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
Chemistry, Physical
Yanke Lin, Tianshuai Wang, Leicheng Zhang, Xudong Peng, Baoling Huang, Maochun Wu, Tianshou Zhao
Summary: This research proposes a method of coating a thin layer containing Al/Li dual-salt onto solid polymer electrolytes to address the issue of dendrite formation and contact loss. By forming a lithiophilic Li-Al alloy-rich layer and a lithiophobic LiF-rich layer, the interfacial adhesion is improved and dendrite suppression is achieved, enabling stable cycling of solid-state Li batteries.
Article
Chemistry, Physical
Qinping Jian, Tianshuai Wang, Jing Sun, Maochun Wu, Tianshou Zhao
Summary: The study formulates a new low-concentration electrolyte to improve the reversibility and stability of zinc anodes in aqueous zinc batteries. By adding DMSO into the electrolyte, a fluorinated interphase is formed on the zinc surface, suppressing dendrite formation and side reactions. This newly formulated electrolyte enables highly reversible zinc plating/stripping and significantly improves the cycle life of zinc batteries.
ENERGY STORAGE MATERIALS
(2022)
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)
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
Materials Science, Multidisciplinary
M. Schellenberger, R. Golnak, W. G. Quevedo Garzon, S. Risse, R. Seidel
Summary: Silicon anodes have a higher theoretical storage capacity than commercial graphite anodes in Li-ion batteries, but the Solid Electrolyte Interphase (SEI) on silicon fails to stabilize the electrolyte sufficiently due to the large volume changes. Researchers have developed a novel X-ray Absorption Spectroscopy (XAS) method to study the SEI on silicon anodes, revealing the main components and possible liquid inclusions within a porous SEI morphology.
MATERIALS TODAY ADVANCES
(2022)
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
Energy & Fuels
Siru Chen, Pingbo Xu, Qingyang Mei, Haiming Xie, Yulong Liu
Summary: To overcome the challenges of using Li metal in batteries, an artificial solid electrolyte interphase with multiple functions is proposed. This technology involves coating Li metal with a magnesium-based inorganic-organic film to reduce side reactions and dendrite formations. Polymer layers are also used to control volume changes caused by lithium plating/stripping. Experimental results show that this approach improves Li ion transport and enhances the stability and performance of Li metal batteries.
JOURNAL OF ENERGY STORAGE
(2023)
Review
Chemistry, Physical
Runze Zhang, Yinglei Wu, Zhenying Chen, Yu Wang, Jinhui Zhu, Xiaodong Zhuang
Summary: All-solid-state Li batteries (ASSLBs) show promise due to their high safety and energy density. Understanding the failure mechanisms of ASSLBs can aid in improving their performance. In situ/operando Raman spectroscopy (IS/O-RS) is commonly used to study ASSLBs, as it can detect molecular structural and compositional changes in the electrodes, solid electrolytes, and their interfaces. This review discusses the applications of IS/O-RS in ASSLB research, including exploring electrode-electrolyte interfaces, electrodes, and solid electrolytes. The optimized use of IS/O-RS can provide valuable insights for improving ASSLB performance.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Yin-Ju Yen, Sheng-Heng Chung
Summary: In this study, a novel lithium-sulfur cell configuration was achieved by using a polysulfide cathode and a sulfide solid electrolyte. The liquid-solid interface provided by the polysulfide catholyte enhanced charge transfer and lithium-ion diffusion. The formation of lithium phosphide and lithium phosphate created an ionically conductive protection layer, optimizing the contact between the polysulfide cathode and the solid electrolyte and stabilizing the active electrodes.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Weibo Huang, Yan Wang, Linze Lv, Guobin Zhu, Qunting Qu, Honghe Zheng
Summary: To construct high-energy-density silicon-based Li-ion batteries, it is crucial to optimize and build a robust solid electrolyte interphase (SEI) to overcome the severe side reactions caused by volume changes in silicon (Si) anodes. This study combines electrolyte design and surface modification to create a phenyl trifluoromethanesulfonimide (PTFSI) interfacial layer on the Si surface, with additive functions. The resulting customized PTFSI interfacial layer modulates the solvation/desolvation reaction mechanism at the electrode interface, forming an artificial SEI structure composed of oligomers and inorganic salts. This structure exhibits fast ionic conductivity, reduces electrolyte consumption, and maintains the integrity of the electrode structure, leading to significantly improved rate capability and cycling performance of the optimized Si@PTFSI anode.
