bluuebunny/crossref_metadata_2025_split huggingface dataset:
New Insights on Electrochemical Parameters in Battery Modeling through 3D Digital Twin Structural Analysis
Authors: Lee Yong Min 
Published: July 2022

Electrochemical parameters such as chemical diffusion coefficients and exchange current densities are very critical in simulating electrochemical battery models. However, conventional experimental methods have not reflect actual status of composite electrodes and cells due to the limitation in analyzing their micro-structures. To address these challenges, we attempted to draw 3D digital twin structures of composite electrodes and cells and then quantify veiled parameters like active surface area. As a result, we could obtain more correct chemical diffusion coefficients and exchange current densities and improve the reliability of electrochemical battery models. In this work, we will introduce how to build and use 3D digital twin structures of composite electrodes for lithium-ion batteries.
[References]
1. J. Park, Y. M. Lee et al., Energy Storage Materials, 19 (2019) 124-129
2. J. Park, Y. M. Lee et al., Advanced Energy Materials, 10(35) (2020) 2001563
3. J. Kim, J. Park, Y. M. Lee et al., ACS Energy Letters, 5(9) (2020) 2995-3004
4. J. Kim, S. Jung, Y. M. Lee et al., Advanced Energy Materials
, Online published (2021)
Optimization of Catholyte in Composite Cathodes for Garnet-Structured Llzo Electrolyte in Solid-State Batteries
Authors: Houache Mohamed , Karkar Zouina , Yim Chae-Ho , Filoso Gina , Niketic Svetlana , Abu-Lebdeh Yaser 
Published: July 2022

The application of Li-ion batteries have been expanding at a rapid rate in recent decades due to the tremendous demands in the market for portable electronics, smart grid, and electric vehicles (EVs). All-solid-state lithium metal battery (ASSLB) is the most promising next-generation energy storage device as they can solve the safety issue resulted from liquid electrolytes.
Among different types of solid-state electrolytes (SSE), garnet-type structure materials have been shown to be very promising for the development of ASSLBs owing to their high Li-ion conductivity (∼10–3 S cm–1 at RT), wide electrochemical stability window (∼6 V vs Li+/Li), and good chemical stability against Li metal. The high interfacial resistance generated by inadequate contact and interfacial reactions is a substantial impediment to the adaptation of ASSLBs. To address this challenge, a catholyte (a small amount of ionic conductors which are mostly derived from the solid electrolyte formulation) is introduced into the cathode formulation. This necessities a re-design of the cathode into a composite cathode with possibly new components such as carbon additives with high aspect ratio and conductive binders. Understanding their individual and combined impacts on performance is essential in the pursuit of optimized systems.
In this work, we designed a series of composite cathode formulations defined with three cathode active materials (LFP, NMC 622 and NMC 811), three carbonaceous additives (carbon black, carbon nanofibers and carbon nanotubes), and a series of organic and inorganic molecular, and polymeric conductors along with LLZO to create a composite cathode with high capacity and stability at high C-rates. A systematic DOE approach has been utilized to evaluate the impact of each component on the electrode and cell performance and the results will be presented.
Cyclic Carbonate-Based, Single-Ion Conducting Polymer Electrolytes for Li-Ion Batteries: Electrolyte Design
Authors: Engler Anthony , Park Habin , Liu Nian , Kohl Paul 
Published: July 2022

Solid polymer electrolytes (SPEs) have been the focus of study to address Li-ion battery issues including thermal runaway by mitigating the danger from volatile solvents. A single ion conductor has a high transference number which eliminates uncontrolled mass transport by immobilizing the anion to the polymer matrix. Problems with undesired side reactions and lithium dendrite growth can also be improved by providing a mechanical barrier. Unfortunately, single-ion conducting SPEs suffer from poor lithium-ion mobility and conductivity due to the immobilized nature of the anions, poor ion-pair dissociation, and the slower time scale diffusion in a polymer matrix compared to liquid electrolytes.
In this study, cyclic carbonate-based polymer electrolytes were synthesized to mimic the beneficial properties of conventional carbonate-based liquid electrolytes, such as high level of ion dissociation and solid electrolyte interphase (SEI) formation. A series of copolymers were synthesized varying the structure and composition of the anionic monomer and polar cyclic carbonate containing monomer. The tertiary hydrogen on these carbonate monomers can act as a crosslinking point in free radical polymerizations or UV curing processes to provide robust mechanical properties to the SPEs at elevated temperatures. Although the inherent conductivities of the single-ion SPEs are on the order of 10-7 mS/cm, the addition of plasticizers can improve these conductivities to 0.1 mS/cm.
Current-Corrected Cycling for True Electrode Performance Measurement
Authors: Yan Zilai , Scott Ben , Glazier Stephen , Obrovac Mark 
Published: July 2022

