Article
Chemistry, Physical
Yuchen Li, Xueying Zheng, Zhang Cao, Yan Wang, Yueyue Wang, Linze Lv, Weibo Huang, Yunhui Huang, Honghe Zheng
Summary: The commercialization of silicon anodes in lithium-ion batteries has been hindered by their low Coulombic efficiency and poor cycling stability. In this study, Li-trapping is identified as a major factor affecting the initial efficiency and stability of silicon anodes. Trapped active Li accounts for about 40% of the irreversible capacity, while trapped inactive Li contributes to about 75% of the total capacity loss after 20 cycles.
ENERGY STORAGE MATERIALS
(2023)
Article
Engineering, Mechanical
Riccardo De Pascalis, Federico Lisi, Gaetano Napoli
Summary: Mechanical instabilities of the solid electrolyte interphase (SEI) layer can lead to battery degradation. The large deformations imposed by rubbery-based electrodes during lithiation and delithiation can cause interphase mechanical instabilities. By considering the theory of nonlinear elasticity and conducting simulations, the critical electrode radius for the instability to occur can be determined. Incorporating the heterogeneity hypothesis of a bilayer SEI improves the model and warns of the errors that can occur by neglecting the microstructure of the shell layer.
EXTREME MECHANICS LETTERS
(2023)
Article
Electrochemistry
Peter J. Weddle, Evan Walter Clark Spotte-Smith, Ankit Verma, Hetal D. Patel, Kae Fink, Bertrand J. Tremolet de Villers, Maxwell C. Schulze, Samuel M. Blau, Kandler A. Smith, Kristin A. Persson, Andrew M. Colclasure
Summary: Understanding and controlling solid-electrolyte interphase (SEI) formation is crucial for the stability of next-generation Li-ion battery technologies. This study develops a continuum-level model informed by first-principle calculations to understand electrolyte degradation and the growth trends of SEI. The model shows good agreement with experimental results and is expected to accelerate our understanding of SEI formation.
ELECTROCHIMICA ACTA
(2023)
Article
Nanoscience & Nanotechnology
Hui Wang, Mouren Miao, Hui Li, Yuliang Cao, Hanxi Yang, Xinping Ai
Summary: By forming an artificial solid electrolyte interphase (ASEI) on the surface of ferrosilicon/carbon (FeSi/C) anode through a designed nucleophilic reaction of polysulfides with vinylene carbonate (VC) and fluoroethylene carbonate (FEC) molecules, it effectively prevents electrolyte infiltration and decomposition while enabling Li+ transport, thus stabilizing the FeSi/C anode interface. The ASEI-modified FeSi/C anode exhibits a large reversible capacity, excellent cycling stability, and greatly elevated cycling coulombic efficiency, potentially serving as a high-capacity anode of LIBs.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Hungu Kang, Soo Jin Cho, Gyu Don Kong, Hyo Jae Yoon
Summary: This paper describes the effect of Li-ion intercalation into a pyrenyl-terminated self-assembled monolayer (SAM) on tunneling performance in a molecular junction. The rectification ratio increased with the concentration of the Li-ion precursor, while treatment with high concentrations of Li-ion resulted in the disappearance of rectification due to the formation of a solid electrolyte interphase (SEI) on the surface of the SAM.
Article
Chemistry, Multidisciplinary
Liang Zhao, Danfeng Zhang, Yongfeng Huang, Kui Lin, Likun Chen, Wei Lv, Yan-Bing He, Feiyu Kang
Summary: Constructing a reinforced and gradient SEI on silicon nanoparticles through an in-situ thiol-ene click reaction is an effective method to improve cycling performance and stability. The modified SEI can homogenize stress and strain during lithiation to reduce expansion and prevent cracking, leading to excellent performance and cycling stability in high-energy-density lithium-ion batteries.
Article
Chemistry, Physical
Franziska Allgayer, Julia Maibach, Fabian Jeschull
Summary: Graphite in potassium-ion batteries shows a faster capacity fade compared to lithium-ion batteries, possibly due to the reactivity of the potassium metal counter electrode or the instability of the solid electrolyte interphase. Previous studies have focused on different electrolyte formulations or charge states of graphite electrodes in potassium half cells. This study compares the surface layers in both charged and discharged states of lithium and potassium half cells, revealing significant differences in SEI composition.
