bluuebunny/crossref_metadata_2025_split huggingface dataset:
(Digital Presentation) Approaches of Pre-Lithiation on Si Anode for Lithium-Ion Batteries
Authors: Wang Lei , Hu Jiazhi , Li Wei , Balogh Michael P 
Published: September 2023

Silicon is one of the most attractive anode materials for next generation high-capacity lithium-ion batteries (LIBs) due to its high specific capacity. However, the large volume change (up to 300%) of silicon during lithiation/delithiation process leads to coupled mechanical and chemical degradation, such as pulverization of silicon particles, formation of unstable solid-electrolyte interphase (SEI), and loss of electrical connectivity, resulting in high irreversible capacity loss and rapid capacity fading. Pre-lithiation is one of the effective approaches to compensate for the loss of active lithium and extend battery cycle life.
In this work, various approaches of pre-lithiation for Si electrodes are systematically studied and compared. Different levels of pre-lithiation dosage are applied to the Si electrodes and the pre-lithiated Si electrodes are evaluated in NMC622/Si full cell configuration. After pre-lithiation, the cell capacity and cycling stability are significantly improved. The impacts of operating voltage window, and N/P ratio on electrochemical performance are also investigated. The morphology of pre-lithiated Si electrodes before and after cycling are also compared via cross section scanning electron microscopy (SEM) to understand the electrode expansion and SEI formation/growth during cycling.
Safety Evaluation of Temperature-Dependent Aging Mechanisms of Li-Ion Batteries Using ARC Tests with Multiple Online Sensors
Authors: Feinauer Max , Abdellatif Abdelaziz , Sichler Peter , Wohlfahrt-Mehrens Margret , Waldmann Thomas 
Published: September 2023

Compared to many other characteristics of Li-ion batteries, the safety behavior is a critical property and should be examined carefully. Especially manufacturers and most studies only focus on the safety of pristine cells. However, the safety behavior can drastically change dependent on the prior aging conditions such as ambient temperature. Especially low temperature aged cells with Li plating show a drastically decreased safety behavior [1]. Moreover, cells aged at higher temperatures with a distinct solid-electrolyte-interface (SEI) layer on the anode show an increased onset of self-heating leading to improved safety [2]. Post-Mortem analysis of aged cells confirmed the two dominating aging mechanisms: Li plating and SEI growth for low and high temperature range, respectively.
Heat-wait-seek (HWS) tests under quasi-adiabatic conditions in an accelerated rate calorimeter (ARC) are a well-known method to evaluate the safety behavior of Li-ion batteries and can reveal critical temperatures such as the onset of self-heating. HWS tests on cells aged at different temperatures until different state-of-health (SOH) reveal the trend that a more pronounced aging increases or decreases the onset of self-heating depending on whether SEI growth or Li plating is the dominating aging mechanism.
In addition to the temperature measurement, multiple sensors for voltage, resistance, strain, and ultrasonic transmission and reflection were placed on the pouch cell for a better understanding of the ongoing processes while the HWS tests. The benefit of these sensors is that they are cheap, allowing them to be widely implemented. Furthermore, an externally coupled mass spectrometer provides information about the gases produced and released after venting of the cell [3]. By Correlating different sensors signals, critical events on the way to the thermal runaway can be reliably identified or even predict in an early stage.
Hence, the HWS tests on Li-ion batteries aged at different temperatures in combination with the multi sensor study provide a comprehensive understanding of the influence of temperature dependent aging state on the safety behavior of Li-ion pouch cells.

Acknowledgment

We gratefully acknowledge the German Federal Ministry of Education and Research (BMBF) for the financial support of the projects AnaLiBa (03XP0347C) and MiCha (03XP0317C) within the AQua cluster.

References

[1] T. Waldmann, M. Wohlfahrt-Mehrens, Electrochimica Acta 230 (2017) 454–460. https://doi.org/10.1016/j.electacta.2017.02.036.
[2] M. Börner, A. Friesen, M. Grützke, Y.P. Stenzel, G. Brunklaus, J. Haetge, S. Nowak, F.M. Schappacher, M. Winter, Journal of Power Sources 342 (2017) 382–392. https://doi.org/10.1016/j.jpowsour.2016.12.041.
[3] A.A. Abd‐El‐Latif, P. Sichler, M. Kasper, T. Waldmann, M. Wohlfahrt‐Mehrens, Batteries & Supercaps 4 (2021) 1135–1144. https://doi.org/10.1002/batt.202100023.

