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Alleviating the anisotropic microstructural change and boosting the lithium ions diffusion by grain orientation regulation for Ni-rich cathode materials

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Journal of Energy Chemistry 2024年第1期88卷 213-222,I0005页

作者： Xinyou He Shilin Su bao zhang Zhiming Xiao Zibo zhang Xing Ou Engineering Research Center of the Ministry of Education for Advanced Battery Materials School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083HunanChina Zhejiang Power New Energy Co.Ltd Zhuji 311899ZhejiangChina

Generally,layered Ni-rich cathode materials exhibit the morphology of polycrystalline secondary sphere composed of numerous primary particles.While the arrangement of primary particles plays a very important role in the properties of Ni-rich cathodes.The disordered particle arrangement is harmful to the cyclic performance and structural stability,yet the fundamental understanding of disordered structure on the structural degradation behavior is unclarified.Herein,we have designed three kinds of LiNi_(0.83)Co_(0.06)Mn_(0.11)O_(2) cathode materials with different primary particle orientations by regulating the precursor coprecipitation process.Combining finite element simulation and in-situ characterization,the Li^(+)transport and structure evolution behaviors of different materials are unraveled.Specifically,the smooth Li^(+)diffusion minimizes the reaction heterogeneity,homogenizes the phase transition within grains,and mitigates the anisotropic microstructural change,thereby modulating the crack evolution behavior.Meanwhile,the optimized structure evolution ensures radial tight junctions of the primary particles,enabling enhanced Li^(+)diffusion during dynamic processes.Closed-loop bidirectional enhancement mechanism becomes critical for grain orientation regulation to stabilize the cyclic performance.This precursor engineering with particle orientation regulation provides the useful guidance for the structural design and feature enhancement of Ni-rich layered cathodes.

关键词： Ni-rich cathode Grain orientation regulation Anisotropic microstructural change Precursor engineering Li~+-ions diffusion

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A Li_(3)P nanoparticle dispersion strengthened ultrathin Li metal electrode for high energy density rechargeable batteries

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Nano Research 2024年第5期17卷 4031-4038页

作者： Lin Fu Xiancheng Wang bao zhang Zihe Chen Yuanjian Li Yongming Sun Provincial Guizhou Key Laboratory of Green Chemical and Clean Energy Technology School of Chemistry and Chemical EngineeringGuizhou UniversityGuiyang 550025China Wuhan National Laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074China School of Physical and Mathematical Sciences Nanyang Technological UniversitySingapore 637371Singapore Institute of Materials Research and Engineering Agency for Science Technology and Research(A*STAR)Singapore 138634Singapore

Achievement of lithium(Li)metal anode with thin thickness(e.g.,≤30µm)is highly desirable for rechargeable high energy density batteries.However,the fabrication and application of such thin Li metal foil electrode remain challenging due to the poor mechanical processibility and inferior electrochemical performance of metallic Li.Here,mechanico-chemical synthesis of robust ultrathin Li/Li_(3)P(LLP)composite foils(~15µm)is demonstrated by employing repeated mechanical rolling/stacking operations using red P and metallic Li as raw materials.The in-situ formed Li+-conductive Li_(3)P nanoparticles in metallic Li matrix and their tight bonding strengthen the mechanical durability and enable the successful fabrication of free-standing ultrathin Li metal composite foil.Besides,it also reduces the electrochemical Li nucleation barrier and homogenizes Li plating/stripping behavior.When matching to high-voltage LiCoO_(2),the full cell with a low negative/positive(N/P)capacity ratio of~1.5 offers a high energy density of~522 W·h·kg^(-1) at 0.5 C based on the mass of cathode and anode.Taking into account its facile manufacturing,potentially low cost,and good electrochemical performance,we believe that such an ultrathin composite Li metal foil design with nanoparticle-dispersion-strengthened mechanism may boost the development of high energy density Li metal batteries.

