Article
Chemistry, Physical
Kristoffer Visti Graae, Xinyu Li, Daniel Risskov Sorensen, Elixabete Ayerbe, Iker Boyano, Denis Sheptyakov, Mads Ry Vogel Jorgensen, Poul Norby
Summary: Silicon-graphite blended electrodes in Li-ion batteries have been investigated to utilize the high capacity of Si while minimizing the negative effects of volume expansion. NMC 811 is an advanced layered oxide cathode material with reduced cobalt content. These two materials show great potential in achieving electric vehicle targets, but their degradation mechanism is not completely understood. In this study, 5 Ah prototype multi-layer pouch cells were fabricated using these materials and studied using neutron and synchrotron X-ray diffraction techniques. The results reveal inhomogeneities across both electrodes during degradation, which are related to the inhomogeneous volume expansion of the Si-graphite anodes.
JOURNAL OF POWER SOURCES
(2023)
Article
Electrochemistry
Calvin D. Quilty, Patrick J. West, Garrett P. Wheeler, Lisa M. Housel, Christopher J. Kern, Killian R. Tallman, Lu Ma, Steven Ehrlich, Cherno Jaye, Daniel A. Fischer, Kenneth J. Takeuchi, David C. Bock, Amy C. Marschilok, Esther S. Takeuchi
Summary: This study investigates the degradation of the cathode in NMC811/graphite batteries under extreme fast charging conditions. The results show that the oxidation state of Ni and Co changed more significantly under a 1C charge rate, but no surface reconstruction of NMC was observed in the recovered electrodes. Furthermore, a greater contraction of the unit cell volume under the 1C rate may reduce structural distortion caused by delithiation.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Energy & Fuels
Chongming Wang, Tazdin Amietszajew, Ruth Carvajal, Yue Guo, Zahoor Ahmed, Cheng Zhang, Gregory Goodlet, Rohit Bhagat
Summary: This study reveals the poor cold aging performance and subsequent premature end-of-life of NMC811, mainly due to lithium plating at the anode side during the charging process.
Article
Electrochemistry
M. A. Cabanero, M. Hagen, E. Quiroga-Gonzalez
Summary: High spatial resolution in-operando Raman spectroscopy was used to study lithium deposition on graphite electrodes, showing that lithium is deposited and intercalated into graphite simultaneously. After 30 minutes, a second mechanism becomes dominant. The evolution of G and D bands of graphite and the lithium concentration in the electrolyte suggest that EC is slowly consumed after lithium plating begins.
ELECTROCHIMICA ACTA
(2021)
Article
Chemistry, Physical
Jinkun Wang, Yun Gao, Jianhong Liu, Hongying Liao, Li Wang, Xiangming He
Summary: This study investigates the phase evolution and Li+ diffusion kinetics in lithium-ion batteries through operando X-ray diffraction. By analyzing the behavior and structural changes of NCM811/Graphite cells at different C-rates, practical suggestions for real-time monitoring and identification of electrode state, materials and electrode structural design, and optimization of charging/discharging protocols are proposed.
Article
Chemistry, Physical
Maximilian Becker, Wengao Zhao, Francesco Pagani, Claudia Schreiner, Renato Figi, Walid Dachraoui, Rabeb Grissa, Ruben-Simon Kuehnel, Corsin Battaglia
Summary: The compatibility of LiNi0.8Mn0.1Co0.1O2 (NMC811) with non-flammable water-in-salt electrolytes is investigated. It is found that the enhanced salt concentration effectively diminishes degradation phenomena and that self-discharge reactions lead to irreversible capacity losses.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Nanoscience & Nanotechnology
Hao Wu, Lihua Zheng, Ning Du, Bowen Sun, Jie Ma, Yingying Jiang, Jiadong Gong, Huan Chen, Lianbang Wang
Summary: The rational design of compact graphite/Si/SiO2 ternary composites enhances packing density and leads to higher areal capacity compared to pure graphite. Introducing Si/SiO2 clusters into void spaces between graphite particles provides an effective strategy for implementing graphite-Si composite anodes in next-generation Li-ion cells.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Electrochemistry
Fang Nan, Wanting Li, Liying Cen, Wenlian Wang, Linan Zhou, Yuanfu Deng
Summary: By using calculation and electrochemical methods, two functional electrolytes containing additives 2-proparylene methane sulfonate (2PMS) and 2-proparylene benzene sulfonate (2PBS) were developed to enhance the long-cycle performance of LiNi0.8Co0.1Mn0.1O2 (NCM811)/graphite batteries. These additives improved the cycling lifetime, rate capability, low temperature discharge, and high temperature calendar performance of the batteries. The study demonstrates the effectiveness of electrolytes with 2PMS (or 2PBS) in NCM811/graphite batteries and provides insights for developing sulfonate-based additive functionalized electrolytes.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Chaoqi Wang, Rui Wang, Zhongyuan Huang, Mihai Chu, Wenhai Ji, Ziwei Chen, Taolue Zhang, Jingjun Zhai, Huaile Lu, Sihao Deng, Jie Chen, Lunhua He, Tianjiao Liang, Fangwei Wang, Jun Wang, Yonghong Deng, Weihua Cai, Yinguo Xiao
Summary: Utilizing in operando neutron diffraction technique, structural characteristics and lithium ion migration pathways of electrodes in LiNi0.5Co0.2Mn0.3O2 /Graphite full cell were revealed. The competition effect between delithiation and magnetic frustration affects the concentration of Li/Ni antisite defects in the cathode, while lithium ions diffuse via different hopping paths in different stages of charge. The study provides insights for designing an optimized pathway for achieving high-performance Li-ion batteries.
