Article
Nanoscience & Nanotechnology
Oguz Bayindir, Ikramul Hasan Sohel, Melek Erol, Ozgur Duygulu, Mehmet Nurullah Ate
Summary: This study introduces a new design paradigm for electrode preparation that significantly enhances the fast-charging capabilities of a graphite anode by controlling crystallographic orientation. By using neodymium magnets under a dynamic magnetic field, the graphite particles align along specific crystal planes, allowing for an 80% charge state in just 50 minutes at a 1C charge rate, compared to 138 minutes for randomly oriented graphite electrodes. The outstanding electrochemical performance of the oriented graphite electrodes was confirmed through various characterization techniques.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Noel Hallemans, Widanalage Dhammika Widanage, Xinhua Zhu, Sanghamitra Moharana, Muhammad Rashid, Annick Hubin, John Lataire
Summary: This article introduces operando EIS as a promising tool for measuring time-varying impedance data of Li-ion batteries. The mathematical principles behind impedance extraction are detailed, and the technique is applied to reproducible experiments to study the nonlinear behavior of the batteries.
JOURNAL OF POWER SOURCES
(2022)
Article
Electrochemistry
Dandan Liu, Yingyuan He, Yongchong Chen, Jingyang Cao, Feng Zhu
Summary: A crack dominated solid electrolyte interface (SEI) resistance is considered in an electrochemical model to investigate the influence of electrode thickness, solid volume fraction and C-rate on the performance of thick graphite electrodes. The simulation results of Li/graphite cells show reasonable agreement with the measured charge and discharge profiles, including the first cycle. The growth of SEI crack explains the periodic evolution of SEI film resistance during the cycles, and the reduction of electrode porosity caused by SEI growth has a larger effect on thick electrodes. A linear relationship is found between the Li plating onset voltages and increasing electrode thicknesses, solid volume fractions, and C-rates.
ELECTROCHIMICA ACTA
(2023)
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
Sergey Yu. Luchkin, Maria A. Kirsanova, Dmitry A. Aksyonov, Svetlana A. Lipovskikh, Victoria A. Nikitina, Artem M. Abakumov, Keith J. Stevenson
Summary: Li-rich layered metal oxides have been extensively studied as potential positive electrode materials for Li-ion batteries. This research investigates the cycling-driven electrochemical activation process in Li-rich materials, which leads to an increase in reversible capacity. The activation process involves oxidation and reduction reactions, with the rate being influenced by the cycling rate.
ACS APPLIED ENERGY MATERIALS
(2022)
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)
Article
Chemistry, Physical
Shuwei Wang, Dongqing Liu, Xingke Cai, Lihan Zhang, Yuanming Liu, Xianying Qin, Rui Zhao, Xiaojie Zeng, Cuiping Han, Chun Zhan, Feiyu Kang, Baohua Li
Summary: Recent research has shown that the capacity and cycling performance of graphite-based hybrid anodes can be greatly improved by regulating the structural uniformity of the electrolyte and achieving an ideal solid electrolyte interface (SEI). The graphite anode with the designed SEI exhibited high initial capacity and cycling stability, outperforming previous graphite-based lithium ion or metal anodes. Pre-depositing limited lithium capacity on the graphite anode coupled with a LiFePO4 cathode resulted in stable cycling performance, highlighting the potential for reversible capacity enhancement through appropriate electrolyte design and SEI structural regulation.
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, Multidisciplinary
David E. Brown, Eric J. McShane, Zachary M. Konz, Kristian B. Knudsen, Bryan D. McCloskey
Summary: In this study, operando electrochemical impedance spectroscopy was used to reliably detect the onset of Li plating on graphite electrodes in three-electrode LIBs. By cross-validating with a highly sensitive ex situ chemical titration, it was determined that this technique can detect very small amounts of plated Li. This technique can also be applied to standard two-electrode LIB systems, making it an important step toward safely implementing fast charging protocols for LIBs in EVs.
CELL REPORTS PHYSICAL SCIENCE
(2021)
Article
Biochemistry & Molecular Biology
Mariusz Radtke, Christian Hess
Summary: By studying Li-rich and catalytically active gamma-LixV2O5 as a cathode, a direct correlation between Raman shift and Faraday current was observed, which can be used for analysis of Butler-Volmer kinetics. The potential of Raman-aided electrochemical detection method is being discussed.