ACS APPLIED ENERGY MATERIALS
(2022)
Review
Nanoscience & Nanotechnology
Lin Han, Tiefeng Liu, Ouwei Sheng, Yujing Liu, Yao Wang, Jianwei Nai, Liang Zhang, Xinyong Tao
Summary: Silicon is promising for lithium storage due to its high capacity and low working platform, but volume changes during cycling lead to material pulverization and electrode cracking. A robust binder is essential for maintaining Si electrode integrity, yet its role in modulating the chemical composition and spatial distribution of the SEI layer is often overlooked.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Jianxin Tian, Taiping Hu, Shenzhen Xu, Rui Wen
Summary: The solid electrolyte interphase (SEI) is a protective film on the electrode surface of a lithium-ion (Li-ion) battery that plays a crucial role in its performance. This study investigates the Li-ion diffusion mechanism within different components of the SEI structure. The results show that the inorganic layer has a much higher Li-ion diffusion coefficient compared to the organic layer, highlighting its important contribution to Li-ion diffusion.
CHINESE CHEMICAL LETTERS
(2023)
Article
Nanoscience & Nanotechnology
Yonglei Zhang, Yinghui Bian, Zichuan Lv, Yuqing Han, Meng-Chang Lin
Summary: This study reveals the reaction mechanism at the Al anode of aqueous electrolyte Al cells and investigates the effects of ASEI on their charge/discharge cycling stability and activity, demonstrating the importance of chloride anions in inducing aluminum corrosion.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Review
Chemistry, Physical
Roman G. Fedorov, Sebastian Maletti, Christian Heubner, Alexander Michaelis, Yair Ein-Eli
Summary: A key challenge in lithium-ion batteries is the instability of electrolytes against anode materials, with the solid-electrolyte interphase (SEI) providing stability at the cost of capacity consumption. Artificial SEIs offer more flexibility to tune properties such as chemical composition and impedance, but must ensure sufficient transport properties for Li-ions and stability.
ADVANCED ENERGY MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Kangsheng Huang, Sheng Bi, Hai Xu, Langyuan Wu, Chang Fang, Xiaogang Zhang
Summary: Gel polymer electrolytes (GPEs) are used as alternatives to liquid electrolytes in lithium-metal batteries (LMBs). Adding diluent 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (TTE) to regulate the electrolyte structure improves the electrochemical stability and ion transport properties of GPEs. The addition of TTE enhances ion association and forms a robust and low-impedance solid electrolyte interface (SEI) on the anode surface. This study provides an effective approach for controlling solvation structures in GPEs, which can advance the design of GPE-based LMBs in the future.
Article
Chemistry, Physical
Aiping Wang, Li Wang, Yanzhou Wu, Yufang He, Dongsheng Ren, Youzhi Song, Bo Zhang, Hong Xu, Xiangming He
Summary: This study explores the ion desolvation processes with and without solid electrolyte interphases (SEIs) using quantum chemistry calculations. It is found that the accelerated ion desolvation in new-concept electrolytes is mainly attributed to SEIs rather than the regulated solvation structure. Based on this understanding, an SEI-aided ion desolvation model is proposed, bridging the SEI and battery kinetics at the atomic scale and redefining the functions of SEIs, which are expected to guide the electrolyte design in batteries.
ADVANCED ENERGY MATERIALS
(2023)
Article
Electrochemistry
Daniel Krotkov, Dan Schneier, Svetlana Menkin, Yonatan Horowitz, Emanuel Peled, Diana Golodnitsky, Sharly Fleischer
Summary: Utilizing Terahertz (THz) time-domain-spectroscopy, the study presents the operando characterization of the silicon/electrolyte interfacial phenomena in a working lithium-ion battery, showing a strong correlation with XPS and electrochemical data.
BATTERIES & SUPERCAPS
(2022)
Article
Chemistry, Physical
Chae Rim Lee, Ho Yeon Jang, Han Jun Leem, Min A. Lee, Wontak Kim, Jongjung Kim, Jun Ho Song, Jisang Yu, Junyoung Mun, Seoin Back, Hyun-seung Kim
Summary: The chemical composition significantly affects the electrical surface properties and thermal stability of solid electrolyte interphase (SEI) on graphite and SiO electrodes. SiO electrodes exhibit inferior electrochemical performance at high temperatures, and improvements can be made by modifying the surface work function or the energy level of the electrolyte additive.
