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Leaching kinetics of fluorine during the aluminum removal from spent li-ion battery cathode materials

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Journal of Environmental Sciences 2024年第4期138卷 312-325页

作者： Shengjie li Jianxin Zhu Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China

The high content of aluminum(Al)impurity in the recycled cathode powder seriously affects the extraction efficiency of Nickel,Cobalt,Manganese,and lithium resources and the actual commercial value of recycled materials,so Al removal is crucially important to conform to the industrial standard of spent li-ion battery cathode *** this work,we systematically investigated the leaching process and optimum conditions associated with Al removal from the cathode powder materials collected in a wet cathode-powder peeling and recycling production line of spent li-ion batteries(liBs).Moreover,we specifically studied the leaching of fluorine(F)synergistically happened along with the removal process of Al,which was not concerned about in other studies,but one of the key factors affecting pollution prevention in the recovery *** mechanism of the whole process including the leaching of Al and F from the cathode powder was indicated by using NMR,FTIR,and XPS,and a defluoridation process was preliminarily investigated in this *** leaching kinetics of Al could be successfully described by the shrinking core model,controlled by the diffusion process and the activation energy was 11.14 kJ/***,the leaching of F was attributed to the dissolution of liPF6and decomposition of PVDF,and the kinetics associated was described by Avrami *** interaction of Al and F is advantageous to realize the defluoridation to some *** is expected that our investigation will provide theoretical support for the large-scale recycling of spent liBs.

关键词： Al removal F leaching Cathode powder Heating alkali leaching Leaching kinetics

Additives strategies to improving cycling stability of li metal batteries by modifying electrode electrolyte interphases

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Progress in Natural Science:Materials International 2024年第2期34卷 338-344页

作者： Yuan li Pengfei Huang Chunyu Cui Xiaoyuan Ma li Chen Zekun li linhai li Yuhong Tian School of Biological and Chemical Engineering Guangxi University of Science and Technology School of College of Chemistry and Chemical Engineering Hunan University Isky Future Energy Institute

li metal batteries（LMBs） have attracted much attention due to the ultra-high theoretical capacity of the li metal anode（LMA）.However,the uncontrollable dendrites growth and low coulombic efficiency hinder their practical ***,we explore 3,5-difluoropyridine（2F-BD） as a novel electrolyte additive to enable highperformance *** 2F-BD additive participates in and modifies the solvation structure of li ions by reducing the coordinated number of PF6-at the electrode surface,leading to the formation of a liF and li3N-rich solid electrolyte interphase（SEI）.The liF component increases the robustness of SEI and suppresses the formation of li dendrites,while the li3N component facilitates the transportation and reaction kinetics of li *** a result,the li‖li symmetric cell presents a stable cycling performance of up to 500 h at a current density of 1 mA *** coupling with liFePO4cathode,the obtained full cell achieves high specific capacities of 106.06 mA h g-1and 84.98 mA h g-1at 2.55 mA cm-2and 5.10 mA cm-2,respectively,and maintains a high capacity retention of84.0% after 1000 cycles at 0.13 mA cm-2,with an average cycling CE of 99.58%.

关键词： Electrolyte additive li dendrites li metal batteries liF and li3N-Rich electrode-electrolyte interphase liFePO4 cathode

SEI/dead li-turning capacity loss for high-performance anode-free solid-state lithium batteries

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Journal of Energy Chemistry 2024年第9期96卷 145-152页

作者： Qianwen Yin Tianyu li Hongzhang Zhang Guiming Zhong Xiaofei Yang Xianfeng li Division of Energy Storage Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Key Laboratory of Long-Duration and Large-Scale Energy Storage Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Laboratory of Advanced Spectro-Electrochemistry and lithium-Ion Batteries Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

