Review
Chemistry, Physical
Ana C. C. Dutra, James A. Dawson
Summary: In the face of the climate emergency, solid-state batteries are expected to revolutionize energy storage by substituting liquid electrolytes with solid counterparts. One promising family of solid electrolytes is antiperovskites, which offer high ionic conductivity, structural versatility, low cost, and stability against metal anodes. This review focuses on the computational design of Li- and Na-based antiperovskite solid electrolytes, discussing topics such as high-throughput screening, synthesis, doping, ion transport mechanisms, grain boundaries, and electrolyte-electrode interfaces, as well as the challenges and future advances in these materials.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Matt J. Clarke, James A. Dawson, Timothy J. Mays, M. Saiful Islam
Summary: The study found that the F-doped system has low conductivity and high activation barriers, while Mg doping has a more favorable impact on lithium ions, leading to higher lithium-ion conductivity and lower migration energy. This suggests a viable doping strategy to enhance the electrochemical performance of antiperovskite solid electrolytes.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Physical
Longyun Shen, Yuhao Wang, Jing Yu, Guodong Zhou, Jiapeng Liu, Matthew J. Robson, Yanguang Zhou, Mohammed B. Effat, Francesco Ciucci
Summary: Li2OHCl is a promising solid-state electrolyte for all-solid-state Li-ion batteries. Strain engineering, achieved through isovalent doping, can improve Li+ conductivity and stabilize the highly conductive cubic phase at room temperature. By introducing tensile strain, Li2OHCl0.921I0.079 achieves a significantly higher ionic conductivity and demonstrates enhanced battery performance compared to Li2OHCl.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Longyun Shen, Yuhao Wang, Jing Yu, Guodong Zhou, Jiapeng Liu, Matthew J. Robson, Yanguang Zhou, Mohammed B. Effat, Francesco Ciucci
Summary: This study investigates the effect of strain on Li+ transport and finds that tensile strain can decrease the migration energy barrier. Tensile strain not only enhances conductivity but also stabilizes the highly conductive cubic phase at room temperature. An optimized composition (Li2OHCl0.921I0.079) achieves an ionic conductivity of 0.50 mS cm-1 at 373 K, five times larger than that of Li2OHCl. Furthermore, introducing tensile strain improves the Li+ conductivity and simultaneously stabilizes the cubic phase at low temperatures, resulting in significantly enhanced battery performance.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
M. A. A. Mohamed, L. Singer, H. Hahn, D. Djendjur, A. Oezkara, E. Thauer, I. G. Gonzalez-Martinez, M. Hantusch, B. Buechner, S. Hampel, R. Klingeler, N. Graessler
Summary: In this study, an antiperovskite (Li2Fe)SeO material was synthesized using a one-step solid-state method. The material showed excellent thermal stability and high cycling performance, making it a promising cathode material for lithium-ion batteries.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Multidisciplinary
Changhong Wang, Shuo Wang, Xudong Liu, Yanlong Wu, Ruizhi Yu, Hui Duan, Jung Tae Kim, Huan Huang, Jiantao Wang, Yifei Mo, Xueliang Sun
Summary: This study investigates the influence of lithium ion and vacant site contents on ionic conductivity by synthesizing a range of solid solutions. It is found that achieving a balance in lithium ion and vacant site content is crucial for optimizing ion transport in a hexagonal close packing anion framework. The highest ionic conductivity and lowest activation energy are achieved in LLZC.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Mikael S. Andersson, Vitalie Stavila, Alexander Skripov, Mirjana Dimitrievska, Malgorzata T. Psurek, Juscelino B. Leao, Olga A. Babanova, Roman Skoryunov, Alexei Soloninin, Maths Karlsson, Terrence J. Udovic
Summary: The study investigates the unique structural and ion dynamical properties of NaCB11H12 dispersed within high-surface-area silica through salt-solution infiltration, revealing the formation of a nanoconfined phase with superionic properties that persist at subambient temperatures. Fast-cation diffusion promoted by high anion mobilities leads to Na+ superionic conductivities of around 0.3 mS/cm at room temperature, indicating future potential for conductivity enhancement in related polyhedral (carba)borate-based salts as solid-state electrolytes in battery applications.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Inorganic & Nuclear
Amanda Berger, Craig E. Buckley, Mark Paskevicius
Summary: A novel and cost-effective method has been developed to synthesize the [CB11H12](-) anion with a 40% yield from [B11H14](-), avoiding the use of expensive and dangerous reagents. This method shows excellent reproducibility in product yield and purity, providing a more feasible pathway for commercial application.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Sifan Ling, Bei Deng, Ruo Zhao, Haibin Lin, Long Kong, Ruiqin Zhang, Zhouguang Lu, Juncao Bian, Yusheng Zhao
Summary: This study investigates the influence of H on the antiperovskite Li2OHX. It is found that H affects the Li-ion transport, crystal stability, electrochemical stability, and electronic conductivity of Li2OHX. Decreasing H content enhances the reduction-resistant ability and cycling stability of Li2OHX.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Mengying Ma, Binbin Chen, Huilin Pan
Summary: Controllable regulation of solution structures in electrolytes for Na-ion batteries is achieved by manipulating solvent interactions, leading to enhanced performance.
