Article
Chemistry, Physical
Pirmin Stueble, Valeriu Mereacre, Holger Gesswein, Joachim R. Binder
Summary: Despite 20 years of research on LiNi0.5Mn1.5O4 (LNMO) cathode active materials for lithium-ion batteries, it has not been possible to utilize their favorable properties in stable battery cells. To overcome this, it is necessary to update the research perspective on LNMO and address persisting misconceptions. A comprehensive summary of the current knowledge on LNMO is provided, along with in-situ high temperature X-ray diffraction study and investigation of different LNMO materials. New evidence contradicting the idea of oxygen defects in LNMO is presented, and a enhanced classification of LNMO based on Ni content is proposed.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Feng Zou, Himamshu C. Nallan, Andrei Dolocan, Qiang Xie, Jianyu Li, Brennan M. Coffey, John G. Ekerdt, Arumugam Manthiram
Summary: The high operating voltage of LNMO cathode in lithium-ion cells leads to electrolyte decomposition and accelerated deterioration of the electrode/electrolyte interface. Aggressive side reactions at the graphite anode cause massive active lithium loss and capacity fade. By coating the graphite surface with an ultra-thin Al2O3 film, undesired reactions are inhibited, drastically improving the capacity and cycling stability of the LNMO/graphite cell.
ENERGY STORAGE MATERIALS
(2021)
Article
Chemistry, Physical
Gozde Oney, Jacob Olchowka, Arnaud Demortiere, Francois Weill, Laurence Croguennec
Summary: In this work, we successfully prepared impurity-free platelet-like LiNi0.5Mn1.5O4via molten salt synthesis. These platelets show multiple surface orientations, including {111}, {112}, and other high-indexed facets, and exhibit energy storage performance equivalent to that of octahedral particles. This ability to tune particle morphology and orientation will provide new opportunities to investigate mechanisms at the individual particle level using spectroscopy and microscopy techniques.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Dongsoo Lee, Zehao Cui, John B. Goodenough, Arumugam Manthiram
Summary: This study reveals the limitations of using lithium argyrodite sulfide solid electrolyte with LNMO cathode in all-solid-state batteries (ASSBs) due to inherent chemical incompatibility and poor oxidative stability. It is found that even using a halide solid electrolyte with high oxidative stability can result in the formation of resistive interphase layers with LNMO in ASSBs. However, through Fe-doping and Li3PO4 protective layer coating, LNMO with the halide solid electrolyte shows stable cycle performance with a stabilized interphase at a high voltage in ASSBs. This work provides guidance for using high-voltage cathodes in ASSBs and emphasizes the importance of stable interphases for stable cycling in ASSBs.
Review
Chemistry, Physical
Tianji Fu, Di Lu, Ziqing Yao, Yujie Li, Chongyang Luo, Tianyan Yang, Shuangke Liu, Yufang Chen, Qingpeng Guo, Chunman Zheng, Weiwei Sun
Summary: In order to reduce production cost and environmental damage, the lithium-ion battery industry has focused on cobalt-free cathode materials. High-voltage spinel LiNi0.5Mn1.5O4 (LNMO) has great potential for commercial production due to its high voltage platform, high theoretical energy density, low environmental impact, and low cost. However, its cycle performance and high temperature stability are poor, hindering large-scale production. Recent studies have made progress in improving the cycle stability of LNMO cathodes and understanding their degradation mechanism. This review summarizes the achievements and discusses future directions for LNMO cathode materials, such as machine learning and AI-assisted virtual experiments.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Taeho Yoon, Jiyong Soon, Tae Jin Lee, Ji Heon Ryu, Seung M. Oh
Summary: This study investigates the local dissolution of CEI and its adverse effects on the electrochemical performance of high-voltage spinel electrode. Corrosive acidic HF generated during electrolyte oxidation damages CEI by leaching inorganic components like LiF and LixPOyFz. However, with the presence of Al2O3 as an HF scavenger, CEI remains relatively stable leading to significantly improved coulombic efficiency.
