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Boosting rate and cycling performance of K-doped Na_(3)V_(2)(PO_(4))_(2)F_(3) cathode for high-energy-density sodium-ion batteries

河南省化学会2016年学术年会

作者： Nai-Teng Wu Xian-Ming Liu Hong-Ru Fu Zhan Zhou Lu-fang Ma College of Chemistry and Chemical Engineering and Henan Key laboratory of Function-Oriented Porous Materials Luoyang Normal University

The degradation of Ni-rich cathode materials exposing in the air is an inherent issue for its large-scale application. Tetraethyl orthosilicate(TEOS) was utilized to dispose of the LiOH and LiCO impurities which generated by the resultant reaction between the residual lithium on the surface of LiNiCoAlO(NCA) cathode materials and the HO and CO in the air. After the reoxidation and coating process in the O atmosphere, a stable coating layer containing Si element was successful formed. The morphology, structure and composition of the as-prepared samples were investigated by X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), scanning scanning electron microscope(SEM) and transmission electron microscopy(TEM). Owing to the facile treatment, the resultant TEOS treated NCA(SNCA) used as lithium ion batteries cathode materials manifest remarkably enhanced cycling performance, attaining 85% capacity retention after 100 cycles at 1 C,which is much better than the fresh NCA(FNCA, 71% retention) and degraded NCA(DNCA, 33%retention) counterparts. All of these results demonstrate that such a treatment with DNCA not only reduces the amount of surface impurities, but also endows the electrode materials the capacity of reduction side reaction and improvement the structural stability.

关键词： degradation recovery Li Ni0.8Co0.15Al0.05O2 cathode materials lithium ion batteries

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Green Energy & Environment 2022年第6期7卷 1253-1262页

作者： Jiexin Zhang YangYang Lai Peng Li Yanxia Wang Faping Zhong Xiangming Feng Weihua Chen Jianjun Liu Xinping Ai Hanxi Yang Yuliang Cao Engineering Research Center of Organosilicon Compounds&materials of Ministry of Education College of Chemistry and Molecular SciencesWuhan UniversityWuhan430072China National Engineering Research Center of Advanced Energy Storage materials Hunan410205China College of Chemistry and Molecular Engineering Zhengzhou UniversityZhengzhou450001China State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of Sciences1295 Dingxi RoadShanghai200050China

As a promising cathode material,Na_(3)V_(2)(PO_(4))_(2)F_(3)(NVPF)has attracted wide attention for sodium-ion batteries(SIBs)because of its high operating voltage and high structural stability.However,the low intrinsic electronic conductivity and insufficient Na ion mobility of NVPF limit its development.Herein,K-doping NVPF is prepared through a facile ball-milling combined calcination method.The effects of K-doping on the crystal structure,kinetic properties and electrochemical performance are investigated.The results demonstrate that the Na_(2.90)K_(0.10)V_(2)(PO_(4))_(3)F_(3)(K0.10-NVPF)exhibits a high capacity(120.8 mAh g^(-1) at 0.1 C),high rate capability(66 mAh g^(-1) at 30 C)and excellent cycling performance(a capacity retention of 97.5%at 1 C over 500 cycles).Also,the occupation site of K ions in the lattice,electronic band structure and Na-ion transport kinetic property in K-doped NVPF are investigated by density functional theory(DFT)calculations,which reveals that the K-doped NVPF exhibits improved electronic and ionic conductivities,and located K^(+) ions in the lattice to contribute to high reversible capacity,rate capability and cycling stability.Therefore,the K-doped NVPF serves as a promising cathode material for high-energy and high-power SIBs.

关键词： Potassium doping Na_(3)V_(2)(PO_(4))_(2)F_(3) cathode materials Sodium ion batteries Long-term stability

Progresses in Sustainable Recycling Technology of Spent Lithium-Ion Batteries

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Energy & Environmental materials 2022年第4期5卷 1012-1036页

作者： Kaidi Du Edison Huixiang Ang Xinglong Wu Yichun Liu Faculty of Chemistry Northeast Normal UniversityChangchunJilin 130024China MOE Key Laboratory for UV Light-Emitting materials and Technology Northeast Normal UniversityChangchunJilin 130024China Natural Sciences and Science Education National Institute of EducationNanyang Technological UniversitySingapore 637616Singapore

