Article
Chemistry, Multidisciplinary
Biao Li, Gwenaelle Rousse, Leiting Zhang, Maxim Avdeev, Michael Deschamps, Artem M. Abakumov, Jean-Marie Tarascon
Summary: The current exploration of high-energy-density cathode materials for Li-ion batteries is mainly focused on Li-rich or Ni-rich oxides, which both have practical challenges. This study combines these two concepts to obtain Li-rich Ni-rich oxides for more practical high-energy-density cathodes.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Liang Fang, Limin Zhou, Mihui Park, Daseul Han, Gi-Hyeok Lee, Seongkoo Kang, Suwon Lee, Mingzhe Chen, Zhe Hu, Kai Zhang, Kyung-Wan Nam, Yong-Mook Kang
Summary: This study identifies that voltage hysteresis in Li-rich layered oxide, Li1.2Ni0.4Mn0.4O2, is highly correlated to cationic reduction during discharge. The incomplete reduction of Ni during discharge is found to be associated with hysteresis. This suggests that oxygen redox is not the sole reason for the evolution of voltage hysteresis.
Article
Multidisciplinary Sciences
Tongchao Liu, Jiajie Liu, Luxi Li, Lei Yu, Jiecheng Diao, Tao Zhou, Shunning Li, Alvin Dai, Wenguang Zhao, Shenyang Xu, Yang Ren, Liguang Wang, Tianpin Wu, Rui Qi, Yinguo Xiao, Jiaxin Zheng, Wonsuk Cha, Ross Harder, Ian Robinson, Jianguo Wen, Jun Lu, Feng Pan, Khalil Amine
Summary: Utilizing Li- and Mn-rich (LMR) cathode materials can increase battery energy density. However, voltage decay issues impede commercialization. In this study, it is revealed that nanostrain and lattice displacement accumulate continuously during operation, leading to structure degradation and oxygen loss, which cause rapid voltage decay. The heterogeneous nature of LMR cathodes results in pernicious phase displacement/strain. Mesostructural design is proposed as a strategy to mitigate lattice displacement and achieve stable voltage and capacity profiles.
Article
Chemistry, Multidisciplinary
Zhenkun Hao, Haoxiang Sun, Youxuan Ni, Gaojing Yang, Zhuo Yang, Zhimeng Hao, Ruihan Wang, Pengkun Yang, Yong Lu, Qing Zhao, Weiwei Xie, Zhenhua Yan, Wei Zhang, Jun Chen
Summary: Layered oxides are commonly used as cathodes in lithium-ion batteries. In this study, a thin and coherent spinel-like phase was constructed on the surface of lithium-rich layered oxides (LLOs) to suppress bulk strain and surface oxygen release. The modified LLOs showed improved structural stability and cycling performance.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Baodan Zhang, Yiming Zhang, Xiaotong Wang, Hui Liu, Yawen Yan, Shiyuan Zhou, Yonglin Tang, Guifan Zeng, Xiaohong Wu, Hong-Gang Liao, Yongfu Qiu, Huan Huang, Lirong Zheng, Juping Xu, Wen Yin, Zhongyuan Huang, Yinguo Xiao, Qingshui Xie, Dong-Liang Peng, Chao Li, Yu Qiao, Shi-Gang Sun
Summary: Element doping/substitution can enhance the structural stability of layered cathodes. The study on Li1.2Ni0.2Mn0.6O2 reveals that the degree of disorder induced by Mg/Ti substitution affects the stability of TM-O, Li+ diffusion, and anion redox reversibility, leading to distinct electrochemical performance.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Ke Zhou, Yining Li, Yang Ha, Maojie Zhang, Walid Dachraoui, Haodong Liu, Chunyang Zhang, Xiangsi Liu, Fengchen Liu, Corsin Battaglia, Wanli Yang, Jianjun Liu, Yong Yang
Summary: Li-rich rock-salt oxide LVTO with high capacity and low capacity decay is reported as a promising material for Li-ion batteries.
CHEMISTRY OF MATERIALS
(2022)
Review
Chemistry, Physical
Xin Cao, Yu Qiao, Min Jia, Ping He, Haoshen Zhou
Summary: This study reviews the potential application of Li-rich and Li-excess oxides as cathode materials for next-generation Li-ion batteries, discusses the challenges in using Li-excess oxides, and explores mechanisms to address these issues. Future research directions in the field are also proposed based on advanced characterizations and theory calculations.