In battery research, galvanostatic cycling is the most widely used method to evaluate electrode performance.1 By applying pre-set current throughout the test, this method often fails to accurately reflect electrode performance at the designed cycling rate (particularly for high-rate cycling) because the actual capacity can be considerably affected by polarization and electrode degradation.2 To address this issue, a current-corrected galvanostatic cycling (CCGC) method is proposed, in which the current is actively adjusted during cycling based on the measured capacity of previous cycles.3 Compared to the traditional galvanostatic cycling (TGC) method, which may result in cycling rates that are hundreds of times faster than the designed rate, the proposed cycling strategy can effectively measure rate-dependent electrode performance precisely at designated rates.
As shown in Figure 1, graphite electrodes were cycled in half cells at different rates ranging from C/20 to 5C using TGC and CCGC methods. For TGC, the capacity decreases quickly at rates higher than C/5 and becomes negligeable when the rate is ≥ 2C. This is because the actual cycling rates are much higher than the designed rates when the capacity becomes lower due to polarization, as shown in Figure 1(b). For instance, at a designed 5C rate, the observed actual cycling rate for TGC is 1200 C – 3600 C, about 500 times higher than the designed rate. In addition to the low capacities at high rates, at C/2 the capacity is not stable, due to the increasing overpotential, which causes staging plateaus to be truncated by the lower potential cutoff.

References

J. Liu et al., Nat. Energy, 4, 180–186 (2019).

C. Heubner, M. Schneider, and A. Michaelis, Adv. Energy Mater., 10, 1902523 (2020).

Z. Yan, B. Scott, S. L. Glazier, and M. N. Obrovac, Batter. Supercaps (2021) doi: 10.1002/batt.202100345.

Figure 1 (a) Lithiation capacity and (b) the actual cycling rate of graphite electrodes cycled at different rates using CCGC and TGC. Reproduced with permission from ref 3. Copyright 2021 Wiley-VCH GmbH.

Figure 1
Garnet-Based Composite Cathodes for All-Solid-State Lithium Batteries
Authors: Ihrig Martin , Laptev Alexander M , Finsterbusch Martin , Fattakhova-Rohlfing Dina , Guillon Olivier , Ye Ruijie 
Published: July 2022

Garnet-based all-solid-state lithium batteries (ASSLB) provide high intrinsic safety, extended operational temperature range, and high energy density. As the first two are intrinsic to the materials system, one prerequisite to obtain high energy densities with such ASSLBs is the manufacturing of composite cathodes. Preferably, cathode active material (CAM) and electrolyte should form an intertwined 3D-network with an intimate extended contact between two phases. The interface between the CAM and the electrolyte should feature high total surface area with a low impedance to enable an efficient charge transfer and transport and minimize the resistance losses in a battery.
Composite solid cathode microstructures can be formed via a co-sintering of solid electrolyte and CAM powders. However, many CAMs such as Li[Ni1-x-yCoxMny]O2 (NMC), Li[Ni1-x-yCoxAly]O2 (NCA) or Li2NiMn3O8 (LMO) cannot withstand sintering temperatures required, for oxide class solid electrolytes as Li7La3Zr2O12 (LLZ) or Li1+xAlxTi2-x(PO4)3, to obtain sintered composite cathodes. Furthermore, the thermodynamic stability of CAMs significantly decreases in the presence of solid electrolytes. Still, several groups have demonstrated that thermodynamic limitations can be significantly lessened via a kinetic control of the process such as reduction of reaction times and a careful control of powder morphology during ceramic sintering process.
Following this work, we demonstrate that Field Assisted Sintering Technique / Spark Plasma Sintering (FAST/SPS) enables fabrication of different functional solid-state battery components within minutes such as dense LLZ separator layers with a high ionic conductivity, thick LiCoCO2 (LCO)/LLZ composite cathodes without any interfacial reactions, and integrated cathode half-cells consisting of a composite cathode and a LLZ separator layer at temperatures as low as 675 °C. . The analysis of these composite cathodes revealed well sintered pure phases and a homogenous distribution of cubic LLZ and cathode active material. Electrochemical tests showed promising electronic and ionic conductivity (0.4 mS cm-1) values and an increased capacity (4 mA cm-2) compared to cathodes with pure active material.
The structural analysis after the electrochemical characterization shows the mechanical integrity of the LLZ/LCO interface, which means that a mechanically stable rigid LLZ/LCO interface can be obtained.
Such a mechanically stable LLZ/LCO cathode allows to analyze possible electrochemistry induced degradation, which is suggested by theoretical work but lacks experimental validation. A detailed analysis of the LLZ/LCO interface by SEM, TEM, Raman, and XRD provide insights into the processes occurring during electrochemical cycling. The findings can pave the way to increase the cycling stability of ceramic all-solid-state batteries via interface optimization

