Article
Electrochemistry
Hiroyuki Fujimoto, Hisao Kiuchi, Shigeharu Takagi, Keiji Shimoda, Ken-ichi Okazaki, Zempachi Ogumi, Takeshi Abe
Summary: Since the commercialization of rechargeable Li ion batteries in the early 1990s, the performance of these devices has continually improved. The present work examined the reaction mechanisms at graphite negative electrodes based on operando synchrotron X-ray diffraction analyses during charge/discharge, showing a series of superlattices formed depending on the amount of Li intercalated into the graphite.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Paul Choi, Bharathy Parimalam, Yubai Li, Shawn Litster
Summary: This study uses high-resolution in-situ/operando Zernike phase contrast X-ray microscopy to directly observe the lithium electrodeposition process and characterizes it using TXM and CT imaging techniques. The results reveal the nucleation and deposition mechanisms of lithium and provide comprehensive morphology of the resulting structure. The study emphasizes the importance of in-situ/operando characterization of commercially-relevant configurations in developing practical dendrite mitigation strategies.
JOURNAL OF POWER SOURCES
(2023)
Article
Electrochemistry
Hiroyuki Fujimoto, Miwa Murakami, Toshiro Yamanaka, Keiji Shimoda, Hisao Kiuchi, Zempachi Ogumi, Takeshi Abe
Summary: The recharge and discharge mechanism of graphite electrodes is still unclear, and the research team used various technologies for real-time analysis, proposed a synchronized real-time analysis method, and studied the details of the intercalation mechanism.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Atsunori Ikezawa, Masato Horiuchi, Hajime Arai
Summary: This study reveals that shape change processes in alkaline secondary batteries with zinc negative electrodes are mainly due to spatially uneven reactions. Uneven reactions lead to relatively short cycle life in some cases, while uniform reactions result in improved durability.
JOURNAL OF POWER SOURCES
(2021)
Article
Electrochemistry
Victor Maurel, Kevin Brousse, Tyler S. S. Mathis, Audrey Perju, Pierre-Louis Taberna, Patrice Simon
Summary: This study presents an experimental setup for measuring the in-plane AC impedance and DC resistance of electrode materials during electrochemical cycling. The measurements allow for tracking of changes in the ionic and electronic contributions to impedance under polarization, providing insights into the transport mechanisms and potential improvements in electrode performance.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Guillaume Tonin, Gavin B. M. Vaughan, Renaud Bouchet, Fannie Alloin, Celine Barchasz
Summary: This study used X-ray techniques to investigate the morphology and heterogeneity of lithium metal electrodes in liquid Li/S cells, revealing the uneven oxidation and pit formation of lithium foil during discharge, with a reduction in current density leading to a more homogeneous lithium stripping/plating process.
JOURNAL OF POWER SOURCES
(2022)
Article
Materials Science, Multidisciplinary
Shahabeddin Dayani, Henning Markoetter, Jonas von Krug von Nidda, Anita Schmidt, Giovanni Bruno
Summary: This paper investigates the overdischarge phenomenon in lithium-ion cells, focusing on the behavior of copper dissolution and deposition. The concentration of dissolved and deposited copper is quantified using nondestructive imaging, revealing a nonuniform distribution pattern for copper deposition on the cathode. The research provides insights for safer battery cell design.
ADVANCED MATERIALS TECHNOLOGIES
(2023)
Review
Chemistry, Physical
Wenzao Li, Diana M. Lutz, Lei Wang, Kenneth J. Takeuchi, Amy C. Marschilok, Esther S. Takeuchi
Summary: To overcome the limitations of static and destructive characterizations of Li-ion battery materials and components, a comprehensive investigation over various length and time scales is essential. Emerging in situ and operando characterization methodologies focusing on multiple size domains are a powerful approach to resolve current challenges and navigate future directions. The necessity and opportunity for in situ and operando characterization of electrochemical energy storage materials and systems are discussed, along with suggestions for future directions to tackle currently intractable issues on Li-ion battery application, failure, and emerging design concepts.