ENERGY STORAGE MATERIALS
(2022)
Article
Chemistry, Physical
Jiafeng Gao, Songlin Zuo, He Liu, Qiwen Jiang, Chenhao Wang, Huanhuan Yin, Ziqi Wang, Jie Wang
Summary: In this study, an interconnected hollow Si-C nanospheres/graphite composite was fabricated to improve the performance of Si anode. The composite anode exhibited high specific capacity, excellent rate performance, and cycling stability, attributed to the high electrical conductivity and buffering effect of graphite, as well as the good compatibility and uniform distribution of hollow Si-C nanospheres and graphite.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Article
Electrochemistry
Marzi Barghamadi, Thomas Ruether, Christian Lechtenfeld, Adam S. Best
Summary: Adding 10%-25% silicon to graphite composite anodes can increase the practical energy density and performance of lithium-ion batteries. Different electrolyte formulations, including ionic liquid-based electrolytes, showed superior performance. The use of ionic liquid-based electrolytes improved safety but slightly reduced discharge capacity. When in contact with ionic liquid-based electrolytes, the cathode temperature increased while the anode temperature decreased, resulting in higher heat generation.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Hongsen Li, Zhengqiang Hu, Qingtao Xia, Hao Zhang, Zhaohui Li, Huaizhi Wang, Xiangkun Li, Fengkai Zuo, Fengling Zhang, Xiaoxiong Wang, Wanneng Ye, Qinghao Li, Yunze Long, Qiang Li, Shishen Yan, Xiaosong Liu, Xiaogang Zhang, Guihua Yu, Guo-Xing Miao
Summary: Research has found that cobalt oxide has larger storage capacity in lithium-ion batteries. The anomalous capacity is associated with the formation of a spin capacitor and the growth of a polymeric film. Operando magnetometry technology provides direct evidence of the catalytic role of metallic cobalt in assisting the polymeric film formation.
ADVANCED MATERIALS
(2021)
Review
Energy & Fuels
Dan Zhang, Weizhuo Zhang, Shengrui Zhang, Xiaohui Ji, Le Li
Summary: This article reviews the synthesis methods and composite strategies of expanded graphite in high-performance lithium-based batteries, and introduces the latest research findings on expanded graphite-based composite materials. The important role of expanded graphite-based composite materials in this field is emphasized, and the remaining challenges are discussed to accelerate the advancement and commercialization of lithium-based battery technology.
JOURNAL OF ENERGY STORAGE
(2023)
Article
Green & Sustainable Science & Technology
Ke Xu, Xiaohan Li, Xuefeng Liu, Yingjie Yu, Xin Zhang, Wen Lei, Zhengwei Xie, Shaowei Zhang, Quanli Jia, Haijun Zhang
Summary: Si-based materials are highly promising candidates for high performance Li-ion batteries, and Si/graphite anode is commonly used to enable commercial applications. However, the poor interfacial bonding strength and limited ability to relieve volume expansion of silicon hinder the cycle performance. In this study, a novel Si-based anode structure with a double protective layer, combining inner graphite and outer TiC, is introduced to improve electrical conductivity, alleviate volume expansion, and suppress side reactions. The Si@G@TiC electrode demonstrates significantly improved cycling performance and retains 85% capacity after 300 cycles at 0.2 A g-1.