关键词： lithium metal anode high energy density battery mechanico-chemical synthesis ultrathin Li/Li_(3)P composite foil low negative/positive capacity ratio

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Understanding the failure mechanism towards developing high-voltage single-crystal Ni-rich Co-free cathodes

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Green Energy & Environment 2024年第6期9卷 1045-1057页

作者： Jixue Shen bao zhang Changwang Hao Xiao Li Zhiming Xiao Xinyou He Xing Ou Engineering Research Center of the Ministry of Education for Advanced Battery Materials School of Metallurgy and EnvironmentCentral South UniversityChangsha410083China Zhejiang Power New Energy Co. Ltd.Zhuji311899China Material Science and Chemistry Engineering College China University of GeosciencesWuhan430074China

Benefited from its high process feasibility and controllable costs,binary-metal layered structured LiNi_(0.8)Mn_(0.2)O_(2)(NM)can effectively alleviate the cobalt supply crisis under the surge of global electric vehicles(EVs)sales,which is considered as the most promising nextgeneration cathode material for lithium-ion batteries(LIBs).However,the lack of deep understanding on the failure mechanism of NM has seriously hindered its application,especially under the harsh condition of high-voltage without sacrifices of reversible capacity.Herein,singlecrystal LiNi_(0.8)Mn_(0.2)O_(2) is selected and compared with traditional LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM),mainly focusing on the failure mechanism of Cofree cathode and illuminating the significant effect of Co element on the Li/Ni antisite defect and dynamic characteristic.Specifically,the presence of high Li/Ni antisite defect in NM cathode easily results in the extremely dramatic H2/H3 phase transition,which exacerbates the distortion of the lattice,mechanical strain changes and exhibits poor electrochemical performance,especially under the high cutoff voltage.Furthermore,the reaction kinetic of NM is impaired due to the absence of Co element,especially at the single-crystal architecture.Whereas,the negative influence of Li/Ni antisite defect is controllable at low current densities,owing to the attenuated polarization.Notably,Co-free NM can exhibit better safety performance than that of NCM cathode.These findings are beneficial for understanding the fundamental reaction mechanism of single-crystal Ni-rich Co-free cathode materials,providing new insights and great encouragements to design and develop the next generation of LIBs with low-cost and high-safety performances.

关键词： Li/Ni antisite defect Dynamic characteristic High-voltage Single-crystal Ni-rich Co-free cathodes Lithium-ion batteries

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Degradation analysis and doping modification optimization for high-voltage P-type layered cathode in sodium-ion batteries

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Journal of Energy Chemistry 2024年第2期89卷 1-9,I0002页

作者： bao zhang Yi Zhao Minghuang Li Qi Wang Lei Cheng Lei Ming Xing Ou Xiaowei Wang National Engineering Laboratory for High-Efficiency Recovery of Refractory Nonferrous Metals School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083HunanChina Zhejiang Power New Energy Co. LTDZhuji 311800ZhejiangChina

Advancing high-voltage stability of layered sodium-ion oxides represents a pivotal avenue for their progress in energy storage applications.Despite this,a comprehensive understanding of the mechanisms underpinning their structural deterioration at elevated voltages remains insufficiently explored.In this study,we unveil a layer delamination phenomenon of Na_(0.67)Ni_(0.3)Mn_(0.7)O_(2)(NNM)within the 2.0-4.3 V voltage,attributed to considerable volumetric fluctuations along the c-axis and lattice oxygen reactions induced by the simultaneous Ni^(3+)/Ni^(4+)and anion redox reactions.By introducing Mg doping to diminished Ni-O antibonding,the anion oxidation-reduction reactions are effectively mitigated,and the structural integrity of the P2 phase remains firmly intact,safeguarding active sites and precluding the formation of novel interfaces.The Na_(0.67)Mg_(0.05)Ni_(0.25)Mn_(0.7)O_(2)(NMNM-5)exhibits a specific capacity of100.7 mA h g^(-1),signifying an 83%improvement compared to the NNM material within the voltage of2.0-4.3 V.This investigation underscores the intricate interplay between high-voltage stability and structural degradation mechanisms in layered sodium-ion oxides.