Article
Multidisciplinary Sciences
Alice J. Merryweather, Christoph Schnedermann, Quentin Jacquet, Clare P. Grey, Akshay Rao
Summary: The key to advancing lithium-ion battery technology, especially fast charging, lies in understanding dynamic processes in functioning materials under realistic conditions in real time. A laboratory-based optical interferometric scattering microscope was introduced to study nanoscopic lithium-ion dynamics in battery materials, allowing for high-throughput material screening. This methodology was applied to study various processes in battery materials, providing insights into battery degradation mechanisms.
Article
Chemistry, Physical
Tuan-Tu Nguyen, Julie Villanova, Zeliang Su, Remi Tucoulou, Benoit Fleutot, Bruno Delobel, Charles Delacourt, Arnaud Demortiere
Summary: Quantitative phase contrast X-ray nano-holotomography was used to analyze the microstructures of high energy density Li-ion electrodes, revealing the negative impacts of excess CBD on electrode performance and offering insights for electrode design optimization.
ADVANCED ENERGY MATERIALS
(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
Shigeharu Takagi, Keiji Shimoda, Jun Haruyama, Hisao Kiuchi, Ken-ichi Okazaki, Toshiharu Fukunaga, Zempachi Ogumi, Takeshi Abe
Summary: In this study, operando structural analyses of graphite electrode in lithium-ion batteries were performed using neutron diffraction and synchrotron radiation X-ray diffraction. The results provide insights into the phase evolution and structural transition of lithium-intercalated graphite. The study reveals that the in-plane structure of graphite transitions from LiC6-type to LiC9-type during lithium de-intercalation, and the LiC9-type arrangement is retained in Li-poor phases. This research is significant for understanding the structural changes in lithium-ion battery materials.
Article
Chemistry, Multidisciplinary
Ashley P. P. Black, Andrea Sorrentino, Francois Fauth, Ibraheem Yousef, Laura Simonelli, Carlos Frontera, Alexandre Ponrouch, Dino Tonti, M. Rosa Palacin
Summary: Synchrotron radiation based techniques are powerful tools for battery research, providing insight into length scales, depth sensitivities, and spatial/temporal resolutions. Operando experiments enable characterization during battery operation and help elucidate reaction mechanisms. This article discusses the state of the art for relevant techniques (scattering, spectroscopy, and imaging) and addresses bottlenecks specific to battery applications, including cell design improvement, multi-modal characterization, and automated data analysis protocols. Accelerated progress is expected in these areas, fostering advancements in battery performance.
Article
Chemistry, Physical
Yuta Kimura, Su Huang, Takashi Nakamura, Nozomu Ishiguro, Oki Sekizawa, Kiyofumi Nitta, Tomoya Uruga, Tomonari Takeuchi, Toyoki Okumura, Mizuki Tada, Yoshiharu Uchimoto, Koji Amezawa
Summary: A method combining operando computed tomography and X-ray absorption near-edge structure spectroscopy (CT-XANES) is proposed in this paper to directly track the evolution of the 3D distribution of local capacity loss in battery electrodes. The method enables a five-dimensional analysis of degradation, including spatial coordinates, time, and chemical state. It quantifies the spatiotemporal dynamics of local capacity degradation and correlates it with overall electrode performance, providing critical insights for identifying degradation factors and developing batteries with long-term stability.
Article
Chemistry, Physical
Anirudha Jena, Zizheng Tong, Behrouz Bazri, Kevin Iputera, Ho Chang, Shu-Fen Hu, Ru-Shi Liu
Summary: Solid Li-ion conductors have the potential to enhance the performance of batteries by widening the cell-potential window and improving safety features. However, the development of all-solid-state batteries (ASSBs) faces challenges such as ion transport, interface reactions, and increased cell resistance. Advanced in situ/operando techniques are being used to explore and address these challenges.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
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
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)