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Unraveling role of double-exchange interaction in electrochemical water oxidation by external magnetic field

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Rare Metals 2024年第1期43卷 289-297页

作者： Jun li Jun-Ming li Hong Hong Dong-Xue liu Qing-Qi Cao Dun-Hui Wang National Laboratory of Solid State Microstructures and Jiangsu Provincial Key Laboratory for Nanotechnology Nanjing UniversityNanjing 210093China School of Electronics and Information Hangzhou Dianzi UniversityHangzhou 310018China

Double-exchange(DE) interaction plays an important role in electrocatalytic oxygen evolution reaction(OER).However,precise achievement of DE interaction often requires foreign dopants or vacancy engineering,leading to destabilization of the catalysts and deterioration of performance.By contrast,the utilization of environmentally friendly,contactless,and continuously adjustable magnetic fields to study the OER process is profitable to avoid aforementioned interference factors and further elucidate the direct relationship_(0.5)between DE interaction and OER activity.Here,by using cobalt hydroxide carbonate(Co(OH)(CO_(3))·xH_(2)O,CoHC) nanostructures as a proof-of-concept study,external magnetic fields are carefully implemented to verify the role of DE interaction during water oxidation reaction.Detailed studies reveal that external magnetic fields effectively enhance the reaction rate of the catalyst,the overpotential decreases from 386 to 355 mV(100 mA·cm^(-2)),while Tafel slopes drastically decline from 93 to 67 mV·dec^(-1)(1.0 T).Moreover,magnetic field increment exhibits robust durability.Through in situ Raman and impedance measurements under external field,it can be found that magnetic field promotes the electron migration between Co^(2+) and Co^(3+) in the CoHC catalysts with the assistance of DE interactions,thus boosting the OER efficiency.

关键词： Magnetic field Double-exchange(DE)interaction Electrocatalysis Oxygen evolution reaction(OER) Cobalt hydroxide carbonate

High cerium content(Nd-Pr-Ce)_(2)Fe_(14)B melt-spun ribbons with high coercivity

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Journal of Rare Earths 2024年第4期42卷 690-695页

作者： Yujiang Zhong junming Wang Zikai Yuan Ruijin liu Minggang Zhu Zhe liu Xin Chen Wei li Zhaohui Guo Division of Functional Materials Central Iron and Steel Research InstituteBeijing100081China Ningbo Jinji Strong Magnetic Material Co. Ltd.Ningbo315172China Jiangxi Jiangwu Rare Metal New Material Co. Ltd.Nanchang330013China

The effects of wheel speeds on the magnetic properties and microstructures of[(Nd,Pr)_(1-x)Ce_(x)]-Fe-B meltspun ribbons were investigated.Compared to melt-spun ribbons with low cerium(Ce)content(x=0.2),amorphous formation can be suppressed at high wheel speed in the ribbons with a relatively high Ce content(x=0.8),and with the increase of the wheel speed,the magnetic properties of the ribbons with high Ce content raise continuously.At high wheel speed,the coercivity mechanism of melt-spun ribbons is mainly pinning field,and the high wheel speed introduces a large number of defects into the matrix as pinning sites.Furthermore,ribbons with high Ce content form a fine and uniform grain structure,so the grain boundary area enlarges,which further hinders the movement of domain walls.The combined effects of the above factors enable ribbons with high Ce content to have excellent magnetic properties(Hcj=0.977 T,Mr=64 m^(2) A/kg)at the wheel speed of 35 m/s.

关键词： Wheel speed Cecontent Microstructure Magnetic properties Rare earths

Electric-Field-Treated Ni/Co_(3)O_(4) Film as High-Performance Bifunctional Electrocatalysts for Efficient Overall Water Splitting

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Nano-Micro Letters 2022年第9期14卷 160-173页

作者： junming li Jun li Jun Ren Hong Hong Dongxue liu lizhe liu Dunhui Wang National Laboratory of Solid State Microstructures Collaborative Innovation Center of Advanced MicrostructuresJiangsu Provincial Key Laboratory for NanotechnologySchool of PhysicsNanjing UniversityNanjing 210093People’s Republic of China Hangzhou Dianzi University Hangzhou 310018People’s Republic of China

Rational design of bifunctional electrocatalysts for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)with excellent activity and stability is of great significance,since overall water splitting is a promising technology for sustainable conversion of clean energy.However,most electrocatalysts do not simultaneously possess optimal HER/OER activities and their electrical conductivities are intrinsically low,which limit the development of overall water splitting.In this paper,a strategy of electric field treatment is proposed and applied to Ni/Co_(3)O_(4) film to develop a novel bifunctional electrocatalyst.After treated by electric field,the conductive channels consisting of oxygen vacancies are formed in the Co_(3)O_(4) film,which remarkably reduces the resistance of the system by almost 2×10^(4) times.Meanwhile,the surface Ni metal electrode is partially oxidized to nickel oxide,which enhances the catalytic activity.The electric-field-treated Ni/Co_(3)O_(4) material exhibits super outstanding performance of HER,OER,and overall water splitting,and the catalytic activity is significantly superior to the state-of-the-art noble metal catalysts(Pt/C,RuO_(2),and RuO_(2)‖Pt/C couple).This work provides an effective and feasible method for the development of novel and efficient bifunctional electrocatalyst,which is also promising for wide use in the field of catalysis.

关键词： Bifunctional electrocatalyst Overall water splitting Co_(3)O_(4)film Oxygen vacancies Electric field

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

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新型城镇化、市场化改革与数字经济发展

统计与信息论坛 2024年第6期39卷 32-44页

作者：李俊铭夏友富对外经济贸易大学国家对外开放研究院北京100029

随着中国正式迈入新发展阶段,高效推进新型城镇化建设,进一步加速数字经济发展,着力构建高水平现代化市场体系已然成为中国“十四五”时期乃至未来助力高质量发展的关键举措。基于中国30个省份2011-2020年的面板数据,综合运用面板向量... 详细信息

随着中国正式迈入新发展阶段,高效推进新型城镇化建设,进一步加速数字经济发展,着力构建高水平现代化市场体系已然成为中国“十四五”时期乃至未来助力高质量发展的关键举措。基于中国30个省份2011-2020年的面板数据,综合运用面板向量自回归模型、耦合协调度模型、双重固定效应模型等方法客观揭示了新型城镇化、市场化改革与数字经济三大系统的互动关系、耦合协调发展程度及其有效驱动因素,得到以下研究结论:第一,新型城镇化能够显著推动地区市场化改革,市场化改革有利于促进数字经济发展;新型城镇化与数字经济则能够彼此支持、相互促进;第二,中国新型城镇化、市场化改革与数字经济的耦合协调程度稳步提升,三大系统间的互动联系愈发密切,协调发展态势已基本形成,但总体呈现由东向西的区域梯度差距分布;第三,固定资产投资、政府干预、科技创新等因素则是驱动三大系统耦合协调发展的关键。由此表明,创新完善宏观调控政策,科学引导,精准施策,统筹推动新型城镇化、市场化改革与数字经济的稳健发展,合理实现三者间的高水平联动,将是当代中国实现经济转型与高质量发展的题中应有之义。

关键词：新型城镇化市场化改革数字经济互动关系耦合协调

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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

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