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

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 materials.In 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 process.The 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 study.The 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/mol.While,the leaching of F was attributed to the dissolution of liPF6and decomposition of PVDF,and the kinetics associated was described by Avrami model.The interaction of Al and F is advantageous to realize the defluoridation to some degree.It 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

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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 application.Here,we explore 3,5-difluoropyridine（2F-BD） as a novel electrolyte additive to enable highperformance LMBs.The 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 ions.As a result,the li‖li symmetric cell presents a stable cycling performance of up to 500 h at a current density of 1 mA cm-2.After 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

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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 batteries.In 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 anode.The polyvinyl chloride(PVC)can effectively resist water and oxygen,which is confirmed by density functional theory.The 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

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Accelerating lithium-sulfur battery reaction kinetics and inducing 3D deposition of li2S using interactions between Fe3Se4 and lithium polysulfides

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Journal of Energy Chemistry 2024年第8期95卷 540-553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 University

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 li2S.To address these issues,a novel composite,using electrospinning technology,consisting of Fe3Se4and porous nitrogen-doped carbon nanofibers was designed for the interlayer of LSBs.The porous carbon nanofiber structure facilitates the transport of ions and electrons,while the Fe3Se4material adsorbs lithium polysulfides（liPSs） and accelerates its catalytic conversion process.Furthermore,the Fe3Se4material interacts with soluble liPSs to generate a new polysulfide intermediate,lixFeSycomplex,which changes the electrochemical reaction pathway and facilitates the three-dimensional deposition of li2S,enhancing the reversibility of LSBs.The designed LSB demonstrates a high specific capacity of1529.6 mA h g-1in the first cycle at 0.2 C.The rate performance is also excellent,maintaining an ultra-high specific capacity of 779.7 mA h g-1at a high rate of 8 C.This investigation explores the mechanism of the interaction between the interlayer and liPSs,and provides a new strategy to regulate the reaction kinetics and li2S deposition in LSBs.

关键词： Adsorption Catalysis Electrostatic spinning Interlayers li2S electrodeposition lithium-sulfur batteries Polysulfide intermediates

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Ultrathin organic solvent nanofiltration membrane with polydopamine-HKUST-1 interlayer for organic solvent separation

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Journal of Environmental Sciences 2024年第7期141卷 182-193页

作者： Haike li Xindong li Guozai Ouyang lijinhong Huang Lang li Wenhao li Wanfu Huang Duokun li Ganzhou Key Laboratory of Basin Pollution Simulation and Control Jiangxi University of Science and TechnologyGanzhou 341000China Innovation Center for Water Quality Security Technology at Ganjiang River Basin Jiangxi University of Science and TechnologyGanzhou 341000China School of Architecture and Design Jiangxi University of Science and TechnologyGanzhou 341000China WA School of Mines:Minerals Energy and Chemical EngineeringCurtin UniversityWA 6845Australia School of Materials Science and Engineering Tiangong UniversityTianjin 300387China

Polydopamine(PDA)and metal-organic skeleton HKUST-1 were co-deposited on the base membrane of hexamethylenediamine(HDA)-crosslinked polyetherimide(PEI)ultrafiltration membrane as the interlayer,and high-throughput organic solvent nanofiltration membrane(OSN)was prepared by interfacial polymerization and solvent activation reaction.The polyamide(PA)layer surface roughness from 28.4 nm in PA/PEI to 78.3 nm in PA/PDA-HKUST-10.6/PEI membrane,reduced the thickness of the separation layer from 79 to 14 nm,and significantly improved the hydrophilic,thermal and mechanical properties.The flux of the PA/PDA-HKUST-10.6/PEI membrane in a 0.1 g/L Congo Red(CR)ethanol solution at 0.6 MPa test pressure reached 21.8 L/(m^(2)·hr)and the rejection of CR was 92.8%.Solvent adsorption test,N,N-dimethylformamide(DMF)immersion experiment,and long-term operation test in ethanol showed that the membranes had high solvent tolerance.The solvent flux test demonstrated that,under the test pressure of 0.6 MPa,the flux of different solvents ranked as follows:methanol(56.9 L/(m^(2)·hr))>DMF(39.6 L/(m^(2)·hr))>ethanol(31.2 L/(m^(2)·hr))>IPA(4.5 L/(m^(2)·hr))>N-hexane(1.9 L/(m^(2)·hr)).The ability of the membranes to retain dyes in IPA/water dyes solution was also evaluated.The flux of the membrane was 30.4 L/(m^(2)·hr)and the rejection of CR was 91.6%when the IPA concentration reached 50%.This OSN membrane-making strategy is economical,environment-friendly and efficient,and has a great application prospect in organic solvent separation systems.

