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Unexpected Li displacement and suppressed phase transition enabling highly stabilized oxygen redox in P3-type Na layered oxide cathode

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Journal of Energy Chemistry 2023年第10期85卷 144-153,I0006页

作者： Myungeun Choi Hobin Ahn Hyunyoung Park Yongseok Lee Jinho Ahn Bonyoung Ku Junseong Kim Wonseok Ko Jungmin Kang Jung-Keun Yoo Duho Kim Jongsoon Kim Department of Energy Science Sungkyunkwan UniversitySuwon 16419Republic of Korea SKKU Institute of Energy Science and Technology(SIEST) Sungkyunkwan UniversitySuwon 16419Republic of Korea Carbon Composites Department Korea Institute of Materials Science(KIMS)Changwon 51508Republic of Korea Department of Mechanical Engineering(Integrated Engineering Program) Kyung Hee University1732Deogyeong-daeroGiheung-guYongin-siGyeonggi-do 17104Republic of Korea Department of KHU-KIST Convergence Science and Technology Kyung Hee University23Kyunghee-daero Dongdaemun-guSeoul 02447Republic of Korea

Oxygen redox is considered a new paradigm for increasing the practical capacity and energy density of the layered oxide cathodes for Na-ion batteries. However, severe local structural changes and phase transitions during anionic redox reactions lead to poor electrochemical performance with sluggish ***, we propose a synergy of Li-Cu cations in harnessing the full potential of oxygen redox, through Li displacement and suppressed phase transition in P3-type layered oxide cathode. P3-type Na_(0.7)[Li_(0.1)Cu_(0.2)Mn_(0.7)]O_(2) cathode delivers a large specific capacity of ~212 mA h g^(-1)at 15 mA g^(-1). The discharge capacity is maintained up to ~90% of the initial capacity after 100 cycles, with stable occurrence of the oxygen redox in the high-voltage region. Through advanced experimental analyses and first-principles calculations, it is confirmed that a stepwise redox reaction based on Cu and O ions occurs for the charge-compensation mechanism upon charging. Based on a concrete understanding of the reaction mechanism, the Li displacement by the synergy of Li-Cu cations plays a crucial role in suppressing the structural change of the P3-type layered material under the oxygen redox reaction, and it is expected to be an effective strategy for stabilizing the oxygen redox in the layered oxides of Na-ion batteries.

关键词： layered oxide cathode Oxygen redox reaction Structural stability Li displacement No phase transition

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Doping Strategy in Nickel-Rich layered oxide cathode for Lithium-Ion Battery

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Renewables 2023年第3期1卷 316-340页

作者： Jiayi Wang Xincheng Lei Shengnan Guo Lin Gu Xin Wang Aiping Yu Dong Su Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190 School of Information and Optoelectronic Science and Engineering&International Academy of Optoelectronics at Zhaoqing South China Normal UniversityGuangzhou 510006 Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials Department of Materials Science and EngineeringTsinghua UniversityBeijing 100084 Department of Chemical Engineering Waterloo Institute for NanotechnologyWaterloo Institute for Sustainable EnergyUniversity of WaterlooWaterlooOntario N2L 3G1

Ni-rich layered oxides have been regarded as the most promising cathode material for next-generation high energy density Li-ion batteries because of their advantages in capacity and ***,these cathodes suffer from irreversible structural degradation,fast capacity attenuation as well as seriously reduced safety in their practical *** strategies with different elements have been employed to address the above *** this review,we summarize the research advances of the elemental doping in a Ni-rich layered oxide *** experimental methods and dopant selection rules are briefly *** we discuss here the effects of the elemental doping from the aspects of the crystal lattice,electronic structure,nanomorphology,and surface *** addition,this review surveys the first-principles calculation and advanced structural characterization techniques,which have played important roles in elucidating the structure-performance ***,perspectives regarding the future of doping strategy are given.

