Review
Chemistry, Multidisciplinary
Chao Chen, Kexin Wang, Hongying He, Emil Hanc, Masashi Kotobuki, Li Lu
Summary: As one of the most promising candidates for solid-state batteries, Li7La3Zr2O12 (LLZO) garnet-type solid electrolyte has high ionic conductivity and good electrochemical stability. However, the reliable and controllable preparation of LLZO ceramics with desirable properties remains a challenge.
Article
Chemistry, Physical
Madison Olson, Jacob Wheaton, Mary Okkema, Nicholas Oldham, Steve W. Martin
Summary: Na4P2S7-6xO4.62xN0.92x (NaPSON) glassy solid electrolytes (GSEs) were studied for their electrochemical properties and processability into thin films. The x = 0.2 composition (NaPSON-2) showed high conductivity, non-crystallizability, stability against Na-metal, and support for symmetric cell cycling. Thin films of NaPSON-2 exhibited unchanged conductivity and slow growth in resistance, while NaPSON-2 disc displayed stability and reaction products in the bulk. The surface stability was attributed to the segregation of trigonally coordinated nitrogen.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Mauricio R. Bonilla, Fabian A. Garcia Daza, Pierre Ranque, Frederic Aguesse, Javier Carrasco, Elena Akhmatskaya
Summary: The study investigates the impact of composite materials on solid-state electrolytes, revealing insights into interfacial Li-ion dynamics through molecular dynamics simulations. The results help explain a previously reported drop in conductivity and pave the way for computational modeling of other conductive filler/polymer combinations as well as the rational design of composite solid-state electrolytes.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Review
Chemistry, Multidisciplinary
Tian Wu, Wei Dai, Meilu Ke, Qing Huang, Li Lu
Summary: Solid-state thin-film mu-batteries are micro-sized energy storage devices with high safety and increased capacity, which face various scientific and technical challenges before practical application. Understanding ion transfer in solid-state electrolytes and the effects of chemistry on electrochemical behaviors is crucial for the development of these batteries.
Review
Energy & Fuels
Moran Balaish, Juan Carlos Gonzalez-Rosillo, Kun Joong Kim, Yuntong Zhu, Zachary D. Hood, Jennifer L. M. Rupp
Summary: This review critically discusses the research status of high-energy-density solid-state batteries, focusing on cost-effective processing and the integration of solid electrolyte materials. The future design of SSBs should consider capturing the thermal processing budget and stability of the oxide solid electrolyte phase.
Article
Chemistry, Physical
Wanzheng Lu, Mingzhe Xue, Cunman Zhang
Summary: SSLB is regarded as a promising candidate for energy storage devices, with LLZO solid-state electrolyte playing a key role, and significant progress has been made in research, although challenges remain to be addressed.
ENERGY STORAGE MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Chunxiang Xian, Shengzhao Zhang, Ping Liu, Lei Huang, Xinping He, Shenghui Shen, Feng Cao, Xinqi Liang, Chen Wang, Wangjun Wan, Yongqi Zhang, Xin Liu, Yu Zhong, Yang Xia, Minghua Chen, Wenkui Zhang, Xinhui Xia, Jiangping Tu
Summary: This study proposes an advanced gel polymer electrolyte for all-solid-state lithium metal batteries, which exhibits high mechanical strength, low flammability, improved ionic conductivity, and good compatibility with the lithium anode. The assembled batteries show enhanced cycling performance and high-rate capacity.
Article
Chemistry, Physical
Young-Woong Song, Hyochan Lee, Sang-Jun Park, Dahee Hwang, Min-Young Kim, Jaekook Kim, Jinsub Lim
Summary: Composite solid electrolytes (CSEs) show promise for various applications due to the combined benefits of solid polymers and inorganic solid electrolytes. In this study, a solvent-assisted ultrasonication process is introduced to effectively disperse particles and inhibit surface resistance in CSEs. Ultrasonicated LLZTO exhibits higher ionic conductivity and Li transference number compared to dry-milled LLZTO, leading to improved performance and stability in battery testing.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Huanyu Zhang, Faruk Okur, Claudia Cancellieri, Lars P. H. Jeurgens, Annapaola Parrilli, Dogan Tarik Karabay, Martin Nesvadba, Sunhyun Hwang, Antonia Neels, Maksym V. Kovalenko, Kostiantyn V. Kravchyk
Summary: Li dendrites form in Li7La3Zr2O12 (LLZO) solid electrolytes due to volume changes and voids at the Li metal/LLZO interface. Dense-porous LLZO membranes provide a solution by storing lithium in the pores, avoiding volume changes and void formation. The reported method of sequential tape-casting allows for the production of bilayer membranes with high performance.