关键词： Interfacial polymerization Organic solvent nanofiltration Interlayer Metal-organic frameworks Polydopamine

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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 material.However,with the increase of nickel content,the interfacial side reactions between the cathode and electrolyte become increasingly serious.Herein,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 method.The 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 process.In addition,the coating layer is electrochemically stable.As a result,the interfacial side reactions during the long cycle are effectively suppressed,and the solid electrolyte interphase layer at the interface is stabilized.The 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 NCM9064.This 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

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Micro-nanofiber composite biomimetic conduits promote long-gap peripheral nerve regeneration in canine models

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Bioactive Materials 2023年第12期30卷 98-115页

作者： Xianhao Dong Yueyue Yang Zheheng Bao Adam C.Midgley feiyi li Shuxin Dai Zhuangzhuang Yang Jin Wang lihua liu Wenlei li Yayuan Zheng Siyang liu Yang liu Weijian Yu Jun liu Meng Fan Meifeng Zhu Zhongyang Shen Gu Xiaosong Deling Kong State Key Laboratory of Medicinal Chemical Biology The Key Laboratory of Bioactive MaterialsMinistry of EducationCollege of Life ScienceNankai UniversityTianjinChina Department of Orthopaedics Tianjin First Central HospitalSchool of MedicineNankai UniversityTianjinChina Department of Radiology Tianjin First Central HospitalTianjin Medical Imaging InstituteSchool of MedicineNankai UniversityTianjinChina Institute of Transplantation Medicine NHC Key Laboratory for Critical Care MedicineTianjin First Central HospitalSchool of MedicineNankai UniversityTianjinChina Haihe Laboratory of Sustainable Chemical Transformations Keyan West RoadTianjin300192China Jiangsu Key Laboratory of Neuroregeneration Jiangsu Clinical Medicine Center of Tissue Engineering and Nerve Injury RepairCo-innovation Center ofNeuroregenerationNMPA Key Laboratory for Research and Evaluation of Tissue Engineering Technology ProductsNantong UniversityNantongChina Outpatient Department Tianjin First Central HospitalSchool of MedicineNankai UniversityTianjinChina Clinical School/College of Orthopedics Tianjin Medical UniversityTianjinChina Department of Joint Tianjin HospitalTianjinChina

Peripheral nerve injuries may result in severe long-gap interruptions that are challenging to repair.Autografting is the gold standard surgical approach for repairing long-gap nerve injuries but can result in prominent donor-site complications.Instead,imitating the native neural microarchitecture using synthetic conduits is expected to offer an alternative strategy for improving nerve regeneration.Here,we designed nerve conduits composed of high-resolution anisotropic microfiber grid-cordes with randomly organized nanofiber sheaths to interrogate the positive effects of these biomimetic structures on peripheral nerve regeneration.Anisotropic microfiber-grids demonstrated the capacity to directionally guide Schwann cells and neurites.Nanofiber sheaths conveyed adequate elasticity and permeability,whilst exhibiting a barrier function against the infiltration of fibroblasts.We then used the composite nerve conduits bridge 30-mm long sciatic nerve defects in canine models.At 12 months post-implant,the morphometric and histological recovery,gait recovery,electrophysiological function,and degree of muscle atrophy were assessed.The newly regenerated nerve tissue that formed within the composite nerve conduits showed restored neurological functions that were superior compared to sheaths-only scaffolds and Neurolac nerve conduit controls.Our findings demonstrate the feasibility of using synthetic biophysical cues to effectively bridge long-gap peripheral nerve injuries and indicates the promising clinical application prospects of biomimetic composite nerve conduits.

