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)
Article
Chemistry, Physical
Hui Chen, Lei Shi, Ke Sun, Kexin Zhang, Qi Liu, Junjie Ge, Xiao Liang, Boyuan Tian, Yalan Huang, Zhaoping Shi, Zizhun Wang, Wei Zhang, Mingjie Liu, Xiaoxin Zou
Summary: Ir-based perovskite oxides have shown promise as electrocatalysts for oxygen evolution reaction (OER) in an acidic medium, but their uncontrollable surface amorphization and structural instability have been major challenges. In this study, we report a high-yield chemical exfoliation method to obtain protonated colloidal nanosheets with an undamaged perovskite framework from Ruddlesden-Popper layered perovskite Sr2IrO4. These protonated perovskite nanosheets show potential to overcome the trade-off between OER activity and structural stability. The 2D morphology and uniformity of these nanosheets enable the fabrication of an ultralow-Ir-loading catalyst film with significantly higher activity and comparable Ir leaching to the IrO2 catalyst film during OER. The presence of structural hydroxyl groups on the surface of protonated nanosheets is found to contribute to the catalytic cycle of OER, representing a non-traditional adsorbate evolution mechanism for the protonated layered perovskite framework.
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
Shuwei Li, Zepeng Liu, Lu Yang, Xi Shen, Qiuyan Liu, Zhiwei Hu, Qingyu Kong, Jun Ma, Jiedong Li, Hong-Ji Lin, Chien-Te Chen, Xuefeng Wang, Richeng Yu, Zhaoxiang Wang, Liquan Chen
Summary: This study comprehensively investigated the oxygen redox reaction and structural reversibility of the Ni-rich layered oxide during deep delithiation. It was found that the redox reaction is caused by cation mixing upon delithiation, and the migration of transition metals leads to the formation of the I41 structure. These findings provide insights into the origin of the oxygen redox and its impact on structural transformations.
Article
Materials Science, Multidisciplinary
Subhayan Roychoudhury, Ruimin Qiao, Zengqing Zhuo, Qinghao Li, Yingchun Lyu, Jung-Hyun Kim, Jun Liu, Eungje Lee, Bryant J. Polzin, Jinghua Guo, Shishen Yan, Yongsheng Hu, Hong Li, David Prendergast, Wanli Yang
Summary: This study investigates the O-K pre-edge of 55 oxides covering all 3d TMs in various elements, structures, and electrochemical states, showing that the O-K pre-edge variation in battery cathodes is dominated by changing TM-d states. The results provide a unique way to project the relative energy positions of low-lying TM states and clarify unusual redox reactions. This work offers a critical clarification on O-K pre-edge interpretation and establishes a benchmark database for characterizing redox reactions in batteries and other energy materials.
ENERGY & ENVIRONMENTAL MATERIALS
(2021)
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
Gwanghyeon Choi, Jaewoon Lee, Sojung Koo, Sangeon Park, Duho Kim
Summary: The concept of "band coherency" is proposed to explain the reversible ORR origin in alkali-excess compounds, with non-discrete transition metal nd-O 2p electron activity, including O and Ru charge variations and thermodynamic-phase stability. Triggering band coherency can achieve high-energy-density properties.
CELL REPORTS PHYSICAL SCIENCE
(2021)
Article
Chemistry, Inorganic & Nuclear
Susu Fang, Shu Zhang, Lianshan Ni, Guoqiang Zou, Hongshuai Hou, Huiqun Liu, Wentao Deng, Xiaobo Ji
Summary: This study presents a method to efficiently prepare submicrometer single-crystal LiNi0.8Co0.1Mn0.1O2 (NCM) cathode material without the need for extreme alkaline environments and complex processes. The prepared NCM exhibits moderate particle size and strong metal-oxygen bonds, which greatly enhance Li+ diffusion kinetics and structure stability. The NCM electrode shows good discharge capacity and superior capacity retention, indicating the effectiveness and flexibility of this strategy for developing submicrometer single-crystal nickel-rich layered cathode materials.