Article
Materials Science, Multidisciplinary
E. A. Il'ina, K. V. Druzhinin, T. A. Kuznetsova, M. E. Ozhiganov
Summary: The high resistance at the interface between cathode and solid electrolyte in all-solid-state power sources is effectively addressed by introducing a low-melting additive (Li3BO3) and lithium-conducting solid electrolyte (Li7La3Zr2O12) in the cathode mass LiNi1/3Co1/3Mn1/3O2. The chemical and thermal stability of the solid electrolyte in contact with LiNi1/3Co1/3Mn1/3O2 and Li3BO3 was investigated using XRD and DSC analysis. The addition of 5 wt% Li3BO3 in LiNi1/3Co1/3Mn1/3O2 resulted in close contact between the solid electrolyte and cathode, significantly reducing the interfacial resistance from 45000 to 85 Omega cm(2) at 300 degrees C.
JOURNAL OF MATERIALS SCIENCE
(2023)
Article
Chemistry, Physical
Humaira S. Bhatti, Shamsa Jabeen, Arif Mumtaz, Ghulam Ali, Sara Qaisar, Shahzad Hussain
Summary: Cobalt-doped Li4Ti5O12 (LTO) powders with varying Cobalt concentrations were synthesized and studied for their structural, optical, electrical, and electrochemical properties. The sample with x = 0.15 showed enhanced electronic and ionic conductivity, reduced bandgap, and increased lattice spacing, leading to improved electrochemical activity. These results highlight the potential of Cobalt-doped LTO as a promising material for energy storage applications.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Materials Science, Multidisciplinary
Stephen J. Turrell, Hyeon Jeong Lee, Marco Siniscalchi, Sudarshan Narayanan, Mauro Pasta, Susannah C. Speller, Chris R. M. Grovenor
Summary: This study demonstrates the successful synthesis of a lithium-rich antiperovskite compound Li3OCl using RF magnetron sputtering. The stabilization of the antiperovskite phase and its distinction from Li2OHCl were confirmed through optimization of the synthesis and characterization processes.
MATERIALS ADVANCES
(2022)
Article
Chemistry, Multidisciplinary
Susumu Fujii, Shenghan Gao, Cedric Tassel, Tong Zhu, Thibault Broux, Koji Okada, Yuto Miyahara, Akihide Kuwabara, Hiroshi Kageyama
Summary: The role of anions in antiperovskites was investigated through theoretical and experimental studies, revealing that replacing polarizable H- anions with ionic F- anions in the M(3)FCh family does not slow down ion diffusion. It was found that the low-frequency rotational modes of the octahedron in cubic M(3)FCh facilitate fast ionic diffusion, showing a correlation between tolerance factor and ionic transport. The cubic iodine-doped Li3FSe exhibited a room-temperature ionic conductivity of 5 x 10(-5) S/cm with a bulk activation energy of 0.18 eV.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Justin Mark, Katherine E. Woo, Weidi Zhu, Bingheng Ji, Shannon J. Lee, Adedoyin N. Adeyemi, Sabyasachi Sen, Kirill Kovnir
Summary: Two new ternary tetrel pnictide phases, Li1.08Ge4.92As7 and Cs0.11Zn0.05Si0.95As, have been synthesized with new structure types. Li1.08Ge4.92As7 displays a novel Ge-As layer motif, while Cs0.11Zn0.05Si0.95As exhibits a 3D framework composed of fragments of the 2D parent-phase SiAs.