JOURNAL OF POWER SOURCES
(2021)
Article
Chemistry, Multidisciplinary
Manuela R. Zimmermann, Subhas C. Bera, Georg Meisl, Sourav Dasadhikari, Shamasree Ghosh, Sara Linse, Kanchan Garai, Tuomas P. J. Knowles
Summary: Understanding the mechanisms of amyloid formation and replication is crucial for studying neurodegenerative disorders like Alzheimer's disease. Secondary nucleation, which involves attachment of soluble species to fibril surfaces leading to the formation of new fibrils in solution, plays a key role in aggregate self-replication. This detailed insight into the process is essential for designing potential inhibitors of amyloid formation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Stephanie L. Spence, Anyang Hu, Meng Jiang, Zhengrui Xu, Zhijie Yang, Muhammad Mominur Rahman, Luxi Li, Yong S. Chu, Xianghui Xiao, Xiaojing Huang, Feng Lin
Summary: In this study, high-spatial-resolution synchrotron X-ray nanodiffraction techniques were used to investigate lattice distortions and structural defects in Spinel LiNi0.5Mn1.5O4 material. The results revealed the presence of different forms of Mn3+ in the material, leading to variations in lattice distributions. It was also found that lattice distortions and structural defects can affect the diffusion of lithium ions.
ACS ENERGY LETTERS
(2022)
Article
Chemistry, Physical
Tayfun Kocak, Xiadong Qi, Xiaogang Zhang
Summary: This study investigates the influence of different water-based binders on the cycle performance of LNMO electrodes. The results show that LNMO electrodes with guar gum binder exhibit relatively stable performance at lower temperatures, while electrodes with polyvinylidene fluoride (PVdF) binder show better capacity retention at higher temperatures.
SOLID STATE IONICS
(2022)
Article
Chemistry, Multidisciplinary
Zehao Cui, Feng Zou, Hugo Celio, Arumugam Manthiram
Summary: It is demonstrated that the performance and lifespan of lithium-ion batteries can be improved by electrochemical modifications on graphite and LNMO materials, providing a possibility for the development of long-life graphite||LNMO full cells.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Fulya Ulu Okudur, Maria Batuk, Joke Hadermann, Mohammadhosein Safari, Dries De Sloovere, Satish Kumar Mylavarapu, Bjorn Joos, Jan D'Haen, Marlies K. Van Bael, An Hardy
Summary: The high-energy positive electrode material LNMO for lithium ion batteries suffers from capacity loss and impedance rise during cycling. In this study, a solution-gel synthesis method was used to coat LNMO particles with amorphous Li-Ti-O for improved Li conduction and surface stability. The surface modification resulted in increased electrochemically active surface area and HF-scavenging capability, leading to enhanced electrochemical performance.
Article
Nanoscience & Nanotechnology
Asako Oishi, Ryoichi Tatara, Eiichi Togo, Hiroshi Inoue, Satoshi Yasuno, Shinichi Komaba
Summary: This study focuses on the development of high-voltage LNMO composite electrodes for lithium-ion batteries. The use of a sulfated alginate binder showed the best performance, significantly improving the electrode's affinity for the electrolyte and forming a protective passivation layer. This research provides a basis for the cost-effective fabrication of high-energy-density LIBs.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Materials Science, Multidisciplinary
Xingfu Zi, Xin Huang, Jiling Song, Hongming Wu, Jianbing Guo
Summary: The application of LiNi0.49Mn1.49-xSrxY0.02O4 (x = 0.02, 0.04, 0.06) synthesized by sol-gel method in high energy density lithium-ion batteries was studied. The doping of Sr and Y improved the microscopic morphology and electrochemical performance of the LNMO material, with the LiNi0.49Mn1.45Sr0.04Y0.02O4 LNMO sample showing the optimal electrochemical performance.
