bluuebunny/crossref_metadata_2025_split huggingface dataset:
How Much Safer Are Solid State Cells? - Quantified Failure Analysis of Next-Generation Solid State Cells during Abuse Testing
Authors: Parks Huw Christopher William , Shearing Paul R , Robinson James B 
Published: December 2024

Solid-state lithium-ion batteries offer a promising solution for electric vehicle energy storage by replacing flammable liquid organic electrolytes with non-flammable solid alternatives, thus significantly enhancing safety levels.1 However, despite this potential, the safety of these batteries remains a subject of debate due to a lack of quantified understanding, and existing standards may not adequately address anticipated failure modes. Consequently, there is a pressing need to characterize and quantify the safety of solid-state cells, considering the unique chemistry of each component. Although solid electrolytes aim to reduce the instances of soft shorts between electrode, one of the major safety concerns in solid-state batteries is the occurrence of internal short circuits (ISCs) under faliure circumstance, which pose significant challenges in terms of durability and safety, particularly in automotive applications. ISCs can lead to rapid and catastrophic discharge of up to 70% of the total cell energy in under 60 seconds, resulting in substantial self-heating and potentially initiating thermal runaway.2

To evaluate the safety of solid-state cells, abuse testing has become a standard practice, involving techniques such as nail penetration, crush testing, accelerating rate calorimetry, and overcharging. These tests expedite ISC occurrences, enabling researchers to gain insights into cell behaviour under extreme conditions and facilitating safety assessments. In this study, we conducted a comprehensive examination by subjecting commercial solid-state cells and Li-ion cells of similar energy to catastrophic failure conditions. In conducting this work, we aim to provide a comparative analysis of the challenges encountered by solid-state cells and to quantify the impact of scale-up on safety and failure events, ranging from cell capacities of 2 Ah to 10’s of Ah, and examining the propagation of failure through battery packs. To achieve this, we utilized a diverse array of abuse testing and characterization techniques, including X-ray CT, SEM, and GCMS. Through this endeavour, we aim to establish a benchmark for solid-state failure analysis and quantification, contributing to the advancement of safer battery technologies.
[1] Mauro Pasta et al 2020 J. Phys. Energy 2 032008
[2] Hossein Maleki and Jason N. Howard 2009 J. Power Sources. 2 568-574
The Critical Role of Pressure Uniformity in Enhancing the Performance and Safety of Solid-State Batteries
Authors: Kim Kyounghwan , Shin Jaeho 
Published: December 2024

All-solid-state batteries represent a significant advancement in energy storage technology, offering higher safety and energy density compared to traditional liquid electrolyte solutions. As the demand for more efficient and robust energy storage solutions grows, particularly for electric vehicles and renewable energy systems, the development of solid-state batteries with the argyrodite Li6PS5Cl as the electrolyte has gained substantial attention. These batteries promise enhanced performance through improved energy density and safety.
However, optimizing these systems requires a deep understanding of the mechanical stresses involved, particularly those related to pressure dynamics within the battery cells. For stable operation of these batteries, high pressure is essential, yet studies analyzing pressure in practical, commercially viable cell configurations are notably scarce. This research focuses on the development and examination of pouch-type cells, which are instrumental in demonstrating how pressure dynamics influence battery performance and longevity in real-world applications. By meticulously monitoring these pressure variations, our study not only assesses operational efficiency but also detects potential short circuits, thereby significantly enhancing battery safety. Additionally, our findings highlight the critical role of pressure uniformity in preventing uneven lithium deposition, a common issue that can lead to performance degradation and reduce the battery's overall lifespan. Through advanced pressure management techniques, this research contributes to the design of more reliable and efficient batteries, paving the way for their commercial viability and widespread adoption
Simultaneous Solid Electrolyte Deposition and Cathode Lithiation for Thin Film Batteries
Authors: Warecki Zoey , Castagna Ferrari Victoria , Ievlev Anton , Sugar Josh D , Kim Nam Soo , Stewart David Murdock , Albertus Paul , Rubloff Gary , Talin Albert Alec 
Published: December 2024

