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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 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

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

A unique Janus PdZn-Co catalyst for enhanced photocatalytic syngas production from CO_(2) and H_(2)O

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Chinese Chemical Letters 2023年第7期34卷 265-268页

作者： Dongxue Zhou Xiangdong Xue Qingjie Luan liguo Zhang baozhen li Xing Wang Wenjun Dong Ge Wang Changmin Hou Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule&Structure ConstructionSchool of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China Shunde Graduate School of University of Science and Technology Beijing Foshan 528399China State Key Laboratory of Inorganic Synthesis&Preparative Chemistry College of Chemistry.Jilin UniversityChangchun 130012China

The development of excellent catalyst to achieve photocatalytic syngas production from CO_(2) and H_(2)O is a prospective and sustainable strategy to alleviate environment and energy crisis. In this study, a unique Janus PdZn-Co catalyst is prepared by annealed the Pd/IRMOF-3(Co, Zn) precursor. Due to the strong interaction, the electron transfers from PdZn terminal to Co terminal in the Janus structure. The electron-received Co terminal facilitates Co sites coordinate with the electrophilic C atom of CO_(2) and the electron-donated PdZn center is easier to coordinate with nucleophilic O atoms of H_(2)O or C=O bonds.The charge redistribution enhances the absorption of CO_(2) and H2O, which promotes H_(2) evolution and CO production. In addition, the carbon shell effectively suppresses the metal core agglomeration and facilitates the electron transmission from photosensitizer to metallic active sites. Meanwhile, the ratio of CO/H_(2) can be regulated(~3:1 to 2:1) by adjusting the proportion of Co and PdZn. The Janus structure and graphite carbon synergistically play a profound impact on improving the photocatalytic performance.The optimized PdZn-Co catalyst exhibits a superior photocatalytic CO production rate(20.03 μmol/h) and the H_(2) generation rate(9.90 μmol/h) with a ratio of CO/H_(2)= 2.02.

关键词： PdZn@C catalyst Janus structure Charge redistribution Absorption modulation Photocatalyst

癫痫共患注意缺陷多动障碍的临床特征及危险因素

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武汉大学学报（医学版） 2024年第4期45卷 480-484页

作者：李娟姚宝珍武汉大学人民医院儿科湖北武汉430060

目的:探讨癫痫儿童共患注意缺陷多动障碍(ADHD)的临床特点,分析癫痫相关因素与ADHD之间的关系,为临床诊治提供参考依据。方法:回顾性收集2018年6月至2021年6月在武汉大学人民医院儿科住院部90例癫痫患儿的详细临床资料,采用美国精神医... 详细信息

目的:探讨癫痫儿童共患注意缺陷多动障碍(ADHD)的临床特点,分析癫痫相关因素与ADHD之间的关系,为临床诊治提供参考依据。方法:回顾性收集2018年6月至2021年6月在武汉大学人民医院儿科住院部90例癫痫患儿的详细临床资料,采用美国精神医学学会修订的《精神障碍诊断与统计手册(第5版)》中ADHD诊断标准进行评估,其中90例癫痫患儿中35例为癫痫共患ADHD患儿(38.9%),55例为单纯癫痫患儿,通过单因素分析和多因素Logistic回归分析确定癫痫共患ADHD的危险因素。结果:癫痫共患ADHD组与单纯癫痫组在性别、癫痫首次发病年龄、抗癫痫药物多药联合、癫痫发作是否控制以及是否有热性惊厥病史差异有统计学意义(χ^(2)=6.194;7.011;12.735;13.502;5.440,P0.05)。结论:男性患儿、癫痫首次发病年龄小于3岁、抗癫痫药物多药联合、癫痫控制与否以及热性惊厥病史是癫痫共患ADHD的危险因素。

关键词：癫痫注意缺陷多动障碍共患病

Covalent-organic frameworks with keto-enol tautomerism for efficient photocatalytic oxidative coupling of amines to imines under visible light

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Science China Chemistry 2021年第12期64卷 2169-2179页

作者： Zhenyu Wu Xiubing Huang Xiangjun li Guangtong Hai baozhen li Ge Wang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule&Structure ConstructionSchool of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing100083China

Photocatalytic oxidation of organic molecules into highly value-added products is an innovative and challenging research which has gradually attracted remarkable attention of scientists.In this work,it is demonstrated that the COF-TpPa with keto-enol tautomerism equilibrium structure shows excellent performance(yield>99%after 8 h)in the selective photocatalytic oxidative coupling of amines to imines under visible light irradiation.It is revealed that three kinds of reactive oxygen species(superoxide radical,hydroxyl radical and singlet oxygen)participate in this photocatalytic oxidation reaction.In addition,hydrogen protons cleaved from the benzyl are proven to be reduced to hydrogen in the conduction band of COF-TpPa in anaerobic atmosphere,accompanied with the formation of imines.The direct hydrogen evolution from amine provides an effective way to extract clean energy from organic molecule as well as the production of value-added chemicals.As a contrast,COF-LZU1 with similar structure and chemical composition to COF-TpPa but without keto-enol tautomerism exhibits worse optical properties and photocatalytic performance.It is also demonstrated that keto-enol tautomerism favors the adsorption of benzylamine based on the characterization results and theoretical calculations.

关键词： covalent-organic frameworks photocatalysts aerobic/anaerobic benzylamine oxidation keto-enol tautomerism

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

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

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

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