Figure 1
Analysing the Effects of High-Intensive Dry Mixing on the Calendering Process and Cell Performance of NMC622 Based Cathodes
Authors: Diener Alexander , Mayer Julian Kristoffer , Zhang Yue , Kwade Arno 
Published: July 2022

A reliable design of production processes for the manufacturing of lithium-ion battery electrodes requires a deep understanding of the interdependency of processes, the resulting electrode microstructure and the influence on the cell performance indicators, like energy density, cycle life and aging. In the present study, the focus lays on the calendering process during which the electrode coating is compacted with the aim of adjusting uniform electrode properties such as mechanical, electrical and electrochemical behavior. Compaction of the electrode coating affects the pore structure and therefore has a crucial influence on the electrical and electrochemical behavior of the cell. Consequently, process and machine parameters have to be adapted in order to generate electrode structures optimized for a desired application. To meet this target, an in-depth understanding of how the calendering process affects the electrode structure beyond the simple reduction of porosity and further how the calendering process itself is affected by the preceding process steps like dry or wet mixing is mandatory.
Thus, the focus of the presented work is to investigate the interdependency between the dry mixing process step and the subsequent calendering process by correlating powder properties adjusted via the dry mixing with the machine behavior during the calendering as well as the resulting coating density. The impact of the calendering process on the electrode microstructure and its correlation with electrode properties by developing process-product-property functions, regarding the above mentioned criteria, is an additional focus of the presented study.
Therefore, powder mixtures of NMC622 with carbon black were created under varying the dry mixing intensity and thus adjusting the carbon black agglomerate size. The created powder mixtures were comprehensively characterized, e.g. particle size distribution and powder conductivity, and then used to build up electrodes which afterwards were compacted to different coating densities. The correlation between the powder properties and the calendering behavior shows a higher compaction resistance with decreasing carbon black agglomerate size. Whereas reducing the carbon black agglomerate size leads to lower electrical resistivity and therefore strongly impacts the C-rate capability.
One-Pot Synthesis of LiAlO2-Coated LiNi0.6Mn0.2Co0.2O2 Cathode Material
Authors: Touag Ouardia , Coquil Gael , Charbonneau Mathieu , Mankovsky Denis , Dollé Mickaël 
Published: July 2022

The chemistry of lithium-ion batteries (LIBs) is an active area of research, notably through the increasing demand for high energy and power density in LIBs, especially for application in electric vehicles (EVs) and hybrid electric vehicles (HEVs).
Among the various cathode materials, LiNixCoyMn1-x-yO2 (NMC) intercalation compounds are the best candidates for applications in high performance LIBs. However, Ni-rich NMC suffers mainly from parasitic side reactions at the interface with the electrolyte, which leads to a lower thermal and electrochemical stability. Surface modification via coating is an effective concept to counter the capacity degradation of NMC and to improve the particles’ structural stability for enhancing their cycle-life [1], [2]. Different processing techniques that usually requires several steps are presented in the literature. However, to facilitate the integration of a new product in the current battery market, it is preferable to reduce the number of steps during the synthesis process. In this work, we propose a one-pot synthesis of LiAlO2-coated LiNi0.6Mn0.2Co0.2O2 particles, by using a continuous stirred-tank reactor (CSTR).
Firstly, the composition and morphology of the coated and uncoated cathode materials are characterized by SEM, TEM, EDX and XPS. Then, the structural characterization of our materials is validated by XRD analysis. Consequently, we will compare the electrochemical performance and thermal stability of coated and uncoated NMC particles.
We will demonstrate that our approach provides an easy way to apply surface treatment onto Ni-rich NMC particles and simplifies the synthesis process at large scale production.
KEYWORDS: Lithium-ion battery, Ni-rich NMC cathode, LiAlO2 coating, surface protection.