INORGANIC CHEMISTRY
(2023)
Article
Nanoscience & Nanotechnology
Jong-Min Ju, Chi Ho Lee, Jung Hyun Park, Jun-Hyeong Lee, Hajin Lee, Jae-Hoon Shin, Seon-Yeong Kwak, Sang Uck Lee, Jong-Ho Kim
Summary: Covalent organic frameworks (COFs) are promising candidates for the controllable design of electrocatalysts. In this study, imidazolium-rich COFs (IMCOFs) with well-defined active sites and characteristic three-dimensional assembly structures were prepared, and their electronic structures were tuned by Co incorporation to elicit bifunctional electrocatalytic activities for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The Co nanoparticle-incorporated IMCOF-derived electrocatalyst exhibited lower overpotentials for the ORR and OER compared with the atomic Co-incorporated IMCOF-derived electrocatalyst. Computational simulations revealed that the imidazole carbon sites of the CoNP-s-IMCOF were the active sites for the ORR and OER, and its p-band center downshifted via charge transfer, facilitating the chemisorption of oxygen intermediates during the reactions. A Zn-air battery with the CoNP-s-IMCOF showed a small voltage gap and excellent durability.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Lina Wang, Lei Shi, Qi Liu, Yalan Huang, Wensheng Yan, Xiao Liang, Xiao Zhao, Hui Chen, Xiaoxin Zou
Summary: We report the synthesis and characterization of honeycomb layered strontium iridate (SrIr2O6) as an efficient electrocatalyst for the acidic oxygen evolution reaction (OER) with robust structural stability. Unlike most iridate catalysts, SrIr2O6 can maintain its crystalline structure during OER instead of forming an amorphous active phase. The edges of SrIr2O6 demonstrate high catalytic activity for OER following the adsorbate evolution mechanism, while the basal planes are catalytically inert. SrIr2O6 exhibits about 10-fold higher intrinsic activity than the benchmark catalyst IrO(2), with minimal iridium leaching (approximately 0.03%) and long-term catalytic stability for over 300 hours.
Article
Chemistry, Physical
Sojung Koo, Jaewoon Lee, Jinwoo Lee, Sangho Yoon, Duho Kim
Summary: This study explores the role of Mn(t2g3)-O hybridized band in activating oxygen redox reactions and suppressing O2 release. The presence of this band is crucial for easily triggering ORRs and inhibiting the formation of very short O-O dimers, providing a new direction for designing high energy density cathodes in lithium-ion batteries.
ENERGY STORAGE MATERIALS
(2021)
Article
Engineering, Environmental
Zhijie Feng, Hui Song, Wei Su, Meng Liu, Yuanhang Li, Riming Chen, Shuyin Xu, Yingchun Lyu, Dongdong Xiao, Bingkun Guo
Summary: This study reports a facile strategy to improve the electrochemical kinetics and structural stability of Li-rich layered oxide cathode materials through a one-step treatment with thiourea at a moderate temperature. The built-in surface reconstruction layer suppresses irreversible oxygen evolution, promotes cation redox, and satisfies the essential requirements of efficient diffusion kinetics.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Nanoscience & Nanotechnology
Yong-Lin Huo, Yi-Jing Gu, Zi-Liang Chen, Xiao-Yu Ma, Yi-Ge Xiong, Hua-Fei Zhang, Fu-Zhong Wu, Xin-Yi Dai
Summary: A technique of stabilizing the crystal structure and reducing the surface oxygen activity is proposed, achieving better voltage attenuation and capacity retention. The addition of a coating layer and highly concentrated oxygen vacancies inhibits structural transformation and oxygen release during the charge and discharge process.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Xin Cao, Haifeng Li, Yu Qiao, Ping He, Yumin Qian, Xiyan Yue, Min Jia, Jordi Cabana, Haoshen Zhou
Summary: The combination of anionic and cationic activities in Li-rich materials has achieved high-energy-density batteries by breaking through the traditional capacity limitation. However, the utilization of anionic oxygen redox reactions often leads to detrimental lattice oxygen release, which accelerates structural distortion and electrochemical performance deterioration. This study found that the introduction of Mn vacancy enables reversible oxygen redox behaviors within layered Li-4/7[square Mn-1/7(6/7)]O-2 with Li-O-vacancy configuration, effectively suppressing lattice oxygen loss and improving the output capacity and long-term cycling stability of batteries.
