Article
Chemistry, Physical
Hideaki Oka, Takamasa Nonaka, Yasuhito Kondo, Yoshinari Makimura
Summary: In this study, an electrochemical cell capable of controlled overcharging and temperature regulation is developed, and the reactions between the electrodes and the electrolyte are investigated during heated overcharging. The results show that higher temperatures during overcharging lead to increased side reactions in the positive electrode, while the negative electrode gradually increases side reactions with increasing temperature in the normal charge-discharge region. The side reactions are induced by the oxidative decomposition of the electrolyte at the positive electrode.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Physical
Hyuntae Lee, Hyeongguk An, Hongjun Chang, Mingyu Lee, Seungsoo Park, Soyeon Lee, Jiwoong Kang, Seungwoo Byon, Bonhyeop Koo, Hochun Lee, Yong Min Lee, Janghyuk Moon, Sujong Chae, Hongkyung Lee
Summary: This study explores the safety risks of fast charging for Li-ion batteries and proposes a new electrolyte design to improve the cycling performance and capacity retention of the batteries.
ENERGY STORAGE MATERIALS
(2023)
Article
Green & Sustainable Science & Technology
Fathima Ali Kayakool, Binitha Gangaja, Shantikumar Nair, Dhamodaran Santhanagopalan
Summary: The recycling and regeneration of graphite from spent Li-ion batteries can be utilized for the fabrication of Li-ion based all-carbon dual-ion batteries, achieving promising electrochemical performance.
SUSTAINABLE MATERIALS AND TECHNOLOGIES
(2021)
Article
Chemistry, Physical
Lorenzo Mezzomo, Nicolo Pianta, Irene Ostroman, Niv Aloni, Diana Golodnitsky, Emanuel Peled, Piercarlo Mustarelli, Riccardo Ruffo
Summary: New generation lithium batteries require better performances, improved safety, and sustainability. Deep Eutectic Solvents (DESs) made with 2,2,2-trifluoroacetamide (TFA) and LiPF6 show promise as safer and more environmentally sustainable electrolyte components. The DES composition tested against Li metal, LiFePO4 (LFP), and high voltage LiNi1-x-yMnxCoyO2 (NMC) demonstrates good electrochemical performance and improved thermal stability compared to a commercial liquid electrolyte.
JOURNAL OF POWER SOURCES
(2023)
Review
Chemistry, Multidisciplinary
Wei Zhong, Ziqi Zeng, Shijie Cheng, Jia Xie
Summary: Prelithiation technology is one of the most effective methods to compensate for the loss of active lithium. This review analyzes the factors inducing lithium loss and investigates the mechanisms and effects of prelithiation. The emerging advanced prelithiation technologies and key issues are systematically summarized. Hybrid replenishment and lithium storage technologies are proposed to provide a reference for developing prelithiation technology.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
M. Henriksen, K. Vaagsaether, J. Lundberg, S. Forseth, D. Bjerketvedt
Summary: The study investigates the laminar burning velocity of gas compositions associated with Li-ion battery failures, ranging from 300 to 1050 mm/s, and the accuracy of different reaction models in predicting these velocities. The results can be used in safety engineering models and provide recommendations for choosing reaction models to predict burning velocities for various gas compositions.
JOURNAL OF POWER SOURCES
(2021)
Article
Electrochemistry
Brendan E. Hawkins, Harrison Asare, Brian Chen, Robert J. Messinger, William West, John-Paul Jones
Summary: This study investigates the failure mechanisms of lithium-ion batteries (LIBs) operating at 100 degrees C, identifies the causes of capacity fade, and demonstrates the potential of electrode replacement for improving performance at high temperatures. The findings are expected to guide the development of electrolyte formulations to enhance electrode interphase stability and enable the use of LIBs at temperatures as high as 100 degrees C.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Madhusoodhanan Lathika Divya, Yun-Sung Lee, Vanchiappan Aravindan
Summary: The intercalation of Li into graphite is crucial in energy storage mechanisms. Research on co-intercalation has shown potential for effective recycling of spent LIBs.