关键词： lithium-ion battery layered oxide cathode doping strategy advanced characterization techniques

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Ultralow-strain Ti substituted Mn-vacancy layered oxides with enhanced stability for sodium-ion batteries

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Journal of Energy Chemistry 2021年第12期30卷 351-357,I0008页

作者： Yanchen Liu Chenchen Wang Meng Ren Hengyi Fang Zhuoliang Jiang Fujun Li Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Renewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin 300071China

Anionic redox reaction(ARR) in layered manganese-based oxide cathodes has been considered as an effective strategy to improve the energy density of sodium-ion ***-vacancy layered oxides deliver a high ARR-related capacity with small voltage hysteresis,however,they are limited by rapid capacity degradation and poor rate capability,which arise from inferior structure changes due to repeated redox of lattice ***,redox-inactive Ti^(4+)is introduced to substitute partial Mn^(4+)to form Na_(2) Ti_(0.5)Mn_(2.5)O_7(Na_(4/7)[□_(1/7)Ti_(1/7)Mn_(5/7)]O_(2),□ for Mn vacancies),which can effectively restrain unfavorable interlayer gliding of Na2 Mn307 at high charge voltages,as reflected by an ultralow-strain volume variation of 0.11%.There is no irreversible O_(2) evolution observed in Na_(2) Ti_(0.5)Mn_(2.5)O_7 upon charging,which stabilizes the lattice oxygen and ensures the overall structural *** exhibits increased capacity retention of 79.1% after 60 cycles in Na_(2) Ti_(0.5)Mn_(2.5)O_7(17.1% in Na_(2) Mn_(3) O_7) and good rate capability(92.1 mAh g^(-1) at 0.5 A g^(-1)).This investigation provides new insights into designing high-performance cathode materials with reversible ARR and structural stability for SIBs.

关键词： Mn vacancy layered oxide cathode Anionic redox reaction Sodium-ion batteries

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Clarification of underneath capacity loss for O3-type Ni, co free layered cathodes at high voltage for sodium ion batteries

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Journal of Energy Chemistry 2023年第2期77卷 479-486,I0012页

作者： Dong Zhou De Ning Jun Wang Jiahua Liu Gaoyuan Zhang Yinguo Xiao Jiaxin Zheng Yongli Li Jie Li Xinzhi Liu Guangdong Provincial Key Laboratory of Magnetoelectric Physics and Devices School of PhysicsSun Yat-sen UniversityGuangzhou 510275GuangdongChina School of Innovation and Entrepreneurship Southern University of Science and TechnologyShenzhen 518055GuangdongChina Centre for Photonics Information and Energy Materials Shenzhen Institutes of Advanced TechnologyChinese Academy of SciencesShenzhen 518055GuangdongChina School of Advanced Materials Peking University Shenzhen Graduate SchoolShenzhen 518055GuangdongChina Institute for Clean Energy Technology North China Electric Power UniversityBeijing 102206China Department of Energy Politecnico di MilanoVia Lambruschini 4Milano 20156Italy Centre for Physical Mechanics and Biophysics School of PhysicsSun Yat-sen UniversityGuangzhou 510275GuangdongChina

Earth abundant O3-type NaFe_(0.5)Mn_(0.5)O_(2)layered oxide is regarded as one of the most promising cathodes for sodium ion batteries due to its low cost and high energy ***,its poor structural stability and cycle life strongly impede the practical ***,the dynamic phase evolution as well as charge compensation mechanism of O3-type NaFe_(0.5)Mn_(0.5)O_(2)cathode during sodiation/desodiation are revealed by a systemic study with operando X-ray diffraction and X-ray absorption spectroscopy,high resolution neutron powder diffraction and neutron pair distribution *** layered structure experiences a phase transition of O3→P3→OP2→ramsdellite during the desodiation,and a new O3’phase is observed at the end of the discharge state(1.5 V).The density functional theory(DFT)calculations and nPDF results suggest that depletion of Na^(+)ions induces the movement of Fe into Na layer resulting the formation of an inert ramsdellite phase thus causing the loss of capacity and structural ***,the operando XAS clarified the voltage regions for active Mn^(3+)/Mn^(4+)and Fe^(3+)/Fe^(4+)redox *** work points out the universal underneath problem for Fe-based layered oxide cathodes when cycled at high voltage and highlights the importance to suppress Fe migration regarding the design of high energy O3-type cathodes for sodium ion batteries.