关键词： composite fiber injuries

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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 material.However,the slow kinetics and poor cycling stability severely restrict its practical applications.In 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 composite.The milled 2liH+MgB_(2)composites were initially hydrogenated to obtain the 2liBH_(4)+MgH_(2)composites.The 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 cycle.Nb_(2)C keeps stable in the composite and acts as an efficient catalyst for the li-Mg-B-H composite.It 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 composite.This 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

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Hard-carbon hybrid li-ion/metal anode enabled by preferred mesoporous uniform lithium growth mechanism

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Journal of Energy Chemistry 2024年第1期88卷 252-259,I0006页

作者： Fang Yan Yan liu Yuan li Yan Wang Zicen Deng Meng li Zhenwei Zhu Aohan Zhou Ting li Jingyi Qiu Gaoping Cao Shaobo Huang Biyan Wang Hao Zhang School of Chemistry and Biological Engineering University of Science and TechnologyBeijing 100083China Research Institute of Chemical Defense Beijing 100191China College of Physics and Engineering Henan University of Science and TechnologyLuoyang 471023HenanChina National Base for International Science&Technology Cooperation School of ChemistryXiangtan UniversityXiangtan 411105HunanChina Materials and Manufacturing Department Beijing University of TechnologyBeijing 100124China

To achieve high energy density in lithium batteries,the construction of lithium-ion/metal hybrid anodes is a promising strategy.In particular,because of the anisotropy of graphite,hybrid anode formed by graphite/li metal has low transport kinetics and is easy to causes the growth of lithium dendrites and accumulation of dead li,which seriously affects the cycle life of batteries and even causes safety problems.Here,by comparing graphite with two types of hard carbon,it was found that hybrid anode formed by hard carbon and lithium metal,possessing more disordered mesoporous structure and lithophilic groups,presents better performance.Results indicate that the mesoporous structure provides abundant active site and storage space for dead lithium.With the synergistic effect of this structure and lithophilic functional groups(–COOH),the reversibility of hard carbon/lithium metal hybrid anode is maintained,promoting uniform deposition of lithium metal and alleviating formation of lithium dendrites.The hybrid anode maintains a 99.5%Coulombic efficiency(CE)after 260 cycles at a specific capacity of 500 m Ah/g.This work provides new insights into the hybrid anodes formed by carbon-based materials and lithium metal with high specific energy and fast charging ability.

关键词： Hard carbon/li metal hybrid anode Mesoporous structure Surface oxygen functional group Fast charging lithium batteries

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Catalytic anode surface enabling in situ polymerization of gel polymer electrolyte for stable li metal batteries

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Nano Research 2024年第6期17卷 5216-5223页

作者： Guocheng li Kang liang Yuanjian li Xiangrui Duan lin Fu Zhao Cai Zhaofu Zhang Jiangnan Dai Yongming Sun Wuhan National Laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074China The Institute of Technological Sciences Wuhan UniversityWuhan 430074China Faculty of Materials Science and Chemistry China University of Geoscience(Wuhan)Wuhan 430074China

Employing quasi-solid-state gel polymer electrolyte(GPE)instead of the liquid counterpart has been regarded as a promising strategy for improving the electrochemical performance of li metal batteries.However,the poor and uneven interfacial contact between li metal anode and GPE could cause large interfacial resistance and electrochemical li stripping/plating inhomogeneity,deteriorating the electrochemical performance.Herein,we proposed that the functional component of composite anode could work as the catalyst to promote the in situ polymerization reaction,and we experimentally realized the integration of polymerized-dioxolane electrolyte and li/li_(22)Sn_(5)/liF composite electrode with low interfacial resistance and good stability by in situ catalyzation polymerization.Thus,the reaction kinetics and stability of metallic li anode were significantly enhanced.As a demonstration,symmetric cell using such a GPE-li/li_(22)Sn_(5)/liF integration achieved stable cycling beyond 250 cycles with small potential hysteresis of 25 mV at 1 mA·cm^(−2)and 1 mAh·cm^(−2),far outperforming the counterpart regular GPE on pure li.Paired with liNi0.5Co0.3Mn0.2O2,the full cell with the GPE-li/li_(22)Sn_(5)/liF integration maintained 85.7%of the original capacity after 100 cycles at 0.5 C(1 C=200 mA·g^(−1)).Our research provides a promising strategy for reducing the resistance between GPE and li metal anode,and realizes li metal batteries with enhance electrochemical performance.

关键词： catalyzation polymerization interface resistance interfacial stability li metal batteries electrochemical performance

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