Article
Engineering, Electrical & Electronic
Mahnaz Ashuri, Mohammad Golmohammad, Alireza Soleimany Mehranjani, Mohammadali Faghihi Sani
Summary: The study utilized the combustion sol-gel technique to prepare an Al-doped LLZO solid electrolyte, showcasing densification properties with two different shrinkage rates. With 0.25 mol Al-dopant, a high bulk conductivity of 5.89 x 10(-4) S cm(-1) was achieved at 1100 degrees C. The effect of Al-doping on electrochemical properties was extensively investigated using AC impedance spectroscopy and distribution of relaxation times (DRT) method.
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
(2021)
Article
Chemistry, Multidisciplinary
Hoang Long Nguyen, Van Tung Luu, Manh Cuong Nguyen, Sung Hoon Kim, Quoc Hung Nguyen, Nungu Israel Nungu, Yun-Seok Jun, Wook Ahn
Summary: All-solid-state Li batteries (ASSLBs) are limited in their application due to their narrow operating temperature range, low ionic conductivity, poor stability, and complex production process. In this study, a simple method combining various battery candidates was employed to solve these limitations and a solid polymer electrolyte with high conductivity and excellent cycling stability was successfully prepared.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Yongtao Wang, Lingqiao Wu, Xianwei Guo, Peipei Ding, Zhiyuan Lin, Yinzhong Wang, Xin Yin, Haijun Yu
Summary: A thin free-standing composite solid electrolyte film with high ionic conductivity and wide electrochemical stability window is prepared using tape casting and solution infusion method. Solid-state lithium metal batteries based on this film and LiCoO2 cathode exhibit good cycling stability and capacity retention with a 4.5 V cut-off voltage.
CHEMICAL COMMUNICATIONS
(2022)
Article
Nanoscience & Nanotechnology
Renming Deng, Bingyuan Ke, Yonghui Xie, Shoulin Cheng, Congcong Zhang, Hong Zhang, Bingan Lu, Xinghui Wang
Summary: Thin-film all-solid-state lithium-sulfur (TFLSBs) batteries were successfully fabricated using vertical graphene nanosheets-Li2S (VGsLi(2)S) composite thin-film cathode, lithium-phosphorous-oxynitride (LiPON) thin-film solid electrolyte, and Li metal anode. The solid-state Li-S system with an unlimited Li reservoir fundamentally eliminated the shuttle effect and maintained a stable VGs-Li2S/LiPON interface, demonstrating excellent long-term cycling stability and high temperature tolerance. This study presents a new development strategy for secure and high-performance rechargeable all-solid-state thin-film batteries.
NANO-MICRO LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Quoc Hung Nguyen, Van Tung Luu, Hoang Long Nguyen, Young-Woo Lee, Younghyun Cho, Se Young Kim, Yun-Seok Jun, Wook Ahn
Summary: The research focused on utilizing a cubic garnet oxide electrolyte and ionic liquid in combination with a polymer electrolyte to produce a composite electrolyte membrane with high ionic conductivity. The composite electrolyte membrane was effective in suppressing lithium dendrite growth, as confirmed through symmetric lithium stripping/plating tests. The full cell showed a high specific capacity and capacity retention after 100 cycles, highlighting the potential of solid polymer electrolytes in enhancing the performance of all-solid-state batteries.
FRONTIERS IN CHEMISTRY
(2021)
Article
Chemistry, Physical
Lei Zhang, Quanchao Zhuang, Runguo Zheng, Zhiyuan Wang, Hongyu Sun, Hamidreza Arandiyan, Yuan Wang, Yanguo Liu, Zongping Shao
Summary: This article provides a review and analysis of garnet-based all-solid-state lithium batteries (ASSLBs), with a focus on the optimization of LLZO structure, preparation of high-quality LLZO-based solid-state electrolytes (SSEs), engineering of the LLZO-based SSEs interface, and the realization of LLZO-based ASSLBs with high energy density.
ENERGY STORAGE MATERIALS
(2022)
Article
Materials Science, Ceramics
Markus Wolf, Daniel Emil Mack, Georg Mauer, Olivier Guillon, Robert Vassen
Summary: This study investigated the deposition of ytterbium disilicate (YbDS) at short stand-off distances and different total feed rates and oxy-fuel ratios. The results showed that the overall degree of crystallinity could be maintained above 90%, with porosities below 10% achieved. However, fully dense coatings were hindered by the accumulation of stresses within the coatings.
