Article
Chemistry, Physical
Yifei Xu, Lina Gao, Qianqian Liu, Qian Liu, Zerui Chen, Wei Zhao, Xueqian Kong, Hao Bin Wu
Summary: Metal-organic frameworks have been developed as solid electrolytes for Li batteries. A study demonstrates metal-organic solid electrolytes with superionic conductivity by grafting hemilabile anionic chains in the pore channels of an Al-based metal-organic framework. The solid electrolyte shows excellent stability and enables remarkable rate performance in Li batteries.
ENERGY STORAGE MATERIALS
(2023)
Article
Materials Science, Ceramics
Chaeeun Kim, Young-Il Kim
Summary: The ionic conductivity of complex rock-salt Li3TaO4 was studied by modifying the low-temperature and high-temperature polymorphs with Li/Ta non-stoichiometry. The results showed that the disordered low-temperature phase had higher ionic conductivity than the ordered high-temperature phase, and the Li/Ta non-stoichiometry contributed to an increase in the ionic conductivity of Li3TaO4.
CERAMICS INTERNATIONAL
(2023)
Article
Chemistry, Physical
Benedikt Soeldner, Kristof Grohe, Peter Neidig, Jelena Auch, Sebastian Blach, Alexander Klein, Suresh K. Vasa, Lars V. Schaefer, Rasmus Linser
Summary: Understanding macromolecular function, interactions, and stability requires detailed assessment of conformational ensembles. Limited by the qualitative or low abundance of solid-state nuclear magnetic resonance internuclear distance information, accurately elucidating the spatial dynamics of solid proteins at physiological temperatures is challenging. However, this study demonstrates unprecedented access to abundant proton-proton internuclear distances, enabling accurate molecular dynamics simulations and providing atomic-level spatial details of conformational dynamics in various biomolecular systems.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Bo Fan, Zebo Guan, Hongjiao Wang, Lilin Wu, Wenzhi Li, Shibang Zhang, Bai Xue
Summary: This study quantitatively investigated the evolution of electrochemical impedance spectra of all-solid-state lithium-sulfur batteries, revealing the characteristics of different interfaces and dynamic processes within the battery. The analysis of impedance spectra indicated that Li diffusion plays a significant role in charge transfer within the active materials.
SOLID STATE IONICS
(2021)
Article
Energy & Fuels
Kieran Mc Carthy, Hemtej Gullapalli, Tadhg Kennedy
Summary: This paper proposes an accurate online model for estimating the capacity of Li-ion batteries. By analyzing the effect of aging on battery impedance characteristics, the model estimates the current battery capacity based on the relationship between capacity fade and impedance increase. Experimental results demonstrate the high accuracy and reliability of the proposed model.
Article
Chemistry, Physical
Julia Moeller, Vanessa van Laack, Katharina Koschek, Patrick Bottke, Michael Wark
Summary: In order to improve the safety of lithium-ion batteries, alternatives to liquid electrolytes are being widely studied. One of the promising alternatives is the plastic-crystal succinonitrile (SN) that can solvate various Li salts. By introducing polymers, the system can be further enhanced with higher melting points and adjustable properties.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Xiaoyu Wang, Yuqi Wang, Yuan Kang, Bing Yao, Xinsheng Peng
Summary: The burgeoning field of miniaturized and portable electronic devices requires advancements in micro-energy storage technology. This study introduces a strategy that utilizes flexible metal-organic framework (MOF) nanosheet-based membranes to enhance the performance of deep eutectic solvent (DES)-based micro-supercapacitors (MSC) through the construction of quasi-solid-state electrolytes. The MSCs engineered with this system exhibit excellent performance in terms of areal-specific capacitance, energy density, and power density, and maintain consistent performance even when subjected to bending.
Article
Chemistry, Multidisciplinary
Xiangsi Liu, Ziteng Liang, Yuxuan Xiang, Min Lin, Qi Li, Zigeng Liu, Guiming Zhong, Riqiang Fu, Yong Yang
Summary: The recent applications of solid-state nuclear magnetic resonance (ssNMR) and magnetic resonance imaging (MRI) techniques in Li/Na batteries are reviewed, emphasizing the importance of investigating battery materials structure, solid electrolyte interfaces, and in situ research.