SUSTAINABLE MATERIALS AND TECHNOLOGIES
(2023)
Article
Chemistry, Multidisciplinary
Wandi Wahyudi, Viko Ladelta, Leonidas Tsetseris, Merfat M. Alsabban, Xianrong Guo, Emre Yengel, Hendrik Faber, Begimai Adilbekova, Akmaral Seitkhan, Abdul-Hamid Emwas, Mohammed N. Hedhili, Lain-Jong Li, Vincent Tung, Nikos Hadjichristidis, Thomas D. Anthopoulos, Jun Ming
Summary: This study reveals the key role of additives in promoting cation desolvation, further demonstrating the importance of nitrate anions in improving battery performance.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Physical
Burak Aktekin, Guiomar Hernandez, Reza Younesi, Daniel Brandell, Kristina Edstrom
Summary: The highly concentrated electrolyte system LiFSI:EC shows excellent electrochemical performance and stability in various cell configurations, including high-capacity and high-voltage electrodes. It exhibits superior conductivity and passivation ability, leading to improved performance in Li-metal-Si/graphite cells and NMC111-Si/graphite cells. However, it shows less compatibility with the high-voltage spinel LNMO electrode.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Physical
Florian Gebert, Matilde Longhini, Fosca Conti, Andrew J. Naylor
Summary: The rapid adoption of lithium-ion batteries, especially in transportation, has raised concerns about their safety, particularly regarding the flammable liquid electrolyte. This study identified and tested eight promising non-flammable liquid electrolytes, finding that the phosphorus-free fluorinated solvents outperformed the phosphate and phosphonate-based solvents in terms of performance and capacity retention.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Physical
Wessel W. A. van Ekeren, Marcelo Albuquerque, Gustav Ek, Ronnie Mogensen, William R. Brant, Luciano T. Costa, Daniel Brandell, Reza Younesi
Summary: To enhance battery safety, the development of non-flammable electrolytes is crucial. A new concept in this field is the use of localized highly concentrated electrolytes (LHCEs), which have lower viscosity, improved conductivity, and reduced costs compared to highly concentrated electrolytes (HCEs) due to the addition of diluent solvents. This study investigates the solvation structures of LHCEs using Raman spectroscopy and NMR spectroscopy, and molecular dynamics simulations reveal the formation of a highly concentrated Li+-TEP solvation sheath that can be protected by the diluents TTE and BTFE. The electrochemical performances of the LHCEs are evaluated in various cell configurations, with the TTE-based electrolyte performing better in full-cells and Li-metal cells compared to the BTFE-based electrolyte.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Abdolkhaled Mohammadi, Sabrine Djafer, Syreina Sayegh, Andrew J. Naylor, Mikhael Bechelany, Reza Younesi, Laure Monconduit, Lorenzo Stievano
Summary: Although lithium metal and anode-free rechargeable batteries (LMBs and AFBs) have great potential as energy storage systems, the formation of high-surface lithium deposits during plating-stripping cycles hinders their practical applications. Efforts have been made to prevent this issue, such as electrolyte modification and electrode surface modification. However, the evaluation of battery performance using Coulombic efficiency (CE) is challenging due to various parameters. This study aims to reveal the interplay of several overlooked parameters and provide insights into the evaluation methods for LMBs and AFBs.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Hangning Liu, Runmeng Liu, Yingjun Ma, Lin Wang, Changhui Sun, Tong Xu, Haidong Liu, Jie Wang
Summary: This study proposes a simple in-situ strategy for the construction of high-dispersive cobalt oxide nanoneedle arrays on a copper foam substrate. The resulting CoO arrays serve as binder-free anodes in lithium-ion batteries, leading to outstanding rate capability and superior long-term cycling stability. This approach streamlines the electrode fabrication steps and holds significant promise for the future development of the battery industry.
Article
Electrochemistry
Florent Mohimont, Ronan Le Ruyet, Reza Younesi, Andrew J. J. Naylor
Summary: Alloy electrodes with high energy density are gaining interest in the field of Li-ion batteries, but they suffer from rapid pulverization and disconnection due to large volume changes. Ga-based liquid alloys, such as galinstan, have been studied as self-healing electrodes due to their ability to store Li and remain in a liquid state at room temperature. However, the lithiation mechanism and practical capacity of galinstan are still unknown. This study used electrochemical measurements, XRD, and SEM analyses to investigate the redox processes and structural properties of galinstan as an electrode material.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Yu-Chuan Chien, Haidong Liu, Ashok S. Menon, William R. Brant, Daniel Brandell, Matthew J. Lacey
Summary: The intermittent current interruption (ICI) method is proposed as a reliable, accurate, and faster alternative to the galvanostatic intermittent titration technique (GITT) for determining Li+ diffusion coefficients. Experimental measurements show that ICI and GITT methods provide consistent results under the assumption of semi-infinite diffusion.