Negi, R.S., et al., Enhancing the Electrochemical Performance of LiNi0.70Co0.15Mn0.15O2 Cathodes Using a Practical Solution-Based Al2O3 Coating. ACS Applied Materials & Interfaces, 2020. 12(28): p. 31392-31400.

Kim, H.-S., et al., Enhanced electrochemical properties of LiNi1/3Co1/3Mn1/3O2 cathode material by coating with LiAlO2 nanoparticles. Journal of Power Sources, 2006. 161(1): p. 623-627.
(Digital Presentation) Thermal Acceleration Model for the Capacity Fade of a Rechargeable Li Ion Battery and Its Validation with 10+ Years of Testing Data
Authors: Ye Hui , Fang Zhi , Tamirisa Prabhakar , Jain Gaurav , Scott Erik 
Published: July 2022

Rechargeable Li ion batteries have become not only a major power source for consumer electronics, but also a critical power source for high demanding applications like electrical vehicles, portable military devices and medical devices. Medtronic, one of the leading medical device companies has developed a breakthrough rechargeable Li ion battery technology-OverdriveTM to power implantable neurostimulators such as Intellis and Interstim Micro. OverdriveTM batteries have exceptional stable performance and fast charging capability. Figure 1 shows design verification test of capacity stability under two different discharge rate, C/24 and C/168; charging rate are 2C for both groups. As shown in Figure 1, there is virtually no capacity fade under C/168 discharge rate cycling and only a few percent capacity loss under C/24 rate cycling for more than 10 years of testing at 37oC.
It is crucial to have a good acceleration testing model to design a rechargeable battery with reliable performance over 10 years of service and to ensure robust design with foreseeing battery material replacement over time. In the early development stage, we established a thermal acceleration capacity fade model for our OverdriveTM battery based on 2 years of testing as shown in Figure 2. Figure 2 shows capacity fade of Overdrive battery cycling at different temperatures up to 10 years. The trend of additional 8 years of data is consistent with model prediction.
This presentation will highlight the performance characteristics of the OverdriveTM battery technology and provide the technical details of thermal acceleration capacity fade model. In addition, we will present how the model has been applied to understand the degradation mechanism of OverdriveTM battery and to improve the battery chemistry.

Figure 1
(Digital Presentation) Ti3C2
Tx
MXene As an Anode in Li- and Na-Ion Batteries: Where Does Electrochemical Capacity Stem from?
Authors: Koriukina Tatiana , Nyholm Leif , Hahlin Maria , Edstrom Kristina 
Published: July 2022