Interest in thin film solid state lithium-ion batteries (TFSSLIBs) continues to grow because of their increased safety over flammable liquid electrolytes and their compatibility with well-established thin-film fabrication methods and characterization techniques. TFSSLIBs are also attractive for addressing fundamental questions because they generally comprise fewer components (no binders or conductive additives), and are commonly used to investigate the formation and evolution of solid electrode/electrolyte interfaces. TFSSLIBs are well suited to study the inherent capacity retention and rate performance of cathode materials in a symmetric battery structure, e.g., cathode/SSE/cathode. V2O5 is a candidate with a high theoretical capacity and insertion chemistry of up to 3 Li ions per V2O5, but which practically is unable to achieve highly reversible cycling of even Li2V2O5 due to the structural phase change upon lithiation. By designing a TFSSLIB model system with a solid electrolyte that forms a stable electrode/electrolyte interface, e.g. lithium phosphorous oxynitride (LiPON), in a symmetric configuration, we are able to study the performance of LixV2O5 thin film cathodes without the additional deleterious effects related to anode performance.
We will discuss the fabrication and cycling performance of two different symmetric V2O5 TFSSLIB configurations. The first is a V2O5/LiPON/LixV2O5 TFSSLIB, where the cyclable lithium in this system is included via simultaneous electrolyte deposition and lithiation of one V2O5 cathode during the RF sputtering process, as discussed in our recent publication.1 The second configuration is an LixV2O5/LiPON/LixV2O5 TFSSLIB where lithium is included during the auto-lithiation step of the first V2O5 electrode as well as during the co-sputtered deposition of the second V2O5 electrode. A comparison of the two TFSSLIB symmetric cell performances will be discussed, as well as a comparison to similar symmetric cells cycled in liquid electrolyte. We show that the deposition of the solid-state electrolyte LiPON onto thin film V2O5 leads to a uniform lithiation of up to 2.2 Li per V2O5, without affecting the Li concentration in the LiPON and its ionic conductivity. In the LixV2O5/LiPON/LixV2O5 system, we demonstrate cycling of >270 mAh/g at a rate of 20C, for 1600 cycles with only 8.4% loss in capacity.
1. Warecki, Z. et. al., Simultaneous Solid Electrolyte Deposition and Cathode Lithiation for Thin Film Batteries and Lithium Iontronic Devices, ACS Energy Lett, 2024, 9, 2065-2074
Modifying Li1.3Al0.3Ti1.7(PO4)3 electrolyte-Anode Interface with Two-Dimensional Materials for All-Solid-State Lithium Batteries
Authors: Tsai Dong-Lun , Yeh Che-Ning 
Published: December 2024

The widespread adoption of lithium batteries in electric vehicles (EVs) and electronic devices is attributed to their extended cycle life and high energy density. However, the utilization of organic liquid electrolytes (LEs), which are highly flammable and volatile, has raised safety concerns. Additionally, severe side reactions between electrodes and LEs decrease the performance of lithium batteries. Recently, the replacement of LEs by solid-state electrolytes (SSEs) has emerged as a promising development for safe and high-energy-density lithium batteries.
Among these, Li1.3Al0.3Ti1.7(PO4)3 (LATP), a NASICON-type SSE, has garnered attention due to its high ionic conductivity (10-4 - 10-3 S/cm) and excellent stability in ambient conditions. However, the strong reducibility of lithium metal anode poses a risk of Ti4+ reduction, leading to the formation of a highly electronic conductive phase such as Li3Al0.3Ti1.7(PO4)3, which may accelerate lithium dendrite growth and increase interfacial resistance.
In our work, we introduce 2D material coatings (e.g., graphene, MoS2, Co3O4, etc.) at the electrode-LATP interface. Leveraging the high mechanical strength and specific surface area of 2D materials, this coating enhances the surface stability of LATP and electrodes, prevents titanium reduction, and inhibits lithium dendrite growth, thereby enhancing cycling performance. The solid-state batteries using LATP with modified coating as SSE exhibit high capacity retention compared to the batteries using bare LATP SSE. Our work provides a promising approach to SSEs with superior ionic conductivity and stability, expanding the candidates of applicable solid electrolytes toward the realization of the next-generation all-solid-state lithium batteries.
Computational Study of Amorphous LiNb0.5P0.5O3 Cathode Coating Material Utilizing Universal Machine Learning Potential
Authors: Yoshikawa Koki , Fujiwara Yoshiya , Luong Huu Duc , Zhou Zizhen , Fujisaki Fumika , Tateyama Yoshitaka 
Published: December 2024