The number of lithium-ion batteries(LIBs)is steadily increasing in order to meet the ever-growing demand for sustainable energy and a high quality of life for humankind.At the same time,the resulting large number of LIB waste certainly poses safety hazards if it is not properly disposed of and will seriously harm the environment due to its inherent toxicity due to the use of toxic substances.Moreover,the consumption of many scarce precious metal resources is behind the mass production of batteries.In the light of severe environmental,resources,safety and recycling problems,recycling spent LIBs have become an essential urgently needed action to achieve sustainable social development.This review therefore critically analyses the value and the need for recycling of spent LIBs from a variety of resources and the environment.A range of existing technologies for recycling and reusing spent LIBs,such as pretreatment,pyrometallurgy,hydrometallurgy,and direct recycled methods,is subsequently summarized exclusively.In addition,the benefits and problems of the methods described above are analyzed in detail.It also introduces recycling progress of other LIB components,such as anodes,separators,and electrolytes,as well as the high-value cathode.Finally,the prospects for recycling LIBs are addressed in four ways(government,users,battery manufacturers,and recyclers).This review should contribute to the development of the recycling of used LIBs,particularly in support of industrialization and recycling processes.

关键词： cathode materials pretreatment recycling spent lithium-ion batteries valuable metals

Uncovering the degradation mechanism induced by ion-diffusion kinetics in large-format lithium-ion pouch cells

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能源化学:英文版 2023年第8期83卷 98-105,I0005页

作者： Shi Zhou Xiaohong Zhang Cong Chen Ming Chen Fanpeng Kong Yingjie Qiao Jiajun Wang Key Laboratory of Superlight materials and Surface Technology Ministry of EducationCollege of Materials Science and Chemical EngineeringHarbin Engineering University Harbin 150001HeilongjiangChina Chongqing Research Institute of Harbin Institute of Technology Chongqing 401135China

Battery electrochemistry in an actual cell is a complicated behavior influenced by the current density,uniformity,and ion-diffusion distance,etc.The anisotropism of the lithiation/delithiation degree is usually inevitable,and even worse,due to a trend of big-size cell design,typically such as 4680 and blade cells,which accelerated a battery failure during repeat lithiation and delithiation of cathodes.Inspire by that,two big-size pouch cells with big sizes,herein,are selected to reveal the ion-diffusion dependency of the cathodes at different locations.Interestingly,we find that the LiCoO_(2) pouch cell exhibits ~5 A h loss after 120 charge-discharge cycles,but a 15 A h loss is verified in a LiNixMnyCO_(1-x)-yO_(2)(NCM) cell.Synchrotron-based imaging analysis indicates that higher ion-diffusion rates in the LiCoO_(2)than that in the LiNixMnyCO_(1-x)-yO_(2)is the determined factor for the anisotropic cathode fading,which is responsible for a severe mechanical issue of particle damage,such as cracks and even pulverization,in the cathode materials.Meanwhile,we verify the different locations at the near-tab and bottom of the electrode make it worse due to the ion-diffusion kinetics and temperature,inducing a spatially uneven electrochemistry in the big-size pouch cell.The findings give an in-depth insight into pouch cell failure and make a guideline for high-energy cell design and development.

关键词： Ah-level lithium-ion pouch cells cathode materials lon-diffusion kinetics X-ray tomography

Mechanism exploration of enhanced electrochemical performance of single-crystal versus polycrystalline LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)

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Rare Metals 2022年第11期41卷 3783-3794页

作者： Tian-Yi Zeng Xiao-Yun Zhang Xing-Yu Qu Mei-Qing Li Pan-Pan Zhang Ming-Ru Su Ai-Chun Dou Ahmad Naveed Yu Zhou Yun-Jian Liu School of Material Science and Engineering Jiangsu UniversityZhenjiang212013China

Single-crystal LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(SC-811),which offers better cycle performance compared to the polycrystalline counterpart,has received great attention.We report herein the synthesis of SC-811 with a grain size of 2-4μm by washing and reheating method,which compares with conventional polycrystalline LiNi_(0.8)-Co_(0.1)Mn_(0.1)O_(2)(PC-811).The discharge capacity of SC-811 reaches 152.1 mAh·g^(-1)after 100 cycles(86.7%capacity retention)at 1.0 C,which is much better than that of PC-811(130.2 mAh·g^(-1),73.8%capacity retention).By using multiscale characterization,the results unveil that SC-811 can not only improve the reversibility of the H2-H3 phase transitions,suppress the generation of micro-cracks and phase transformations,but also mitigate the undesired side reactions between electrode and electrolyte.Besides,the Li-O bond of SC-811 is longer than that of PC-811,which is conducive to the de-intercalation of Li-ions,thereby enhancing the structural stability.This finding provides an impressive strategy to sustain structural stability and improve the cycling life of Ni-rich layered cathodes.

