrations instead of high-velocity gases the powder production unit is much smaller and suitable for research and alloy development.
[1] J. Zhao, Z. Wei, N. Chen, F. Meng, R. Tian, Y. Zeng, F. Du, Energy Storage Mater
2024, 65, DOI 10.1016/j.ensm.2023.103127.
[2] B. Fu, G. Liu, Y. Zhang, Z. Liu, X. Xie, G. Fang, S. Liang, ACS Energy Lett
2024, 3292.
[3] Z. Zhao-Karger, Y. Xiu, Z. Li, A. Reupert, T. Smok, M. Fichtner, Nat Commun
2022, 13, DOI 10.1038/s41467-022-31261-z.
[4] D. Gu, Y. Yuan, J. Liu, D. Li, W. Zhang, L. Wu, F. Cao, J. Wang, G. Huang, F. Pan, J Power Sources
2022, 548, DOI 10.1016/j.jpowsour.2022.232076.
[5] F. Liu, G. Cao, J. Ban, H. Lei, Y. Zhang, G. Shao, A. Zhou, L. zhen Fan, J. Hu, Journal of Magnesium and Alloys
2022, 10, DOI 10.1016/j.jma.2022.09.004.
[6] X. You, X. Zhang, C. Yu, Y. Chen, H. Li, Y. Hou, L. Tian, N. Yang, G. Xie, Journal of Rare Earths
2023, 41, DOI 10.1016/j.jre.2022.04.011.
[7] S. B. Wang, Q. Ran, R. Q. Yao, H. Shi, Z. Wen, M. Zhao, X. Y. Lang, Q. Jiang, Nat Commun
2020, 11, DOI 10.1038/s41467-020-15478-4.
[8] L. Cao, M. Zheng, G. Dong, J. Xu, R. Xiao, T. Huang, J Mater Sci Technol
2025, 211, 278.
[9] A. Priyadarshi, S. Bin Shahrani, T. Choma, L. Zrodowski, L. Qin, C. L. A. Leung, S. J. Clark, K. Fezzaa, J. Mi, P. D. Lee, D. Eskin, I. Tzanakis, Addit Manuf
2024, 83, DOI 10.1016/j.addma.2024.104033.
Enhancing Ni-Rich Lithium Metal Battery Performance By Mitigating Transition Metal Migration with Functional Separators and Additives
Authors: Seo Junhyeok , Kim Minjae , Cho Jaegu , Cho Kuk Young 
Published: December 2024

Achieving high energy density in lithium-ion batteries remains an ongoing challenge. To meet this requirement, electrodes with high capacity are essential. Lithium metal batteries, employing high-nickel NMC cathodes and lithium metal anodes, represent next-generation secondary batteries that can fulfill these demands. Despite the advantage of high energy density in lithium metal batteries, they tend to exhibit unstable long-term charge-discharge behavior due to issues such as dendrite formation on lithium metal and the collapse of active materials in the cathode.
Therefore, we aim to mitigate the crosstalk of transition metals in the cathode, thereby enhancing cell performance. To achieve this, we have developed a functional separator designed to shield the migration of dissolved transition metal ions. By incorporating this new functional separator along with an additive that stabilizes the cathode active material, we have successfully reduced the migration of dissolved ions by 84% and significantly improved cycle performance.
Investigation of the Temperature Behavior of Silicon-Rich Multilayer Pouch Lithium-Ion Battery Cells and Its Effect on Cycle Life and Rate Capability
Authors: Bosch Hannah , Diller Felix 
Published: December 2024