All-solid-state batteries using sulfide-based solid electrolytes (SSEs) have been expected as promising next-generation batteries, but the low chemical stability of SSEs causes interfacial side reactions with cathode active materials (CAMs), resulting in degraded battery performance.[1] To mitigate this issue, cathode coating material (CCM) like LiNbO3 on the CAM has been introduced to prevent direct contact with the SSE.[2] Recently, it was reported that amorphous LiNb0.5P0.5O3 suppresses the interfacial side reactions compared to amorphous LiNbO3.[3] Though several computational studies on crystalline CCMs exist[4], accurate modelling of the amorphous CCM has been still challenging. In this work, adopting a universal machine learning potential (MLP) that allows reasonable level of accuracy and speed both[5], we investigated characteristics of the amorphous LiNb0.5P0.5O3. Pair distribution functions (PDFs) of amorphous LiNbO3 calculated by melt quench method[6] using first-principles (VASP[7, 8]) and MLP techniques are shown in Fig. 1 (a). The similarity indicates that MLP can calculate the amorphous structures with sufficient accuracy. We also calculated lithium and oxygen vacancy formation energies in amorphous LiNb(1-x)P
x
O3 (x = 0, 0.5, 1.0) using MLP (Fig. 1 (b)). The lithium vacancy formation energy increases with the P content, indicating that phosphorus contributes to the stabilization of Li in the CCM. Meanwhile, the oxygen vacancy formation energy is the highest for LiNb0.5P0.5O3 (x = 0.5), implying that the coexistence of Nb and P suppresses oxygen desorption associated with cation valence changes. These results can be regarded as one of the reasons for the reduced interfacial side reactions using LiNb0.5P0.5O3 as a CCM. We are also calculating lithium diffusion coefficients, density of states, and comparing the properties to crystalline CCMs, which will be discussed in the presentation.
Acknowledgement:
This study is based on the project of ‘Evaluation of All-Solid-State Battery Material and Foundational Technology Development for Next Generation (SOLiD-Next, JPNP23005)’, commissioned by the New Energy and Industrial Technology Development Organization (NEDO).
References:
[1] Q. Zhang et al., Adv. Mater., 31, 1901131 (2019).
[2] A. Banerjee et al., Chem. Rev., 120, 6878 (2020).
[3] Y. Morino et al., ACS Appl. Mater. Interfaces, 15, 36086 (2023).
[4] H. Chen et al., Chem. Mater., 35, 5657 (2023).
[5] S. Takamoto et at., Nat. Commun., 13, 2991 (2022).
[6] M. D. Kluge et at., Phys. Rev. B, 36, 4234, (1987).
[7] P. E. Blöch, Phys. Rev. B, 50, 17953 (1994).
[8] G. Kresse et al., Phys. Rev. B, 59, 1758 (1999).

Figure 1
(Invited) Factors Guiding the Stability Sulfide and Oxide Solid-State Electrolyte Interphases with Lithium Metal
Authors: Mitlin David 
Published: December 2024

Site-specific microstructural analysis combined with interphase design is employed to understand the origin of solid-state electrolyte failure, and to promote extended electrochemical stability. For example, stable anode-free all-solid-state battery (AF-ASSB) with an argyrodite is achieved by tuning wetting of lithium metal on “empty” copper current-collector by coating it with a thin composite film of thermodynamically stable Li2Te and Cu microparticles. Cryo-FIB sectioning demonstrates a dense and uniform electrodeposit, with minimal voiding or dendrites at the collector-SSE interface. Unmodified Cu current-collector promotes inhomogeneous Li electrodeposition/dissolution, leading to a thick non-uniform solid electrolyte interphase (SEI) interspersed with voids. As another example, thin intermetallic Li2Te–LiTe3 bilayer derived from 2D tellurene stabilizes the Li-argyrodite SEI, allowing state-of-the-art electrochemical performance with conventional foils. The Li2Te–LiTe3 bilayer impedes SSE decomposition and suppresses voiding. Unmodified Li–LPSCl undergoes reduction decomposition that extends deep into the SSE, causing reactivity-induced voids in both metal and SEI. For the first time, short-circuiting Li metal dendrite is directly identified, employing 1.5 mm diameter "mini" symmetrical cell and cryogenic focused ion beam (cryo-FIB) electron microscopy. The branching sheet-like dendrite traverses intergranularly, filling the interparticle voids and forming an SEI around it. A separate study on dendrites in garnet LLZTO demonstrates that the compact's grain size distribution and internal porosity critically affect electrical short-circuiting, indicating the importance of local electronic properties. Lithium dendrites propagate intergranularly through regions where LLZTO grains are statistically smaller than the bulk average. Metal also accumulates in the otherwise empty pores of sintered compact present along the dendrite path.