INTERNATIONAL JOURNAL OF APPLIED CERAMIC TECHNOLOGY
(2022)
Article
Chemistry, Physical
Markus Mann, Michael Kuepers, Grit Haeuschen, Martin Finsterbusch, Dina Fattakhova-Rohlfing, Olivier Guillon
Summary: LLZO is a promising oxide-ceramic solid electrolyte for all-solid-state batteries, with dopants like Al, Ta, Nb, Ga, and W enhancing its ionic conductivity. The study investigates the impact of hafnium impurities on tantalum-doped LLZO, finding that hafnium has limited effect on the material's performance up to a certain concentration level. This research has implications for reducing the cost of LLZO by using lower grade zirconium sources.
Article
Materials Science, Ceramics
Moritz Kindelmann, Moritz L(ukas) Weber, Mark Stamminger, Rahel Buschhaus, Uwe Breuer, Martin Bram, Olivier Guillon
Summary: Due to the increasing applications of ceramic components in reactive etching processes, there is a growing interest in understanding the specific erosion behavior of highly etch-resistant materials like yttrium oxide (Y2O3). However, the existing investigations in this field have limited comparability, leading to a lack of general understanding of the erosion mechanisms. In order to address this issue, this study systematically investigates the erosion behavior of Y2O3 under various plasma etching parameters and identifies three distinct erosion regimes.
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
(2022)
Article
Materials Science, Ceramics
Alexander Bauer, Md Yusuf Ali, Hans Orthner, Sven Uhlenbruck, Hartmut Wiggers, Dina Fattakhova-Rohlfing, Olivier Guillon
Summary: Through spray flame synthesis, La2Zr2O7 nanoparticles were prepared and added to Li7La3Zr2O12 powder, resulting in a significant improvement in ionic conductivity at lower temperatures, leading to a more than twofold increase in conductivity while operating at a reduced sintering temperature.
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
(2022)
Article
Materials Science, Multidisciplinary
Walter Sebastian Scheld, Sandra Lobe, Sven Uhlenbruck, Christian Dellen, Yoo Jung Sohn, Linda Charlotte Hoff, Frank Vondahlen, Olivier Guillon, Dina Fattakhova-Rohlfing
Summary: A rapid photonic sintering process was used to obtain compact films of cathode active material of lithium batteries. The films showed homogeneous densification and structural consistency, and exhibited good electrochemical activity.
Article
Materials Science, Multidisciplinary
Xin Lu, Chih-Long Tsai, Shicheng Yu, Hongying He, Osmane Camara, Hermann Tempel, Zigeng Liu, Anna Windmueller, Evgeny Alekseev, Shibabrata Basak, Li Lu, Ruediger-A Eichel, Hans Kungl
Summary: This article discusses the importance and current development status of lithium-ion conductive solid electrolytes in all-solid-state batteries. Phosphosulfide electrolytes are considered the most promising materials with high conductivity and stability. The article is divided into two parts, providing a detailed discussion on the compositions, structures, processing, and performance of different phosphosulfide electrolytes. Future research will focus on the development of new electrolytes and improvement of their performance.
FUNCTIONAL MATERIALS LETTERS
(2022)
Article
Electrochemistry
Anna Windmueller, Tatiana Renzi, Hans Kungl, Svitlana Taranenko, Emmanuelle Suard, Francois Fauth, Mathieu Duttine, Chih-Long Tsai, Ruoheng Sun, Yasin Emre Durmus, Hermann Tempel, Peter Jakes, Christian Masquelier, Ruediger-A. Eichel, Laurence Croguennec, Helmut Ehrenberg
Summary: Positive electrodes with high energy densities for Lithium-ion batteries often rely on toxic and costly transition metals. This study synthesized iron-based spinel materials and investigated their properties using various experimental methods. Unexpected results were observed and the relationship between material performance and electrolyte was also revealed.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Walter Sebastian Scheld, Sandra Lobe, Christian Dellen, Martin Ihrig, Grit Hauschen, Linda Charlotte Hoff, Martin Finsterbusch, Sven Uhlenbruck, Olivier Guillon, Dina Fattakhova-Rohlfing
Summary: Rapid thermal annealing techniques are promising for processing ceramic materials, especially those containing elements with high vapor pressure. In this study, the sintering method RTP was used to fabricate composite ceramic cathodes of LLZO and LCO, effectively mitigating secondary phase formation between the two materials.
