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Revealing the working mechanism of a multi-functional block copolymer binder for lithium-sulfur batteries

Journal of energy Chemistry 2021年第8期30卷 1-8,I0001页

作者： xin He Zhimeng Liu Guoping Gao xiaotao Liu Michal Swietoslawski Jun Feng Gao Liu Lin-Wang Wang Robert Kostecki energy storage&Distributed Resources division Lawrence Berkeley National Laboratory1 Cyclotron Road94720 BerkeleyUSA Materials sciences division Lawrence Berkeley National Laboratory94720 BerkeleyUSA The Molecular Foundry Lawrence Berkeley National Laboratory94720 BerkeleyUSA Department of Materials science&Engineering Southern University of Science and Technology(SUSTech)Shenzhen 518055China

The lithium-sulfur(Li-S)battery is one of the most promising substitutes for current energy storage systems because of its low cost,high theoretical capacity,and high energy ***,the high solubility of intermediate products(i.e.,lithium polysulfides)and the resultant shuttle effect lead to rapidly fading capacity and a low coulombic efficiency,which hinder the practical application of Li-S *** this study,block copolymers are constructed with both an ethylene oxide unit and a styrene unit and then used as binders for Li-S *** performance improvements are attributed to the synergistic effects contributed by the different units of the block *** ethylene oxide unit traps polysulfide,which bonds strongly with the intermediate lithium polysulfide,and enhances the transport of lithium ions to reach high ***,the styrene unit maintains cathode integrity by improving the mechanical properties and elasticity of the constructed block copolymer to accommodate the large volume *** enabling multiple functions via different units in the polymer chain,high sulfur utilization is achieved,polysulfide diffusion is confined,and the shuttle effect is suppressed during the cycle life of Li-S batteries,as revealed by operando ultraviolet-visible spectroscopy and S Kedge x-ray absorption spectroscopy.

关键词： Lithium sulfur batteries Polymer binder Block copolymer Ultraviolet-visible spectroscopy x-ray absorption spectroscopy

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An advanced low-cost cathode composed of graphene-coated Na_(2.4)Fe_(1.8)(SO_(4))_(3) nanograins in a 3D graphene network for ultra-stable sodium storage

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Journal of energy Chemistry 2021年第3期30卷 564-570页

作者： Yongjin Fang Qi Liu xiangming Feng Weihua Chen xinping Ai Liguang Wang Liang Wang Zhiyuan Ma Yang Ren Hanxi YangYuliang Cao College of Chemistry and Molecular sciences Engineering Research Center of Organosilicon Compounds&Materials of Ministry of EducationWuhan UniversityWuhan 430072HubeiChina Department of Physics City University of Hong KongTat Chee AvenueKowloonHong KongChina College of Chemistry and Molecular Engineering Zhengzhou UniversityZhengzhou 450001HenanChina x-ray science division Advanced Photon SourceArgonne National Laboratory9700 South Cass AvenueLemontIL 60439USA

Iron-based electrodes have attracted great attention for sodium storage because of the distinct cost ***,exploring suitable iron-based electrodes with high power density and long duration remains a big ***,a spray-drying strategy is adopted to construct graphene-coated Na_(2.4)Fe_(1.8)(SO_(4))_(3) nanograins in a 3D graphene microsphere *** unique structural and compositional advantages endow these electrodes to exhibit outstanding electrochemical properties with remarkable rate performance and long cycle *** analyses further explain the outstanding electrochemical properties from the structural aspect.

关键词： Na_(2.4)Fe_(1.8)(SO_(4))_(3) Polyanions Spray-drying Cathode Sodium-ion batteries

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Understanding Lithium-ion Transport in Sulfolane- and Tetraglyme-Based Electrolytes Using Very Low-Frequency Impedance Spectroscopy

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energy & Environmental Materials 2023年第1期6卷 368-376页

作者： Janet SHo Oleg A.Borodin Michael SDing Lin Ma Marshall A.Schroeder Glenn R.Pastel Kang xu energy sciences division Sensors and Electron Devices DirectorateUS Army Research LaboratoryAdelphi MD 20783USA