Anode-free solid-state lithium metal batteries(AF-SSLBs)have the potential to deliver higher energy density and improved safety beyond lithium-metal ***,the unclear mechanism for the fast capacity decay in AF-SSLBs,either determined by dead li or solid electrolyte interface(SEI),limits the proposal of effective strategies to prolong cycling *** clarify the underlying mechanism,herein,the evolution of SEI and dead li is quantitatively analyzed by a solid-state nuclear magnetic resonance(ss-NMR)technology in a typical liPF6-based polymer *** results show that the initial capacity loss is attributed to the formation of SEI,while the dead li dominates the following capacity loss and the growth rate is 0.141 mA h cm^(−2)cycle−*** reduce the active li loss,the combination of inorganic-rich SEI and self-healing electrostatic shield effect is proposed to improve the reversibility of li deposition/dissolution behavior,which reduces the capacity loss rate for the initial SEI and following dead li generation by 2.3 and 20.1 folds,*** a result,the initial Coulombic efficiency(ICE)and stable CE increase by 15.1%and 15.3%in li-Cu cells,which guides the rational design of high-performance AF-SSLBs.

关键词： Solid-state lithium batteries Solid-state NMR Anode-free SEI Dead li

Synergy effect of regulated li-plating and functional solid electrolyte interphase on graphite anodes

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Nano Research 2024年第9期17卷 8077-8085页

作者： Panpan Wang Baojia Xia Jianling li State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China Shanghai Institute of Microsystem and Information Technology Chinese Academy of SciencesShanghai 201800China

The growth of li dendrites poses potential safety hazard to lithium-ion batteries(liBs),and eliminating li dendrites thoroughly stills face tough difficulties ***,regulating li-plating is a critical optimization-direction to address the ***,a“graphite-li hybrid”anode with high reversibility is realized under the constant-capacity lithiation(CCL).Within CCL,the uniform distribution of li-plating on the graphite surface is successfully *** evolution in different states of solid electrolyte interphase(SEI)is investigated in detail to study the interaction between the potentials and impedance during the process of liintercalation and *** the potential below 0 V and the state of charge(SOC)of 110%relative to the theoretical capacity,the F-rich SEI with high stability is constructed to hinder the emergency of li dendrites and maintain the intact structure of graphite anode under long *** cell presents more than 100%Coulombic efficiency(CE)with the 900 cycles,demonstrating the reversible li-plating and the utilization of *** the CCL half-cell provides a good cycling performance and specific capacity of 900 cycles at 0.5 C,it is attributed to the synergy effect of stable inorganic-rich SEI and regulated active li-plating.

关键词： "graphite-li hybrid"anode li-plating reversibility solid electrolyte interphase(SEI)

Highly-chlorinated inert and robust interphase without mineralization of oxide enhancing high-rate li metal batteries

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Chinese Chemical Letters 2024年第6期35卷 239-243页

作者： Long li Kang Yang Chenpeng Xi Mengchao li Borong li Gui Xu Yuanbin Xiao Xiancai Cui Zhiliang liu lingyun li Yan Yu Chengkai Yang Key Laboratory of Advanced Materials Technologies International(HongKong Macao and Taiwan)Joint Laboratory on Advanced Materials TechnologiesSchool of Materials Science and EngineeringFuzhou UniversityFuzhou 350108China College of Material Sciences and Chemical Engineering Harbin Engineering UniversityHarbin 150001China

Side reactions and dendrite growth triggered by the unstable interface and inhomogeneous deposition have become the biggest obstacle to the commercialization for lithium metal *** this study,a highly-chlorinated organic-inorganic hybrid interfacial protective layer is developed by rationally tuning the interfacial passivation and robustness to achieve the convenient and efficient li metal *** polyvinyl chloride(PVC)can effectively resist water and oxygen,which is confirmed by density functional *** organic-dominant solid electrolyte interphases(SEI)with lithium chloride are investigated by the X-ray photoelectron spectroscopy(XPS)with little mineralization of oxide,such as li_(2)O and li_(2)CO_(3).With such artificial SEI,a uniform and dense lithium deposition morphology are formed and an ultra-long stable cycle of over 500 h are achieved even at an ultra-high current density of 10 m A/cm^(2).Moreover,the simple and convenient protected anode also exhibits excellent battery stability when paired with the liNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)and liFePO_(4)(LFP)cathode,showing great potential for the commercial application of lithium metal batteries.