BATTERIES & SUPERCAPS
(2021)
Article
Chemistry, Physical
Elna J. K. Nilsson, Christian Brackmann, Annika Ahlberg Tidblad
Summary: With the increasing use of battery electric vehicles, fire incidents involving Li-ion batteries have become a growing concern. This study aims to enhance the understanding of the combustion process of gas mixtures vented from Li-ion batteries. Using simulation of ignition and laminar flames, the research reveals significant variations in laminar burning velocity, flame temperature, and heat release for different gas mixtures. Factors such as the content of carbonates, hydrogen gas, and inert carbon dioxide are found to be influential in laminar flames.
JOURNAL OF POWER SOURCES
(2023)
Review
Chemistry, Multidisciplinary
Zhiming Zhao, Husam N. Alshareef
Summary: This review provides an extensive overview of the current status and future prospects of sustainable dual-ion batteries beyond Li-ion. These new batteries utilize abundant and low-cost cations, holding significant promise for large-scale energy storage solutions.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Huarong Xia, Yuxin Tang, Oleksandr I. Malyi, Zhiqiang Zhu, Yanyan Zhang, Wei Zhang, Xiang Ge, Yi Zeng, Xiaodong Chen
Summary: A new deep-cycling architecture has been developed to break the theoretical capacity limit of conventional Li-ion batteries, which offers higher capacity and energy storage efficiency by utilizing movable ions in both electrolyte and electrodes. This architecture shows 57.7% more capacity and 84.4% retention after 2000 cycles, indicating its potential for next-generation energy storage devices.
ADVANCED MATERIALS
(2021)
Review
Chemistry, Physical
Xin Cao, Yu Qiao, Min Jia, Ping He, Haoshen Zhou
Summary: This study reviews the potential application of Li-rich and Li-excess oxides as cathode materials for next-generation Li-ion batteries, discusses the challenges in using Li-excess oxides, and explores mechanisms to address these issues. Future research directions in the field are also proposed based on advanced characterizations and theory calculations.
ADVANCED ENERGY MATERIALS
(2022)
Article
Nanoscience & Nanotechnology
Naijie Wang, Xiangqun Chen, Qiu Sun, Ying Song, Tiezhu Xin
Summary: A self-standing and flexible polyurethane-based single-ion conductor membrane was prepared by tethering the trifluoromethanesulfonamide anion to polyurethane. The polymer electrolyte exhibited excellent ionic conductivity, mechanical properties, lithium-ion transfer number, thermal stability, and a broad electrochemical window. Consequently, the plasticized electrolyte membrane showed exceptional stability and reliability in a Li||Li symmetric battery.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Shiyuan Zhou, Qizheng Zheng, Shi Tang, Shi-Gang Sun, Hong-Gang Liao
Summary: Li metal batteries (LMBs) have great potential for next-generation energy storage due to their high energy density and low electrochemical potential. The formation/dissolution of Li metal at the solid-electrolyte interface (SEI) layer has been a major concern, as it leads to battery degradation in practical conditions. In the past decade, in situ electrochemical transmission electron microscopy (EC-TEM) has been developed to track the reactions at the electrode/electrolyte interfaces. This perspective provides a brief introduction to liquid cell development, discusses different configurations of EC-TEM, and focuses on recent advances and future prospects of liquid-cell EC-TEM for LMB research.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Jae Yeon Yoo, Tae Yeong Kim, Dong-Min Shin, Yongku Kang, Mi Hye Wu, Yun Chan Kang, Do Youb Kim
Summary: Lithium (Li) composites with Li-ionic conductive Al-doped Li7La3Zr2O12 (LLZO) particles (Li/LLZO) are fabricated using a mechanical kneading process. These composites effectively regulate the Li-ion flux and suppress the Li dendritic growth by creating faster pathways for Li-ion migration. As a result, Li-metal-based cells utilizing the Li/LLZO composite anodes demonstrate significantly enhanced cycle stability compared to cells employing pure Li anodes.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Anna T. S. Freiberg, Simon Qian, Johannes Wandt, Hubert A. Gasteiger, Ethan J. Crumlin