ENERGY STORAGE MATERIALS
(2022)
Article
Chemistry, Physical
Yu-Hsing Lin, Liang-Ting Wu, Yu-Ting Zhan, Jyh-Chiang Jiang, Yuh-Lang Lee, Jeng-Shiung Jan, Hsisheng Teng
Summary: Lithium-metal batteries with limited-Li anodes are crucial for high-energy storage. We engineer the self-assembly formation of solid-electrolyte interphase (SEI) in a gel polymer electrolyte (GPE) to control Li-deposition behavior and enhance reversibility.
ENERGY STORAGE MATERIALS
(2023)
Article
Engineering, Environmental
His Muhammad Bintang, Lee Seongsoo, Sunghee Shin, Byung Gon Kim, Hun-Gi Jung, Dongmok Whang, Hee-Dae Lim
Summary: The use of a Sn anode paired with a novel electrolyte composed of eutectic succinonitrile (SN) combined with fluoroethylene carbonate (FEC) has been demonstrated to improve the stability of the solid electrolyte interphase (SEI) and buffer large volume changes, leading to superior cycle performance of the Sn anode compared to conventional electrolytes. The synergistic effects of the novel electrolyte components result in a mechanically rigid SEI mainly composed of favorable inorganics, demonstrating potential for enhanced electrochemical performance of Sn anodes and other alloying-based anode materials.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Applied
Yangfan Lin, Juner Chen, Han Zhang, Jianhui Wang
Summary: The in-situ construction of high-quality solid electrolyte interphase (SEI) using synergistic additives of LiNO3 and ethylene sulfite (ES) results in improved mechanical strength and ion conductivity, effectively suppressing Li-dendrite growth and side reactions and achieving high Coulombic efficiency (CE) and capacity retention.
JOURNAL OF ENERGY CHEMISTRY
(2023)
Article
Chemistry, Physical
Haneol Kang, Hoon Kim, Chuleun Yeom, Moon Jeong Park
Summary: In this study, electrolyte additives were designed and synthesized for lithium batteries with an Si-graphite composite (SGC) anode to improve their rate performance and cycle stability. A hybrid artificial solid-electrolyte interphase (SEI) was formed on the anode surface through a combination of fluoroethylene carbonate (FEC) and dilithium vinylphosphonate (VPLi), resulting in enhanced capacity retention and rate capability.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Trisha R. Nickerson, Emma N. Antonio, Dylan P. McNally, Michael F. Toney, Chunmei Ban, Anthony P. Straub
Summary: Polyamide reverse osmosis (PA-RO) membranes have high water permeability and salt rejection, making them important for addressing water shortages. However, current membranes face challenges with selectivity, fouling, and predicting performance. This Perspective highlights the need for molecular understanding of selectivity and transport mechanisms of PA-RO and other polymer membranes to guide future developments and improve predictive models. It discusses current understanding of ion, water, and polymer interactions in PA-RO membranes, explores their impact on transport properties, and underscores advances in characterization techniques and computational methods for studying transport phenomena.
Article
Chemistry, Physical
Aashutosh Mistry, Venkat Srinivasan, Hans-Georg Steinrueck
Summary: Current flowing through the electrolyte involves the motion of ions and solvent, concentration profiles, and the electric field. Traditionally, understanding electrolyte transport relied on macroscopic voltage measurements, but recent advances in imaging and spectroscopic techniques allow direct probing of velocity and concentration profiles. This detailed information opens up exciting opportunities, from verifying theories about transport in Li-ion electrolytes to new approaches for measuring and quantifying transport in complex electrolytes. This paper discusses these emerging directions.
ADVANCED ENERGY MATERIALS
(2023)
Article
Polymer Science
Grant E. Bauman, Jonathan D. Hoang, Michael F. Toney, Timothy J. White
Summary: The anisotropy of liquid crystalline elastomers (LCEs) is derived from the interaction-facilitated orientation of the molecular constituents. In this study, we investigated the correlation between the thermomechanical response of LCEs subjected to mechanical alignment and measurements of the Hermans orientation parameter. By systematically preparing LCEs with varying concentrations of liquid crystalline mesogens, we were able to control the degree of achievable order. The results showed that the liquid crystalline content defines the temperature of actuation, while the orientation parameter of the LCE is intricately correlated to both the total actuation strain and the rate of thermomechanical response.