关键词： Sodium ion batteries layered oxide cathode Iron migration Operando X-ray absorption spectroscopy Neutron measurements

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Designing a durable high-rate K_(0.45)Ni_(0.1)Fe_(0.1)Mn_(0.8)O_(2) cathode for K-ion batteries:A joint study of theory and experiment

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Science China Materials 2022年第7期65卷 1741-1750页

作者： Rongbin Dang Qing-Bo Yan Enyue Zhao Na Li Kang Wu Zhongjun Chen Zhonghua Wu Xiangfeng Liu Zhongbo Hu Xiaoling Xiao College of Materials Science and Optoelectronic Technology Center of Materials Science and Optoelectronics EngineeringUniversity of Chinese Academy of SciencesBeijing 100049China Songshan Lake Materials Laboratory Dongguan 523808China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China

K-ion batteries(KIBs)hold great promise for large-scale energy ***,the absence of suitable cathode materials limits their practical ***,rationally designing advanced cathode materials for KIBs remains an open *** this work,based on density functional theory calculations,we find that the bond stability of Fe–O is higher than that of Co–O in layered transitional metal(TM)***,the K-ion migration in the Fe-based layered TM oxide has a significantly lower activation energy barrier than that in the Co-based *** on this theoretical prediction,we successfully synthesized a low-cost K_(0.45)Ni_(0.1)Fe_(0.1)Mn_(0.8)O_(2)cathode,which shows excellent structural stability and superior K-storage properties,including durable cycle life and high-rate ***,the designed K_(0.45)Ni_(0.1)Fe_(0.1)Mn_(0.8)O_(2)cathode possesses a great full-cell performance with a discharge capacity of~75 mA h g^(-1) and capacity retention of~80%after 100 *** results show that Fe has better structural stability and K-ion diffusion than high-cost Co in layered oxide cathodes,and this finding provides new insights into the design of low-cost and high-performance KIB layered *** work highlights the feasibility of a theory-guided experiment in screening promising battery materials.

关键词： K-ion batteries layered oxide cathode density functional theory K_(0.45)Ni_(0.1)Fe_(0.1)Mn_(0.8)O_(2)

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Al, Zr dual-doped cobalt-free nickel-rich cathode materials for lithium-ion batteries

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Progress in Natural Science:Materials International 2023年第1期33卷 108-115页

作者： Xinxin Tan Wenjie Peng Meng Wang Gui Luo Zhixing Wang Guochun Yan Huajun Guo Qihou Li Jiexi Wang School of Metallurgy and Environment Central South University BASF ShanShan Battery Materials Co. LTD Engineering Research Center of the Ministry of Education for Advanced Battery Materials Central South University Hunan Provincial Key Laboratory of Nonferrous Value-Added Metallurgy Central South University

Nickel-rich and cobalt-free cathode materials have obvious advantages in the aspects of energy density and economic efficiency. However, these materials are restricted from being used in commercial lithium-ion batteries due to the problems of poor structural stability and rate capability. In this study, the aluminum and zirconium dual-doped Co-free Ni-rich LiNi0.96Mn0.04O2cathode material(NMAZ) is prepared by a facile high-temperature solid-phase method. The obtained NMAZ shows low cation disordering degree owing to the stability of transition metal slabs induced by strong Al–O and Zr–O bonds. Besides, the kinetics of lithium-ion diffusion is significantly improved by larger c-axis and the fast lithium-ion conducting Li2ZrO3layer on the interface. As a result, NMAZ shows an improved capacity retention of 70.3% at 1C after 100 cycles under an elevated temperature(45°C), compared with 50.5% of pure LiNi0.96Mn0.04O2. In addition, it exhibits splendid rate performance even at higher C-rate and better thermal stability compared to bare LiNi0.96Mn0.04O2. Hence, the Al, Zr dualdoped modification is beneficial to improving the structural stability and electrochemical performance of the Ni-rich and Co-free layered oxide cathodes for Li-ion batteries.

关键词： Lithium-ion batteries Ni-rich Co-free layered oxide cathode Dual-doping

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