Summary: A new operando spectro-electrochemical setup was developed to study oxygen depletion from the surface of layered transition metal oxide particles at high degrees of delithiation. By analyzing the O 1s spectra of the particles and comparing it to the Ni 2p3/2 intensity, the metal-to-oxygen ratio of the metal oxide close to the particle surface can be calculated, providing insight into the formation of an oxygen-depleted phase. This new setup enables a deeper understanding of interfacial changes of layered oxide-based cathode active materials for Li-ion batteries upon cycling.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Electrochemistry
Stefan Oswald, Hubert A. Gasteiger
Summary: The composition of layered transition metal oxides as cathode active materials is trending towards higher nickel contents for increased capacity and energy. The stability of these materials at high degrees of delithiation is determined by their composition, rather than the stability window of the electrolyte. Short-term cycling experiments and online electrochemical mass spectrometry reveal that capacity fade and lattice oxygen release are concurrent processes contributing to CAM degradation.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Clara Berg, Robert Morasch, Maximilian Graf, Hubert A. Gasteiger
Summary: A comparison is made between graphite and microsilicon anodes in terms of their temperature-dependent kinetic charge-transfer resistances and ion transport resistances. It is found that the charge-transfer resistance dominates at low temperatures, while at high temperatures, the pore resistance dominates for both electrode types. Additionally, when fast-charging, the thinner silicon electrode has lower overpotentials due to lower ion transport losses in the electrolyte phase.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Tom Boetticher, Anu Adamson, Sebastian Buechele, Ethan D. Alter, Michael Metzger
Summary: This study investigates the impact of dimethyl terephthalate (DMT) as a redox shuttle molecule on lithium-ion battery performance. The results show that DMT lowers the coulombic efficiency, increases the charge endpoint capacity slippage, and dramatically accelerates the reversible self-discharge of LFP/graphite pouch cells. Gas chromatography-mass spectrometry analysis reveals that DMT is stable over weeks in cells with LiPF6, but only for several days in cells with LiFSI. A well-insulating solid-electrolyte interphase layer derived from vinylene carbonate can prevent DMT from shuttling. However, alternative measures such as eliminating PET components would be the best way to prevent DMT-induced self-discharge of lithium-ion batteries.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Tobias Teufl, Daniel Pritzl, L. Hartmann, Sophie Solchenbach, Manuel A. Mendez, Hubert A. Gasteiger
Summary: Fluoroethylene-carbonate (FEC) is commonly used in lithium-ion batteries as a co-solvent for high-voltage cathodes and silicon-based anodes. However, its limited thermal stability when used with LiPF6 can trigger detrimental side reactions, producing vinylene-carbonate (VC) and HF at elevated temperatures. These side reactions not only increase impedance but also lead to transition metal dissolution. Comparatively, FEC has no advantage over ethylene-carbonate (EC) in high-voltage operation without lattice oxygen evolution. Extended charge/discharge cycling at 45 degrees C shows that the thermal decomposition of FEC leads to cell bulging due to the oxidation of VC above approximately 4.4-4.5 V vs. Li+/Li.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Franziska Friedrich, Alexander Kunz, Andreas Jossen, Hubert A. Gasteiger
Summary: Using isothermal micro-calorimetry, the heat generation of lithium- and manganese-rich layered oxides (LMR-NCMs) during the first cycle is investigated. It is found that irreversible structural rearrangements during activation lead to a considerable generation of heat. Only a fraction of the lost electrical work is converted into waste heat, suggesting that the heat flow profile of the first charge is unique.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Christian Sedlmeier, Robin Schuster, Carina Schramm, Hubert A. Gasteiger
Summary: Impedance measurements are a powerful tool to investigate interfaces in lithium-ion batteries. This study presents a straightforward approach to implement a micro-reference electrode (mu-RE) for electrode-resolved impedance and potential measurements in all-solid-state batteries. The mu-RE consists of an insulated gold wire sandwiched between two Li6PS5Cl/polymer separator sheets and is activated by in situ electrochemical lithiation. The results show the importance of the cell assembly configuration in providing a reservoir of cyclable lithium.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Robert Morasch, Hubert A. Gasteiger, Bharatkumar Suthar