Due to its high energy density and fast charge capability, silicon is an excellent active material, especially in electrical vehicles (EV) applications. The fast charging capability can be reasoned through its higher potential against Li/Li+ when compared to graphite, reducing the risk of Li-plating. As a result of the volume change of silicon during the (de-) lithiation processes, a continuous reformation of the solid electrolyte interface (SEI) takes place. FEC is used as an additive or as a co-solvent to improve the SEI formation. It reported in literature that FEC decomposes at elevated temperatures starting from 45°C [1]. As such elevated temperatures can easily be reached, especially during the charge step in applications where bigger battery formats are used, the temperature behavior of high silicon wt% Lithium-Ion Batteries should be investigated more thoroughly.
To the best of our knowledge, a focus on the temperature behavior of multilayer pouch cells (MLP) with a very high silicon content (70wt%) has not been subject of research so far. Therefore, this study gives important insights into the electrochemical and thermal behavior of silicon within bigger battery formats.
MLP cells with 5 Ah were built and tested for their rate capabilities and their temperature behavior. The cells consisted of 70wt% of silicon as the anode material and a high nickel cathode material. Rate tests were conducted at 10 °C, 25 °C and 40 °C with MLP cells. The resistances were measured at three States of Charge points 25%, 50%, and 75% to investigate the temperature impact on the resistance. Additionally, the cycle lifetimes of the MLP cells were investigated at different fast charging C-rates (C/2, 2C, 5C) until 80% State of Health (SoH) at 25 °C.
These results give important information on the performance of silicon based 5Ah lithium-ion batteries in a bigger format. The temperature behavior needs to be understood, as the battery‘s thermal management has to be adapted accordingly, especially for application purposes such as EVs.
The study is investigated in the project “CAESAR”, funded by the German Federal Ministry for Economic Affairs and Climate Action (BMWK) under grant number 03El3046F. We thank BASF SE for the NCM cathode material, Wacker Chemie AG for the silicon anode material and E-Lyte for the electrolyte.
[1] T. Teufl, D. Pritzl, L. Hartmann, S. Solchenbach, M. Mendez, H. Gasteiger, “Implications oft he Thermal Stability of FEC-Based Electrolytes for Li-Ion Batteries”, J. Electrochem. Soc., 2023, 170, 020531, DOI: 10.1149/1945-7111/acbc52.
Analysis of Lithium-Ion Distribution Uniformity and Artifacts in Lipon Solid Electrolyte Material Based on Esm
Authors: Choi Youngwoo , Kim Seonghyun , Cho Su-Ho , Ahn Chi Won , Hong Seungbum 
Published: December 2024

The advancement of electronic devices, such as electric vehicles and drones, has led to an increased focus on battery research. Lithium-ion batteries are widely used for their high energy density and long cycle life. However, using liquid electrolytes in these batteries presents several challenges, including leakage risks, flammability, and the formation of dendrites, which can lead to safety hazards and reduced battery performance.
Solid electrolytes offer several advantages, such as enhanced safety, prevention of leakage, and suppression of dendrite formation. These benefits can potentially address the issues associated with liquid electrolytes. However, solid electrolytes also face challenges, including difficulties in manufacturing, lower ionic conductivity, and mechanical stability issues, which hinder their commercialization. Uniform distribution of lithium ions within solid electrolytes is crucial to ensure consistent performance and prevent the formation of hotspots that can lead to battery failure.
Electrochemical Strain Microscopy (ESM) is a powerful technique that can analyze ion concentration and conductivity by detecting the strain generated in the material due to ionic movement. When applied to solid electrolyte materials, ESM provides valuable insights into the uniformity of ion distribution and ion conduction pathways. This capability is particularly beneficial in developing and optimizing solid electrolytes, where understanding and controlling ion distribution is critical to improving battery performance and reliability.
This study verified the uniformity of ion concentration in LiPON, a representative solid electrolyte material, based on ESM images. Simultaneously, by comparing Trace and Retrace images at different scan speeds, the impact of scan speed on ESM imaging was assessed, and the causes of artifacts occurring during the ESM imaging process were identified. Furthermore, methodologies to reduce these artifacts were proposed.
Exploring High-Entropy Thin Films for Advanced Energy Storage Applications
Authors: Serikkazyyeva Assel , Mashekova Aiym , Yegamkulov Mukagali , Nurpeissova Arailym , Mukanova Aliya , Bakenov Zhumabay 
Published: December 2024

High-entropy thin films (HETF) represent a novel and promising avenue in the field of materials science, offering unique properties and functionalities that hold great potential for energy storage applications. This work delves into the synthesis, characterization, and application of HETF in energy storage systems.
Through the integration of multiple elements in equimolar or near-equimolar ratios, HETF exhibit exceptional mechanical strength, thermal stability, and corrosion resistance. Moreover, their tunable compositions and structures allow for tailored electrochemical properties, enhancing the performance and efficiency of energy storage devices.
This presentation will discuss recent advancements in the fabrication techniques of high-entropy thin films, elucidate their fundamental electrochemical mechanisms, and highlight their applications in various energy storage platforms, including batteries, supercapacitors, and beyond. By elucidating the potential of high-entropy thin films, this research aims to contribute to the development of next-generation energy storage technologies, paving the way towards sustainable and efficient energy solutions.
Effective Conductive Networks from Carbon Materials for Lithium-Ion Batteries
Authors: Baumgartner Julian F. , Kravchyk Kostiantyn V. , Kovalenko Maksym V. 
Published: December 2024