Review
Chemistry, Multidisciplinary
Hao A. Nguyen, Grant Dixon, Florence Y. Dou, Shaun Gallagher, Stephen Gibbs, Dylan M. Ladd, Emanuele Marino, Justin C. Ondry, James P. Shanahan, Eugenia S. Vasileiadou, Stephen Barlow, Daniel R. Gamelin, David S. Ginger, David M. Jonas, Mercouri G. Kanatzidis, Seth R. Marder, Daniel Morton, Christopher B. Murray, Jonathan S. Owen, Dmitri V. Talapin, Michael F. Toney, Brandi M. Cossairt
Summary: In this review, the demand and design rules for solution-processed semiconductors with narrow photoluminescence line widths are discussed. The current state of emission line width for various colloidal materials is compared, and some conclusions and prospects are summarized.
Article
Chemistry, Physical
Lucas Q. Flagg, Jonathan W. Onorato, Christine K. Luscombe, Vinayak Bhat, Chad Risko, Ben Levy-Wendt, Michael F. Toney, Christopher R. McNeill, Guillaume Freychet, Mikhail Zhernenkov, Ruipeng Li, Lee J. Richter
Summary: Organic mixed ionic-electronic conductors (OMIECs) have the potential for various new technologies, but their complex behavior inhibits material design. This report presents the use of RXRD to determine the structure of a doped polymer OMIEC. The insights from RXRD provide important information on ion location and doping behavior, contributing to a better understanding of transport in OMIECs.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Nayon Park, Ryan A. Beck, Kevin K. Hoang, Dylan M. Ladd, Jared E. Abramson, Ricardo A. Rivera-Maldonado, Hao A. Nguyen, Madison Monahan, Gerald T. Seidler, Michael F. Toney, Xiaosong Li, Brandi M. Cossairt
Summary: We demonstrate the colloidal, layer-by-layer growth of metal oxide shells on InP quantum dots (QDs) at room temperature. The presence of surface-localized dark states near the band edges due to native InP QD surface oxides gives rise to nonradiative pathways, which can be reduced by replacing surface indium with zinc to form a ZnO shell. A synthetic strategy using stoichiometric amounts of common atomic layer deposition precursors in alternating cycles was developed for layer-by-layer growth. The results show the potential of controlling QD interfaces and contribute to the understanding of the connections between structural complexity and PL properties in colloidal optoelectronic materials.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Julian A. Steele, Eduardo Solano, David Hardy, Damara Dayton, Dylan Ladd, Keith White, Peng Chen, Jingwei Hou, Haowei Huang, Rafikul Ali Saha, Lianzhou Wang, Feng Gao, Johan Hofkens, Maarten B. J. Roeffaers, Dmitry Chernyshov, Michael F. Toney
Summary: Recent reports have increasingly utilized synchrotron-based grazing incident wide angle X-ray scattering (GIWAXS) to study metal halide perovskite thin films, which has proven to be invaluable for understanding structure-property relationships that limit optoelectronic performance. The GIWAXS technique is compatible with in situ and operando setups, and a growing research community has successfully used it to study kinetic and dynamic features in halide perovskite materials. This article aims to accelerate the learning curve for new experimentalists by providing a comprehensive framework for effective GIWAXS experiments.
ADVANCED ENERGY MATERIALS
(2023)
Article
Multidisciplinary Sciences
Joshua T. Del Mundo, Sintu Rongpipi, Hui Yang, Dan Ye, Sarah N. Kiemle, Stephanie L. Moffitt, Charles L. Troxel, Michael F. Toney, Chenhui Zhu, James D. Kubicki, Daniel J. Cosgrove, Esther W. Gomez, Enrique D. Gomez
Summary: In this study, grazing-incidence wide-angle X-ray scattering (GIWAXS) with a humidity chamber was used to investigate the properties of onion cell walls. The results showed that the lattice spacing of cellulose (110/110) slightly decreased upon drying, while the lattice parameters of (200) remained unchanged. The intensity of (110/110) diffraction increased relative to (200) in hydrated samples. Density functional theory models confirmed the changes in crystalline properties during drying. GIWAXS also revealed a peak attributed to pectin chain aggregation.