Summary: The proposed expression for the exchange current density has been widely used for modeling Li-ion battery materials, but its applicability needs validation. In this study, the kinetic behavior of NCM 111 was analyzed using EIS and compared with the proposed theory. The results show that the charge transfer kinetics follow the proposed theory for lower concentrated electrolytes, but deviate at higher salt concentrations.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Rafael B. Berk, Thorsten Beierling, Lukas Metzger, Hubert A. Gasteiger
Summary: This study investigates the influence of the hydroxide precursor on the physical properties of cathode active material (CAM) for lithium-ion batteries during industrial production. The evolution of secondary particle size and morphology of Ni0.8Co0.1Mn0.1(OH)2 during coprecipitation is observed, revealing a two-stage particle formation mechanism: seeding phase and growth phase. The degree of turbulence in the seeding phase affects the size and number of seeds, which subsequently influences the growth rate and morphology of the secondary particles.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Secil Unsal, Michele Bozzetti, Yen-Chun Chen, Robin Girod, Anne Berger, Justus S. Diercks, Sofia Gialamoidou, Jike Lyu, Marisa Medarde, Hubert A. Gasteiger, Vasiliki Tileli, Thomas J. Schmidt, Juan Herranz
Summary: Non-noble metal catalysts (NNMCs) are a promising alternative to expensive Pt-based materials for catalyzing the oxygen reduction reaction (ORR) in proton exchange membrane fuel cell (PEMFC) cathodes. By studying catalysts with different particle sizes and porosities, it was found that smaller aggregate size and higher porosity lead to improved mass transport properties and peak power density.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Hussein Hijazi, Ziwei Ye, Libin Zhang, Jay Deshmukh, Michel B. Johnson, Jeff R. Dahn, Michael Metzger
Summary: This study investigates the cycling performance and failure mechanisms of sodium-ion pouch cells with layered NaCa0.03[Mn0.39Fe0.31Ni0.22Zn0.08]O-2 positive electrodes and hard carbon negative electrodes. The results show that limiting the upper cut-off voltage to 3.80 V improves capacity retention, reduces voltage polarization, and lowers gas generation. The failure analysis reveals that the charge transfer resistance of the negative electrode dominates the impedance of the full cell.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Yan-Sheng Li, Davide Menga, Hubert A. Gasteiger, Bharatkumar Suthar
Summary: In this study, the impact of electronic resistance on the performance of PGM-free CCLs in PEMFCs was investigated. It was found that adding carbon additives can significantly improve fuel cell performance. Four-point probe measurements revealed a significant difference in resistance between the in-plane and through-plane direction of the CCLs, attributed to the anisotropic morphology of the CCLs.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Anne Berger, Yen-Chun Chen, Jacqueline Gatzemeier, Thomas J. Schmidt, Felix N. Buechi, Hubert A. Gasteiger
Summary: This study aims to analyze the impact of fabricating a GDL with an MPL that intrudes into the GDL-S on the structure of GDL-S and PEMFC performance. The results provide design guidelines for improved GDLs.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Anu Adamson, Kenneth Tuul, Tom Botticher, Saad Azam, Matthew D. L. Garayt, Michael Metzger
Summary: Polyethylene terephthalate (PET) tape, widely used in lithium-ion batteries, has been found to have chemical instability. This study demonstrates that replacing PET with chemically stable polypropylene tape can effectively eliminate reversible self-discharge in LiFePO4-graphite cells.
Article
Electrochemistry
Rafael B. Berk, Thorsten Beierling, Lukas Metzger, Hubert A. Gasteiger
Summary: This study investigates the relationship between residual sulfur content, crystallinity, and the pH value during the synthesis of Ni0.8Co0.1Mn0.1(OH)2, as well as the inhibition of crystallite growth due to sulfate adsorption. Adsorption/desorption experiments demonstrate the possibility to decouple secondary particle morphology and residual impurity content.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)