Related Work:

Mechanical Milling - induced Microstructure Changes in Argyrodite LPSCl Solid-State Electrolyte Critically Affect Electrochemical Stability,
Advanced Energy Materials.
2024, in-press.

Dendrite Growth—Microstructure—Stress—Interrelations in Garnet Solid-State Electrolyte.
Advanced Energy Materials.
2024, 2303062. https://doi.org/10.1002/aenm.202303062
Stable Anode‐Free All‐Solid‐State Lithium Battery through Tuned Metal Wetting on the Copper Current Collector.
Advanced Materials

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Tuned Reactivity at the Lithium Metal–Argyrodite Solid State Electrolyte Interphase.
Advanced Energy Materials
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Li Metal Surface Modification to Stabilize Lithium-Argyrodite Interface for Sulfide-Based All-Solid-State Lithium Metal Batteries
Authors: Sim Hui-Tae , Oh Myungkeun , Park Ye-Eun , Kim Hyojin , Cho Yun-Sun , PARK Seongjin , Kim Dong-Won 
Published: December 2024

Since the commercialization of lithium-ion batteries, they have faced limitation in safety and energy density. All-solid-state lithium metal batteries (ASSLMBs) can be a solution to address these issues. Among many types of solid electrolytes, sulfide-based solid electrolytes have been attracted great attention because of their high ion conductivity and ductile property. However, many researchers have reported that the interface between lithium metal and solid electrolyte is highly unstable. The lithium dendrite growth can be also occurred in the ASSLMBs by voids, cracks, grain boundaries in solid electrolyte and side reactions between lithium metal and solid electrolyte. Therefore, it is imperative to develop a protective layer that can suppress lithium dendrites and side reactions.
In our work, we removed native resistive surface layer formed on pristine lithium metal and reconstructed solid electrolyte interphases (SEI) with uniform, ion-conductive and excellent physical properties by dipping solution containing lithium nitrate in nitromethane and dimethoxyethane. The modified lithium metal is denoted as Li@NDL (lithium @ nitromethane-dimethoxyethane-lithium nitrate). We confirmed that nitromethane reacted with LiOH and Li2O on native surface of lithium to form Li3N and organic layer, which enhanced ionic conductivity and mechanical strength. The symmetric lithium cell with Li@NDL increased critical current density to 2.8 mA cm-2 and exhibited outstanding cycling stability without short circuit over 1000 hours. ASSLMB comprising Li@NDL anode and 4 mAh cm-2 NCM composite cathode maintained 80% retention after 200th cycles at 0.5 C, demonstrating our work can provide a novel surface modification of lithium metal for ASSLMBs.
All-Solid-State Li-S Cells: The Importance of Interfaces
Authors: Cruddos Joshua , Cruddos Josh , Robinson James B , Zeier Wolfgang 
Published: December 2024

All solid-state batteries have long been considered the next leap forward in energy storage devices, owing to their improved safety and higher theoretical energy density than their liquid counterparts. However, even with these improvements, heavy metal positive electrode materials such as lithium nickel oxides (NMC) and lithium iron Phosphate (LFP) are not gravimetrically energy dense enough to meet the growing energy requirements of modern-day applications. One promising candidate is the lithium sulfur (Li-S) chemistry due to the high theoretical capacity and abundance of sulfur. However, designing positive electrodes with high sulfur content that is able to withstand the large sulfur morphology expansion, alongside minimizing the excess Li storage in the negative electrode has remained elusive. A solution to this is the development of “anode-free” or zero excess lithium (ZEL) cells which minimise inactive materials and mitigate the challenges of handling Li metal foils during fabrication. These offer a further enhanced energy density, additional safety improvements and more control of the negative electrode interface. However, the inefficiency of lithium plating and stripping leads to rapid capacity degradation due to the absence of an excess lithium inventory.
Here we present, to our knowledge, the development of the first zero-excess (anode free) all solid state LiS battery, composed of an Li2S-based catholyte combined with an Li6PS5CL solid electrolyte and a Ni/In negative electrode. The cell displays good capacity retention, 350 mAh g-1 Li2S after 50 cycles, and good rate capability, up to 2C. Since zero-excess cell degradation is primarily afforded to Li losses at the negative electrode, our study focuses on understanding this degradation and its relationship with the interfacial resistance at the anode-electrolyte interface. In addition, we show the affect of replacing Indium with an ionically conductive amorphous thin film as a method to reduce interfacial resistance which improves the gravimetric energy density of the cell. Finally, using X-ray computer tomography, we investigate the formation of cracks and void shifts and their subsequent effect on cycling performance, alongside the importance of pressure to enable long cycling life.

