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Revisiting the capacity-fading mechanism of P2-type sodium layered oxide cathode materials during high-voltage cycling

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Journal of Energy Chemistry 2022年第6期31卷 16-25,I0002页

作者： Meidan Jiang Guannan Qian Xiao-Zhen Liao Zhouhong Ren Qingyu Dong Dechao Meng Guijia Cui Siqi Yuan Sang-Jun Lee Tian Qin Xi Liu Yanbin Shen Yu-Shi He Liwei Chen Yijin Liu Linsen Li Zi-Feng Ma Department of Chemical Engineering Shanghai Electrochemical Energy Device Research Center(SEED)School of Chemistry and Chemical EngineeringFrontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai 200240China Stanford Synchrotron Radiation Lightsource SLAC National Accelerator LaboratoryMenlo ParkCA 94025United States In-Situ Center for Physical Sciences School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China Suzhou Institute of Nanotech and Nanobionics(SINANO) Chinese Academy of SciencesSuzhou 215123JiangsuChina Shanghai Jiao Tong University Sichuan Research Institute Chengdu 610213SichuanChina

P2-type sodium layered oxide cathode (Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)P2-NNMO) has attracted great attention as a promising cathode material for sodium ion batteries because of its high specific capacity. However, this material suffers from a rapid capacity fade during high-voltage cycling. Several mechanisms have been proposed to explain the capacity fade, including intragranular fracture caused by the P2-O2 phase transion, surface structural change, and irreversible lattice oxygen release. Here we systematically investigated the morphological, structural, and chemical changes of P2-NNMO during high-voltage cycling using a variety of characterization techniques. It was found that the lattice distortion and crystal-plane buckling induced by the P2-O2 phase transition slowed down the Na-ion transport in the bulk and hindered the extraction of the Na ions. The sluggish kinetics was the main reason in reducing the accessible capacity while other interfacial degradation mechanisms played minor roles. Our results not only enabled a more complete understanding of the capacity-fading mechanism of P2-NNMO but also revealed the underlying correlations between lattice doping and the moderately improved cycle performance.

关键词： Phase transition layered cathode Buckling Capacity fading mechanism Sodium-ion batteries

Manipulating Na occupation and constructing protective film of P2-Na_(0.67)Ni_(0.33)Mn_(0.67)O_(2) as long-term cycle stability cathode for sodium-ion batteries

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Journal of Energy Chemistry 2024年第1期88卷 603-611,I0013页

作者： Yiran Sun Pengfei Zhou Siyu Liu Zhongjun Zhao Yihao Pan Xiangyan Shen Xiaozhong Wu Jinping Zhao Junying Weng Jin Zhou School of Chemistry and Chemical Engineering Shandong University of TechnologyZibo 0255000ShandongChina School of Materials Science and Engineering Shandong University of TechnologyZibo 255049ShandongChina

P2-Na_(0.67)Ni_(0.33)Mn_(0.67)O_(2)(NNMO)is promising cathode material for sodium-ion batteries(SIBs)due to its high specific capacity and fast Na+diffusion ***,the irreversible P2-O_(2)phase transformation,Na+/vacancy ordering,and transition metal(TM)dissolution seriously damage its cycling stability and restrict its commercialization ***,Na occupation manipulation and interface stabilization are proposed to strengthen the phase structure of NNMO by synergistic Zn/Ti co-doping and introducing lithium difluorophosp(LiPO_(2)F_(2))film-forming electrolyte *** Zn/Ti co-doping regulates the occupancy ratio of Nae/Nafat Na sites and disorganizes the Na+/vacancy ordering,resulting in a faster Na+diffusion kinetics and reversible P2-Z phase transition for P2-Na_(0.67)Ni_(0.28)Zn_(0.05)Mn_(0.62)Ti_(0.05)O_(2)(NNZMTO).Meanwhile,the LiPO_(2)F_(2)additive can form homogeneous and ultrathin cathode-electrolyte interphase(CEI)on NNZMTO surface,which can stabilize the NNZMTO-electrolyte interface to prevent TM dissolution,surface structure transformation,and micro-crack *** studies of in situ and ex situ characterizations and theoretical calculations were used to elucidate the storage mechanism of NNZMTO with Li PO_(2)F_(2)*** a result,the NNZMTO displays outstanding capacity retention of 94.44%after 500 cycles at 1C with 0.3 wt%Li PO_(2)F_(2),excellent rate performance of 92.5 mA h g^(-1)at 8C with 0.1 wt%Li PO_(2)F_(2),and remarkable full cell *** work highlights the important role of manipulating Na occupation and constructing protective film in the design of layered materials,which provides a promising direction for developing high-performance cathodes for SIBs.