ADVANCED ENERGY MATERIALS
(2022)
Article
Nanoscience & Nanotechnology
Yuan Yang, Naifang Hu, Yu-Han Zhang, Yue Zheng, Zhiwei Hu, Chang-Yang Kuo, Hong-Ji Lin, Chien-Te Chen, Ting-Shan Chan, Cheng-Wei Kao, Yongcheng Jin, Jun Ma, Guanglei Cui
Summary: Li-rich layered oxide (LLO) cathode materials with mixed cationic and anionic redox reactions have higher specific capacity but a low practical specific capacity in sulfide all-solid-state lithium-ion batteries (ASSLBs). This study qualitatively and quantitatively analyzes the capacity contribution of each redox reaction in LLO during the first charging process. The results show that the cationic redox is almost complete, while the anionic redox is severely limited due to sluggish transport kinetics and interface reaction. The poor intrinsic conductivity and interface stability jointly restrict the capacity release of LLO in sulfide ASSLBs.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Michael Merz, Bixian Ying, Peter Nagel, Stefan Schuppler, Karin Kleiner
Summary: This study investigates the reversible and irreversible charge exchange reactions of Li- and Mn-rich layered oxides, and demonstrates the relationship between O-O formation in the bulk and reduction/oxidation processes of Ni, Co, and Mn. It also discusses the reversibility of charge compensation reactions and differences between O-O formation and oxygen release during activation.
CHEMISTRY OF MATERIALS
(2021)
Article
Chemistry, Physical
Aleksandra A. Savina, Anatolii V. Morozov, Ivan A. Moiseev, Anton O. Boev, Dmitry A. Aksyonov, Leiting Zhang, Polina A. Morozova, Victoria A. Nikitina, Egor M. Pazhetnov, Erik J. Berg, Stanislav S. Fedotov, Jean-Marie Tarascon, Evgeny V. Antipov, Artem M. Abakumov
Summary: Due to the excellent discharge capacity provided by oxygen redox activity, Li-rich layered oxide positive electrode materials have attracted great attention. However, there is still no consensus regarding the role of ionocovalency of transition metal-oxygen chemical bonding in the reversibility of oxygen redox and the local crystal and electronic structure transformations. In this study, we successfully manipulated the cationic/anionic redox contributions to the overall electrochemical activity and investigated the importance of enhancing the covalency of the TM-O bonding for anchoring the reversibility of the charge compensation mechanism.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Xin He, Jue Wu, Zhuoying Zhu, Haodong Liu, Ning Li, Dong Zhou, Xu Hou, Jun Wang, Haowei Zhang, Dominic Bresser, Yanbao Fu, Matthew J. Crafton, Bryan D. McCloskey, Yan Chen, Ke An, Ping Liu, Anubhav Jain, Jie Li, Wanli Yang, Yong Yang, Martin Winter, Robert Kostecki
Summary: This study provides a comparative study of transition metals and oxygen redox activities in Li-rich materials operated at different current rates. It reveals a reaction gradient of lattice oxygen redox reactions and a dynamic compatibility between the oxidation processes of lattice oxygen and transition metals. The study also proposes a detailed mechanism of structural distortion and the role of oxygen vacancies in Li+ diffusion.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Review
Chemistry, Multidisciplinary
Wei Zhong, Ziqi Zeng, Shijie Cheng, Jia Xie
Summary: Prelithiation technology is one of the most effective methods to compensate for the loss of active lithium. This review analyzes the factors inducing lithium loss and investigates the mechanisms and effects of prelithiation. The emerging advanced prelithiation technologies and key issues are systematically summarized. Hybrid replenishment and lithium storage technologies are proposed to provide a reference for developing prelithiation technology.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Weiyuan Huang, Cong Lin, Jimin Qiu, Shunning Li, Zhefeng Chen, Haibiao Chen, Wenguang Zhao, Guoxi Ren, Xiaoyuan Li, Mingjian Zhang, Feng Pan
Summary: The search for high-performance cathode materials is an important challenge for lithium-ion batteries. In this study, a strategy of delocalizing superstructure units within transition-metal layers was demonstrated to enhance the layer stability of a Li-excess Mn-rich layered oxide cathode. This resulted in a high capacity and energy density after cycling.
Article
Chemistry, Multidisciplinary
Jiming Peng, Yu Li, Zhiqiang Chen, Gemeng Liang, Sijiang Hu, Tengfei Zhou, Fenghua Zheng, Qichang Pan, Hongqiang Wang, Qingyu Li, Jianwen Liu, Zaiping Guo
Summary: A surface-coating strategy using NiFe2O4 was developed to enhance the performance of Li-rich layered oxides in lithium-ion batteries, resulting in improved cycle stability and rate capability. This strategy effectively traps surface lattice oxygen and restrains cation migration, decoupling the surface oxygen redox from cation movement.