Article
Chemistry, Physical
Leiting Zhang, Chrysi Tsolakidou, Sathiya Mariyappan, Jean-Marie Tarascon, Sigita Trabesinger
Summary: Identification of gaseous decomposition products from irreversible side-reactions helps understand the inner workings of rechargeable batteries. This study focused on gas evolution processes in Na-ion batteries through online electrochemical mass spectrometry, revealing differences in SEI stability and electrolyte reduction between Na-ion and Li-ion systems. The findings provide insights for developing more durable electrode-electrolyte interphases for higher specific energy and improved cycling stability in Na-ion batteries.
ENERGY STORAGE MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Katja Lahtinen, Eeva-Leena Rautama, Hua Jiang, Samuli Rasanen, Tanja Kallio
Summary: The study found that the structure and capacity of aged LiCoO2 can be restored through re-lithiation, providing a new method for the recycling of used batteries.
Article
Chemistry, Physical
Xingwei Liu, Xiaohui Shen, Hui Li, Peng Li, Laibing Luo, Haiman Fan, Xiangming Feng, Weihua Chen, Xinping Ai, Hanxi Yang, Yuliang Cao
Summary: This study introduces a simple and effective strategy to prepare electrochemically compatible PC-based electrolytes, utilizing a weakly coordinating diethyl carbonate co-solvent to enhance the reduction tolerance of PC solvent. By incorporating a film-forming additive, an electrochemically stable PC-based electrolyte that allows reversible Li+ intercalation on the graphite electrode is obtained.
ADVANCED ENERGY MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Chuangchao Sun, Xiao Ji, Suting Weng, Ruhong Li, Xiaoteng Huang, Chunnan Zhu, Xuezhang Xiao, Tao Deng, Liwu Fan, Lixin Chen, Xuefeng Wang, Chunsheng Wang, Xiulin Fan
Summary: This study designs two electrolytes that enable extreme fast charging of a microsized graphite anode, achieving high ionic conductivity, low desolvation energy, and a protective solid electrolyte interphase (SEI). These electrolytes provide principles for the practical design of fast-charging lithium-ion batteries (LIBs) with graphite anodes.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Physical
Ander Orue, Mikel Arrese-Igor, Rosalia Cid, Xabier Judez, Nuria Gomez, Juan Miguel Lopez del Amo, William Manalastas, Madhavi Srinivasan, Catleya Rojviriya, Michel Armand, Frederic Aguesse, Pedro Lopez-Aranguren
Summary: In this study, high-voltage Li metal cells with LiNi0.6Mn0.2Co0.2O2 active material were assembled using a composite electrolyte containing Li7La3Zr2O12 garnet, which showed improved cycling stability. Additive lithium hydroxide (LiOH) played a key role in enhancing the cyclability of the cells by inducing the cleavage of the labile S-F bond and increasing the concentration of LiF in the solid-electrolyte interface layer. It was emphasized that SEI-forming additives should be considered for stable SEI interfacial engineering design to expand the performance boundary of solid-state batteries.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Physical
Parameswara R. Chinnam, Leidong Xu, Lu Cai, Nikolaus L. Cordes, Sangwook Kim, Corey M. Efaw, Daniel J. Murray, Eric J. Dufek, Hongyi Xu, Bin Li
Summary: Research at a pouch cell level is crucial for the commercialization of lithium-sulfur batteries. This study investigates the failure mechanisms of Li-S pouch cells through in operando pressure analysis, identifying factors influencing performance and proposing real-time methods for morphology diagnosis and improvement.
ADVANCED ENERGY MATERIALS
(2022)
Article
Energy & Fuels
Parameswara R. Chinnam, Tanvir R. Tanim, Eric J. Dufek, Charles C. Dickerson, Meng Li
Summary: Lithium plating is a key challenge for extreme fast charging in graphite-based lithium-ion batteries, and there is currently a lack of comprehensive understanding of key plating-related electrochemical signatures. The diagnostics for lithium plating during fast charging face sensitivity and reliability issues.
JOURNAL OF ENERGY STORAGE
(2022)
Article
Chemistry, Physical
Ningshengjie Gao, Sangwook Kim, Parameswara Chinnam, Eric J. Dufek, Andrew M. Colclasure, Andrew Jansen, Seoung-Bum Son, Ira Bloom, Alison Dunlop, Stephen Trask, Kevin L. Gering
Summary: This paper discusses the selection, testing, and validation of electrolyte candidates for Li-ion cells with a focus on achieving extreme fast charge (XFC). Laboratory testing results match predictions from the Advanced Electrolyte Model, indicating that combinations of low molecular weight solvents are crucial for fast charge electrolytes.