Figure 1
High-Capacity Metal Oxide Electrodes for Lithium-Ion Batteries
Authors: Katiyar Ram S. , Oli Nischal , Florez Gomez Jose Fernando , Zuluaga Gomez Claudia , Katiyar Rajesh , Wu Xianyong , Morell Marrero Gerardo 
Published: September 2023

It is of paramount importance to develop rechargeable lithium-ion batteries (LIBs) with higher energy to meet the demands of emerging energy storage applications. Currently, LIBs use LiCoO2 as the cathode and graphite as the anode, which shows moderate capacity of ~140 mAh g-1 and ~350 mAh g-1, respectively. As a result, the energy density is limited to 120-160 Wh kg-1. In this context, we have investigated a layered-spinel material (Li2MnO3, LiMn2O4, LiNi2/3Mn1/6Co1/6O2, NMC 811,LiFePO4) as a high-capacity cathode. This cathode exhibits a theoretical capacity of ~ 250 mAh g-1, and in our preliminary work, we demonstrated a high capacity of ~ 250 mAh g-1. We also find that this cathode shows high voltage of 4.5 V and stable cycling over 50 cycles. On the anode side, we investigated BiFeO3(BFO) as a potential high-capacity anode, which delivers a high capacity of ~750 mAh g-1, double the capacity of graphite. In the following research, we will explore the possibility of assembling Li-ion full cells using these two materials in order to demonstrate high energy density.
The Li-ion storage mechanism in these two materials will also be thoroughly investigated by electrochemical and physical characterizations, such as electrochemical impedance spectroscopy (EIS), ex-situ XRD, and X-ray photoelectron spectroscopy.
Effects of Cathode Loadings on the Performance of the LiNi0.8Mn0.1Co0.1O2 Cathode in Lithium Batteries
Authors: Velasquez Kevin , Wang Xin , Meng Xiangbo 
Published: September 2023

LiNixMnyCozO2 (NMCs, x + y + z = 1) represent one promising cathode material for next-generation lithium-ion batteries (LIBs) and beyond, due to their high specific capacity and low cost.1-3 The current commercialized batteries tend to utilize high loadings of cathode materials and thin Li anodes for producing higher energy densities. However, a systematic study on the effects of cathode loadings is missing. To this end, we recently conducted a comparative study on the effects of different cathode loadings on the performance of LiNi0.8Mn0.1Co0.1O2 (NMC811). The NMC811 loading ranges from 2 – 14 mg/cm2. The resultant Li||NMC811 cells were tested for their capacity retention and sustainable capacity at different C-rates. Our study revealed that the cathode loadings have remarkably affected the cell performance. With increasing NMC811 loadings, the cells are more liable to fade in their capacity, due to a faster growth of solid electrolyte interface (SEI) on NMC811 particles and thereby a more sluggish Li-ion transportation. We also noticed that the Li anode side had remarkable effects on the Li||NMC811 cells. Particularly, we demonstrated that a polymeric surface coating via molecular layer deposition could protect the Li anode from degradation and thereby sustain Li||NMC811 cells for a better performance. Therefore, we concluded that the performance of the Li||NMC811 cells suffers from the issues of both the NMC811cathode and Li anode. It is significant to address their issues simultaneously for high performance.

References:

[1] X. Wang, J. Cai, Y. Ren, M. Benamara, X. Zhou, Y. Li, Z. Chen, H. Zhou, X. Xiao, Y. Liu, X. Meng, High-performance LiNi0.8Mn0.1Co0.1O2 cathode by nanoscale lithium sulfide coating via atomic layer deposition, Journal of energy chemistry 69 (2022) 531-540.
[2] X.W. Wang, X.B. Meng, J.S. Park, ATOMIC LAYER DEPOSITION FOR EMERGING THIN-FILM MATERIALS AND APPLICATIONS Introduction, Journal of Materials Research 35(7) (2020) 655-655.
[3] X. Meng, X.-Q. Yang, X. Sun, Emerging Applications of Atomic Layer Deposition for Lithium-Ion Battery Studies, Advanced Materials 24(27) (2012) 3589-3615.
Redox Mediator Relithiation of End-of-Life Lithium-Ion Battery Cathode Materials
Authors: Kirwa Cyrus Kibichi , Coyle Jaclyn , Luo Hongmei 
Published: September 2023