ADVANCED ENERGY MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Rabeb Grissa, Alla Abramova, Sacris-Jeru Tambio, Margaud Lecuyer, Marc Deschamps, Vincent Fernandez, Jean-Marc Greneche, Dominique Guyomard, Bernard Lestriez, Philippe Moreau
ACS APPLIED MATERIALS & INTERFACES
(2019)
Article
Chemistry, Multidisciplinary
Heng Zhang, Chunmei Li, Gebrekidan Gebresilassie Eshetu, Stephane Laruelle, Sylvie Grugeon, Karim Zaghib, Christian Julien, Alain Mauger, Dominique Guyomard, Teofilo Rojo, Nuria Gisbert-Trejo, Stefano Passerini, Xuejie Huang, Zhibin Zhou, Patrik Johansson, Maria Forsyth
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2020)
Article
Chemistry, Multidisciplinary
Marin Puget, Viacheslav Shcherbakov, Sergey Denisov, Philippe Moreau, Jean-Pierre Dognon, Mehran Mostafavi, Sophie Le Caer
Summary: The nature of the primary species formed in FEC depends on the amount of FEC in the solution, which will affect its performance in the electrolyte.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Physical
Jianhan Xiong, Nicolas Dupre, Philippe Moreau, Bernard Lestriez
Summary: This study successfully visualized the polymer binder in silicon-based electrodes using a specific electrolyte solvent composition and advanced microscopy techniques, laying the foundation for high-performance lithium-ion batteries for electric vehicle applications.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Analytical
Mouad Essani, Jean-Yves Mevellec, Baptiste Charbonnier, Philippe Moreau, Hilel Moussi, Pierre Weiss, Jean Le Bideau, Maxime Bayle, Bernard Humbert, Patricia Abellan
Summary: The development of instruments combining multiple characterization and imaging tools has driven advancements in material science, engineering, biology, and other related fields. This study reports the use of a cryo-FIB-SEM-mu Raman instrument to assess the accuracy of cryo-fixation methods for studying vitreous materials with high water content, providing a reliable approach to avoid imaging artifacts.
ANALYTICAL CHEMISTRY
(2022)
Article
Engineering, Chemical
Helene Roberge, Philippe Moreau, Estelle Couallier, Patricia Abellan
Summary: This study used scanning electron microscopy combined with focused ion beam to analyze the structural features determining the filtration performance of commercially available polyacrylonitrile (PAN) UF and polyethersulfone (PES) MF membranes at the nanometer scale. The results provide key information about the structural parameters of the selective layer and the percentage of blind pores, and suggest that current models are insufficient to fully describe asymmetric membranes with thin selective layers.
JOURNAL OF MEMBRANE SCIENCE
(2022)
Article
Chemistry, Physical
Lucas Huet, Philippe Moreau, Nicolas Dupre, Thomas Devic, Lionel Roue, Bernard Lestriez
Summary: The physical crosslinking of polymeric binders through coordination chemistry improves the electrochemical performance of silicon-based negative electrodes by stabilizing the electrode and the solid electrolyte interphase (SEI) layer. Scanning electron microscopy coupled with energy dispersive X-ray spectroscopy reveals the homogeneous coordination of carboxylated binder with Zn cations and its layering on the silicon surface. The SEI formed after the first cycle is denser with Zn-coordinated binder and preferentially observed on binder-depleted zones. This results in a lower SEI impedance, a higher first cycle coulombic efficiency, and a 40% improvement of capacity retention after 50 cycles for highly loaded electrodes of over 6 mAh cm(-2).
Article
Nanoscience & Nanotechnology
Angelica Laurita, Liang Zhu, Pierre-Etienne Cabelguen, Jeremie Auvergniot, Jonathan Hamon, Dominique Guyomard, Nicolas Dupre, Philippe Moreau
Summary: In this study, advanced microscopy and spectroscopy techniques were used to investigate the surface of Ni-rich layered transition metal oxides. The results demonstrate that even under usual storage conditions after synthesis, the surface of the material is chemically different from the nominal values.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Yanis Levieux-Souid, Jean-Frederic Martin, Philippe Moreau, Nathalie Herlin-Boime, Sophie Le Caer
Summary: Understanding aging phenomena in batteries is crucial for designing efficient, safe, and reliable energy storage devices. This study demonstrates that radiation chemistry can be used as a valuable tool to screen the behavior of electrolytes within a few hours, yielding similar performance ratings to electrochemical cycling. Controlled irradiation can predict battery cycling behavior and propose mechanisms involved in the degradation processes of different electrolytes.