Figure 1
High Energy Density Sulfide-Based All-Solid-State Batteries by Tailoring Electronic Conductivity within Composite Cathode
Authors: Shin Hyeon-ji , Kim Jun Tae , Han Da-Seul , Nam Kyung-Wan , Jung Hun-Gi 
Published: December 2024

The sulfide-based all-solid-state batteries (ASSBs) has guaranteed having excellent safety by using non-combustible inorganic solid-electrolyte (SE). SE separator can transport Li ion selectively and there is no concentration gradient in theory, enabling fast charging. In addition, due to high ionic conductivity of sulfide-based SE comparable to liquid based electrolyte, high capacity and high energy density ASSBs of 5mAh cm-2 have been developed to a stage close to commercialization.
So far, among the many issues of ASSBs, the performance improvement has been achieved by focusing on interfacial deterioration issues. However, recent several studies have analyzed and identified the cause of inhomogeneous reaction in composite cathode, which lead to capacity degradation quickly. It had been confirmed that the inhomogeneous reaction was caused by not only loosely contact and isolated active materials but also restriction Li conductivity in nano-crystal boundaries of active materials, resulting in localizing overcharge-discharge and decreasing in capacity and rate capability. As one of intrinsic properties of ASSBs, the solid-solid contact induce the limitation of lithium ion mobility and it also triggered insufficient electronic conduction pathway increasing charge transfer resistance.
In order to develop high-energy density and high power ASSB, the ability of the conductivity for electron and ion must be balanced through the formation of a well-developed electronic percolating pathway. In this study, the inhomogeneous reactivity that can be maximized in thick electrodes is alleviated by improving the electron transfer path in the composite cathode. To uniformly transfer electrons in the composite cathode, we introduced argyrodite type SE coating with 2D conductive material under solvent environment. This approach is effective on forming a continuous electronic pathway for homogeneous reactivity as well as reduce SE oxidation by preventing direct contact between SE and cathode active material. As a result, we obtained a high initial capacity of 206 mAh g-1 using a single LiNi0.8Co0.1Mn0.1O2 cathode and SE coated with 2D conductive material, and confirmed that approximately 90% rapacity maintained after 200th cycle.
Effects of Electrolyte Composition on the Electrochemistry of Organic Mixed Conducting Polymer Electrodes
Authors: De La Fuente Duran Ana , Siemons Nicholas Daniel , Marks Adam , Magni Arianna , Salleo Alberto , Chueh William C. , Mefford Tyler 
Published: December 2024

Organic mixed ionic-electronic conductors (OMIECs) are semiconducting conjugated polymers that can transport both electrons and ions throughout their bulk. This property is enabled by electrochemical ion-insertion redox reactions that co-dope the polymer with mobile ions and electrons (or holes). These redox and mixed conduction capabilities provide functionality for applications including organic batteries, actuators, and organic electrochemical transistors. These various applications are enabled by a few fundamental OMIEC redox processes that involve polymer-electrolyte and polymer-electrode interfaces as well as mobile ions and significant amounts of incorporated solvent. Understanding the role of electrolyte in changing these redox processes can enable improved performance across a variety of devices.
This work sets out to identify the role of electrolyte composition in changing the electrochemistry of a conjugated ladder polymer through a multi-faceted experimental and theoretical approach. We primarily focus our efforts on BBL, more formally called poly(benzimidazobenzophenanthroline). Using rotating disk electrochemistry, we find that electrolyte can cause a significant change in the voltage windows in which BBL is redox-active. Using operando UV-Vis and Raman spectroscopy measurements, we identify changes in BBL electrochemistry when operated in different electrolytes. To gain further insights about the redox mechanisms for this polymer, we use DFT to model our operando Raman data and principal component analysis to propose a charging mechanism that accounts for this electrolyte-dependent performance. Our results suggest that the accessible redox states of this polymer can dramatically change based on a modification of its local environment.