JOURNAL OF POWER SOURCES
(2022)
Article
Energy & Fuels
Moritz L. Weber, Moritz Kindelmann, Egbert Wessel, Alexandros Sarantopoulos, Norbert H. Menzler, Regina Dittmann, Rainer Waser, Olivier Guillon, Christian Lenser, Felix Gunkel
Summary: Metal exsolution is a dynamic process driven by reducing atmosphere and elevated temperatures, which leads to the self-assembly of nanoparticles at the surface of complex perovskite catalysts. The characteristics of metal exsolution catalysts can be highly inhomogeneous, and the anisotropic surface properties of ceramic oxides have been found to significantly affect the exsolution behavior.
JOURNAL OF PHYSICS-ENERGY
(2023)
Article
Chemistry, Multidisciplinary
Andrea Schreiber, Melanie Rosen, Katja Waetzig, Kristian Nikolowski, Nikolas Schiffmann, Hartmut Wiggers, Michael Kuepers, Dina Fattakhova-Rohlfing, Wilhelm Kuckshinrichs, Olivier Guillon, Martin Finsterbusch
Summary: All-solid-state batteries are a promising research topic for their high energy density and safety. However, implementing oxide ceramic electrolytes in industrial cells remains challenging. To address this, researchers proposed a target cell design combining two promising oxidic electrolytes, LLZO and LATP, and assessed their environmental impact. In-depth life cycle assessment revealed surprising similarities between oxide-based all-solid-state batteries and conventional Li-ion batteries.
Article
Chemistry, Multidisciplinary
An-Yuan Hou, Chih-Yang Huang, Chih-Long Tsai, Chun-Wei Huang, Roland Schierholz, Hung-Yang Lo, Hermann Tempel, Hans Kungl, Ruediger-A. Eichel, Jeng-Kuei Chang, Wen-Wei Wu
Summary: LLZO-based all-solid-state Li batteries (SSLBs) have the potential for enhanced safety and improved energy density, but the rigid nature of ceramics poses challenges in the SSLB fabrication and interfacial stability during electrochemical cycling. This study demonstrates a promising LLZO-based SSLB with high areal capacity and stable cycle performance. In operando TEM is used to investigate the delithiation/lithiation process and capacity degradation mechanism on an atomic scale. The capacity degradation is attributed to interfacial delamination and the oxygen deficiency of LiCoO2.
Article
Chemistry, Multidisciplinary
Xin Lu, Anna Windmueller, Dana Schmidt, Sandro Schoener, Roland Schierholz, Chih-Long Tsai, Hans Kungl, Xunfan Liao, Shicheng Yu, Hermann Tempel, Yiwang Chen, Rudiger-A. Eichel
Summary: The structural and morphological changes of Li10GeP2S12 were studied over a comprehensive heat treatment range (50 - 700 degrees C) using a ball milling-heating method. The formation process was divided into four zones based on phase composition: Educt, Intermediary, Formation, and Decomposition zones. Diversified intermediate phases and multi-phasic lithium phosphosulfides were found to be involved in the formation and decomposition of Li10GeP2S12. The phase composition exhibited deviations around the transition temperatures of different formation zones, with the sample decomposing into complex phases at 650 degrees C.
Article
Nanoscience & Nanotechnology
Xin Lu, Anna Windmueller, Dana Schmidt, Sandro Schoener, Chih-Long Tsai, Hans Kungl, Xunfan Liao, Yiwang Chen, Shicheng Yu, Hermann Tempel, Ruediger-A. Eichel
Summary: A glassy-ceramic Li10GeP2S12 solid electrolyte with high Li-ion conductivity can be produced through a single-step high-energy ball milling method. The as-milled sample exhibits high ionic conductivity at room temperature, and heat treatment can further improve its crystallinity and ionic conductivity.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Walter Sebastian Scheld, Kwangnam Kim, Christian Schwab, Alexandra C. Moy, Shi-Kai Jiang, Markus Mann, Christian Dellen, Yoo Jung Sohn, Sandra Lobe, Martin Ihrig, Michael Gregory Danner, Chia-Yu Chang, Sven Uhlenbruck, Eric D. Wachsman, Bing Joe Hwang, Jeff Sakamoto, Liwen F. Wan, Brandon C. Wood, Martin Finsterbusch, Dina Fattakhova-Rohlfing
Summary: Solid-state batteries with LLZO garnet electrolyte are being widely studied as a robust and safe alternative to traditional lithium-ion batteries. This research focuses on understanding the chemical reactions between the composite LiCoO2-LLZO cathode and the LLZO separator and their impact on battery performance.
ADVANCED FUNCTIONAL MATERIALS
(2023)