Article
Chemistry, Multidisciplinary
Qinong Shao, Panyu Gao, Chenhui Yan, Mingxi Gao, Wubin Du, Jian Chen, Yaxiong Yang, Jiantuo Gan, Zhijun Wu, Chenyang Zhang, Gairong Chen, Xusheng Zheng, Yue Lin, Yinzhu Jiang, Wenping Sun, Yongfeng Liu, Mingxia Gao, Hongge Pan
Summary: Introducing an additional redox couple in Li- and Mn-rich layered oxides cathode significantly enhances cycling stability and inhibits oxygen release, with S2- ions playing a crucial role in stabilizing the oxygen lattice. The findings suggest a potential direction to improve the cycling stability of high-energy anion-redox cathode materials for rechargeable metal-ion batteries.
ADVANCED MATERIALS
(2022)
Article
Materials Science, Multidisciplinary
William Judge, Henry Chan, Subramanian Sankaranarayanan, Ross J. Harder, Jordi Cabana, Mathew J. Cherukara
Summary: In this study, we propose a machine learning approach to identify crystalline line defects in samples from raw X-ray diffraction data without the need for image reconstruction, demonstrating the potential of automated machine learning approaches.
Review
Nanoscience & Nanotechnology
Zhenpeng Yao, Yanwei Lum, Andrew Johnston, Luis Martin Mejia-Mendoza, Xin Zhou, Yonggang Wen, Alan Aspuru-Guzik, Edward H. Sargent, Zhi Wei Seh
Summary: This Perspective highlights the recent advances in machine learning-driven energy research and proposes a set of key performance indicators to compare the benefits of different ML-accelerated workflows in the field of renewable energy.
NATURE REVIEWS MATERIALS
(2023)
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)
Editorial Material
Chemistry, Physical
Jordi Cabana, Thomas Alaan, George W. Crabtree, Po-Wei Huang, Akash Jain, Megan Murphy, Jeanne N'Diaye, Kasinath Ojha, George Agbeworvi, Helen Bergstrom, Simon Gersib, Hassan Harb, Adrien Stejer, Genesis Quiles-Galarza, Oliver Rodriguez, Isabella Caruso, Josue M. Goncalves, Grace Y. Chen, Carlos A. Fernandez, Hanqing Pan, Kabian Ritter, Yingjie Yang, Haozhe Zhang, Ana Cristina Garcia-Alvarez, Stefan Ilic, Khagesh Kumar, Rachel Silcox, Yu Yao, Hakhyeon Song, Stoyan Stoyanov, Mohit Saraf, Celine H. Chen, S. M. Supundrika Subasinghe, Reginaldo Gomes, Shuangyan Lang, Eamonn Murphy, Arashdeep Singh Thind, Yu Zheng
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Ahmad Jaradat, Chengji Zhang, Sanket Shashikant Sutar, Nannan Shan, Shuxi Wang, Sachin Kumar Singh, Taimin Yang, Khagesh Kumar, Kartikey Sharma, Shahriar Namvar, Ahmadiparidari Alireza, Tomas Rojas, Vikas Berry, Jordi Cabana-Jimenez, Zhehao Huang, Arunkumar Subramanian, Anh T. Ngo, Larry A. Curtiss, Amin Salehi-khojin
Summary: This study introduces a new medium-entropy cathode catalyst, (NbTa)(0.5)BiS3, combined with an ionic liquid-based electrolyte blend, which enables high-rate reversible electrochemistry in Li-CO2 batteries. The Li-CO2 battery with this catalyst exhibits superior performance, with a high current density of 5000 mA g(-1) and a capacity of 5000 mAh g(-1) for up to 125 cycles. The enhanced rate performance is attributed to the greater stability of the multi-element (NbTa)(0.5)BiS3 catalyst due to its higher entropy.