关键词： Soidum ion batteries Layer cathode materials P-type High-voltage performance Degradation analysis

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Recycling of spent lithium-ion batteries to resynthesize high-performance cathode materials for sodium-ion storage

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Tungsten 2024年第3期6卷 574-584页

作者： Hai-Qiang Gong Xing-Yuan Wang Long Ye bao zhang Xing Ou National Engineering Laboratory for High-Efficiency Recovery of Refractory Nonferrous Metals School of Metallurgy and Environment Central South University

The spent lithium-ion batteries recovery has been brought into focus widely for its environmental imperatives and potential profits from the metal components,such as lithium,cobalt,nickel and manganese.However,the weaker pollution and fewer profits of LiMn2O4cathode dispel the enthusiasm and responsibility of industry companies.Thus,a simplified and efncient method to regenerate the sodium-ion cathode materials and separate Li from spent LiMn2O4materials for the profit improvement is proposed.In detail,adjusting the parameters of carbothermal reduction process appropriately,the LiMn2O4spinel structure is destroyed within a short period time and transformed into simple metal oxide.As anticipated,nearly 95 wt.%lithium can be obtained and recovered during the water leaching,while 99 wt.% of manganese can be extracted in acid solution.Noted that the leaching residue can return to the carbothermic reduction,leading to a closed-loop economic recycling process.The regenerated Na0.67Ni0.3Mn0.7O2cathode displays excellent electrochemical performance with superior cycling stability(the initial capacity reaches 95.9 mAh·g-1,and the retention rate reached 98.3% after 100 cycles at 1 C).The delicate strategy of sodium-ion cathode material regenerated from spent LiMn2O4aims to realize lithium separation and material utilization of manganese simultaneously,providing the instructive suggestion to rise up the recycling profits of spent batteries.

关键词： Manganese Spent battery LiMn 2 O 4 cathode Recycling Regenerated Na 0.67 Ni 0.3 Mn 0.7 O 2 Sodium-ion storage

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Graphite recycling from spent lithium-ion batteries for fabrication of high-performance aluminum-ion batteries

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Rare Metals 2024年第5期43卷 2161-2171页

作者： Li Wang Chao Wang Jing-Yi zhang Jia-Cheng Qiu Xu-Wang Fu Zi-Rui zhang Jian-Min Feng Lei Dong Cong-Lai Long De-Jun Li Xiao-Wei Wang bao zhang Jia-Feng zhang Rui-Rui Zhao College of Physics and Materials Science Tianjin Normal University National Engineering Laboratory for High Efficiency Recovery of Refractory Nonferrous Metals School of Metallurgy and Environment Central South University School of Chemistry South China Normal University

Efficient extraction of electrode components from recycled lithium-ion batteries （LIBs） and their highvalue applications are critical for the sustainable and ecofriendly utilization of resources.This work demonstrates a novel approach to stripping graphite anodes embedded with Li+from spent LIBs directly in anhydrous ethanol which can be utilized as high efficiency cathodes for aluminum-ion batteries （AIBs）.Recycled graphite （RG） with foam morphology and crystal structure defects was obtained under the action of ultrasonic peeling and gas generation reaction between residual lithium-graphite interlayer compound and ethanol.The inherent open structure of RG facilitates the intercalation/deintercalation of chloralum anions （AlCl4-） and enhances its AIB cathode performance.The electrochemical measurements revea that the RG cathode has a specific capacity of 123 m Ah·g-1at a current of 5 A·g-1,which is 1.55 times higher than tha of unprocessed natural graphite and 1.25 times higher than that of commercial artificial graphite.Additionally,the RG cathode demonstrated remarkable stability,retaining its high particular capacity of 138.15 mAh·g-1even through2000 times at 10 A·g-1in a low-cost electrolyte consisting of an ionic liquid/urea/AlCl3mixture.This work offers a novel approach to reusing of graphite anode waste materials from LIBs.