With the increasing interest in highly concentrated electrolyte systems,correct determination of the cation transference number is ***-field gradient NMR technique,which measures self-diffusion coefficients,is often applied on liquid electrolytes because of the wide accessibility and simple sample ***,since the assumptions of this technique,that is,complete salt dissociation,all ions participating in motion,and all of them moving independently,no longer hold true in concentrated solutions,the transference numbers,thus obtained are often *** the present work,impedance spectroscopy at a frequency range of 1 MHz to 0.1 mHz was used to examine the concentration effect on lithium-ion transference number under anion-blocking conditions T abc Liþfor two electrolytes:lithium bis(fluorosulfonyl)imide(LiFSI)in sulfolane(SL)and lithium bis(trifluorosulfonyl)imide(LiTFSI)in tetraglyme(G4).The T abc Liþof the former was almost an order of magnitude higher than that of the *** also appeared to increase with increasing concentration while the latter followed an opposite *** faster Li^(+)transport in the SL system is attributed to the formation of a liquid structure consisting of extended chains/bridges of SL molecules and the anions,which facilitate a cation-hopping/ligand-exchanged-typed diffusion mechanism by partially decoupling the cations from the anions and solvent *** G4 system,in contrast,is dominated by the formation of long-lived,stable[Li(G4)]+solvation cages that results in a sluggish Li+*** difference between the two transport mechanisms is discussed via comparison of the bulk ionic conductivity,viscosity,ion self-diffusion coefficients,and the Onsager transport coefficients.

关键词： anion-blocking conditions ion correlations low-frequency impedance spectroscopy transference number

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High Fe^(LS)(C)electrochemical activity of an iron hexacyanoferrate cathode boosts superior sodium ion storage

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Carbon energy 2023年第5期5卷 67-77页

作者： Junhong Guo Fan Feng Shiqiang Zhao Zhenhai Shi Rui Wang Meng Yang Fangfang Chen Suli Chen Zi-Feng Ma Tianxi Liu Key Laboratory of Synthetic and Biological Colloids Ministry of EducationInternational Joint Research Laboratory for Nano Energy CompositesSchool of Chemical and Material EngineeringJiangnan UniversityWuxiChina Department of Chemical Engineering Shanghai Electrochemical Energy Devices Research CenterShanghai Jiao Tong UniversityShanghaiChina College of Chemistry and Materials Engineering Wenzhou UniversityWenzhouChina

Sodium iron hexacyanoferrate(FeHCF)is one of the most promising cathode materials for sodium-ion batteries(SIBs)due to its low cost theoretical ***,the low electrochemical activity of Fe^(LS)(C)in FeHCF drags down its practical capacity and potential ***,FeHCF with high Fe^(LS)(C)electrochemical activity(C-FeHCF)is synthesized via a facile citric acid-assisted solvothermal *** the cathode of SIBs,C-FeHCF shows superior cycling stability(ca.87.3%capacity retention for 1000 cycles at 10 C)and outstanding rate performance(ca.68.5%capacity retention at 50 C).Importantly,the contribution of Fe^(LS)(C)to the whole capacity was quantitatively analyzed via combining dQ/dV and discharge curve for the first time,and the index reaches 44.53%for C-FeHCF,close to the theoretical ***-situ x-ray diffraction proves the structure stability of C-FeHCF during charge-discharge process,ensuring its superior cycling ***,the application feasibility of the C-FeHCF cathode in quasi-solid SIBs is also *** quasi-solid SIBs with the C-FeHCF cathode exhibit excellent electrochemical performance,delivering an initial discharge capacity of 106.5 mAh g^(−1) at 5 C and high capacity retention of 89.8%over 1200 *** work opens new insights into the design and development of advanced cathode materials for SIBs and the beyond.

关键词： cathode material electrochemical activity sodium-ion batteries sodium iron hexacyanoferrate structural evolution

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Copper-hydride nanoclusters with enhanced stability by N- heterocyclic carbenes

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Nano research 2021年第9期14卷 3303-3308页

作者： Hui Shen Lingzheng Wang Omar Lopez-Estrada Chengyi Hu Qingyuan Wu Dongxu Cao Sami Malola Boon KTeo Hannu Hakkinen Nanfeng Zheng State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsNational&Local Joint Engineering Research Center of Preparation Technology of NanomaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Departments of Physics and Chemistry Nanoscience CenterUniversity ofjyvdskyldFI-40014 JyvdskyldFinland