ADVANCED FUNCTIONAL MATERIALS
(2023)
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
Chemistry, Physical
Indrani Roy, Khagesh Kumar, Haifeng Li, Neelam Sunariwal, Grant C. B. Alexander, John W. Freeland, Fanny Rodolakis, Jordi Cabana
Summary: The capacity of transition-metal oxides as Li-ion battery cathodes is limited by instabilities that arise when high states of charge are achieved. Oxyfluorides with a disordered rocksalt structure have emerged as attractive alternatives, but the role of F in their electrochemical function, particularly when cationic redox produces high formal oxidation states, remains to be ascertained. The results obtained from X-ray absorption spectroscopy confirm the existence of Mn-F covalent interactions in Li2MnO2F and Li2Mn2/3Nb1/3O2F, suggesting the possibility of designing battery cathodes by manipulating the covalent interactions between transition metals and two different anions.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Jacob Jan Markut, Jordi Cabana, Neal P. Mankad, Donald J. Wink
Summary: A symmetry activity using student-built models was developed to engage students in identifying symmetry elements for seven molecules. The activity utilized 2D representations, 3D concrete models, and student-created drawings. The results showed consistent student engagement and increased ability to identify symmetry elements.
JOURNAL OF CHEMICAL EDUCATION
(2023)
Article
Chemistry, Physical
Khagesh Kumar, Sasawat Jamnuch, Leily Majidi, Saurabh Misal, Alireza Ahmadiparidari, Michael A. Dato, George E. Sterbinsky, Tianpin Wu, Amin Salehi-Khojin, Tod A. Pascal, Jordi Cabana
Summary: In this study, researchers investigated the electronic structure changes of MoS2 nanosheets during the carbon dioxide reduction reaction (CO2RR) through experimental and computational methods. They discovered the existence of Mo-CO2 binding in the active state, which perturbs the hybridized Mo 4d-S 3p states and is influenced by electrochemically induced sulfur vacancies. These findings provide insights into the excellent performance of MoS2 in CO2RR and could be used as a screening criterion for improving the activity and selectivity of transition-metal dichalcogenides (TMDCs) in general.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Eva Allen, Youngho Shin, William Judge, Mark Wolfman, Vincent De Andrade, Stephanie M. Cologna, Jordi Cabana
Summary: To overcome the instability issues in Ni-rich cathode materials, researchers have been exploring heterogenous architectures with elemental gradients tailored within particles. In this study, the entire three-dimensional structure of a secondary particle was nondestructively resolved using differential X-ray absorption spectroscopy (XAS) through transmission X-ray microscopy (TXM). The relationship between particle location and elemental content was quantified with high statistical significance. The results demonstrated reduced elemental heterogeneity after high-temperature synthesis while gradients still remained. This methodology can guide synthesis and ensure that improvements in electrochemical performance are linked to precise elemental distributions at the nanoscale.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Junghwa Kim, Shashwat Anand, Colin Gilgenbach, Ian D. Johnson, Megan Murphy, Tina Chen, Matthew Moy, Aubrey Penn, Jordi Cabana, Gerbrand Ceder, Brian J. Ingram, James M. LeBeau
Summary: This study directly investigates the atomic transport pathways of cations in spinel magnesium chromate using STEM, revealing the reversible occupation of interstitial sites by Cr atoms and the formation of vacancies induced by electron irradiation, leading to irreversible phase transitions.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Melissa C. Cendejas, Oscar A. Paredes Mellone, Unni Kurumbail, Zisheng Zhang, Jacob H. Jansen, Faysal Ibrahim, Son Dong, John Vinson, Anastassia N. Alexandrova, Dimosthenis Sokaras, Simon R. Bare, Ive Hermans
Summary: Hexagonal boron nitride is a highly selective catalyst for the oxidative dehydrogenation of propane. The activity of the catalyst is attributed to the formation of an amorphous boron oxyhydroxide surface layer, and the reaction mechanism involves both surface mediated and gas phase propagated radical reactions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Analytical
Karina Bzheumikhova, John Vinson, Rainer Unterumsberger, Malte Wansleben, Claudia Zech, Kai Schuler, Yves Kayser, Philipp Honicke, Burkhard Beckhoff
Summary: Using calibrated experimental data, this study demonstrates the applicability of theoretical XAS and XES calculations for titanium and its oxides at different energy edges. The results show that the OCEAN package is a versatile tool for analyzing and interpreting the electronic structure of materials, but also highlight some discrepancies between experimental data and theoretical calculations, indicating limitations of the approach.
JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY
(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.