Article
Nanoscience & Nanotechnology
Shihao Li, Haiyan Zhang, Huangxu Li, Shuai Zhang, Bin Zhu, Sha Wang, Jingqiang Zheng, Fangyan Liu, Zhian Zhang, Yanqing Lai
Summary: Li-rich Mn-based layered oxide cathodes show promise for lithium-ion batteries due to their high-voltage platform and ultrahigh specific capacity, but anionic redox can lead to oxygen release issues. By synthesizing LLO materials with varying lithium vacancy contents, it was found that lithium vacancies are crucial in enhancing anionic redox activity and reversibility.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Zhenpeng Yao, Maria K. Y. Chan, Chris Wolverton
Summary: This study investigates the delithiation and (re)lithiation reactions of super alkali-rich material Li5FeO4 using first-principles calculations. The study reveals non-equilibrium pathways during the charge and discharge processes. A phase transformation from tetrahedrally coordinated to octahedral coordinated structure is observed upon delithiation, with asymmetric kinetic barrier for Fe-ion migration explaining the difficulties in reaction reversibility.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Physical
Maciej P. Polak, Ryan Jacobs, Arun Mannodi-Kanakkithodi, Maria K. Y. Chan, Dane Morgan
Summary: Using multi-fidelity datasets and a machine learning approach, we have significantly reduced the time required for predicting impurity transition levels in semiconductors. The model trained on these datasets shows improved accuracy and does not require high-fidelity values, reducing computational cost. This approach has the potential to predict transition levels in various semiconductor materials.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Materials Science, Multidisciplinary
Arun Mannodi-Kanakkithodi, Maria K. Y. Chan
Summary: The combination of halide perovskites, high-throughput computations, and machine learning shows great promise in providing novel materials for solar cell and optoelectronic technologies. By using density functional theory (DFT) calculations and machine learning algorithms, we can predict and identify impurity atoms that have optoelectronic activity. This accelerated screening can help in identifying problematic impurities and tuning the conductivity and photovoltaic absorption of perovskite materials.
JOURNAL OF MATERIALS SCIENCE
(2022)
Article
Electrochemistry
Jehee Park, Kyojin Ku, Seoung-Bum Son, Jihyeon Gim, Youngsik Kim, Eungje Lee, Christopher Johnson
Summary: This study investigates the effect of electrolytes on the electrochemical performance of Fe-based layered oxide cathodes in sodium-ion batteries. The poor cathode-electrolyte interfacial stability is found to critically impact cell performance, with the reactive Fe4+ state leading to electrolyte decomposition and impedance rise. NaPF6 shows superior performance over NaClO4, and the FEC additive has a beneficial effect on cathode stability.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Eric Schwenker, Venkata Surya Chaitanya Kolluru, Jinglong Guo, Rui Zhang, Xiaobing Hu, Qiucheng Li, Joshua T. Paul, Mark C. Hersam, Vinayak P. Dravid, Robert Klie, Jeffrey R. Guest, Maria K. Y. Chan
Summary: This paper introduces an open-source automation framework called ingrained, which solves the correspondence between simulation and experimental images and fuses atomic resolution image simulations into the corresponding experimental images.
Article
Energy & Fuels
Xiang Liu, Gui-Liang Xu, Venkata Surya Chaitanya Kolluru, Chen Zhao, Qingtian Li, Xinwei Zhou, Yuzi Liu, Liang Yin, Zengqing Zhuo, Amine Daali, Jing-Jing Fan, Wenjun Liu, Yang Ren, Wenqian Xu, Junjing Deng, Inhui Hwang, Dongsheng Ren, Xuning Feng, Chengjun Sun, Ling Huang, Tao Zhou, Ming Du, Zonghai Chen, Shi-Gang Sun, Maria K. Y. Chan, Wanli Yang, Minggao Ouyang, Khalil Amine
Summary: The presence of domain boundaries in single-crystal cathodes hinders the redox stability of oxygen at high voltages. Eliminating domain boundaries enhances reversible lattice oxygen redox and inhibits irreversible oxygen release, leading to improved electrochemical performance.
Article
Instruments & Instrumentation
In Hui Hwang, Mikhail A. Solovyev, Sang Wook Han, Maria K. Y. Chan, John P. Hammonds, Steve M. Heald, Shelly D. Kelly, Nicholas Schwarz, Xiaoyi Zhang, Cheng Jun Sun
Summary: The Argonne X-ray Emission Analysis Package (AXEAP) can convert X-ray emission spectroscopy (XES) data in real time, reducing the amount of stored data, and includes data processing for non-resonant and resonant XES images.