The unique properties of the Ti3C2
Tx
MXene continue to attract attention within the energy storage field. Many of the previous reports on the use of this material in Li- and Na-ion batteries mainly concentrate on modifying the surface of the MXene or the cycling protocol in attempts to achieve higher specific capacities. Very few studies have, on the other hand, addressed the nature of the electrochemical reactions taking place during the electrochemical cycling of the material.
This study aims at gaining a deeper understanding of the electrochemical behavior of freestanding Ti3C2
Tx
electrodes without any binder and conductive additive. The results obtained with these electrodes, which were manufactured by vacuum filtration of MXene suspension in deionized water, are used to identify the electrochemical reactions yielding the observed capacities obtained in Li-metal cells using 1 M LiPF6 in EC:DEC (50:50 vol%) as the electrolyte and in Na-metal cells containing 1 M NaFSI in TEG-DME. Constant current and cyclic voltammetry cycling as well as in-house ex-situ XPS and synchrotron-based ex-situ HAXPES and XAS were used to identify the redox processes taking place upon the charging and discharging of the MXene electrodes.
The results, obtained when cycling the freestanding Ti3C2
Tx
MXene electrodes in Li-metal cells, indicate that the reversible capacity can be explained by redox reactions involving Ti species present in the Ti3C2
Tx
surface layer. The charge storage mechanism is hence faradic. The results of XAS measurements carried out in the transmission mode likewise indicate that the redox reactions are surface confined and do not involve the inner C-Ti-C layer of the Ti3C2
Tx
MXene.
When cycling material between 0 and 3 V vs. Na+/Na in Na-metal cells, the specific capacity of the Ti3C2
Tx
electrodes increases progressively with the cycle number (from 5 mAh/g on the first cycles to 50 mAh/g on the 200th cycle using a cycling rate of 10 mA/g). This effect is suggested to be connected to the deposition of sodium at about 0 V vs. Na+/Na as this count yield an activation of the electrodes. Comparisons of the cycling behavior of freestanding Ti3C2
Tx
electrodes with those of monolithic TiO2 (amorphous) nanotube electrodes with nanotubes lengths of about 4 μm suggest that the behavior of the Ti3C2
Tx
electrodes cannot be explained by the expected spontaneous formation of TiO2 on the surface of Ti3C2
Tx
electrodes. The capacity for the TiO2 nanotube anode was relatively high, i.e., 160 mAh/g, on the first cycle but was seen to decrease to about 90 mAh/g after 100 cycles when cycling at a rate of 10 mA/g. The reasons for the differences seen between the Ti3C2
Tx
and TiO2 nanotube electrodes will be discussed based on the general electrochemical behavior of the Ti3C2
Tx
electrodes.
(Digital Presentation) Modeling Thermal Behavior and Safety of Large Format All-Solid-State Lithium Metal Cells Under Thermal Ramp and Short Circuit Conditions
Authors: Johnson Nathan B , Albertus Paul 
Published: July 2022

We are submitting this abstract in the understanding that a virtual option is likely to be offered for the Spring, 2022 ECS meeting. We are only interested in the virtual option for this presentation.
It has often been posited that solid-state batteries are inherently safer than liquid electrolyte Li-ion batteries because there is no flammable organic solvent present in the battery. However, thermal safety is a multi-faceted issue with other considerations such as onset temperature, maximum temperature, total heat generation, maximum heating rate, etc. These considerations need to be looked at in greater detail, including their dependence on the volumetric and gravimetric energy densities. Safety concerns become even more important as stable graphite anodes are replaced with potentially highly reactive and energetic lithium metal anode. In this presentation, we will report on our work using differential scanning calorimetry (DSC) heat flow data to construct a transient, 2D model of heat generation and temperature distribution in a large format cell with a LixCoO2 cathode, Li7La3Zr2O12 solid electrolyte, and lithium metal anode. We will present on the thermal runaway behavior of this cell chemistry during a thermal ramp test in an oven and due to the formation of an internal short circuit. Our analysis will focus on the total amount of heat generated, onset temperature for self heating, maximum temperature, and maximum heating rate. We also analyze how the battery state of charge affects these properties. Related work in our group focuses on collecting DSC data for Li metal solid state cells and may also be highlighted.
Using Data Science and Machine Learning to Predict the Failure Rate of Pin Diodes
Authors: Gallagher James C , Mastro Michael , Koehler Andrew , Ebrish Mona , Jacobs Alan G. , Hite Jennifer K. , Gunning Brendan P. , Kaplar Robert J. , Hobart Karl D. , Anderson Travis J. 
Published: July 2022

GaN research is important to the development of next generation power conversion technology because its large Baliga figure of merit GaN gives it the potential to outperform SiC. Presently, commercialized GaN technology is based on lateral high electron mobility transistors (HEMTs); however, large areas would be required for high voltage applications thus there is motive to switch to vertical GaN. Current GaN substrate manufacturing technology is known to produce inconsistent quality with a varying concentration of defects. These defects are known to cause catastrophic device failure, thus there is motive to develop quick, non-destructive techniques to predict the quality of the wafer before undergoing the expensive fabrication process. This talk focuses on using data science and machine learning to predict the quality of the diodes.
This work demonstrated that Raman spectroscopy can be used to detect high crystal stress points, which strongly correlates with an increased leakage current. Optical profilometry images can be used to detect defects that cause catastrophic failures; however, the presence of benign defects makes it difficult to predict the device quality using a simple algorithm. Thus, a machine learning algorithm relate optical profilometry images to device performance of subsequently processed device. The results showed that this algorithm was 91% accurate at predicting the forward bias behavior of devices, and it is possible that the devices it could accurately predict failures due to device processing errors.
This work was supported by the Office of Naval Research.