Conductive networks are integral components in Li-ion battery electrodes, serving the dual function to provide electrons to the active material while its porosity ensures Li-ion electrolyte accessibility to deliver and release Li-ions, thereby ultimately determining the electrochemical performance, regardless of the active material. In the realm of academic research, the task of fabricating an electrode equipped with an effective conductive network emerges as a daunting challenge, profoundly influencing a researcher's ability to showcase the intrinsic electrochemical performance of an emerging active material. Amidst the plethora of conductive additives available for battery electrodes, researchers often find themselves navigating a labyrinth of choices, grappling with decisions on a suitable additive and the optimal methodology for electrode preparation.
This review talk seeks to provide fundamental understanding and practical guidelines for designing battery electrodes with effective conductive networks across various length scales.[1] This involves meticulous selection of specific carbon conductive additives from the plethora of options, and exploring effective integration methods into the electrode, all tailored to the unique characteristics of the active materials and the specific research objectives.
[1] J. F. Baumgärtner, K. V. Kravchyk, M. V. Kovalenko, Adv.
Energy Mater.
2024, Manuscript Accepted.

Figure 1
Single-Membrane pH-Decoupling Aqueous Battery Using Proton-Coupled Electrochemistry for pH Recovery
Authors: Xi Dawei , Yang Zheng , Alfaraidi Abdulrahman , Aziz Michael J. 
Published: December 2024

Aqueous redox flow batteries (ARFBs) constitute a promising technology for cost-effective and scalable storage of intermittent renewable energy from sources like wind and solar. For long discharge-duration storage (> 8 h), these batteries offer a unique advantage by decoupling energy storage from power generation, providing a level of design versatility and scalability that traditional rechargeable batteries can hardly match. Typically, the negolyte and posolyte of ARFBs exhibiting long-term operation have roughly the same pH. In contrast, pH-decoupling aqueous redox flow batteries (ARFBs) utilize different pH values in the negolyte and the posolyte, enabling the cell to achieve higher cell voltages and support a broader range of redox pair combinations. Managing the crossover of acid and base, along with an economical and straightforward method to recover their crossover, is critical for long-term operation of pH-decoupling ARFBs. We have previously investigated the crossover of acid and base in multichamber pH-decoupling ARFBs and developed a small, but adequately-sized bipolar membrane (BPM) sub-cell for pH recovery.1 Here, we introduce a new pH-decoupling design utilizing a conventional single-membrane ARFB architecture. This approach reduces the ohmic area-specific resistance while maintaining an acceptably low level of acid-base crossover. We explore various electrolyte pairs, ranging from solutions to semi-solids, anions to cations, acids to bases, showing that this design allows flexibility in electrolyte combinations. The setup can result in improved energy efficiency, higher areal power density, and reduced capital costs. Along with different cells, we demonstrated how proton-coupled electrochemical reactions can serve as proton pumps, enabling in-situ or ex-situ pH recovery in these pH-decoupling setups and discussed its relationship to BPM pH recovery.
1. Xi, D., Alfaraidi, A.M., Gao, J. et al. Mild pH-decoupling aqueous flow battery with practical pH recovery. Nat Energy (2024). https://doi.org/10.1038/s41560-024-01474-1

Figure 1
Microemulsion-Solubilized Menadione As a Redox Flow Battery Negolyte: Electrochemical Surface-Enhanced Raman Spectroscopy Insights
Authors: Sharma Bhavya , Barth Brian , Zawodzinski Thomas A. 
Published: December 2024