JOURNAL OF SYNCHROTRON RADIATION
(2022)
Article
Multidisciplinary Sciences
Xiuquan Zhou, Venkata Surya Chaitanya Kolluru, Wenqian Xu, Luqing Wang, Tieyan Chang, Yu-Sheng Chen, Lei Yu, Jianguo Wen, Maria K. Y. Chan, Duck Young Chung, Mercouri G. Kanatzidis
Summary: Advancements in modern technologies rely on materials discovery, which in turn requires the development of synthesis science. This study presents an efficient methodology for rational material discovery using high-temperature solutions or fluxes with adjustable solubility. By systematically varying temperature and flux ratios, the researchers were able to synthesize previously unreported compounds and determine their structural characteristics. This methodology provides a general strategy for the rational discovery of inorganic solids.
Article
Chemistry, Physical
Srisuda Rojsatien, Arun Mannodi-Kanakkithodi, Trumann Walker, Tara Nietzold, Eric Colegrove, Barry Lai, Zhonghou Cai, Martin Holt, Maria K. Y. Chan, Mariana Bertoni
Summary: X-ray absorption near edge structure (XANES) coupled with X-ray microscopy is a powerful tool to probe the fingerprint of local structures. This study investigates the use of linear combination fitting (LCF) of XANES spectra for Cu doping in CdTe. The results show that the experimental data can be accurately represented by Cu2Te and Cu1.43Te standards. The study also proposes a framework to semi-quantitatively study local structures using binary mixtures of simulated standards.
RADIATION PHYSICS AND CHEMISTRY
(2023)
Article
Chemistry, Physical
Junghoon Yang, Sungwon Park, Sungsik Lee, Jungpil Kim, Di Huang, Jihyeon Gim, Eungje Lee, Gilseob Kim, Kyusung Park, Yong-Mook Kang, Eunsu Paek, Sang-Don Han
Summary: Further development of electrochemical devices and electric vehicles requires advanced secondary batteries with higher energy density, longer lifetime and enhanced thermal safety. Increasing the cell operating voltage can extend the energy density but may lead to irreversible structural changes, mechanical failure, and parasitic reactions at the electrode-electrolyte interface, causing capacity fading, battery failure, and safety issues.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Joydeep Munshi, Alexander Rakowski, Benjamin H. Savitzky, Steven E. Zeltmann, Jim Ciston, Matthew Henderson, Shreyas Cholia, Andrew M. Minor, Maria K. Y. Chan, Colin Ophus
Summary: A fast and robust pipeline for strain mapping of crystalline materials is crucial for technological applications. We propose a deep-learning method using a Fourier space, complex-valued deep-neural network to invert complex electron diffraction patterns. Our method, trained with a large number of samples, outperforms conventional analysis methods in both simulated and experimental datasets.
NPJ COMPUTATIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Zachary D. Hood, Anil U. Mane, Aditya Sundar, Sanja Tepavcevic, Peter Zapol, Udochukwu D. Eze, Shiba P. Adhikari, Eungje Lee, George E. Sterbinsky, Jeffrey W. Elam, Justin G. Connell
Summary: Sulfide-based solid-state electrolytes (SSEs) have high ionic conductivity and favorable mechanical properties, making them promising for next-generation solid-state batteries. Thin Al2O3 coatings grown on Li6PS5Cl powders using atomic layer deposition simultaneously address the stability issues and improve cell performance. These coated powders exhibit higher ionic conductivities, lower electronic conductivities, and improved stability at the Li-SSE interface, leading to significantly improved battery cycle life.
ADVANCED MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Davis Unruh, Venkata Surya Chaitanya Kolluru, Arun Baskaran, Yiming Chen, Maria K. Y. Chan
Summary: Advances in instrumentation have resulted in a vast amount of information on materials chemistry, structures, and transformations, but interpreting microscopy and spectroscopy data is becoming more challenging due to their growing volume and complexity. This article discusses the use of theoretical modeling, artificial intelligence/machine learning (AI/ML), and AI/ML combined with theory for interpreting microscopy and spectroscopy data.
Article
Chemistry, Multidisciplinary
Arun Mannodi-Kanakkithodi, Maria K. Y. Chan
Summary: This study develops a framework based on high-throughput computations and machine learning to design and predict mixed cation halide perovskite alloys. By simulating and computing multiple properties, including stability and optical properties, 392 promising compounds were screened as potential absorbers, revealing compositional trends in mixed cation halide perovskites.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Review
Chemistry, Multidisciplinary
Byunghoon Ryu, Luqing Wang, Haihui Pu, Maria K. Y. Chan, Junhong Chen
Summary: Machine learning is a valuable tool in the study of 2D materials, enabling predictions and discoveries that lead to a better understanding of their properties. It accelerates research and reduces costs.
CHEMICAL SOCIETY REVIEWS
(2022)