关键词： layered cathode Zn/Ti co-doping Na occupation Electrolyte additive Sodium-ion batteries

Constructing a stable interface on Ni-rich LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) cathode via lactic acid-assisted engineering strategy

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Journal of Energy Chemistry 2024年第3期90卷 412-422,I0010页

作者： Weijian Tang Chengzhi Hu AFei Li Xiaoqin Huang Zhangxian Chen Jianhui Su Weixin Zhang Institute of Energy Hefei Comprehensive National Science CenterHefei 230031AnhuiChina School of Chemistry and Chemical Engineering Hefei University of Technology and Anhui Key Laboratory of Controllable Chemical Reaction&Material Chemical EngineeringHefei 230009AnhuiChina School of Electrical Engineering and Automation Hefei University of TechnologyHefei 230009AnhuiChina

Ni-rich layered oxides are potential cathode materials for next-generation high energy density Li-ion batteries due to their high capacity and low ***,the inherently unstable surface properties,including high levels of residual Li compounds,dissolution of transition metal cations,and parasitic side reactions,have not been effectively addressed,leading to significant degradation in their electrochemical *** this study,we propose a simple and effective lactic acid-assisted interface engineering strategy to regulate the surface chemistry and properties of Ni-rich LiNi_(0.8)Co_(0.1)Mr_(0.1)O_(2) *** novel surface treatment method successfully eliminates surface residual Li compounds,inhibits structural collapse,and mitigates cathode-electrolyte interface film *** a result,the lactic acidtreated LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) achieved a remarkable capacity retention of 91.7% after 100 cycles at 0.5 C(25℃) and outstanding rate capability of 149.5 mA h g^(-1) at 10 C,significantly outperforming the pristine ***,a pouch-type full cell incorporating the modified LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) cathode demonstrates impressive long-term cycle life,retaining 81.5% of its capacity after 500 cycles at 1 *** importantly,the thermal stability of the modified cathode is also dramatically *** study offers a valuable surface modification strategy for enhancing the overall performance of Ni-rich cathode materials.

关键词： Residual Li Lactic acid Surface modification Carbon coating layered cathode Ni-rich

Doping of group IVB elements for nickel-rich cobalt-free cathodes

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Journal of Energy Chemistry 2023年第11期86卷 559-568,I0012页

作者： Shengnan Guo Xincheng Lei Jiayi Wang Jie Su Yingying Wang Xiaozhi Liu Pengxiang Ji Kangning Zhao Xuefeng Wang Lin Gu Zhenpeng Yao Dong Su National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Center of Hydrogen Science Shanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Metal Matrix Composites School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials Department of Materials Science and EngineeringTsinghua UniversityBeijing 100084China

Hetero-element doping is a promising strategy to improve the cycling stability of nickel-rich cobalt-free cathodes for the next-generation high energy-density Li ion *** make doping effective,it is important to understand the mechanism of how the dopants regulate the electronic band,lattice parameter adjusting,or hetero-phase formation to achieve high *** this study,we investigate LiNi_(0.9)Mn_(0.1)O_(2)cathodes doped with IVB grouping elements via multiple characterization *** utilizing in situ XRD and TEM methods,we found that the stronger Ti-O bond effectively improves the cathode stability via a dual protection ***,the bulk lattice of cathode is wellpreserved during cycling as a result of the suppressed H_(2)-H_(3)phase transition,while a in situ formed Ti-rich surface layer can prevent continuous surface *** a result,the 5%Ti doped LiNi_(0.9)Mn_(0.1)O_(2)cathode exhibits a high capacity retention of 96%after 100 ***,despite IVB group elements Zr and Hf have stronger bonding energy with oxygen,their larger ionic radii actually impede their diffusion into the cathode,thereby they can not improve the cycling *** findings uncover the functional origin of doped elements with their dynamic modification on cathode structure,providing mechanistic insights into the design of nickel-rich cobalt-free cathodes.