Copper-hydrides have been intensively studied for a long time due to their utilization in a variety of technologically important chemical ***,poor stability of the species severely hinders its isolation,storage and operation,which is worse for nano-sized *** report here an unprecedented strategy to access to ultrastable copper-hydride nanoclusters(NCs),namely,using bidentate N-heterocyclic carbenes as stabilizing ligands in addition to *** this work,a simple synthetic protocol was developed to synthesize the first large copper-hydride nanoclusters(NCs)stabilized by N-heterocyclic carbenes(NHCs).The NC,with the formula of Cu3i(RS)25(NHC)3H6(NHC=1,4-bis(1-benzyl-1 H-benzimidazol-1-ium-3-yl)butane,RS=4-fluorothiophenol),was fully characterized by high resolution Fourier transform ion cyclotron resonance mass spectrum,nuclear magnetic resonance,ultra-violet visible spectroscopy,density functional theory(DFT)calculations and single-crystal x-ray ***,the title cluster exhibits unprecedented Cu4 tetrahedron-based vertex-sharing(TBVS)superstructure(fusion of six Cu4 tetrahedra).Moreover,the ultrahigh thermal stability renders the cluster a model system to highlight the power of NHCs(even other carbenes)in controlling geometrical,electronic and surface structure of polyhydrido copper clusters.

关键词： metal clusters copper-hydride N-hetercxylic carbene stability superatom

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High-rate performance magnesium batteries achieved by direct growth of honeycomb-like V_(2)O_(5)electrodes with rich oxygen vacancies

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Nano research 2023年第4期16卷 4880-4887页

作者： Dongzheng Wu Yichao Zhuang Fei Wang Yang Yang Jing Zeng Jinbao Zhao College of Chemistry and Chemical Engineering State-Province Joint Engineering Laboratory of Power Source Technology for New Energy VehicleState Key Laboratory of Physical Chemistry of Solid SurfacesEngineering Research Center of Electrochemical TechnologyMinistry of EducationCollaborative Innovation Center of Chemistry for Energy MaterialsXiamen UniversityXiamen 361005China School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China

Rechargeable magnesium batteries(RMBs)have emerged as a promising next-generation electrochemical energy storage technology due to their superiority of low price and high ***,the practical applications of RMBs are severely limited by immature electrode ***,the high-rate cathode materials are highly ***,we propose a dualfunctional design of V_(2)O_(5)electrode with rational honeycomb-like structure and rich oxygen vacancies to enhance the kinetics *** result demonstrates that oxygen vacancies can not only boost the intrinsic electronic conductivity of V_(2)O_(5),but also enhance the Mg^(2+)diffusion kinetics inside the cathode,leading to the good high-rate ***,ex-situ x-ray diffraction(xRD),transmission electron microscopy(TEM),and x-ray photoelectron spectroscopy(xPS)characterizations reveal that Mg^(2+)is mainly intercalated from the(101)plane of V_(2)O_(5)−x based on the insertion-type electrochemical mechanism;meanwhile,the highly reversible structure evolution during Mg^(2+)insertion/extraction is also *** work proposes that the dual-functional design of electrode has a great influence in enhancing the electrochemical performance of cathode materials for RMBs.

关键词： V2O5 rechargeable magnesium batteries oxygen vacancies kinetics electronic conductivity

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In situ study on medium-range order evolution during the polyamorphous phase transition in a Pd-Ni-P nanostructured glass

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Journal of Materials science & Technology 2022年第30期125卷 145-156页

作者： Shu Fu Sinan Liu Jiacheng Ge Junjie Wang Huiqiang Ying Shangshu Wu Mengyang Yan Li Zhu Yubin Ke Junhua Luan Yang Ren xiaobing Zuo Zhenduo Wu Zhen Peng Chain-Tsuan Liu xun-Li Wang Tao Feng Si Lan Herbert Gleiter Institute of Nanoscience School of Materials Science and EngineeringNanjing University of Science and TechnologyNanjing 210094P.R.China Department of Physics City University of Hong Kong83 Tat Chee AvenueKowloonHong Kong SARP.R.China Spallation Neutron Source science center Dongguan 523803P.R.China Department of Materials science and Engineering City University of Hong KongHong KongP.R.China x-ray science division Argonne National LaboratoryLemontIllinois 60439USA center of Neutron Scattering and Applied Physics City University of Hong Kong Dongguan Research InstituteDongguan 52300P.R.China School of Materials science and Engineering Jiangsu UniversityZhenjiang 212013P.R.China center of Neutron Scattering City University of Hong Kong Shenzhen Research Institute8 Yuexing 1st RoadShenzhen Hi-Tech Industrial ParkShenzhen 518057P.R.China