JOURNAL OF MATERIALS SCIENCE
(2023)
Article
Chemistry, Physical
Xinwei Jiao, Lalith Rao, Junwei Yap, Chan-Yeop Yu, Jung-Hyun Kim
Summary: This work presents a strategy of blending LLZT garnet solid electrolyte into LNMO high-voltage spinel cathode to enhance electrochemical performances and stabilities of electrode/electrolyte interphase layers. The 5 wt% LLZT blended LNMO cathode delivered improved capacity, cycle life, and rate capability. The improvement mechanism includes LLZT improving Li+ transport properties of the CEI layer and scavenging moisture/proton in the electrolyte and oxidative decomposition products.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Analytical
Tayfun Kocak, Langyuan Wu, Jiang Wang, Umut Savaci, Servet Turan, Xiagong Zhang
Summary: Vanadium-doped LMNO spinel cathode material shows excellent cycling performance at high temperatures, with higher capacity retention compared to pristine and other doped materials, indicating it is an effective solution for improving high-temperature durability.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2021)
Article
Chemistry, Physical
Hua Zhang, Liubin Ben, Hailong Yu, Wenbin Qi, Wenwu Zhao, Xuejie Huang
Article
Materials Science, Multidisciplinary
Wenbin Qi, Liubin Ben, Hailong Yu, Wenwu Zhao, Guangjin Zhao, Xuejie Huang
PROGRESS IN NATURAL SCIENCE-MATERIALS INTERNATIONAL
(2020)
Article
Chemistry, Physical
Feng Tian, Yongzheng Zhang, Zhongzhu Liu, Robson de Souza Monteiro, Rogerio Marques Ribas, Peng Gao, Yongming Zhu, Hailong Yu, Liubin Ben, Xuejie Huang
Summary: Doping with 1 mol% Nb5+ significantly improves the cycling performance of LiNi0.8Co0.1Mn0.1O2 cathode material, showing a 96.9% capacity retention after 300 cycles at 1C. The enhancement is attributed to stabilization of the layered structure, mitigation of Ni2+ migration, improved lithium diffusion kinetics, and reduced lattice expansion/shrinkage during cycling.
SOLID STATE IONICS
(2021)
Article
Energy & Fuels
Yida Wu, Liubin Ben, Yuanjian Zhan, Hailong Yu, Wenbin Qi, Wenwu Zhao, Xuejie Huang
Summary: The novel hydrothermal method of coating LiNi0.5Mn1.5O4 surface with Li3PO4 was shown to be effective in improving cycling performance, with the introduction of small amounts of additional metal ions (such as Co) helping achieve a uniform coating. X-ray photoelectron microscopy and scanning transmission electron microscopy revealed that the additional metal ions diffuse into the surface structure of LiNi0.5Mn1.5O4, connecting Li3PO4 with the bulk material. As a result, the high-voltage LiNi0.5Mn1.5O4 half-cell with optimal Li3PO4 coating demonstrated significantly improved discharge capacity retention compared to the bare counterpart.
Article
Chemistry, Physical
Hongxiang Ji, Liubin Ben, Shan Wang, Zhongzhu Liu, Robson Monteiro, Rogerio Ribas, Hailong Yu, Peng Gao, Yongming Zhu, Xuejie Huang
Summary: The research demonstrates that by precisely controlling the coating concentration and temperature, Nb2O5 can effectively bond to the surface of LiMn2O4 spinel cathode material, significantly improving the electrochemical performance. However, at high coating concentrations, Nb5+ ions diffuse into the cathode structure, leading to a decrease in cycling performance.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Nanoscience & Nanotechnology
Hongxiang Ji, Liubin Ben, Hailong Yu, Ronghan Qiao, Wenwu Zhao, Xuejie Huang
Summary: A fast, simple, and inexpensive electrolysis process was used to prepare a Ni(OH)2 precursor mixed with LiOH/LiNO3 salts to obtain a LiNiO2 cathode material, which exhibited excellent layered structure and good cycling performance.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Correction
Nanoscience & Nanotechnology
Hongxiang Ji, Liubin Ben, Hailong Yu, Ronghan Qiao, Wenwu Zhao, Xuejie Huang
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Electrochemistry
Mengyu Tian, Liubin Ben, Zhou Jin, Hongxiang Ji, Hailong Yu, Wenwu Zhao, Xuejie Huang
Summary: The anode composed of Si nanoparticles and Sn nanowires shows excellent cycling performance at low temperatures, attributed to high lithium-ion chemical diffusion coefficient, low increase of charge transfer impedance, and high lithium intercalation kinetics.
