Article
Chemistry, Physical
William H. Smith, Saeed Ahmadi Vaselabadi, Colin A. Wolden
Summary: This study introduces a method for the production of lithium sulfide through room-temperature metathesis. The synthesized lithium sulfide material exhibits high ionic conductivity and can be used as a critical component in next-generation batteries.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Enyue Zhao, Lunhua He, Zhigang Zhang, Jean-Marie Doux, Darren H. S. Tan, Erik A. Wu, Grayson Deysher, Yu-Ting Chen, Jinkui Zhao, Fangwei Wang, Ying Shirley Meng
Summary: By utilizing temperature-dependent neutron powder diffraction combined with maximum entropy method analysis, a previously unreported Li lattice site was identified in the argyrodite Li6PS5Cl solid-state electrolyte. This discovery offers a more comprehensive understanding of the Li diffusion model in argyrodites, providing structural guidance for designing novel high-conductivity solid-state electrolytes.
CHEMICAL COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Ajay Gautam, Marcel Sadowski, Michael Ghidiu, Nicolo Minafra, Anatoliy Senyshyn, Karsten Albe, Wolfgang G. Zeier
Summary: The study shows that controlling site-disorder in Li6PS5Br by adjusting synthesis conditions can enhance lithium ion diffusion pathways and increase ionic conductivity. Experimental results and ab initio molecular dynamics simulations corroborate each other, highlighting the importance of this modulation method for design and optimization of argyrodites.
ADVANCED ENERGY MATERIALS
(2021)
Article
Chemistry, Physical
Taesoon Hwang, You-Jin Lee, So Ri Lee, Yoon-Cheol Ha, Maenghyo Cho, Sang-Min Lee, Kyeongjae Cho
Summary: This study proposes a method to improve the stability of sulfide-based solid electrolytes by introducing oxygen to replace sulfur. The experimental results show that the introduction of oxygen can suppress structural decomposition and oxygen penetration, while maintaining sufficient ionic conductivity.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Physical
Yuvaraj Subramanian, Rajesh Rajagopal, Sung Kang, Kwang-Sun Ryu
Summary: This study improved the interface stability of Li-argyrodites through metal and oxygen substitution, and evaluated their structural and electrochemical performances. The results showed that MoO2 substitution can enhance critical current density and ionic conductivity.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Electrochemistry
Artur Tron, Ander Orue, Pedro Lopez-Aranguren, Alexander Beutl
Summary: This study investigates the critical parameters and standardized measurement methods of argyrodite electrolytes, providing a foundation for the development of all-solid-state lithium batteries. The formation of dendrites is identified as the main cause of electrolyte breakdown, and the critical current density is highlighted as an important indicator of sustainable current for the electrolyte.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Ananya Banik, Yunsheng Liu, Saneyuki Ohno, Yannik Rudel, Alberto Jimenez-Solano, Andrei Gloskovskii, Nella M. Vargas-Barbosa, Yifei Mo, Wolfgang G. Zeier
Summary: This study systematically investigates the influence of cationic and anionic substitution on the electrochemical stability of lithium-ion conducting argyrodite solid electrolytes. The results show that oxidative stability does not change with different substitutions. Chemical bonding analysis reveals that the valence band edges are mostly populated by nonbonding orbitals or unbound sulfide anions, indicating that simple substitutions cannot improve oxidative stabilities in sulfide-based solid electrolytes.
ACS APPLIED ENERGY MATERIALS
(2022)
Review
Electrochemistry
Chongxing Li, Shuxian Zhang, Xianguang Miao, Cong Wang, Chengxiang Wang, Zhiwei Zhang, Rutao Wang, Longwei Yin
Summary: This review summarizes the basic physical and chemical properties, material synthesis strategies, chemical or electrochemical stabilities, and interface engineering of lithium argyrodite solid-state electrolytes in all-solid-state lithium batteries. It also provides an overview of recent achievements and critical challenges, as well as prospects for integrating lithium argyrodite SSEs into ASSLBs.
BATTERIES & SUPERCAPS
(2022)
Article
Chemistry, Physical
Felix Walther, Florian Strauss, Xiaohan Wu, Boris Mogwitz, Jonas Hertle, Joachim Sann, Marcus Rohnke, Torsten Brezesinski, Juergen Janek
Summary: This study improves the performance of all-solid-state batteries (ASSBs) by using a Li2CO3/LiNbO3 coating, which suppresses the interfacial reaction between the cathode active material and solid electrolyte, leading to a significant enhancement in battery performance.
CHEMISTRY OF MATERIALS
(2021)
Article
Nanoscience & Nanotechnology
Ziqi Zhang, Chuang Yu, Ruonan Xu, Linfeng Peng, Haotian Ren, Junzhao Zhang, Long Zhang, Shijie Cheng, Jia Xie
Summary: This work demonstrates the enhancement of Li6PS5I conductivity by introducing more iodine in the structure. The Li5.5PS4.5I1.5 electrolyte synthesized through mechanical milling shows high ionic conductivity at room temperature. However, there are challenges regarding its stability towards high-voltage cathodes and its activation energy for lithium-ion transport in the cathode/electrolyte interface.