ADVANCED MATERIALS
(2021)
Article
Nanoscience & Nanotechnology
Aamir Iqbal Waidha, Thimo Ferber, Manuel Donzelli, Niloofar Hosseinpourkahvaz, Vanita Vanita, Klaus Dirnberger, Sabine Ludwigs, Rene Hausbrand, Wolfram Jaegermann, Oliver Clemens
Summary: The research demonstrates that as the ceramic weight fraction increases in the composites, the ionic conductivity is reduced, and alternative lithium-ion transport pathways become accessible compared to filler-free electrolytes. The study explores the role of the chemical and morphological properties of the ceramic filler in polymer-rich and ceramic-rich composite electrolytes, highlighting the significant contribution of the intrinsic conductivity of the ceramic filler to the overall conductive process in the ceramic-rich systems. Additionally, the stability of the garnet/PEO interface is investigated using X-ray photoelectron spectroscopy, and its impact on lithium-ion transport is studied via EIS.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Nanoscience & Nanotechnology
Eric Jianfeng Cheng, Kiyoshi Kanamura, Yosuke Kushida, Takeshi Abe
Summary: Solid-state Li-metal batteries have the potential for high safety and high energy densities, but their practical application is limited by the large interfacial resistance. In this study, a low interfacial resistance was achieved by depositing an LCO film onto an Al-doped LLZO substrate and pre-coating LCO particles with LBO. The all-solid-state Li/LLZO/LBO-LCO cells demonstrated high capacity retention and the degradation mechanism was investigated using EIS and in-situ SEM analysis.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Nanoscience & Nanotechnology
Eric Jianfeng Cheng, Kiyoshi Kanamura, Yosuke Kushida, Takeshi Abe
Summary: Garnet-type LLZO is a stable solid-state fast-ion conductor, but the large interfacial resistance between LLZO and cathode materials limits its practical application. By using pre-coated LCO particles and LBO method, the interfacial resistance was successfully reduced on the LLZO substrate, achieving relatively high capacity retention.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Gustavo M. Hobold, Kyeong-Ho Kim, Betar M. Gallant
Summary: Despite its potential as a candidate for meeting energy targets of Li-ion batteries, the lithium metal anode has not achieved the necessary Coulombic efficiency for long cycle life. The limitations are due to the solid electrolyte interphase (SEI), which stabilizes and protects the deposited lithium. The study quantifies the effect of Li+ exchange with the SEI on Coulombic efficiency and reveals a chemistry-dependent picture of SEI evolution. These findings have implications for high-CE electrolyte design targeting high rates.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Nanoscience & Nanotechnology
Leon Katzenmeier, Leif Carstensen, Aliaksandr S. Bandarenka
Summary: This study investigates the temperature dependence of the depletion layer properties in a model solid-state ion conductor using electrochemical impedance spectroscopy. The results show that the thickness of the depletion layer is proportional to the temperature, and the activation energy inside the layer increases compared to the bulk electrolyte.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Multidisciplinary Sciences
Mokwon Kim, Hyunpyo Lee, Hyuk Jae Kwon, Seong-Min Bak, Cherno Jaye, Daniel A. Fischer, Gabin Yoon, Jung O. Park, Dong-Hwa Seo, Sang Bok Ma, Dongmin Im
Summary: A newly proposed strategy involves designing a highly conductive ruthenium-based composite as a carbon-free cathode to improve the cycle life and capacity of solid-state lithium-oxygen batteries. By utilizing this approach, the batteries achieved a specific capacity of 200 milliampere hour per gram over 665 discharge/charge cycles, showcasing a notable improvement compared to existing cathodes.
Article
Chemistry, Physical
Sumit Khatua, Y. Bhaskara Rao, K. Ramakrushna Achary, L. N. Patro
Summary: LiZr2(PO4)3 (LZP), a Li-ion conducting solid electrolyte with NASICON structure, has shown potential for safer all-solid-state Li-ion batteries. This study successfully synthesized LZP with rhombohedral structure at room temperature using a modified sol-gel method with lower sintering temperature (900°C). The effect of sintering temperature on the structure and transport behavior of LZP was investigated, showing that LZP sintered at 900°C had the highest total conductivity, indicating the significant role of grain boundary conductions.