Understanding the electron transfer processes of quinone electrolytes is pivotal for advancing organic redox flow batteries (RFBs) and optimizing their performance. In this study, we employed electrochemical surface enhanced Raman spectroscopy (EC-SERS) to investigate the electron transfer mechanism of microemulsion (μE) - solubilized menadione, a quinone based vitamin. Combining electrochemistry and SERS offers sub-second time and high spatial resolutions, with excellent sensitivity and selectivity. Recently menadione was used in a μE RFB, where electrochemical reversibility was demonstrated to be µE dependent. The electron transfer mechanisms for menadione solubilized in a μE has yet to be reported. By coupling ultramicroelectrode techniques with SERS we investigate the redox behavior of menadione within the context of redox flow batteries.
Our research centered on the elucidating the proton coupled electron transfer pathways for menadione in μEs. The reaction mechanism for a quinone is strongly dependent on the protic nature of the solvent. μEs have the unique property of combining both aqueous and non-aqueous phases at a nanometer scale in a single stable solution. We examine the effects of aqueous phase pH and oil phase hydrogen-bond donor strength on the electrochemical mechanism for a quinone confined to the oil phase. We also address the role of μE morphology on the possible mechanism. We speculate the role of μE ordering on long-term quinone stability. Ultimately, knowledge of the mechanism will provide insight into kinetics and thermodynamic parameters which determine RFB performance.
Revisiting Microemulsion Electrochemistry
Authors: Barth Brian , Imel Adam , Zawodzinski Thomas A. 
Published: December 2024

We present a study of electron transfer kinetics in microemulsion (µE) electrolytes and address possible mechanisms. This work is motivated by our exploration of µEs as redox flow battery (RFB) electrolytes. Our previous studies characterize µEs using small angle neutron scattering, pulsed-field gradient nuclear magnetic resonance spectroscopy, conductivity measurements, and phase behavior diagrams. Results from these studies on ferrocene and menadione redox probes demonstrated surprisingly facile kinetics in bicontinuous sodium dodecyl sulfate µEs at a planar glassy carbon electrode. While preliminary screening with cyclic voltammetry identified these systems as possible RFB electrolyte candidates, electrochemical reversibility was strongly dependent on µE composition. This draws attention to the role of µE properties such as bulk and near-surface ordering, interfacial packing, and dynamics on electron transfer. Ultimately, the realization of µE RFBs requires a fundamental understanding of µE electrochemistry including kinetics and the underlying mechanisms, which are currently unclear.
In this talk, we re-evaluate µE electrochemistry. Historical interpretations often assumed identical bulk and near-surface ordering and a constant electrochemical surface area, independent of µE composition and electrode properties. We address limitations of these assumptions. Furthermore, we compare more recently suggested electron transfer mechanisms in emulsions to µEs. We probe the impact of domain size on the potential mechanism from the perspective of the electroneutrality approximation, including the effects of µE composition, morphology, and interfacial fluidity. In addition, both oil- and water-soluble, and inner- and outer-sphere redox probes are utilized with the aim of understanding the role of the structured µE solvent in the electron transfer process. We leverage insights from these fundamental studies and suggest possible implications for improving the current state of µE RFBs.
(Invited) Development of All Solid-State Batteries with Sulfide Solid Electrolytes: From Materials to Characterizations
Authors: Kim Jung-Hyun 
Published: December 2024

Sulfide-based solid electrolytes (SEs), such as lithium (Li) - argyrodites (e.g., Li6PS5X, where X = Cl, Br, I), have attracted significant attention among various inorganic materials due to their high ionic conductivity (> 10-3 S/cm) and manufacturability of all solid-state batteries (SSBs). However, the practical application of these materials is still challenging due to several technical issues, including problems with the electrode-electrolyte interphase and Li-dendrite growth, which compromise the safety and lifespan of SSBs. In this presentation, I will highlight our recent efforts to (i) identify the failure modes of sulfide-based SSBs and (ii) propose viable solutions to address these challenges.
To begin, I will illustrate the dynamics of lithium-dendrite growth through liquid electrolytes in conventional lithium-ion batteries compared to solid electrolytes in SSBs. I will explore and highlight both the similarities and differences in the behaviors of lithium-dendrite growth across these systems.
Electrochemical methods are routinely employed to assess the performance and failure modes of SSBs. A key technique in R&D is the critical current density (CCD) technique, which evaluates the dynamic stability of the lithium/solid electrolyte (Li/SE) interface by incrementally increasing the current density until the interface/bulk fails. However, we found that the effectiveness of this technique is heavily influenced by three factors: (i) cell design, (ii) cell materials, and (iii) electrochemical measurement protocols. The impact of each factor on CCD values and the methods proposed to achieve reproducible CCD measurements will be discussed in detail. In addition, the distribution of relaxation times (DRT) technique serves as a powerful tool for identifying failure modes in SSB cells. I will present representative DRT behaviors observed in SSB cells, identifying the underlying degradation processes that contribute to cell failure.
Finally, I will discuss our recent efforts to enhance the stability of interfaces, thereby improving the performance of SSBs. One approach involves improving the properties of lithium-argyrodite SE by tuning their chemical compositions.