关键词： Aluminum ion batteries Lithium-ion batteries Graphite anode Recycling

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Critical Solvation Structures Arrested Active Molecules for Reversible Zn Electrochemistry

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Nano-Micro Letters 2024年第8期16卷 64-78页

作者： Junjie Zheng bao zhang Xin Chen Wenyu Hao Jia Yao Jingying Li Yi Gan Xiaofang Wang Xingtai Liu Ziang Wu Youwei Liu Lin Lv Li Tao Pei Liang Xiao Ji Hao Wang Houzhao Wan Hubei Yangtze Memory Laboratories Wuhan 430205People’s Republic of China Hubei Key Laboratory of Micro‑Nanoelectronic Materials and Devices School of MicroelectronicsHubei UniversityWuhan 430062People’s Republic of China School of Physical and Mathematical Sciences Nanyang Technological UniversitySingapore 637371Singapore School of Optical and Electronic Information Huazhong University of Science and TechnologyWuhan 430074People’s Republic of China Institute of Optoelectronics Technology China Jiliang UniversityHangzhou 310018People’s Republic of China

Aqueous Zn-ion batteries(AZIBs)have attracted increasing attention in next-generation energy storage systems due to their high safety and economic.Unfortunately,the side reactions,dendrites and hydrogen evolution effects at the zinc anode interface in aqueous electrolytes seriously hinder the application of aqueous zinc-ion batteries.Here,we report a critical solvation strategy to achieve reversible zinc electrochemistry by introducing a small polar molecule acetonitrile to form a“catcher”to arrest active molecules(bound water molecules).The stable solvation structure of[Zn(H_(2)O)_(6)]^(2+)is capable of maintaining and completely inhibiting free water molecules.When[Zn(H_(2)O)_(6)]^(2+)is partially desolvated in the Helmholtz outer layer,the separated active molecules will be arrested by the“catcher”formed by the strong hydrogen bond N-H bond,ensuring the stable desolvation of Zn^(2+).The Zn||Zn symmetric battery can stably cycle for 2250 h at 1 mAh cm^(-2),Zn||V_(6)O_(13) full battery achieved a capacity retention rate of 99.2%after 10,000 cycles at 10 A g^(-1).This paper proposes a novel critical solvation strategy that paves the route for the construction of high-performance AZIBs.

关键词： Zinc-ion battery Critical solvation Helmholtz layer Arrest active molecule Reversible zinc anode

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Key technology and application of AB_(2) hydrogen storage alloy in fuel cell hydrogen supply system

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Materials Reports(Energy) 2024年第1期4卷 113-122页

作者： Ming Yao Jianguang Yuan bao zhang Youhua Yan Shaoxiong Zhou Ying Wu School of Energy Power and Machinery Engineering North China Electric Power UniversityNo.2 BeinongluChangping DistrictBeijing 102206China Institute of Energy Power Innovation North China Electric Power UniversityNo.2 BeinongluChangping DistrictBeijing 102206China Jiangsu JITRI Advanced Energy&Materials Research Institute Co. LtdNo.5 ChongyinanluXinbei DistrictChangzhou 213000China

At present,there is limited research on the application of fuel cell power generation system technology using solid hydrogen storage materials,especially in hydrogen-assisted two-wheelers.Considering the disadvantages of low hydrogen storage capacity and poor kinetics of hydrogen storage materials,our primary focus is to achieve smooth hydrogen ab-/desorption over a wide temperature range to meet the requirements of fuel cells and their integrated power generation systems.In this paper,the Ti_(0.9)Zr_(0.1)Mn_(1.45)V_(0.4)Fe_(0.15) hydrogen storage alloy was successfully prepared by arc melting.The maximum hydrogen storage capacity reaches 1.89 wt% at 318 K.The alloy has the capability to absorb 90% of hydrogen storage capacity within 50 s at 7 MPa and release 90% of hydrogen within 220 s.Comsol Multiphysics 6.0 software was used to simulate the hydrogen ab-/desorption processes of the tank.The flow rate of cooling water during hydrogen absorption varied in a gradient of(0.02 t x)m s^(-1)(x=0,0.02,0.04,0.06,0.08,0.1,0.12).Cooling water flow rate is positively correlated with the hydrogen absorption rate but negatively correlated with the cost.When the cooling rate is 0.06 m s^(-1),both simulation and experimentation have shown that the hydrogen storage tank is capable of steady hydrogen desorption for over 6 h at a flow rate of 2 L min^(-1).Based on the above conclusions,we have successfully developed a hydrogen-assisted two-wheeler with a range of 80 km and achieved regional demonstration operations in Changzhou and Shaoguan.This paper highlights the achievements of our team in the technological development of fuel cell power generation systems using solid hydrogen storage materials as hydrogen storage carriers and their application in twowheelers in recent years.