Article
Nanoscience & Nanotechnology
Lucas Huet, Driss Mazouzi, Philippe Moreau, Nicolas Dupre, Michael Paris, Sebastien Mittelette, Danielle Laurencin, Thomas Devic, Lionel Roue, Bernard Lestriez
Summary: This study proposes a simple and versatile method for preparing Zn(II)-poly(carboxylates) reticulated binders, which significantly improve the electrochemical performance of silicon-based negative electrodes. The formation of carboxylate-Zn(II) coordination bonds is investigated, and mechanical characterizations reveal better cohesion, adhesion, hardness, and elastic modulus of the coordinated binder. Operando dilatometry experiments show reduced electrode expansion and improved capacity retention of over 30% after 60 cycles for the coordinatively reticulated electrodes.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Review
Chemistry, Physical
Nassima Kana, Kaouther Touidjine, Sarah Olivier-Archambaud, Effrosyni Gkaniatsou, Michael Paris, Nicolas Dupre, Nicolas Gautier, Philippe Moreau, Clemence Sicard, Bernard Lestriez, Thomas Devic
Summary: Silicon is a promising alternative to graphite for lithium-ion battery negative electrodes due to its high capacities. Coating silicon particles with metal-organic frameworks (MOFs) has shown improved electrochemical performance. However, a 20 nm thick layer of MOF on the surface of silicon particles did not result in significant modifications of the electrochemical performance in practical electrode loading conditions.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Lucas Huet, Driss Mazouzi, Philippe Moreau, Nicolas Dupre, Michael Paris, Sebastien Mittelette, Danielle Laurencin, Thomas Devic, Lionel Roue, Bernard Lestriez
Summary: This study proposes a simple and versatile method for preparing Zn(II)-poly(carboxylates) reticulated binders by adding Zn(II) precursors into a preoptimized poly(carboxylic acids) binder solution. These binders significantly improve the electrochemical performance of silicon-based negative electrodes. The formation of carboxylate-Zn(II) coordination bonds is investigated using rheology and spectroscopic techniques. Mechanical characterizations show that the coordinated binder offers better electrode coating cohesion and adhesion, as well as higher hardness and elastic modulus, even in the presence of a carbonate solvent. Operando dilatometry experiments demonstrate that the electrode expansion during lithiation is reduced, mitigating electrode mechanical failure. These coordinatively reticulated electrodes outperform their uncoordinated counterparts with an improved capacity retention of over 30% after 60 cycles.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Angelica Laurita, Liang Zhu, Pierre-Etienne Cabelguen, Jeremie Auvergniot, Dominique Guyomard, Philippe Moreau, Nicolas Dupre
Summary: Li-7 MAS NMR quantification of lithiated species reveals increased Li extraction during electrode preparation process. The study also suggests a new reaction involving Li2O as reagent and the formation of LiF in the degradation of PVdF binder.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Morgane Denis, Hubert Chevreau, Pablo Salcedo-Abraira, Philippe Moreau, Nicolas Dupre, Michael Paris, Philippe Poizot, Thomas Devic
Summary: Recently, metal-organic frameworks (MOFs) that combine organic and inorganic redox-active moieties have attracted attention in electrochemical energy storage. In this study, we focused on MIL-53(M) (M = Al, Fe) analogues based on 2,5-dioxo-1,4-benzenedicarboxylate, as this ligand has shown interesting electrochemical activity in the solid state. We attempted to chemically lithiate the title solids through various synthetic paths and characterized the resulting solids using several techniques. We found that the lithiation process differed significantly for M = Al and Fe, and evaluated the electrochemical extraction/uptake of Li+ in the lithiated derivatives. Although their storage capacities were moderate, the presence of a minor amount of M3+ cations improved the long term capacity retention.
MOLECULAR SYSTEMS DESIGN & ENGINEERING
(2023)
Article
Materials Science, Multidisciplinary
Helene Roberge, Philippe Moreau, Estelle Couallier, Patricia Abellan
Summary: Detailed structural characterization of fouling in membranes is crucial for understanding filtration performance. Electron microscopy combined with labeling techniques can differentiate biomolecules, but specific protocols for differentiating biomolecules in fouled membranes are challenging due to the need for preserving membrane state and the inability of probes to penetrate fouled membranes. This study presents a heavy metal staining technique compatible with cryofixation to identify and differentiate biomolecules in fouling. The technique enhances contrast and reveals the strong interaction between proteins and lipids in fouling.
MICROSCOPY AND MICROANALYSIS
(2023)