CHEMISTRY OF MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Jinfeng Dong, Yilin Jiang, Yandong Sun, Jue Liu, Jun Pei, Wei Li, Xian Yi Tan, Lei Hu, Ning Jia, Ben Xu, Qian Li, Jing-Feng Li, Qingyu Yan, Mercouri G. Kanatzidis
Summary: GeMnTe2 adopts a cubic rock salt structure and can be tuned by alloying with SbTe to achieve high power factor and low thermal conductivity. The GeMnTe2-15.1%SbTe composition exhibits a ZTave of 0.96 in the temperature range of 400-823 K.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Siqi Liu, Weiliang Qi, Jue Liu, Xiangjian Meng, Samira Adimi, J. Paul Attfield, Minghui Yang
Summary: The synthesis of transition metal (M = V, Mo, and W) doped cobalt nitride catalyst for solar to hydrogen energy conversion is reported. The as-prepared cobalt nitride was found to contain lattice defects. M-doping improved charge carrier separation efficiency and reaction kinetics by altering the electronic structure and properties of cobalt nitride. The optimal V-Co3.75N0.14-Eosin-Y system exhibited a hydrogen evolution rate of 21.21 μmol·mg-1·h-1 and a quantum efficiency of 38% at 405 nm excitation wavelength, surpassing previous hybrid photocatalysts.
Article
Chemistry, Physical
Ping-Chun Tsai, Sunil Mair, Jeffrey Smith, David M. M. Halat, Po-Hsiu Chien, Kwangnam Kim, Duhan Zhang, Yiliang Li, Liang Yin, Jue Liu, Saul H. H. Lapidus, Jeffrey A. A. Reimer, Nitash P. P. Balsara, Donald J. J. Siegel, Yet-Ming Chiang
Summary: Through combined experiments and modeling, the first instance of a double paddle-wheel mechanism, leading to fast sodium ion conduction in the antiperovskite Na3-xO1-x(NH2)(x)(BH4), is shown. As the concentration of amide (NH2-) cluster anions is increased, large positive deviations in ionic conductivity above that predicted from a vacancy diffusion model are observed. Using various characterization techniques, the cluster anion rotational dynamics are found to influence cation mobility, resulting in significantly higher sodium ion conductivity at x = 1 compared to the vacancy mechanism alone.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yuanpeng Zhang, Jue Liu, Matthew G. Tucker
Summary: This paper revisits the three fundamental origins of the Lorentz factor for neutron time-of-flight powder diffraction. It presents a detailed derivation of the Lorentz factor in the context of diffuse scattering modeling in reciprocal space, assuming perfect periodicity. The total scattering pattern is constructed in its discrete form, and it is shown that the Lorentz factor becomes 1/Q(2) (or d(2)). The paper also discusses practical data reduction and demonstrates that the existence of the Lorentz factor is independent of the normalization process using vanadium measurement.
ACTA CRYSTALLOGRAPHICA A-FOUNDATION AND ADVANCES
(2023)
Article
Chemistry, Multidisciplinary
Kun Lin, Wenbin Zhang, Chengyi Yu, Qiang Sun, Yili Cao, Wenjie Li, Suihe Jiang, Qiang Li, Qiang Zhang, Ke An, Yan Chen, Dunji Yu, Jue Liu, Kenichi Kato, Qinghua Zhang, Lin Gu, Xiaojun Kuang, Yu Tang, Jun Miao, Xianran Xing
Summary: Chemical heterogeneity, as a counterintuitive strategy, is proposed to design high-performance zero thermal expansion (ZTE) alloys. In a Hf-Ti-Fe alloy with excess Fe in the Hf/Ti sublattice, the introduction of chemical heterogeneity at the micro level regulates local magnetic interactions and triggers a dispersed magnetic phase transition, resulting in remarkable ZTE behavior. The strategy of local chemical heterogeneity opens up an avenue to design ZTE and related functional materials directly via microstructure engineering.