SCRIPTA MATERIALIA
(2022)
Article
Materials Science, Multidisciplinary
Sangwon Park, Jin-Woong Lee
Summary: All solid-state batteries are considered as the ultimate solution to the safety issues of conventional lithium-ion batteries, and modifying the microscopic structure and Li diffusional behaviors of argyrodites can enhance their performance. The study showed that at an appropriate cooling rate, impurities in Li5.5PS4.5Cl1.5 gradually decreased and lattice size differences decreased, leading to improved ionic conductivity. The effect of cooling rates on crystallographic atomic arrangements and their correlation with ionic conductivities were experimentally verified.
KOREAN JOURNAL OF METALS AND MATERIALS
(2021)
Article
Chemistry, Physical
Bernhard T. Leube, Christopher M. Collins, Luke M. Daniels, Benjamin B. Duff, Yun Dang, Ruiyong Chen, Michael W. Gaultois, Troy D. Manning, Frederic Blanc, Matthew S. Dyer, John B. Claridge, Matthew J. Rosseinsky
Summary: A tetragonal argyrodite material, Li7Zn0.5SiS6, with more than 7 mobile cations has been successfully synthesized through solid state synthesis and exploration of phase diagram. The crystal structure of Li7Zn0.5SiS6 has been determined and it undergoes a transition from ordered structure to disordered structure at high temperature. The material has multiple types of Li sites and the incorporation of Zn2+ affects the Li distribution. This study expands our understanding of structure-property relationships in argyrodite materials.
CHEMISTRY OF MATERIALS
(2022)
Article
Electrochemistry
Zhichao Zhang, Yongtao Tian, Gaozhan Liu, Ming Wu, Hao He, Xiayin Yao
Summary: A promising all-solid-state lithium battery electrolyte material with high ionic conductivity and favorable stability has been developed in this study, demonstrating potential applications with its high lithium ion conductivity and good cycling stability.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Jae Min Lee, Young Seon Park, Ji-Woong Moon, Haejin Hwang
Summary: Wet-mechanical milling and post-annealing at 500 degrees C for 4 h were used to synthesize Li6PS5Cl electrolyte powder with excellent electrochemical properties. The choice of solvent does not significantly affect ionic conductivity but does have an impact on electronic conductivity. The use of xylene and toluene can produce Li6PS5Cl electrolyte powder with low electronic and comparable ionic conductivities.
FRONTIERS IN CHEMISTRY
(2021)
Article
Physics, Condensed Matter
V. A. Konstantinov, A. Krivchikov, A. Karachevtseva, V. V. Sagan
Summary: The isochoric thermal conductivity of crystalline 1,1-difluoroethane (F-152a freon) was measured in the dynamically orientationally disordered (DOD) phase, showing an increase in thermal conductivity with temperature that can be described by a thermo-activation mechanism with constant activation energy and density-dependent pre-exponential factor. Bridgman coefficient was found to be 6.0 +/- 0.5. The study suggests that thermal conductivity of other molecular crystals with dynamic orientational disorder can be similarly described, and discusses possible reasons for this thermal activation behavior.
SOLID STATE COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Nathan J. Gimble, Leslie A. Kraynak, Jacob D. Schneider, Maxwell C. Schulze, Amy L. Prieto
Summary: The study analyzed the impact of adding fluoro-ethylene carbonate (FEC) on the formation of solid electrolyte interface (SEI) and battery performance in sodium ion half-cell batteries using X-Ray Photoelectron Spectroscopy (XPS). The results suggest that FEC plays a significant role in determining the chemical environments of SEI, which in turn affects battery performance.
JOURNAL OF POWER SOURCES
(2021)
Article
Electrochemistry
Emma J. Hopkins, Sarah Frisco, Ryan T. Pekarek, Caleb Stetson, Zoey Huey, Steven Harvey, Xiang Li, Baris Key, Chen Fang, Gao Liu, Guang Yang, Glenn Teeter, Nathan R. Neale, Gabriel M. Veith
Summary: The addition of CO2 in the electrolyte results in a thinner SEI layer dominated by LiF, leading to improved cycling performance by reducing irreversible side reactions. CO2 plays a similar role to additives like fluorinated ethylene carbonate and vinylene carbonate in terms of enhancing the polymeric components in the SEI.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Maxwell C. Schulze, Nathan R. Neale
ACS ENERGY LETTERS
(2021)
Review
Chemistry, Physical
Eric Amerling, Haipeng Lu, Bryon W. Larson, Annalise E. Maughan, Alan Phillips, Evan Lafalce, Luisa Whittaker-Brooks, Joseph J. Berry, Matthew C. Beard, Z. Valy Vardeny, Jeffrey L. Blackburn
Summary: Research on derivatives of both bulk and low-dimensional metal halide perovskite semiconductors has grown significantly in the past decade, but the understanding and intentional applications of electronic doping have lagged behind. Successful electronic doping of these materials likely requires careful consideration and application of established doping strategies and mechanisms in the semiconductor field.