SURFACES AND INTERFACES
(2023)
Article
Chemistry, Physical
Maria Gombotz, Katharina Hogrefe, Alexandra Wilkening, Bernhard Gadermaier, Martin Wilkening
Summary: Nanostructured materials prepared by high-energy ball milling exhibit different properties compared to coarse-grained materials, with a large fraction of point defects and structurally disordered interfacial regions. This study investigated how the overall conductivity of SmF3 can be enhanced through mechanical treatment and how aliovalent substitution can further improve anion transport. The results showed a significant increase in total conductivity and electrical relaxation frequencies when transitioning from nano-SmF3 to Sm1-x Bax F3-x for x = 0.1.
ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Katharina Hogrefe, Nicolo Minafra, Isabel Hanghofer, Ananya Banik, Wolfgang G. Zeier, H. Martin R. Wilkening
Summary: Solid electrolytes are crucial for future energy storage systems, and Li-bearing argyrodites are considered to be leading materials for Li+ ion conductivity. In this study, the effect of cation substitution on Li+ ion dynamics was investigated, revealing the microscopic origins of improved ion transport efficiency.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Olha Skurikhina, Maria Gombotz, Mamoru Senna, Martin Fabian, Matej Balaz, Klebson Lucenildo Da Silva, Marcela Achimovicova, H. Martin R. Wilkening, Bernhard Gadermaier
Summary: This study investigates the ion transport properties of K2Ti6O13 using broadband impedance spectroscopy, revealing that K+ is the main charge carrier and the size of the mobile cation correlates with conductivity and activation energy.
ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS
(2022)
Article
Materials Science, Multidisciplinary
Michael Sternad, Georg Hirtler, Michael Sorger, Daniel Knez, Kamil Karlovsky, Magdalena Forster, H. Martin R. Wilkening
Summary: Miniaturized and rechargeable energy storage systems are expected to revolutionize information sharing in various fields, while also significantly impacting sectors such as medicine, security, autonomous driving, and artificial intelligence.
ADVANCED MATERIALS TECHNOLOGIES
(2022)
Correction
Chemistry, Physical
Isabel Hanghofer, Gunther J. Redhammer, Sebastian Rohde, Ilie Hanzu, Anatoliy Senyshyn, H. Martin R. Wilkening, Daniel Rettenwander
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Lukas Schweiger, Katharina Hogrefe, Bernhard Gadermaier, Jennifer L. M. Rupp, H. Martin R. Wilkening
Summary: Solids with high Li+ dynamics are crucial for high performance all-solid-state batteries. Molecular dynamics simulations suggest that introducing local disorder can enhance the ionic conductivity of LGPS. However, experimental evidence shows that ball-milling has a negative impact on Li+ ion transport in LGPS.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Inorganic & Nuclear
Maria Gombotz, Alexandra Wilkening, H. Martin R. Wilkening
Summary: This study investigates the ion dynamics of interfacial Li2S in lithium-ion batteries. Nanostructured Li2S was prepared through high-energy ball milling, and its temperature-dependent ionic conductivity was studied using impedance spectroscopy. The results show that ball-milled Li2S exhibits significantly higher ion conductivity and lower average activation energy compared to the unmilled counterpart. Structural disorder, stress, and local distortions are believed to be responsible for these changes in macroscopic transport parameters.
ZEITSCHRIFT FUR NATURFORSCHUNG SECTION B-A JOURNAL OF CHEMICAL SCIENCES
(2022)
Article
Energy & Fuels
Patrick Posch, Sarah Lunghammer, Alexandra Wilkening, Katharina Hogrefe, H. Martin R. Wilkening
Summary: In this study, nucleus-specific Li-7 and Na-23 nuclear magnetic resonance (NMR) spectroscopy was used to investigate the motion processes in mixed-conducting Li4Na (x) Ti5O12 materials. The results show that the diffusivity of Li+ ions increases significantly in the early stages of chemical sodiation, while there is limited data on the diffusion properties of Na+ ions. In addition, the formation of interfacial solid solutions was observed at very low sodiation levels (x = 0.1), and these regions covered almost the entire crystallite area at x = 0.5, enabling facile long-range ion transport.