Engineering multiscale structural hierarchies in glassy alloys enable a broad spectrum of potential *** glasses were born in hierarchical structures from atomic-to-nanometer ***,the frozen-in structures in traditional metallic glasses prepared by rapid quenching techniques are challenging to ***,we show that a PdNiPbulk nanostructured glass of polyamorphous interfacial structures was prepared by inert-gas condensation with a laser evaporation source,and its multiscale structures could be ***-situ scattering experiment results reveal polyamorphous phase transitions occurred in the interfacial regions,which are accompanied by the evolution of medium-range order and the nanoscale heterogeneous structures during the condensation process of glassy nanoparticles under high pressure and the following heating ***,changes in the cluster connectivity resulting from repacking of the local ordering induced by pressure and temperature could be *** thermophysical and mechanical properties,including boson peaks,hardness,and elasticity modulus,could be changed as a function of heat-treatment *** findings would shed light on the synthesis of bulk nanostructured glassy alloys with tailorable thermodynamic and dynamical behavior as well as mechanical properties based on the understanding of metastability for polyamorphous interfacial phases.

关键词： Bulk nanostructured glasses Medium-range order Polyamorphous phase transition

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Heterostructure engineering in electrode materials for sodium-ion batteries:Recent progress and perspectives

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escience 2023年第5期3卷 1-11页

作者： Eric Gabriel Chunrong Ma Kincaid Graff Angel Conrado Dewen Hou Hui xiong Micron School of Materials science and Engineering Boise State UniversityBoiseID83725USA x-ray sciences division Argonne National LaboratoryLemontIL60439USA College of Textiles&Clothing Qingdao UniversityQingdao266071China Key Laboratory of Bio-Fibers and Eco-Textiles Qingdao UniversityQingdao266071China center for Nanoscale Materials Argonne National LaboratoryLemontIL60439USA center for Advanced energy Studies Idaho FallsID83401USA

Sodium-ion batteries(SIBs)have stepped into the spotlight as a promising alternative to lithium-ion batteries for large-scale energy storage ***,SIB electrode materials,in general,have inferior performance than their lithium counterparts because Nat is larger and heavier than *** engineering is a promising strategy to overcome this intrinsic limitation and achieve practical *** provide a brief review of recent progress in heterostructure engineering of electrode materials and research on how the phase interface influences Nat storage and transport *** strategies for the design and fabrication of heterostructures(in situ methods)are discussed,with a focus on the heterostructure formation *** heterostructure's influence on Nat storage and transport properties arises primarily from local distortions of the structure and chemomechanical coupling at the phase interface,which may accelerate ion/electron diffusion,create additional active sites,and bolster structural ***,we offer our perspectives on the existing challenges,knowledge gaps,and opportunities for the advancement of heterostructure engineering as a means to develop practical,highperformance sodium-ion batteries.

关键词： Heterostructure Sodium-ion batteries Electrode materials Heterogeneous materials Interface engineering Intergrowth

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Investigation of the sodium storage mechanism of iron fluoride hydrate cathodes using x-ray absorption spectroscopy and mossbauer spectroscopy

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Journal of energy Chemistry 2023年第2期77卷 535-542,I0014页

作者： Ghulam Ali Muhammad Akbar Faiza Jan Iftikhar Qamar Wali Beata Kalska Szostko Dariusz Satuła Kyung Yoon Chung energy storage research center Korea Institute of Science and TechnologyHwarang-ro 14 gil 5Seongbuk-guSeoul 02792South Korea USPCAS-E National University of Sciences and Technology(NUST)H-12Islamabad 44000Pakistan division of energy&Environment Technology KIST SchoolKorea University of Science and Technology(UST)Hwarang-ro 14-gil-5Seongbuk-guSeoul 02792South Korea NUTECH School of Applied sciences and Humanities National University of TechnologyIslamabad 44000Pakistan University of Białystok Faculty of ChemistryCiołkowskiego 1K15-424 BiałystokPoland University of Białystok Faculty of PhysicsCiołkowskiego 1L15-424 BiałystokPoland