关键词： Li ion battery layered cathode Cycling stability Doping effect In situXRD

The Puzzles in Fast Charging of Li-Ion Batteries

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Energy & Environmental Materials 2022年第4期5卷 1005-1007页

作者： Sheng Shui Zhang Battery Science Branch FCDD-RLS-CESensors and Electron Devices DirectorateU.S.Army Research LaboratoryAdelphi MD 20783-1138USA

Fast charging of Li-ion cells faces two aspects of challenges,1)accelerated capacity fade and 2)inferior charging *** is commonly believed that the former is due to Li plating and its resultant reactions with electrolyte at the graphite anode,which results in a loss in the inventory of Li+ions and an increase in the cell’s *** the latter is ascribed to the high voltage polarization in relation to the slow transport of Li+ions between two ***,there are many other hidden facts that essentially affect the fast charging performances of Li-ion *** commentary intends,from the view of materials,to uncover these hidden factors,including failure of the solid electrolyte interphase and exfoliation of the graphite structure at the anode,structural degradation of the Ni-rich layered cathode materials,as well as the high solvation and desolvation activation energies of Li+ions in the ***,some solutions to the fast-charging problems of Li-ion cells are proposed based on the understanding of these hidden factors.

关键词： electrolyte fast charging graphite anode layered cathode Li-ion battery

Challenges and modification strategies of high-voltage cathode materials for Li-ion batteries

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Chinese Journal of Structural Chemistry 2023年第10期42卷 67-79页

作者： Yue Wang Caixia Xu Xingtao Tian Siyu Wang Yan Zhao Institute of NBC Defense PLA ArmyBeijing102205China School of Energy and Power Engineering Jiangsu UniversityZhenjiang212013China

Li-ion batteries(LIBs)have gained wide recognition as effective energy storage devices and power supply sources due to their exceptional volumetric energy density,mass energy density and cycling *** cathode materials,a key component of LIBs,play a crucial role in determining the electrochemical performance of these ***,there is an increasing demand to explore and investigate suitable high-energy electrode materials that can provide greater capacity and output voltage for the next generation of *** paper aims to provide a comprehensive overview of the latest researches on five typical high-voltage cathode ***,this review will focus on the detailed analysis of their crystalline structures,reaction mechanisms during cycling,current research status and strategies aimed at improving or enhancing their overall electrochemical ***,the insights presented in this review will help researchers design and develop high-energy cathode materials with improved performance for the next generation of LIBs.

关键词： Research advances Li-ion batteries Lithium iron phosphate layered cathode Lithium-rich oxides Lithium manganate

Recent progress on the modification of high nickel contentNCM:Coating,doping,and single crystallization

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Interdisciplinary Materials 2022年第3期1卷 330-353页

作者： Junqing Yan Hao Huang Junfan Tong Wei Li Xiaohang Liu Haoxuan Zhang Heqin Huang Weidong Zhou State Key Laboratory of Organic-Inorganic Composites Beijing Advanced Innovation Center for Soft Matter Science and EngineeringBeijing University of ChemicalBeijingChina Department of Chemical Catalysts&Battery Materials BASF Advanced Chemicals Co.Ltd.BASF(China)Co.Ltd.ShanghaiChina