Lithium-ion batteries (LIBs) are ideal for electric vehicles and electronic devices because of their high-power density and outstanding cycle life. The need for recycled LIBs material is pivotal for the sustainability of the renewable energy industry. The recycling process needs to be both economically and environmentally conscious. Direct recycling is cheaper and generates the least amount of waste compared to pyrometallurgical and hydrometallurgical processes.
Direct recycling explored in this work is useful for reclaiming precious minerals from the End-of-Life (EOL) LIBs material. Redox mediator relithiation restores the lithium content rapidly and at low cost without sensitivity to EOL material with varying lithium deficiency. The redox mechanism relithiates EOL cathode material by shuttling charges very fast between lithium metal and EOL cathode material. The redox mediator is oxidized to create lithium rich solvent and reduced to relithiate EOL cathode material. However, the process is sensitive to pH changes. The redox reaction creates acidic solvent, which may cause lithium leaching. Therefore, use of lithium hydroxide (LiOH) to remove impurities on the surface of the EOL material and as a lithium source creates a basic solution to prevent lithium leaching and relithiate EOL material. This approach will potentially pave way for fast quality cathode material recovery at a low cost.

Figure 1
(Invited) Quantitative Measurement of the Safety Performance of Li-Ion Batteries
Authors: Kim Chisu , Perea Alexis , Rozon David , Dubé Joël 
Published: September 2023

Safety is one of the essential requirements that should be taken into account and prioritized in the course of the development phases of lithium secondary batteries for any commercial applications. Even though different safety test standards exist to simulate the electric, mechanical, and thermal abuse conditions, there are only limited methods that can be used to quantify the safety performance of the cell.
This study aims to compare the quantitative measurement techniques of safety evaluation and identify the methods to define the design parameters influencing the eventual safety performance of the full cells. The nail penetration, hot box, ARC (Accelerated Rate Calorimeter) and overcharging test are performed using the pouch cells (1-3 Ah) with different cell designs and aging conditions.
It is found that hot box and nail penetration results are well correlated with the OCV (open circuit voltage) of the cells, suggesting that the OCV threshold can be used as a new quantitative indicator of the safety performance. Using this indicator, the cells having different P/E (power-to-energy ratio) designs and different electrolyte formulations are compared to identify the conditions to promote the safety performance of the cells.

Figure 1
(Invited) Overcoming Challenges in Transitioning Electroreduction of CO2 to a Deployable Technology
Authors: Kenis Paul 
Published: September 2023

Since 2010, the electrochemical reduction of CO2 has evolved from a barely studied topic to one of the most active research areas in the field of electrochemistry. The need to reduce global CO2 emissions has driven the vigorous pursuit of different electrocatalysts, electrodes, and electrolyzer configurations that are able to reduce CO2 to different value added intermediates or products ever more selectively and efficiently. With many catalysts now available, attention has started to shift to topics such as catalyst stability, electrode durability, and electrolysis operation optimization. These efforts increasingly are tied to ever more-detailed techno-comic and life cycle analyses.
This presentation will provide an overview where some of these ‘beyond CO2RR catalyst discovery’ efforts are. What about durability of electrodes in different cell configurations? What should larger electrolyzer stack designs looks like, and how should they be operated to maximize performance (rate and/or selectivity)? How to optimize performance in light of dilute CO2 feeds from industrial point sources or from direct air capture, with these feeds containing different contaminants and/or oxygen? A separate idea is to pursue a co-conversion approach where conversion of an industrial waste stream or conversion of a renewable feed (e.g., from biomass) into a valued-added chemical on the anode is performed in parallel with electroreduction of CO2 on the cathode. This presentation will explore some of these aforementioned challenges based on our work as well as the work by others.
Modeling Chemical Microenvironments in Porous Copper Electrodes for CO2 Reduction at Elevated Current Densities
Authors: Bui Justin C , Boehme Annette , Lees Eric W. , Atwater Harry A. , Bell Alexis T. , Weber Adam Z. 
Published: September 2023