JOURNAL OF PHYSICS-ENERGY
(2023)
Article
Chemistry, Physical
Jonas Spychala, H. Martin R. Wilkening, Alexandra Wilkening
Summary: Li2OHCl is a suitable Li+ ionic conductor composed of abundant elements excluding Li. Its low melting point enables easy synthesis methods. However, the clear picture of Li+ self-diffusion is still challenging to prove, as it is suggested to be coupled to OH- rotational dynamics in Li2OHCl.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Maria Gombotz, Caroline Hiebl, Florian Stainer, H. Martin R. Wilkening
Summary: The development of ceramic proton conductors is of great interest due to their potential use in energy storage systems. Li6La3ZrTaO12 (LLZTO) has been found to exhibit rapid Li+ diffusivity. By treating a single crystal in water or glacial acetic acid, mobile Li+ ions can be exchanged with protons, resulting in a mixed proton-lithium ionic conductor. In this study, the diffusion of H+ protons and Li+ ions in the exchanged LLZTO has been investigated using element-specific H-1 and Li-7 NMR spectroscopy. The results show slower long-range Li-7 diffusion but relatively high H+ diffusivity, albeit slower than Li+ dynamics. By measuring spin-lattice relaxation and self-diffusion coefficient D(H) of H+ dynamics, energy barriers and transport properties have been determined, suggesting the potential of designing fast transport pathways for protons in ceramics.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Materials Science, Multidisciplinary
Patrick Bottke, Katharina Hogrefe, Julia Kohl, Suliman Nakhal, Alexandra Wilkening, Paul Heitjans, Martin Lerch, H. Martin R. Wilkening
Summary: The visualization of atomic or ionic jump processes on a nanometer length scale is important for understanding diffusion pathways in solid electrolytes. This study used high-resolution 6Li nuclear magnetic resonance (NMR) spectroscopy to investigate Li+ exchange processes in Li3VF6. The results confirmed the preferred diffusion pathways and provided further insights into ion dynamics between corner-shared Li-bearing polyhedra.
MATERIALS RESEARCH BULLETIN
(2023)
Article
Chemistry, Physical
Alexander Komar, Dirk Wilmer, Martin R. Wilkening, Ilie Hanzu
Summary: The determination of stray capacitance in impedance measuring cells is crucial for studying solid ion conductors. We present a general method that accurately determines stray capacitance and can be applied to various impedance cells or sample holders for temperature conductivity measurements. Experimental calibration on a 2032-type coin cell sample holder demonstrates the reliability of our method for impedance measurements of air sensitive materials. Our method serves as an example of good practice in the field of solid electrolytes, solid state batteries, and dielectric materials investigations.
SOLID STATE IONICS
(2023)
Review
Electrochemistry
Erwin Hueger, Lukas Riedel, Jing Zhu, Jochen Stahn, Paul Heitjans, Harald Schmidt
Summary: Li-Nb-O-based insertion layers are used in Li-ion batteries to protect electrodes and electrolytes and enhance Li transport. This study reviews the suitability of different Li-Nb-O-based compounds for battery operation, especially amorphous LiNbO3 films. Experimental results show that the amorphous LiNbO3 films have higher porosity and better Li diffusivity compared to other similar metal oxides. The films exhibit high reversible capacity and fast cycling, which make them suitable for improved battery performance.
Article
Chemistry, Multidisciplinary
Jian-Fang Wu, Zheyi Zou, Bowei Pu, Lukas Ladenstein, Shen Lin, Wenjing Xie, Shen Li, Bing He, Yameng Fan, Wei Kong Pang, H. Martin R. Wilkening, Xin Guo, Chaohe Xu, Tao Zhang, Siqi Shi, Jilei Liu
Summary: The softness of sulfur sublattice and rotational PS4 tetrahedra in thiophosphates lead to liquid-like ionic conduction, while the existence of such conduction in rigid oxides remains unclear. This study discovers 1D liquid-like Li-ion conduction in LiTa2PO8 and its derivatives, enabled by doping strategies, with low activation energy and short mean residence time of Li ions on interstitial sites. The findings provide principles for the future design of improved solid electrolytes without modifications to achieve stable ionic transport.
ADVANCED MATERIALS
(2023)