关键词： Li-ion batteries(LIBs) cathode materials Single-crystal Capacity retention Phase transitions

Regeneration of spent LiFePO4 as a high-performance cathode material by a simultaneous coating and doping strategy

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International Journal of Minerals,Metallurgy and materials 2023年第6期30卷 1162-1170页

作者： Hui Tong Yi Li Gaoqiang Mao Chaolei Wang Wanjing Yu Yong Liu Mudan Liu School of Metallurgy and Environment Central South UniversityChangsha 410083China Guangdong Provincial Key Laboratory of Development and Comprehensive Utilization of Mineral Resources Guangzhou 510560China National&Regional Joint Engineering Research Center of Nonferrous Metal Resource Recycling Changsha 410083China Engineering Research Center of the Ministry of Education for Advanced Battery materials Central South UniversityChangsha 410083China Institute of Resources Utilization and Rare Earth Development Guangdong Academy of SciencesGuangzhou 510560China

With the number of decommissioned electric vehicles increasing annually,a large amount of discarded power battery cathode material is in urgent need of treatment.However,common leaching methods for recovering metal salts are economically inefficient and polluting.Meanwhile,the recycled material obtained by lithium remediation alone has limited performance in cycling stability.Herein,a short method of solid-phase reduction is developed to recover spent LiFePO4 by simultaneously introducing Mg2+ions for hetero-atom doping.Issues of particle agglomeration,carbon layer breakage,lithium loss,and Fe3+defects in spent LiFePO4 are also addressed.Results show that Mg2+addition during regeneration can remarkably enhance the crystal structure stability and improve the Li+diffusion coefficient.The regenerated LiFePO4 exhibits significantly improved electrochemical performance with a specific discharge capacity of 143.2 mAh·g^(−1)at 0.2 C,and its capacity retention is extremely increased from 37.9%to 98.5%over 200 cycles at 1 C.Especially,its discharge capacity can reach 95.5 mAh·g^(−1)at 10 C,which is higher than that of spent LiFePO4(55.9 mAh·g^(−1)).All these results show that the proposed regeneration strategy of simultaneous carbon coating and Mg2+doping is suitable for the efficient treatment of spent LiFePO4.

关键词： spent LiFePO4 solid-phase reduction repair and regeneration cathode materials lithium-ion batteries

Building Better Full Manganese‑Based cathode materialsfor Next‑Generation Lithium‑Ion Batteries

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Electrochemical Energy Reviews 2023年第1期6卷 148-185页

作者： Jin Song Hangchao Wang Yuxuan Zuo Kun Zhang Tonghuan Yang Yali Yang Chuan Gao Tao Chen Guang Feng Zewen Jiang Wukun Xiao Tie Luo Dingguo Xia Beijing Key Laboratory of Theory and Technology for Advanced Battery materials School of Materials Science and EngineeringPeking UniversityBeijing 100871China College of Chemistry and Molecular Science Wuhan UniversityWuhan 430072HubeiChina College of Engineering Peking UniversityBeijing 100871China

Lithium-manganese-oxides have been exploited as promising cathode materials for many years due to their environmental friendliness,resource abundance and low biotoxicity.Nevertheless,inevitable problems,such as Jahn-Teller distortion,manganese dissolution and phase transition,still frustrate researchers;thus,progress in full manganese-based cathode materials(FMCMs)has been relatively slow and limited in recent decades.Recently,with the fast growth of vehicle electrification and large-scale energy-storage grids,there has been an urgent demand to develop novel FMCMs again;actually,new waves of research based on FMCMs are being created.Herein,we systematically review the history of FMCMs,correctly describe their structures,evaluate the advantages and challenges,and discuss the resolution strategies and latest developments.Additionally,beyond FMCMs,a profound discussion of current controversial issues,such as oxygen redox reaction,voltage decay and voltage hysteresis in Li_(2)MnO_(3)-based cathode materials,is also presented.This review summarizes the effectively optimized approaches and offers a few new possible enhancement methods from the perspective of the electronic-coordination-crystal structure for building better FMCMs for next-generation lithium-ion batteries.

