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Unveiling the correlation between structural alterations and enhanced high-voltage cyclability in Na-deficient P3-type layered cathode materials via Li incorporation

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Electron 2024年第1期2卷 164-176页

作者： Xiaoxia Yang Suning Wang Hang Li Jochi Tseng Zhonghua Wu sylvio indris Helmut Ehrenberg Xiaodong Guo Weibo Hua School of Chemical Engineering and Technology Xi'an Jiaotong UniversityXi'anChina School of Chemical Engineering Sichuan UniversityChengduChina Institute for Applied Materials(IAM) Karlsruhe Institute of Technology(KIT)Eggenstein‐LeopoldshafenGermany Diffraction and Scattering Division Japan Synchrotron Radiation Research Institute(JASRI)KoutoSayo‐choSayo‐gunHyogoJapan Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijingChina

With exceptional capacity during high-voltage cycling,P3-type Nadeficient layered oxide cathodes have captured substantial attention.Nevertheless,they are plagued by severe capacity degradation over cycling.In this study,tuning and optimizing the phase composition in layered oxides through Li incorporation are proposed to enhance the high-voltage stability.The structural dependence of layered Na_(2/3)LixNi_(0.25)Mn_(0.75)O_(2)þδoxides on the lithium content(0.0≤x≤1.0)offered during synthesis is investigated systematically on an atomic scale.Surprisingly,increasing the Li content triggers the formation of mixed P2/O3-type or P3/P2/O3-type layered phases.As the voltage window is 1.5-4.5 V,P3-type Na2/3Ni_(0.25)Mn_(0.75)O_(2)(NL0.0NMO,R3m)material exhibits a sequence of phase transformations throughout the process of(de)sodiation,that is,O3⇌P3⇌O30⇌O3″.Such complicated phase transitions can be effectively suppressed in the Na2/3Li_(0.7)Ni_(0.25)Mn_(0.75)O_(2.4)(NL_(0.7)NMO)oxide with P2/P3/O3-type mixed phases.Consequently,cathodes made of NL0.7NMO exhibit a substantially enhanced cyclic performance at high voltages compared to that of the P3-type layered NL0.0NMO cathode.Specifically,NL0.7NMO demonstrates an outstanding capacity retention of 98%after 10 cycles at 1 C within 1.5-4.5 V,much higher than that of NL0.0NMO(83%).This work delves into the intricate realm of bolstering the high-voltage durability of layered oxide cathodes,paving the way for advanced sodium-ion battery technologies.

关键词： high-voltage cycling Li incorporation phase transition sodium ion batteries triphasic composites

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Elucidation of the sodiation/desodiation mechanism in Ca_(0.5)Ti_(2)(PO_(4))_(3)/C as promising electrode for sodium batteries: New insights into the phase transitions

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Journal of Energy Chemistry 2022年第7期31卷 36-44,I0002页

作者： Abdelhaq Nassiri Noha Sabi Angelina Sarapulova Yingjin Wei Bouchaib Manoun sylvio indris Alexandr Missyul Helmut Ehrenberg Ismael Saadoune IMED-Lab Faculty of Science and Technology-Cadi Ayyad University(UCA)Av.A.El KhattabiP.B.549MarrakeshMorocco Institute for Applied Materials(IAM) Karlsruhe Institute of Technology(KIT)P.O.Box 364076021 KarlsruheGermany Key Laboratory of Physics and Technology for Advanced Batteries(Ministry of Education) Jilin Engineering Laboratory of New Energy Materials and TechnologyCollege of PhysicsJilin UniversityChangchun 130012JilinChina MSN Mohamed VI Polytechnic UniversityLot 660Hay Moulay RachidBen Guerir 43150Morocco CELLS-ALBA Synchrotron E-08290 Cerdanyola del VallesBarcelonaSpain Technology Development Cell(Techcell) Technology Transfer Office(TTO)Mohamed VI Polytechnic UniversityLot 660Hay Moulay RachidBen Guerir 43150Morocco

The structure evolution and electrochemical performance of Na SICON-type Ca_(0.5)Ti_(2)(PO_(4))_(3) for sodium batteries are presented.This phosphate was synthesized by a solid-state method,and the obtained particles were coated with carbon using sucrose.This compound crystallizes in the rhombohedral system with space group R-3.The presence of carbon in the Ca_(0.5)Ti_(2)(PO_(4))_(3)/C composite was confirmed by Raman and Thermogravimetric analysis.The electrochemical performance of Ca_(0.5)Ti_(2)(PO_(4))_(3)/C was investigated in the potential window 1.5–3.0 V vs.sodium metal at different scan rates.The compound is able to initially intercalate/deintercalate 1.6/1.15 Na per formula unit,respectively.In operando synchrotron diffraction was done in the potential window 0.02–3.0 V vs.Na|Na+and revealed the occurrence of several reaction regions upon first discharge.Up to 4 Na+ion per formula unit can be inserted during the first discharge.An intensive refinement of the synchrotron X-ray diffraction(SXRD)patterns of discharged Ca_(0.5)Ti_(2)(PO_(4))_(3) evidenced the existence of five regions depending on the sodium content while the crystal structures of new phases were elucidated for the first time where sodium insertion occurs in the unusual M3 and M’3 sites of the Na SICON structure.