关键词： AB_(2)hydrogen storage alloy Hydrogen storage tanks Simulation Hydrogen-electric coupling system Power-assisted two-wheelers

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A tunable ionic covalent organic framework platform for efficient CO_(2) catalytic conversion

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Frontiers of Chemical Science and Engineering 2024年第1期18卷 25-36页

作者： Ting Li Ji Xiong Minghui Chen Quan Shi Xiangyu Li Yu Jiang Yaqing Feng bao zhang School of Chemical Engineering and Technology Tianjin UniversityTianjin 300350China Guangdong Laboratory of Chemistry and Fine Chemical Industry Jieyang Center Jieyang 522000China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

The cycloaddition reaction between epoxides and CO_(2) is an effective method to utilize CO_(2) resource.Covalent organic frameworks(COFs)provide a promising platform for the catalytic CO_(2) transformations on account of their remarkable chemical and physical properties.Herein,a family of novel vinylene-linked ionic COFs named TE-COFs(TTE-COF,TME-COF,TPE-COF,TBE-COF)has been facilely synthesized from N-ethyl2,4,6-trimethylpyridinium bromide and a series of triphenyl aromatic aldehydes involving different numbers of nitrogen atoms in the central aromatic ring.The resulting catalyst TTE-COF with excellent adsorption capacity(45.6 cm3·g^(-1),273 K)exhibited outstanding catalytic performance,remarkable recyclability and great substrate tolerance.Moreover,it was also observed that the introduction of nitrogen atom in the precursor led to a great improvement in the crystallinity and CO_(2) adsorption capacity of TE-COFs,thus resulting to a progressively improved catalytic performance.This work not only illustrated the influence of monomer nitrogen content on the crystallinity and CO_(2) adsorption capacity of TE-COFs but also provided a green heterogeneous candidate for catalyzing the cycloaddition between CO_(2) and epoxides,which shed a light on improving the catalytic performance of the CO_(2) cycloaddition reaction by designing the covalent organic frameworks structures.

关键词： CO_(2)cycloaddition nreaction covalent organic frameworks cyclic carbonate vinylene-linked synergetic effects

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Testing Linearity in Functional Partially Linear Models

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Acta Mathematicae Applicatae Sinica 2024年第3期40卷 875-886页

作者： Fan-rong ZHAO bao-xue zhang School of Mathematical Sciences Shanxi UniversityTaiyuan 030006China School of Statistics Capital University of Economics and BusinessBeijing 100070China

For the functional partially linear models including flexible nonparametric part and functional linear part,the estimators of the nonlinear function and the slope function have been studied in existing literature.How to test the correlation between response and explanatory variables,however,still seems to be missing.Therefore,a test procedure for testing the linearity in the functional partially linear models will be proposed in this paper.A test statistic is constructed based on the existing estimators of the nonlinear and the slope functions.Further,we prove that the approximately asymptotic distribution of the proposed statistic is a chi-squared distribution under some regularity conditions.Finally,some simulation studies and a real data application are presented to demonstrate the performance of the proposed test statistic.

关键词： asymptotic theory functional partially linear model Nadaraya-Watson estimate test statistic

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