Elucidation of a reaction mechanism is the most critical aspect for designing electrodes for highperformance secondary ***,we investigate the sodium insertion/extraction into an iron fluoride hydrate(FeF_(3)·0.5H_(2)O)electrode for sodium-ion batteries(SIBs).The electrode material is prepared by employing an ionic liquid 1-butyl-3-methylimidazolium-tetrafluoroborate,which serves as a reaction medium and precursor for F^(-)*** crystal structure of FeF_(3)·0.5H_(2)O is observed as pyrochlore type with large open 3-D tunnels and a unit cell volume of 1129A^(3).The morphology of FeF_(3)·0.5H_(2)O is spherical shape with a mesoporous *** microstructure analysis reveals primary particle size of around 10 *** FeF_(3)·0.5H_(2)O cathode exhibits stable discharge capacities of 158,210,and 284 mA h g^(-1) in three different potential ranges of 1.5-4.5,1.2-4.5,and 1.0-4.5 V,respectively at 0.05 C *** specific capacities remained stable in over 50 cycles in all three potential ranges,while the rate capability was best in the potential range of 1.5-4.5 *** electrochemical sodium storage mechanism is studied using x-ray absorption spectroscopy,indicating higher conversion at a more discharged ***-situ M?ssbauer spectroscopy strengthens the results for reversible reduction/oxidation of *** results will be favorable to establish high-performance cathode materials with selective voltage window for SIBs.

关键词： Iron fluoride Sodium-ion batteries Pyrochlore x-ray absorption spectroscopy Mössbauer spectroscopy

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Medium-range order endows a bulk metallic glass with enhanced tensile ductility

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Journal of Materials science & Technology 2023年第28期159卷 10-20页

作者： Sinan Liu Weixia Dong Zhiqiang Ren Jiacheng Ge Shu Fu Zhenduo Wu Jing Wu Yu Lou Wentao Zhang Huaican Chen Wen Yin Yang Ren Joerg Neuefeind Zesheng You Ying Liu xun-Li Wang Si Lan Herbert Gleiter Institute of Nanoscience School of Materials Science and EngineeringNanjing University of Science and TechnologyNanjing 210094China Department for Physics City University of Hong Kong83 Tat Chee AvenueKowloonHong Kong SARChina City University of Hong Kong Shenzhen research Institute Shenzhen 518057China City University of Hong Kong(Dongguan) Dongguan 523000China Cryo-TEM center Southern University of Science and TechnologyShenzhen 518055China Spallation Neutron Source science center Institute of High Energy Physics(IHEP)Chinese Academy of Sciences(CAS)Dongguan 523808China Guangdong-Hong Kong-Macao joint Laboratory for Neutron Scattering science and Technology 1 Zhongziyuan RoadDalangDongguan 523803China Chemical and Engineering Materials division Oak Ridge National LaboratoryOak RidgeTennessee37831USA

Developing ductile bulk metallic glasses(BMGs)can benefit from an in-depth understanding of the structure-property relation during plastic ***,endowing BMGs with tensile ductility in BMGs needs to reveal the response of critical structure units during ***,we report the experimental results of an in-situ synchrotron high-energy x-ray study of a Zr-based BMG under uniaxial tension after preprocessing by canning compression of the three-dimensional compressive stress *** is revealed that the canning-compressed BMG(CC-BMG)sample has better tensile ductility and higher ultimate strength than the as-cast sample,which possesses heterogeneous and loosely packed local struc-tures on medium-range *** experimental results revealed two stages of plastic deformation in the CC-BMGs compared with one stage of plastic deformation in the as-cast ***,the shift in the first sharp diffraction peak along the tension direction for the canning-compressed sample is substan-tially more pronounced than that of the as-cast ***,the real-space analysis illustrates a competition mechanism between the 2-atom and 3-atom connection modes on medium-range order during the plastic deformation of the ***,the ordering on the medium-range scale de-creases in the first plastic deformation stage but increases in the second plastic deformation ***-fore,a structural crossover phenomenon occurs in the CC-BMG during plastic *** results demonstrate a structure-property correlation for the CC-BMGs of heterogeneous medium-range ordered structures,which may be beneficial for endowing BMGs with ductility based on medium-range order engineering techniques.

关键词： Bulk metallic glass Medium-range order Tensile ductility Structure-property relation

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