关键词： Highly-chlorinated Water/oxygen resistance Stable interphase Dendrite-free lithium metal batteries High-rate

Accelerating lithium-sulfur battery reaction kinetics and inducing 3D deposition of li_(2)S using interactions between Fe_(3)Se_(4)and lithium polysulfides

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Journal of Energy Chemistry 2024年第8期95卷 540-553,I0012页

作者： Yihan lin liheng li Longjie Tan Yongliang li Xiangzhong Ren Peixin Zhang Chuanxin He lingna Sun College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060GuangdongChina

Although lithium-sulfur batteries(LSBs)exhibit high theoretical energy density,their practical application is hindered by poor conductivity of the sulfur cathode,the shuttle effect,and the irreversible deposition of li_(2)*** address these issues,a novel composite,using electrospinning technology,consisting of Fe_(3)Se_(4)and porous nitrogen-doped carbon nanofibers was designed for the interlayer of *** porous carbon nanofiber structure facilitates the transport of ions and electrons,while the Fe_(3)Se_(4)material adsorbs lithium polysulfides(liPSs)and accelerates its catalytic conversion ***,the Fe_(3)Se_(4)material interacts with soluble liPSs to generate a new polysulfide intermediate,li_(x)FeS_(y)complex,which changes the electrochemical reaction pathway and facilitates the three-dimensional deposition of li_(2)S,enhancing the reversibility of *** designed LSB demonstrates a high specific capacity of1529.6 mA h g^(-1)in the first cycle at 0.2 *** rate performance is also excellent,maintaining an ultra-high specific capacity of 779.7 mA h g^(-1)at a high rate of 8 *** investigation explores the mechanism of the interaction between the interlayer and liPSs,and provides a new strategy to regulate the reaction kinetics and li_(2)S deposition in LSBs.

关键词： lithium-sulfur batteries Polysulfide intermediates li_(2)S electrodeposition Interlayers Electrostatic spinning Adsorption Catalysis

Theoretical Design of Defects as a Driving Force for Ion Transport in li3OBr Solid Electrolyte

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Energy & Environmental Materials 2024年第3期7卷 147-157页

作者： Xingyun Luo Yanlu li Xian Zhao State Key Lab of Crystal Materials and Institute of Crystal Materials Shandong University Center for Optics Research and Engineering Shandong University

Due to ever-increasing concerns about safety issues in using li ionic batteries,solid electrolytes have extensively *** li-rich antiperovskite li3OBr has been considered as a promising solid electrolyte candidate,but it still suffers challenges to achieve a high ionic conductivity owing to the high intrinsic symmetry of the crystal ***,we presented a design strategy that introduces various point defects and grain boundaries to break the high lattice symmetry of li3OBr crystal,and their effect and microscopic mechanism of promoting the migration of li-ion were explored *** has been found that liiare the dominant defects responsible for the fast li-ion diffusion in bulk li3OBr and its surface,but they are easily trapped by the grain boundaries,leading to the annihilating of the Frenkel defect pair V'li+li,and thus limits the V'lidiffusion at the grain *** VBrdefect near the grain boundaries can effectively drive V'liacross the grain boundary,thereby converting the carrier of li+migration from li,in the bulk and surface to V'liat the grain boundary,and thus improving the ionic conductivity in the whole li3OBr *** work provides a comprehensive insight into the li+transport and conduction mechanism in the li3OBr *** opens a new way of improving the conductivity for all-solid-state li electrolyte material through the defect design.

关键词： defects density functional theory ionic migration solid electrolyte

Boosting the performance of liNi_(0.90)Co_(0.06)Mn_(0.04)O_(2) electrode by uniform li_(3)PO_(4) coating via atomic layer deposition

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Chinese Chemical Letters 2024年第5期35卷 499-503页

作者： Mingjiao Lu Zhixing Wang Gui Luo Huajun Guo Xinhai li Guochun Yan Qihou li Xianglin li Ding Wang Jiexi Wang School of Metallurgy and Environment Central South UniversityChangsha 410083China BASF ShanShan Battery Materials Co. Ltd.Changsha 410006China Engineering Research Center of the Ministry of Education for Advanced Battery Materials Central South UniversityChangsha 410083China Hunan Provincial Key Laboratory of Nonferrous Value-Added Metallurgy Central South UniversityChangsha 410083China School of Physics and Chemistry Hunan First Normal UniversityChangsha 410205China National and Local Joint Engineering Laboratory for lithium-ion Batteries and Materials Preparation Technology Key Laboratory of Advanced Battery Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093China