ENERGY STORAGE MATERIALS
(2022)
Article
Engineering, Chemical
Adam Yonge, Gabriel S. Gusmao, Rakesh Batchu, M. Ross Kunz, Zongtang Fang, Rebecca Fushimi, Andrew J. Medford
Summary: This paper proposes a framework for quantifying initial state uncertainties in transient measurements using the temporal analysis of products (TAP) reactor. Two methods are introduced to approximate parameter variances and provide insights into the structural certainty of the model. The initial state covariance matrix can be merged with the experimental noise covariance matrix to provide a unified description of parameter uncertainties for TAP experiments.
Article
Chemistry, Physical
Pete Barnes, Yunxing Zuo, Kiev Dixon, Dewen Hou, Sungsik Lee, Zhiyuan Ma, Justin G. Connell, Hua Zhou, Changjian Deng, Kassiopeia Smith, Eric Gabriel, Yuzi Liu, Olivia O. Maryon, Paul H. Davis, Haoyu Zhu, Yingge Du, Ji Qi, Zhuoying Zhu, Chi Chen, Zihua Zhu, Yadong Zhou, Paul J. Simmonds, Ariel E. Briggs, Darin Schwartz, Shyue Ping Ong, Hui Xiong
Summary: A nanostructured rock-salt Nb2O5 electrode formed through amorphous-to-crystalline transformation during cycling with Li+ exhibits superb cycling stability and high capacity at high rates.
Article
Chemistry, Physical
Matthew S. Barclay, Christopher K. Wilson, Simon K. Roy, Olga A. Mass, Olena M. Obukhova, Rostyslav P. Svoiakov, Anatoliy L. Tatarets, Azhad U. Chowdhury, Jonathan S. Huff, Daniel B. Turner, Paul H. Davis, Ewald A. Terpetschnig, Bernard Yurke, William B. Knowlton, Jeunghoon Lee, Ryan D. Pensack
Summary: An elusive oblique packing arrangement in molecules is achieved using mechanically interlocked molecules. The spatial arrangement of molecules is controlled by templating and chemical substitution. The distinct signature of oblique packing is observed in the absorption spectra and validated by theoretical modeling. Fine control of packing is demonstrated by fluorinating the macrocycle of the molecules.
Article
Chemistry, Physical
Matthew S. Barclay, Jonathan S. Huff, Ryan D. Pensack, Paul H. Davis, William B. Knowlton, Bernard Yurke, Jacob C. Dean, Paul C. Arpin, Daniel B. Turner
Summary: In this study, the measured spectra of two laser dyes are fitted to microscopic models of femtosecond coherence spectra (FCS) arising from molecular vibrations. Coherent quantum-beat signals are classified as fundamentals or overtones and their Huang-Rhys factors and anharmonicity values are quantified. This work solidifies the use of FCS for analysis of coherent quantum beats arising from molecular vibrations.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Matthew S. Barclay, Azhad U. Chowdhury, Austin Biaggne, Jonathan S. Huff, Nicholas D. Wright, Paul H. Davis, Lan Li, William B. Knowlton, Bernard Yurke, Ryan D. Pensack, Daniel B. Turner
Summary: DNA is a re-configurable, biological information-storage unit, but there is still much to learn about its heterogeneous structural dynamics. In this study, femtosecond, two-dimensional electronic spectroscopy is used to probe local conformations in different DNA samples. The analysis reveals a strong excitation-emission correlation in only the double-stranded DNA-Cy5 complex, indicating inhomogeneous broadening. Molecular dynamics simulations support the conclusion that this broadening is caused by a specific conformer found only in the double-stranded DNA-Cy5 complex. These insights will contribute to future studies on DNA's structural heterogeneity.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Nicholas D. Wright, Jonathan S. Huff, Matthew S. Barclay, Christopher K. Wilson, German Barcenas, Katelyn M. Duncan, Maia Ketteridge, Olena M. Obukhova, Alexander I. Krivoshey, Anatoliy L. Tatarets, Ewald A. Terpetschnig, Jacob C. Dean, William B. Knowlton, Bernard Yurke, Lan Li, Olga A. Mass, Paul H. Davis, Jeunghoon Lee, Daniel B. Turner, Ryan D. Pensack, Ryan D. Pensack
Summary: This study characterized the electronic structure and excited-state dynamics of a series of indolenine-based squaraine dyes incorporating electron donating and/or electron withdrawing substituents. The results showed that the introduction of these substituents increased the static dipole moment difference (delta d) while maintaining a large transition dipole moment (mu). However, asymmetrically substituted dyes exhibited a significant nonradiative decay pathway that drastically reduced their excited-state lifetime (tau), indicating the need for strategies such as rigidifying the pi-conjugated network to ensure long tau.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Correction