关键词： Sodium-ion batteries Phosphates Synchrotron Mechanism Energy storage

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Probing thermally-induced structural evolution during the synthesis of layered Li-, Na-, or K-containing 3d transition-metal oxides

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eScience 2022年第2期2卷 183-191页

作者： Weibo Hua Xiaoxia Yang Nicola PMCasati Laijun Liu Suning Wang Volodymyr Baran Michael Knapp Helmut Ehrenberg sylvio indris School of Chemical Engineering and Technology Xi'an Jiaotong UniversityXi'anShaanxi710049China Institute for Applied Materials(IAM) Karlsruhe Institute of Technology(KIT)Hermann-von-Helmholtz-Platz 1D-76344Eggenstein-LeopoldshafenGermany College of Materials Science and Engineering Guilin University of TechnologyGuilin541004China Paul Scherrer Institut(PSI) WLGA/2295232Villigen PSISwitzerland Deutsches Elektronen-Synchrotron(DESY) Notkestr.85Hamburg22607Germany

Layered alkali-containing 3d transition-metal oxides are of the utmost importance in the use of electrode materials for advanced energy storage applications such as Li-,Na-,or K-ion batteries.A significant challenge in the field of materials chemistry is understanding the dynamics of the chemical reactions between alkali-free precursors and alkali species during the synthesis of these compounds.In this study,in situ high-resolution synchrotron-based X-ray diffraction was applied to reveal the Li/Na/K-ion insertion-induced structural transformation mechanism during high-temperature solid-state reaction.The in situ diffraction results demonstrate that the chemical reaction pathway strongly depends on the alkali-free precursor type,which is a structural matrix enabling phase transi-tions.Quantitative phase analysis identifies for the first time the decomposition of lithium sources as the most critical factor for the formation of metastable intermediates or impurities during the entire process of Li-rich layered Li[Li_(0.2)Ni_(0.2)Mn_(0.6)]O_(2) formation.Since the alkali ions have different ionic radii,Na/K ions tend to be located on prismatic sites in the defective layered structure(Na_(2/3-x)[Ni_(0.25)Mn_(0.75)]O_(2) or K_(2/3-x)[Ni_(0.25)Mn_(0.75)]O_(2))during calcination,whereas the Li ions prefer to be localized on the tetrahedral and/or octahedral sites,forming O-type structures.

关键词： In situ sXRD Structural evolution 3d transition-metal oxides Layered structure High-temperature solid-state reaction

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Enhanced room-temperature Na^(+) ionic conductivity in Na_(4.92)Y_(0.92)Zr_(0.08)Si_(4)O_(12)

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eScience 2023年第6期3卷 935-945页

作者： Aikai Yang Kai Yao Mareen Schaller Enkhtsetseg Dashjav Hang Li Shuo Zhao Qiu Zhang Martin Etter Xingchen Shen Huimin Song Qiongqiong Lu Ruijie Ye Igor Moudrakovski Quanquan Pang sylvio indris Xingchao Wang Qianli Ma Frank Tietz Jun Chen Olivier Guillon Forschungszentrum Jülich GmbH Institute of Energy and Climate ResearchMaterials Synthesis and Processing(IEK-1)52425 JülichGermany Institute of Mineral Engineering(GHI) RWTH Aachen UniversityForckenbeckstraße 3352074 AachenGermany Institute for Applied Materials-Energy Storage Systems(IAM-ESS) Karlsruhe Institute of Technology(KIT)76344 Eggenstein-LeopoldshafenGermany Renewable Energy Conversion and Storage Center(RECAST) Haihe Laboratory of Sustainable Chemical TransformationsKey Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)College of ChemistryNankai UniversityTianjin 300071China Deutsches Elektronen-Synchrotron(DESY) Notkestrasse 8522607 HamburgGermany Laboratoire de Cristallographie et Sciences des Materiaux(CRISMAT) CNRSENSICAEN14000 CaenFrance Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials School of Materials Science and EngineeringPeking UniversityBeijing 100871China Institute of Materials Henan Academy of SciencesHenan Key Laboratory of Advanced Conductor MaterialsZhengzhou 450046China Max Planck Institute for Solid State Research Heisenbergstraße 170569 StuttgartGermany State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources Key Laboratory of Advanced Functional MaterialsAutonomous RegionInstitute of Applied ChemistryCollege of ChemistryXinjiang UniversityUrumqiXinjiang 830046China Forschungszentrum Jülich GmbH Helmholtz Institute Münster(IEK-12)52425 JülichGermany Jülich Aachen Research Alliance JARA-Energy52425 JülichGermany

Developing cost-effective and reliable solid-state sodium batteries with superior performance is crucial for stationary energy storage.A key component in facilitating their application is a solid-state electrolyte with high conductivity and stability.Herein,we employed aliovalent cation substitution to enhance ionic conductivity while preserving the crystal structure.Optimized substitution of Y^(3+)with Zr^(4+)in Na_(5)YSi_(4)O_(12) introduced Naþion vacancies,resulting in high bulk and total conductivities of up to 6.5 and 3.3 mS cm^(-1),respectively,at room temperature with the composition Na_(4.92)Y_(0.92)Zr_(0.08)Si_(4)O_(12)(NYZS).NYZS shows exceptional electrochemical stability(up to 10 V vs.Naþ/Na),favorable interfacial compatibility with Na,and an excellent critical current density of 2.4 mA cm^(-2).The enhanced conductivity of Naþions in NYZS was elucidated using solid-state nuclear magnetic resonance techniques and theoretical simulations,revealing two migration routes facilitated by the synergistic effect of increased Naþion vacancies and improved chemical environment due to Zr^(4+)substitution.NYZS extends the list of suitable solid-state electrolytes and enables the facile synthesis of stable,low-cost Naþion silicate electrolytes.

关键词： Solid-state electrolytes Sodium superionic conductors Na_(4.92)Y_(0.92)Zr_(0.08)Si_(4)O_(12) High conductivity Ultra-wide electrochemical window

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