ELECTROCHIMICA ACTA
(2021)
Article
Chemistry, Physical
Tian Rao, Peng Gao, Zimeng Zhu, Shan Wang, Liubin Ben, Yongming Zhu
Summary: The dual-doped LNO cathode material with magnesium and manganese exhibits higher capacity retention, more stable charge transfer impedance, and Li+ diffusion coefficient, improving its structural stability and cycling performance compared to the bare LNO counterpart.
SOLID STATE IONICS
(2022)
Article
Chemistry, Multidisciplinary
Mengyu Tian, Liubin Ben, Hailong Yu, Ziyu Song, Yong Yan, Wenwu Zhao, Michel Armand, Heng Zhang, Zhi-Bin Zhou, Xuejie Huang
Summary: This study proposes a new designer cathode additive that improves the solid electrolyte interphase layer on high-energy anodes by forming an ultrathin sulfur coating on the cathode, leading to enhanced cycling efficiency for lithium-ion batteries.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Feng Tian, Liubin Ben, Hailong Yu, Hongxiang Ji, Wenwu Zhao, Zhongzhu Liu, Robson Monteiro, Rogerio M. Ribas, Yongming Zhu, Xuejie Huang
Summary: X-ray nano-computed tomography and deep learning were used to study the structural evolution of LiNi0.8Co0.1Mn0.1O2 during cycling at 55 degrees C. Two types of intergranular cracks were observed, with the open cracks showing a significant increase in volume and a decrease in capacity retention. Further analysis revealed that migration of transition metal ions and reduction of these ions predominantly occurred in the open crack regions.
Article
Nanoscience & Nanotechnology
Hongxiang Ji, Ronghan Qiao, Hailong Yu, Shan Wang, Zhongzhu Liu, Robson Monteiro, Rogerio Ribas, Yongming Zhu, Liubin Ben, Xuejie Huang
Summary: The morphology of LiNiO2 cathode material was engineered using a small amount of Nb2O5 during the electrolysis synthesis of Ni(OH)(2) precursor, resulting in improved electrochemical performance. The engineered LNO cathode material exhibited increased mechanical strength and electrical contact, and reduced the H2-H3 phase transition effects.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Mengyu Tian, Zhou Jin, Ziyu Song, Ronghan Qiao, Yong Yan, Hailong Yu, Liubin Ben, Michel Armand, Heng Zhang, Zhi-bin Zhou, Xuejie Huang
Summary: This study proposes a new method to address the low conductivity and large volume changes of silicon-based anodes by introducing elemental sulfur and building a sulfur-mediated gradient interphase (SMGI) layer. The results show that lithium-ion batteries using this method exhibit good performance in terms of high energy density and cycle life.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Peng Ju, Liubin Ben, Yang Li, Hailong Yu, Wenwu Zhao, Yuyang Chen, Yongming Zhu, Xuejie Huang
Summary: The particle morphology of LiNi0.90Co0.05Mn0.05O2 (NCM90) cathode materials can be engineered by processing in pressurized oxygen atmospheres, resulting in small primary particle size and increased particle number. The use of deep learning to evaluate their morphological information reveals that the randomized orientation of primary particles and the homogenized distribution of small primary particles effectively eliminate the accumulation of cycling-induced local strain, leading to excellent electrical cycling performance.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Inorganic & Nuclear
Yang Li, Liubin Ben, Hailong Yu, Wenwu Zhao, Xinjiang Liu, Xuejie Huang
Summary: The study investigates the coating of tungsten oxide on the surface of LiNi0.6Co0.2Mn0.2O2 cathode material and its impact on the electrochemical cycling performance. The coated tungsten oxide primarily accumulates on the (003) facet, reducing lattice expansion during charge and oxygen release, thereby lowering strain and improving the cycling performance. This research provides new insights for enhancing the performance of lithium-ion battery cathode materials.