SCIENTIFIC REPORTS
(2023)
Article
Chemistry, Physical
Nicholas J. Weadock, Tyler C. Hemamala, Julian A. Vigil, Aryeh Gold-Parker, Ian C. Smith, Ballal Ahammed, Matthew J. Krogstad, Feng Ye, David Voneshen, Peter M. Gehring, Andrew M. Rappe, Hans-Georg Steinrueck, Elif Ertekin, Hemamala I. Karunadasa, Dmitry Reznik, Michael F. Toney
Summary: This study determines the true structure of two hybrid lead-halide perovskites using single-crystal diffuse scattering, neutron inelastic spectroscopy, and molecular dynamics simulations. The research reveals a remarkable collective dynamics that induces longer-range intermolecular correlations and may increase charge carrier lifetimes and affect halide migration.
Article
Environmental Sciences
Valerie A. Niemann, Marten Huck, Hans-Georg Steinrueck, Michael F. Toney, William A. Tarpeh, Sharon E. Bone
Summary: This study investigated the fouling of RO membranes by calcium and silicon under realistic feed conditions using mu-X-ray fluorescence (mu-XRF) mapping and mu-X-ray absorption near-edge fine structure (mu-XANES) spectroscopy. The results showed that both calcium and silicon were abundant in the fouling layer. Additionally, organic compounds were closely related to the presence of calcium and silicon on the RO membrane. These findings provide important insight into the mechanism of RO membrane fouling.
Article
Chemistry, Multidisciplinary
Tim Pruessner, Dennis Meinderink, Siqi Zhu, Alejandro G. Orive, Charlotte Kielar, Marten Huck, Hans-Georg Steinrueck, Adrian Keller, Guido Grundmeier
Summary: This study investigates the molecular adhesion of a pilus-derived peptide that promotes the formation of biofilms in Pseudomonas aeruginosa. The results suggest that the interaction between the peptide and the surface is mainly mediated by coordination and hydrogen bonding.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Kerry Sun, Chuntian Cao, Dingyi Zhao, Xiao Tong, Seong-Min Bak, Yonghua Du, Feng Wang, Daniel A. Steingart
Summary: The superionic solid-state argyrodite electrolyte Li6PS5Br can enhance the safety and energy density of lithium and lithium-ion batteries. However, this electrolyte still suffers from electrode degradation, and the stability of LFP against Li6PS5Br is not inherently guaranteed.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Luis Kitsu Iglesias, Emma N. Antonio, Tristan D. Martinez, Liang Zhang, Zengqing Zhuo, Steven J. Weigand, Jinghua Guo, Michael F. Toney
Summary: This study elucidates the mechanism of sodium storage in hard carbon anodes and provides insights into the preferred pore sizes, extent of pore filling, and the influence of defect concentration. It is observed that sodium in larger pores exhibits increased pseudo-metallic sodium character, and higher pyrolysis temperatures enhance the capacity of sodium stored in the pores. Additionally, sodium intercalation between graphene layers occurs simultaneously with pore filling in the plateau region. The findings highlight strategies to design superior hard carbon anodes for sodium-ion batteries.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Dario Gomez Vazquez, Travis P. Pollard, Julian Mars, Ji Mun Yoo, Hans-Georg Steinrueck, Sharon E. Bone, Olga Safonova, Michael F. Toney, Oleg Borodin, Maria R. Lukatskaya
Summary: By using coordinating anions like acetate, a WIS-like Zn coordination environment can be achieved even in relatively dilute conditions, enabling prolonged cycling of Zn metal anodes.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Stephanie L. Moffitt, Chuntian Cao, Maikel F. A. M. Van Hest, Laura T. Schelhas, Hans-Georg Steinrueck, Michael F. Toney
Summary: In this study, the existence of vertically heterogeneous thermally induced structural relaxation in amorphous In-Zn-O (a-IZO) thin films was observed using in situ X-ray reflectivity, which has not been previously observed. Thermal annealing was found to influence the electrical performance of the films. These findings are important for the development of a-IZO-based devices.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)