关键词： Energy storage Lithium-ion batteries cathode materials Manganese oxides

Precisely quantifying bulk transition metal valence evolution in conventional battery electrode by inverse partial fluorescence yield

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Journal of Energy Chemistry 2022年第6期31卷 363-368,I0010页

作者： Kehua Dai Weiwei Shao Beibei Zhao Wenjuan Zhang Yan Feng Wenfeng Mao Guo Ai Gao Liu Jing Mao Wanli Yang College of Chemistry Tianjin Normal UniversityTianjin 300387China Advanced Light Source Lawrence Berkeley National LaboratoryBerkeleyCA 94720United States College of Physics and materials Science Tianjin Normal UniversityTianjin 300387China Energy Storage and Distributed Resources Division Energy Technologies AreaLawrence Berkeley National LaboratoryBerkeleyCA 94720United States School of materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina

Precisely quantifying transition metal(TM) redox in bulk is a key to understand the fundamental of optimizing cathode materials in secondary batteries. At present, the commonly used methods to probe TM redox are hard X-ray absorption spectroscopy(hXAS) and soft X-ray absorption spectroscopy(sXAS).However, they are both facing challenges to precisely quantify the valence states of some transition metals such as Mn. In this paper, Mn-L iPFY(inverse partial fluorescence yield) spectra extracted from Mn-L m RIXS(mapping of resonant inelastic X-ray scattering) is adopted to quantify Mn valence states. Mn-L i PFY spectra has been considered as a bulk-sensitive, non-distorted probe of TM valence states.However, the exact precision of this method is still unclear in quantifying practical battery electrodes.Herein, a series of LiMn_(2)O_(4) electrodes with different charge and discharge states are prepared. Based on their electrochemical capacity(generally considered to be very precise), the precision of Mn iPFY in quantifying bulk Mn valence state is confirmed, and the error range is unraveled. Mn-L mRIXS iPFY thus is identified as one of the best methods to quantify the bulk Mn valence state comparing with hXAS and sXAS.

关键词： cathode materials Valence state of transition metals Lithium-ion batteries Mapping of resonant inelastic X-ray scattering Inverse partial fluorescence yield

Yolk-Shell P3-Type K_(0.5)[Mn_(0.85)Ni_(0.1)Co_(0.05)]O_(2):A Low-Cost cathode for Potassium-Ion Batteries

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Energy & Environmental materials 2022年第1期5卷 261-269页

作者： Jiaxin Hao Ke Xiong Jiang Zhou Apparao M.Rao Xianyou Wang Huan Liu Bingan Lu School of Physics and Electronics State Key Laboratory of Advanced Design and Manufacturing for Vehicle BodyHunan UniversityChangsha 410082China Key Laboratory of Environmentally Friendly Chemistry and Applications of Ministry of Education Hunan Province Key Laboratory of Electrochemical Energy Storage and ConversionSchool of ChemistryXiangtan UniversityXiangtan 411105China School of materials Science and Engineering Central South UniversityChangsha 410083China Department of Physics and Astronomy Clemson Nanomaterials InstituteClemson UniversityClemson SC 29634USA College of materials Science and Engineering Hunan University of Scienceand TechnologyXiangtan 411201China Fujian Strait Research Institute of Industrial Graphene Technologies Quanzhou 362000China

Low-cost preparation methods for cathodes with high capacity and long cycle life are crucial for commercializing potassium-ion batteries(PIBs).Presently,the charging/discharging strain that develops in the active cathode material of PIBs causes cracks in the particles,leading to a sharp capacity fade.Here,to abate the strain release and the need for an industrially relevant process,a simple low-cost co-precipitation method for synthesizing yolk-shell P3-type K_(0.5)[Mn_(0.85)Ni_(0.1)Co_(0.05)]O_(2) (YS-KMNC)was reported.As cathode material for PIBs,the YS-KMNC delivers a high reversible capacity(96 mAh g^(-1) at 20 mA g^(-1))and excellent cycle stability(80.5%retention over 400 cycles at a high current density of 200 mA g^(-1)).More importantly,a full battery assembled with the YS-KMNC cathode and a commercial graphite anode exhibits a high operating voltage(0.5-3.4 V)and an excellent cycling performance(84.2%retention for 100 cycles at 100 mA g^(-1)).Considering the low-cost,simple production process and high performance of YS-KMNC cathode,this work could pave the way for the commercial development of PIBs.

关键词： cathode materials K_(0.5)[Mn_(0.85)Ni_(0.1)Co_(0.05)]O_(2) strain release volume expansion yolk-shell structure