Chemistry, Physical
Logan Ward, Susan Barbinec, Eric J. Dufek, David A. Howey, Venkatasubramanian Viswanathan, Muratahan Aykol, David A. C. Beck, Benjamin Blaiszik, Bor-Rong Chen, George Crabtree, Simon Clark, Valerio De Angelis, Philipp Dechent, Matthieu Dubarry, Erica E. Eggleton, Donal P. Finegan, Ian Foster, Chirranjeevi Balaji Gopal, Patrick K. Herring, Victor W. Hu, Noah H. Paulson, Yuliya Preger, Dirk Uwe-Sauer, Kandler Smith, Seth W. Snyder, Shashank Sripad, Tanvir R. Tanim, Linnette Teo
Article
Chemistry, Physical
KatelynM. Duncan, Hannah M. Byers, Madaline E. Houdek, Simon K. Roy, Austin Biaggne, Matthew S. Barclay, Lance K. Patten, Jonathan S. Huff, Donald L. Kellis, Christopher K. Wilson, Jeunghoon Lee, Paul H. Davis, Olga A. Mass, Lan Li, Daniel B. Turner, John A. Hall, William B. Knowlton, Bernard Yurke, Ryan D. Pensack
Summary: In this study, the electronic structure and excited-state dynamics of monomers and aggregates of four asymmetric polymethine dyes templated via DNA were characterized. The asymmetric polymethine dye monomers exhibited large transition dipole moments (mu), appreciable static dipole moment differences (Delta d), and long excited-state lifetimes (tau(p)). Dye Dy 754 displayed the strongest propensity for aggregation and exciton delocalization, with promising values of the excitonic hopping parameter (J).
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Yiqin Hu, Zongtang Fang, Monica Vasiliu, David A. Dixon
Summary: The dehydration and dehydrogenation of ethanol on (TiO2)(n), n = 2-4 nanoclusters were studied using density functional theory. Physisorption and chemisorption of ethanol on the trimer and tetramer at the bridge Ti site were found to be thermodynamically favorable compared to the Ti site with a terminal Ti+O. Different reaction coordinates for dehydration were predicted for the dimer, trimer, and tetramer. The results of the nanoclusters for n = 3 and 4 are in line with experimental findings on the reactivity of ethanol on TiO2 (110) surface sites.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Nanoscience & Nanotechnology
Zhenzhen Yang, Tanvir R. Tanim, Haoyu Liu, Ira Bloom, Eric J. Dufek, Baris Key, Brian J. Ingram
Summary: During XFC of lithium-ion batteries, LLI and reaction mechanisms at the anode/electrolyte interface are crucial factors. The causes of LLI and their quantification are still challenging. This study investigates the evolution and interactions of aging mechanisms at the anode/electrolyte interface. The results provide a comprehensive analytical framework for understanding anodic degradation mechanisms and assessing XFC lithium-ion battery capacity fade.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Instruments & Instrumentation
J. S. Huff, K. M. Duncan, C. J. van Galen, M. S. Barclay, W. B. Knowlton, B. Yurke, P. H. Davis, D. B. Turner, R. J. Stanley, R. D. Pensack
Summary: Developmental details of a high-sensitivity Stark absorption spectrometer with a laser-driven light source are reported. The spectrometer exhibits minimal intensity fluctuations, drift, and 1/f noise, with additional features of balanced detection and multiplex sampling. Measurements show low noise amplitudes.
REVIEW OF SCIENTIFIC INSTRUMENTS
(2023)
Article
Chemistry, Physical
Nicholas D. Wright, Jonathan S. Huff, Matthew S. Barclay, Christopher K. Wilson, German Barcenas, Katelyn M. Duncan, Maia Ketteridge, Olena M. Obukhova, Alexander I. Krivoshey, Anatoliy L. Tatarets, Ewald A. Terpetschnig, Jacob C. Dean, William B. Knowlton, Bernard Yurke, Lan Li, Olga A. Mass, Paul H. Davis, Jeunghoo Lee, Daniel B. Turner, Ryan D. Pensack
Summary: Molecular (dye) aggregates are a materials platform of interest in various fields, and this study characterizes the properties of certain asymmetric squaraine dyes and suggests strategies to enhance their interaction.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)