Electrochemical CO2 reduction (CO2R) presents a promising pathway toward the reuse of CO2 emitted during the production of industrial commodities (e.g., cement, steel, and plastics) to form value-added commodities and fuels at ambient temperatures and pressures with renewably generated electrons. Copper (Cu) catalysts demonstrate the ability to convert CO2 to multicarbon (C2+) products. Additionally, 3-D structured porous Cu electrodes can facilitate the operation of CO2R to C2+ at significantly elevated current densities by enhancing the delivery of CO2 to catalytic active sites on Cu, offering the potential to translate lab-scale understanding to industrial operation. Nonetheless, there still exist selectivity limitations in porous electrode systems due to poor control of the chemical microenvironment, (i.e., the local pH, CO2 activity, and CO intermediate management), in these complex electrodes. Therefore, resolving microenvironment in porous Cu electrodes will be critical to advancing these systems towards industrialization.
In this talk, we explore the use of continuum modeling to resolve and understand the effects of mass transfer and chemical environment in electrochemical CO2 reduction in porous Cu electrodes. We explore two scenarios of porous Cu electrodes performing electrochemical CO2 reduction. The first is the operation of a device employing a bipolar membrane (BPM) in reverse bias, wherein modeling reveals that the proton flux generated by the BPM substantially lowers the pH of the porous electrode and promotes selective CH4 and HCOOH generation. The second is the use of a micro-structured porous electrode that employs an anion-exchange membrane and more selectively generates C2+ products. 2-D modeling reveals heterogeneities in the porous electrode enable hotspots of increased pH that locally enhance C2+ selectivity. Ultimately, this talk underscores the powerful ability of continuum modeling to resolve microenvironments at spatial resolutions beyond what is achievable experimentally, as well as to link changes in microenvironment to changes in local selectivity. These simulations will rationalize and guide the engineering of microenvironment in next-generation porous electrodes for CO2 reduction to C2+ products at industrial scales.
Real-Time, Non-Invasive Magnetic Field Imaging for Diagnosing Current Flow Patterns inside Fault-Simulated Li-Ion Batteries
Authors: Shin Yewon , Lee Mingyu , Lee Hongkyung 
Published: September 2023

With the growing popularity of Li-ion batteries in electric-powered mobility, securing battery safety has become a common goal of the battery community. Battery failures are commonly caused by small, undetectable defects that can form during manufacturing and operation, ranging from materials to the cell level. Although the small errors inside the cells trigger catastrophic failures, tracing them and distinguishing cell failure modes without cell anatomy remains challenging. Given that several defects within the cell could cause abnormal current flow compared to the normal cells, visualization of the current inside the battery is informative to find and trace the invisible defects that cannot be detected using imaging tools for the internal structure of fully packaged commercial cells.
This study presents a real-time, non-invasive magnetic field imaging (MFI) method that can signal the magnetic field induced by battery current flow inside the Li-ion pouch cell during cycling (Figure 1). MFI can offer high-speed scanning in a few minutes (~100 mm/min) and spatially high resolution (0.161 mm2) and immediately measure the magnetic field with no need for shielding commonly required for MRI measurement. Based on the Biot-Savart law, we validated magnetic field-current correlation through the MFI of current-carrying 1D straight wires and 2D planes. Then, we found the optimal pouch cell structure for visualizing the current flow patterns using MFI and successfully converted the MFI contour map of the pouch cells into the normalized current distribution. To demonstrate the efficacy of current pattern analysis, we have collected MFI results of fault-simulated batteries (FSBs) to distinguish failure modes that intentionally possess cell manufacturing faults, such as lead-tab contact failure, electrode alignment, and stacking faults. Magnetic field offset using countercurrent-carrying, pouch cell-shaped 2D conductor underneath can selectively detect the failure spots where the current abnormally flows. It is believed that direct visualization of current distribution patterns and figuring out the pattern changes during operation can expedite the non-destructive, immediate diagnosis of commercial cells and troubleshoot safety-related challenges.

Figure 1. Single-layer pouch cells and in operando MFI analysis during charging. (a) Scheme for internal structure of single-layer pouch cell (60 × 90 mm2) with counter-side, center-aligned tabs (CS-C cell). (b) Actual image of CS-C cell and MFI scan and applied current directions during the cell charging. MFI mapping images for (c) Bx
, (d) By
and (e) Bz
vector fields at the cell. White arrows within each MFI contour map indicate the current flow prediction. Applying current density: 5.09 mA cm−2, the cell was situated 6 mm below the sensor (z-distance: 2.5 mm, scanned side: Cathode-side up). The total number of scanned data points are 1699 (11 cm) and 64 (16 cm) in y- and x-directions, respectively.