CELL REPORTS PHYSICAL SCIENCE
(2023)
Article
Chemistry, Physical
Sanghyeon Kim, Nathan T. Hahn, Timothy T. Fister, Noel J. Leon, Xiao-Min Lin, Haesun Park, Peter Zapol, Saul H. Lapidus, Chen Liao, John T. Vaughey
Summary: Calcium-ion batteries (CIBs) have potential for next-generation energy storage due to the low redox potential and abundance of calcium compounds. This study reports the use of elemental Se as a high-capacity cathode material for CIBs operating via a conversion mechanism in a Ca metal battery at room temperature. The Se electrodes exhibit reversible specific capacity and a discharge plateau near 2.0 V (vs Ca2+/Ca). The electrochemical reaction between calcium and selenium is investigated using operando synchrotron-based techniques and discussed.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Xinbin Yu, Jisue Moon, Yongqiang Cheng, Luke Daemen, Jue Liu, Sung Wng Kim, Abinash Kumar, Miaofang Chi, Victor Fung, Anibal J. Ramirez-Cuesta, Zili Wu
Summary: NH3 synthesis is a critical industrial process. Ru catalysts have high activity in this reaction but are susceptible to hydrogen poisoning. By using supports like electrides and hydrides, the problem of hydrogen poisoning can be alleviated. However, there is limited research on the structural dynamics of Ru/electride catalysts during the reaction.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Sreya Paladugu, Peter C. Metz, Si Luo, Meijun Li, Jue Liu, Harry Meyer, Yiqing Wu, Zili Wu, Katharine Page
Summary: This study investigates the structural evolution of ceria nanorods under redox gas environments with Pt loading, which is important for catalysis applications. The results show that Pt-CeO2 nanorods are more easily reducible than CeO2 rods, and no evidence of oxygen vacancy ordered surface reconstruction is found.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Nanoscience & Nanotechnology
Xuyu Dong, Kun Lin, Chengyi Yu, Wenbin Zhang, Wenjie Li, Qian Zhang, Qiang Zhang, Jue Liu, Yili Cao, Xianran Xing
Summary: This work presents a single phase and nearly isotropic zero thermal expansion (ZTE) alloy (Hf0.8Nb0.2)Fe2.5 with dimensionally stable properties over a wide temperature range of 5-460 K. The introduction of excess Fe breaks the dual-phase structure, increases the magnetic ordering temperature, and induces spin reorientation, resulting in the ZTE behavior. The design concept of changing the internal magnetic interaction through non-stoichiometric regulation provides support for the discovery of novel ZTE materials.
SCRIPTA MATERIALIA
(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)
Article
Chemistry, Physical
Kira E. Wyckoff, Linus Kautzsch, Jonas L. Kaufman, Brenden R. Ortiz, Anna Kallistova, Ganesh Pokharel, Jue Liu, Keith M. Taddei, Kamila M. Wiaderek, Saul H. Lapidus, Stephen D. Wilson, Anton van der Ven, Ram Seshadri
Summary: Controlling the magnetic properties of functional inorganic materials with a kagome-derived network is achieved by electrochemically controlling the lithium content. The electronic occupancy and consequent magnetic properties are varied by inserting up to two additional lithium ions into LiScMo3O8. The measurements and calculations reveal the evolution from a diamagnetic band insulator to a geometrically frustrated magnet and back to a diamagnetic insulator as the lithium content changes.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yanming Sun, Yili Cao, Shixin Hu, Maxim Avdeev, Chin-Wei Wang, Sergii Khmelevskyi, Yang Ren, Saul H. Lapidus, Xin Chen, Qiang Li, Jinxia Deng, Jun Miao, Kun Lin, Xiaojun Kuang, Xianran Xing
Summary: By high-temperature synthesis, researchers have achieved tunable thermal expansion in the kagome cubic (Fd-3m) intermetallic (Zr,Nb)Fe-2 materials. By magnetic doping, they have obtained a near-zero thermal expansion coefficient, which has significant applications in advanced technologies.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
A. Dive, K. Kim, S. Kang, L. F. Wan, B. C. Wood
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Inorganic & Nuclear
Callista M. Skaggs, Dong-Choon Ryu, Hari Bhandari, Yan Xin, Chang-Jong Kang, Saul H. Lapidus, Peter E. Siegfried, Nirmal J. Ghimire, Xiaoyan Tan
Summary: Polycrystalline IrGe4 with a chiral crystal structure is synthesized and exhibits metallic behavior and non-saturating magnetoresistance under an applied magnetic field.
INORGANIC CHEMISTRY
(2023)