Ultra-high nickel material is considered to be a promising cathode ***,with the increase of nickel content,the interfacial side reactions between the cathode and electrolyte become increasingly ***,an atomically controllable ionic conductor li_(3)PO_(4)(LPO)coating is deposited on the liNi_(0.90)Co_(0.06)Mn_(0.04)O_(2)(NCM9064)based electrode by the atomic layer deposition *** results shows that the LPO coating is uniformly and densely covered on the surface of secondary particles of NCM9064,helping to prevent the direct contact between the electrolyte and cathode during the chargingdischarging *** addition,the coating layer is electrochemically *** a result,the interfacial side reactions during the long cycle are effectively suppressed,and the solid electrolyte interphase layer at the interface is *** electrode with 20 layers of LPO deposition(ALD-LPO-20)exhibits an excellent capacity retention of 81%after 200 cycles in 2.8-4.3 V at 25℃,which is 18%higher than the unmodified material(ALD-LPO-0).Besides,the moderate LPO coating improves the rate capability and high temperature cycling performance of *** study provides a method for the modification of ultra-high nickel cathode materials and corresponding electrodes.

关键词： Ultra-high nickel material liNi_(0.90)Co_(0.06)Mn_(0.04)O_(2) Atomic layer deposition li_(3)PO_(4) Ionic conductor

Layered niobium carbide enabling excellent kinetics and cycling stability of li-Mg-B-H hydrogen storage material Layered niobium carbide enabling excellent kinetics

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Rare Metals 2024年第3期43卷 1153-1166页

作者： li-Wen Lu Hui Luo Guang-Xu li Yun li Xin-Hua Wang Cun-Ke Huang Zhi-QiangLan Wen-Zheng Zhou Jin Guo Mohammad Ismail Hai-Zhen liu Guangxi Novel Battery Materials Research Center of Engineering Technology Guangxi Colleges and Universities Key Laboratory of Blue Energy and Systems IntegrationSchool of Physical Science and TechnologyGuangxi UniversityNanning530004China State Key Laboratory of Featured Metal Materials and life-Cycle Safety for Composite Structures Nanning530004China School of Mechanical and Electrical Engineering Quzhou College of TechnologyQuzhou324000China Department of Materials Science and Engineering Zhejiang UniversityHangzhou310027China Faculty of Ocean Engineering Technology and Informatics Universiti Malaysia Terengganu21030Kuala NerusTerengganuMalaysia Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin300071China

The li-Mg-B-H composite(2liBH_(4)+MgH_(2))has a high capacity of 11.4 wt%as a hydrogen storage ***,the slow kinetics and poor cycling stability severely restrict its practical *** this work,a layered Nb_(2)C MXene was first synthesized and then introduced to tailor the kinetics and cycling stability of the li-Mg-B-H *** milled 2liH+MgB_(2)composites were initially hydrogenated to obtain the 2liBH_(4)+MgH_(2)*** 2liBH_(4)+MgH_(2)+5wt%Nb_(2)C can release 9.0 wt%H_(2)in 30 min at 400℃,while it is only 2.7 wt%for the undoped 2liBH_(4)+MgH_(2).The dehydrogenation activation energies of MgH_(2)and liBH_(4)are 123 and 154 kJ·mol^(-1)respectively for the 5 wt%Nb_(2)C-doped composite,lower than the undoped composite(164 and 165 kJ·mol^(-1)).The 2liBH_(4)+MgH_(2)+5 wt%Nb_(2)C possesses excellent cycling stability,with the reversible capacity only slightly reduced from 9.4 wt%for the 1st cycle to 9.3 wt%for the 20th ***_(2)C keeps stable in the composite and acts as an efficient catalyst for the li-Mg-B-H *** is believed that both the layered structure and the active Nb element contribu te to the enhanced hydrogen storage performances of the li-Mg-B-H *** work confirms that the Nb_(2)C MXene with layered stru cture has a significant enhancing impact on the li-Mg-B-H hydrogen storage materials,which is different from the bulk NbC.

关键词： Hydrogen storage lithium borohydride Magnesium hydride Nb_(2)C MXene