Figure 1
(Invited) Additives Approach to Improve the Performance of LiNi0.5Mn1.5O2 5V Cathodes
Authors: Liao Chen , Wang Bingning , Doan Hieu , Gim Jihyeon , Abraham Daniel P. , Son Seoung-Bum , Trask Stephen E. , Qin Yang , Jansen Andrew N. 
Published: September 2023

The high voltage spinel cathode of LiNi0.5Mn1.5O2 has an average working voltage of 4.7 V, high-rate performance with faster diffusion properties, and is viewed as one of the promising cathode materials for high energy lithium-ion batteries. The lack of Co in such cathode materials is also advantageous due to the issues of artisan mining and geopolitical tensions associated with Co mining. However, the high working voltages in LiNi0.5Mn1.5O2 exceeds the stability of electrolyte window and the redox center in the cathode materials is mainly Ni2+ while Mn stays at the 4+ charge state. Due to the dominance of the Mn elements in the cathode, acid leaching from the impurity of the electrolytes can cause Mn dissolution, and the degradation of LNMO//Gr is associated with transition metal dissolution and crosstalk to the anode side, causing loss of inventory Li loss. For example, the decomposition of ethylene carbonate leads to formation of glycolic acid and difluorophosphoric acid (HPO2F2).
Using additives in the electrolyte formulation is an economic way of improving the performance without significant change in either the processing industry or manufacturing technology, and here we present the approach of using a combinatorial approach to optimize the additives for LNMO//Gr full cells. The degradation mechanism will also be discussed. Machine learning (ML) method has been used effectively to predict molecular structures, preferred quantity, as well as formation of interfaces.1-3 In this study, we used ML to formulate the high-performance additives with both improved capacity retention and reduced initial and final impedance.

Okamoto, Y.; Kubo, Y., Ab Initio Calculations of the Redox Potentials of Additives for Lithium-Ion Batteries and Their Prediction through Machine Learning. ACS Omega
2018,
3 (7), 7868-7874.

Bhowmik, A.; Castelli, I. E.; Garcia-Lastra, J. M.; Jørgensen, P. B.; Winther, O.; Vegge, T., A perspective on inverse design of battery interphases using multi-scale modelling, experiments and generative deep learning. Energy Storage Materials
2019,
21, 446-456.

Hildenbrand, F.; Aupperle, F.; Stahl, G.; Figgmeier, E.; Sauer, D. U., Selection of Electrolyte Additive Quantities for Lithium-Ion Batteries Using Bayesian Optimization. Batteries & Supercaps
2022,
5 (7), e202200038.
Temperature-Dependent Electrochemical Impedance Spectroscopy of Li/Li Symmetric Cells and Li/MnO2 Batteries
Authors: Katırcı Gökberk , Ülgüt Burak , Civan Fazlı Eren , Zabara Mohammed 
Published: September 2023

Understanding the electrochemical properties of Lithium metal is a crucial step for developing and optimizing rechargeable batteries with lithium metal anodes. During discharge, the lithium metal is oxidized, generating dissolved lithium cations. Transport of the ions to the electrolyte is a significant part of this process. To investigate this process, temperature-dependent EIS experiments are done to independently measure the resistance due to this transport and, eventually, the activation energy.
Electrochemical Impedance Spectroscopy (EIS) is a non-destructive analysis method mainly employed for studying the characteristics of electrochemical energy storage systems. EIS can be invaluable in isolating and studying buried interfaces without physically separating individual components. The anodic process, specifically the charge transfer through the solid-electrolyte interface can be studied without any influence of the rest of the processes.
In this study, we built and measured the Potentiostatic EIS of both symmetric (Li/Li) and batteries (Li/MnO2). Button size (CR 2032) cells were constructed with different battery-grade electrolytes. A symmetric cell can isolate the processes related to metallic lithium. In contrast, a battery type (with an anode and a cathode) can differentiate the effect of the cathode on the anode. A broad range of temperatures (15ᵒC to 65ᵒC) was achieved with a Peltier-powered, homemade climate chamber. The limiting factors were selected according to the freezing and boiling temperatures of the electrolyte systems. Cycling of symmetric cells and discharging of batteries were performed, and the cells were measured after cycling/discharging.
The evaluation of the spectra as a function of temperature and states-of-charge can give a comprehensive understanding of metallic Li and the oxidation process. The resistance modeling the transport as well as the capacitance values were investigated as functions of temperature. The change in resistance values at different temperatures resulted in not only Arrhenius behavior but also regions where Arrhenius behavior is violated.
Interpretation of the temperature dependence provides a detailed understanding of the underlying electrochemical phenomena involving the metallic lithium anode. The effect of electrolytes on Li+ conductance can also be interpreted from the achieved results.