High nickel content layered cathodes,represented by NCM(LiNi_(x)Co_(y)Mn_(z)O_(2),x+y+z=1),are now widely employed in the market of electric vehicles,owing to their high energy *** the gradual increase of nickel content and capacity,the issues on cycling life and safety become more *** this review,various strategies for improving the performance of high nickel NCM are summarized on the aspects of surface coating,ionic doping,and singlecrystal *** coating strategy was separately described according to the physical property of coating species,including inert material coating,Li^(+)-conductor coating,electronic conductor coating,and mixed conductor *** coating species help to suppress the interfacial oxidation of electrolytes by NCM,improving the cycling life and *** elemental doping in the crystal lattice of NCM is then presented in the aspects of cation,anion,and mixed-ion doping,which are beneficial to stabilize the layered structure during charge–discharge and so promote the electrochemical *** quite recent years,the strategy of single-crystal NCM was demonstrated to be a promising pathway,owing to the dramatically reduced surface area and grain ***,the remaining unsolved challenges and future strategies for further development of NCM cathode materials are outlined.

关键词： coating doping high nickel NCM layered cathode lithium-ion batteries

Precipitate-stabilized surface enabling high-performance Na_(0.67)Ni_(0.33-x)Mn_(0.67)Zn_(x)O_(2) for sodium-ion battery

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eScience 2022年第5期2卷 529-536页

作者： Kuan Wang Zhengfeng Zhang Sulan Cheng Xiao Han Junjie Fu Manling Sui Pengfei Yan Beijing Key Laboratory of Microstructure and Properties of Solids Faculty of Materials and ManufacturingBeijing University of TechnologyBeijing100124China

Electrode interfacial degradations are the key challenges for high-performance rechargeable batteries,usually mitigated through surface modification/coating ***,we report a novel mechanism to enhance the surface stability of P2 layered cathodes by introducing a high density of dopant-enriched *** on microscopic analysis,we show that forming a high density of precipitates at the grain surface can effectively suppress surface cracking and corrosion,which not only improves the surface/interface stability but also effectively suppresses the intergranular cracking *** the doping level can lead to a greater density of precipitates at the surface region,which results in higher surface stability and increased cycling stability of the P2 layered cathode for a sodium-ion *** further reveal that prolonged cycling can induce the formation of a precipitate-free surface region due to the loss of Zn dopant and *** in-depth microanalysis reveals cycling-induced dynamic structural evolution of the P2 layered cathodes,highlighting that dopant segregation-induced precipitation is a new approach to achieving high interfacial stability.

关键词： layered cathode TEM Precipitate Sodium-ion battery Surface stability

Coating of Al_2O_3 on layered Li(Mn_(1/3)Ni_(1/3)Co_(1/3))O_2 using CO_2 as green precipitant and their improved electrochemical performance for lithium ion batteries

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Journal of Energy Chemistry 2013年第3期22卷 468-476页

作者： Yingqiang Wu Linhai Zhuo Jun Ming Yancun Yu Fengyu Zhao State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of Sciences Laboratory of Green Chemistry and Process Changchun Institute of Applied ChemistryChinese Academy of Sciences University of Chinese Academy of Sciences

Li（Mn1/3Ni1/3Co1/3）O2 cathode materials were fabricated by a hydroxide precursor method. A1203 was coated on the surface of the Li（Mn1/3Ni1/3Co1/3）O2 through a simple and effective one-step electrostatic self-assembly method. In the coating process, a NaHCO3- H2CO3 buffer was formed spontaneously when CO2 was introduced into the NaAlO2 solution. Compared with bare Li（Mn1/3Ni1/3Co1/3）O2, the surface-modified samples exhibited better cycling performance, rate capability and rate capability retention. The Al2O3-coated Li（Mn1/3Ni1/3Co1/3）O2 electrodes delivered a discharge capacity of about 115 mAh.g-1 at 2 A.g-1, but only 84 mAh.g-1 for the bare one. The capacity retention of the Al2O3-coated Li（Mn1/3Ni1/3Co1/3）O2 was 90.7% after 50 cycles, about 30% higher than that of the pristine one.

关键词： electrochemistry alumina coating layered cathode lithium-ion batteries