NATURE COMMUNICATIONS
(2023)
Article
Electrochemistry
Girish D. D. Salian, Alma Mathew, Ritambhara Gond, Wessel van Ekeren, Jonathan Hojberg, Christian Fink Elkjaer, Matthew J. J. Lacey, Satu Kristiina Heiskanen, Daniel Brandell, Reza Younesi
Summary: This study investigates a 1 M lithium bis(fluorosulfonyl) imide (LiFSI) electrolyte in sulfolane (SL) without ethylene carbonate for LiNi0.5Mn1.5O4-graphite full-cells. The focus is on evaluating the anodic stability of the SL electrolyte and the passivation layers formed on LiNi0.5Mn1.5O4 (LNMO) and graphite, along with resistance measurements using intermittent current interruption (ICI) technique during cycling. The results show that the sulfolane electrolyte degrades more at higher potentials, contradicting previous reports of higher oxidative stability. However, the formed passivation layers due to electrolyte degradation prevent further degradation. The study provides new insights into the oxidative/anodic stability of sulfolane-based electrolyte.
BATTERIES & SUPERCAPS
(2023)
Article
Electrochemistry
Ali Jamal, Girish D. Salian, Alma Mathew, Wandi Wahyudi, Rodrigo P. Carvalho, Ritambhara Gond, Satu Kristiina Heiskanen, Daniel Brandell, Reza Younesi
Summary: This study presents the use of TMSPi and LiDFOB as film-forming additives in a conventional LiPF6-containing carbonate-based electrolyte solution to suppress the degradation of high-voltage lithium-ion battery electrolytes. TMSPi oxidizes on the LNMO cathode surface to form a stable cathode electrolyte interphase (CEI) layer, while LiDFOB has the potential to form a solid electrolyte interphase (SEI) on the graphite anode surface. The combination of these two additives effectively inhibits electrolyte degradation and improves capacity retention of high-voltage LIBs.
Article
Electrochemistry
Mads C. Heintz, Jekabs Grins, Aleksander Jaworski, Gunnar Svensson, Thomas Thersleff, William R. Brant, Rebecka Lindblad, Andrew J. Naylor, Kristina Edstrom, Guiomar Hernandez
Summary: Silicon powder kerf loss from diamond wire sawing can be used as a raw material for lithium-ion battery negative electrodes. The kerf particles contain approximately 50% amorphous silicon. Thorough investigation of the amorphicity and other relevant features was conducted. In-situ X-ray powder diffraction experiments demonstrated the significance of the powders for battery applications.
Article
Chemistry, Multidisciplinary
Yonas Tesfamhret, Haidong Liu, Erik J. Berg, Reza Younesi
Summary: Transition metal (TM) dissolution is influenced by cathode-electrolyte interaction and affects both the loss of redox-active material from the cathode and the stability of the solid electrolyte interphase (SEI) at the counter electrode. The limited anodic stability of typical carbonate-based electrolytes, specifically ethylene carbonate (EC), poses challenges for high-voltage cathode performance. Tetramethylene sulfone (SL) has been used as a co-solvent to investigate the TM dissolution behavior of LiN0.8C0.17Al0.03 (NCA) and LiMn2O4 (LMO) as a more anodically stable substitute for EC. Electrolytes containing SL show reduced TM dissolution compared to EC, but they have lower cycling stability due to their reduced ability to support Li-ion transport.
Article
Chemistry, Multidisciplinary
Le Anh Ma, Alexander Buckel, Andreas Hofmann, Leif Nyholm, Reza Younesi
Summary: Knowledge about capacity losses related to the solid electrolyte interphase (SEI) in sodium-ion batteries (SIBs) is still limited. This study investigates capacity losses caused by changes in the SEI layer under different electrolyte conditions, and finds that the amount of capacity lost depends on the interplay between the electrolyte chemistry and the thickness and stability of the SEI layer.
Article
Chemistry, Physical
Felix Massel, Burak Aktekin, Yi-Sheng Liu, Jinghua Guo, Magnus Helgerud Sorby, Daniel Brandell, Reza Younesi, Maria Hahlin, Laurent-Claudius Duda
Summary: This study investigated the first lithiation cycle of the positive electrode material LNMO using XAS and RIXS techniques. The results revealed that charge compensation in LNMO primarily occurs within the Ni-O bonds. RIXS analysis provided insights into the distribution of holes between Ni and O ions during delithiation. Additionally, the study highlighted the presence of non-trivial anionic activity.
Article
Chemistry, Physical
Lars Olow Simon Colbin, Charles Aram Hall, Ahmed S. Etman, Alexander Buckel, Leif Nyholm, Reza Younesi
Summary: This article investigates the impact of different electrolyte solutions on the anodic dissolution or passivation of aluminum in sodium-ion batteries. It is found that the type of electrolyte is critical for the presence of anodic dissolution, while the solvent alters the dissolution process.