ACS ENERGY LETTERS
(2021)
Article
Electrochemistry
Daniel Korff, Andrew M. Colclasure, Yeyoung Ha, Kandler A. Smith, Steven C. DeCaluwe
Summary: This study presents a 1D model of a Li-Sulfur battery, which allows for comparing different mechanisms and investigating the influence of polysulfide intermediates on battery performance. The model is also used to explore cathode design strategies and the impact of polysulfide concentrations.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Electrochemistry
Yeyoung Ha, Trevor R. Martin, Sarah Frisco, Leah Rynearson, Maxwell C. Schulze, Sang-Don Han, Stephen E. Trask, Brett L. Lucht, Glenn Teeter, Nathan R. Neale
Summary: The unstable electrode/electrolyte interface is the main cause of degradation in silicon-based anodes for lithium-ion batteries. Developing functional electrolyte additives can stabilize the dynamic Si/electrolyte interface and benefit the development of high-energy-density Li-ion batteries. Among the evaluated polymerizable electrolyte additives with different functional groups, the fluorine-containing additives show the best passivation effect on the Si electrode and enhance the performance of the full cell.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Maxwell C. Schulze, Fernando Urias, Nikita S. Dutta, Zoey Huey, Jaclyn Coyle, Glenn Teeter, Ryan Doeren, Bertrand J. Tremolet de Villers, Sang-Don Han, Nathan R. Neale, G. Michael Carroll
Summary: Silicon is a promising candidate for the next-generation anode of rechargeable lithium-ion batteries due to its high theoretical capacity and abundance. However, the cycle life of silicon-based composite anodes is limited by volume changes and reactive interfacial chemistries. In this study, surface-functionalized silicon nanocrystals were synthesized to fabricate a silicon composite electrode with controllable electrolyte interphase. The cured electrode showed improved silicon utilization, high coulombic efficiency, and retained 72% of its capacity after 1000 charge/discharge cycles when paired with a capacity-matched cathode.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Zoey Huey, Yeyoung Ha, Sarah Frisco, Andrew Norman, Glenn Teeter, Chun-Sheng Jiang, Steven C. DeCaluwe
Summary: In this study, the SEI on composite Si-Gr anodes was characterized using multi-modal characterization techniques to reveal the relationship between SEI chemical composition and structure with its functional properties. By combining multiple analysis methods, a comprehensive understanding of the SEI was obtained. The study found that the SEI has a bilayer structure and a direct correlation between elemental Li and F, suggesting that most Li in the SEI exists as lithium fluoride (LiF). Furthermore, there is an inverse relationship between lithium carbonate and LiF concentration in the SEI, providing insight into the detailed chemistry of SEI formation and evolution.
JOURNAL OF POWER SOURCES
(2023)
Article
Electrochemistry
Yeyoung Ha, Stephen E. Trask, Yicheng Zhang, Andrew N. Jansen, Anthony Burrell
Summary: The LTO/LMO system shows promise for behind-the-meter storage applications due to its critical-material-free chemistry, offering good safety and long lifetime. By designing the LTO/LMO cells with different loadings and electrolyte properties, their capacity retention and performance can be enhanced.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
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
Electrochemistry
Ankit Verma, Maxwell C. Schulze, Andrew Colclasure, Marco-Tulio Fonseca Rodrigues, Stephen E. Trask, Krzysztof Pupek, Christopher S. Johnson, Daniel P. Abraham
Summary: The impact of electrolyte fluorination on the calendar fade of blended silicon-graphite anodes is explored. Unfluorinated electrolyte shows higher cell resistance compared to fluorinated electrolyte, with slower rate of parasitic capacity loss for the LiBOB system. The results suggest that fluorinated electrolyte performs better in calendar life.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Maxwell. C. C. Schulze, Kae Fink, Jack Palmer, Gerard. M. M. Carroll, Nikita. S. S. Dutta, Christof Zwiefel, Chaiwat Engtrakul, Sang-Don Han, Nathan. R. R. Neale, Bertrand Tremolet J. de Villers
Summary: Silicon anodes have high energy density potential but suffer from poor lifetimes due to mechanical and chemical reactivity issues. This study presents a pitch carbon-coated silicon composite anode that reduces reactivity with carbonate-based electrolytes. By minimizing particle size and employing conformal coatings, the anode retains 75% capacity after 1000 cycles when paired with a high voltage cathode. However, increasing energy density leads to severe mechanical degradation, posing a challenge for future work.
BATTERIES & SUPERCAPS
(2023)
Article
Chemistry, Physical
Trevor R. Martin, Ryan T. Pekarek, Jaclyn E. Coyle, Maxwell C. Schulze, Nathan R. Neale
Summary: This study reveals the evolution of PAA during electrode fabrication and its impact on electrode performance using in situ spectroscopy techniques. The results show that PAA undergoes a chemical change to form a polyether network polymer during cross-linking reaction. Additionally, PAA acts as an interfacial material that conducts lithium ions, limits solvent molecule access to the Si surface, and stabilizes the electrode against parasitic lithium inventory loss.
JOURNAL OF MATERIALS CHEMISTRY A
(2021)