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Electron donor enabling Mn-Fe based layer oxide cathode with durable sodium ion storage 认领 引用
1
作者 Yanzhe Zhang Zechen Li +4 位作者 Zheng Li Wenwen Sun Xuanyi Yuan Haibo Jin Yongjie Zhao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2025年第10期740-748,共9页
Enhancing the specific capacity of P2-type layered oxide cathodes via elevating the upper operation voltage would inevitably deteriorate electrochemical properties owing to the irreversible anionic redox reaction at h... Enhancing the specific capacity of P2-type layered oxide cathodes via elevating the upper operation voltage would inevitably deteriorate electrochemical properties owing to the irreversible anionic redox reaction at high voltage.In this work,the strategy of the electron donor was utilized to address this issue.Remarkably,the earth-abundant P2-layered cathode Na2/3Al1/6Fe1/6Mn2/3O2with the presence of K2S renders superior rate capability(187.4 and 79.5 mA h g-1at 20 and 1000 mA g-1)and cycling stability(a capacity retention of 85.6% over 300 cycles at 1000 mA g-1)within the voltage region of 2-4.4 V Na+/Na.Furthermore,excellent electrochemical performance is also demonstrated in the full cell.Detailed structural analysis of as-proposed composite cathode illustrates that even at 4.4 V irreversible phase transition can be avoided as well as a cell volume variation of only 0.88%,which are attributed to the enhanced performance compared with the control group.Meanwhile,further investigation of charge compensation reveals the crucial role of sulfur ions in actively control of reversible redox reaction of oxygen species in the lattice structure.This work inspires a new strategy to enhance the structural stability of layered sodium ion cathode materials at high voltages. 展开更多
关键词 Sodium-ion batteries P2-type layered oxide cathode High voltage Electron donor Anion redox reaction
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Regulating the local electronic structure of low-cost Fe/Mn-based layered oxide cathodes for rapid and stable sodium storage 认领 引用
2
作者 Wei Zhao Shaohua Luo +3 位作者 Zhaozhan Shi Rui Huang Shengxun Yan Lixiong Qian 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第2期893-904,I0019,共12页
The P2-type Fe/Mn-based layered oxides,with cost advantages and high theoretical capacity,are considered one of the promising cathode materials for sodium-ion batteries(SIBs).However,the commercial development of thes... The P2-type Fe/Mn-based layered oxides,with cost advantages and high theoretical capacity,are considered one of the promising cathode materials for sodium-ion batteries(SIBs).However,the commercial development of these materials is impeded by two main factors:the MnO6 structure distortion induced by the Jahn-Teller(J-T)effect of Mn3+,and the unfavorable phase transitions that occur during the insertion and extraction of Na+.Here,we present a strategy to improve structural stability by incorporating cost-effective,robust Al-O bonds.This approach induces localized adjustments in the electronic structu re and a pinning effect,which limits the deformation of the transition metal(TM)layers,strengthens the electrostatic bonding within the TM layers,and expands the Na layer spacing.Consequently,the Na0.67Fe0.4Mn0.54Al0.06O2 cathode demonstrates a capacity of 168.8 mAh g-1 at 0.1 C,maintaining89.2%of its original capacity after 200 cycles at 1 C.Through in situ electrochemical impedance spectroscopy(EIS)with dynamic resistance transformation(DRT)analysis,ex situ X-ray absorption spectroscopy(XAS),and in situ X-ray diffraction(XRD),the study demonstrates a reduction in the J-T effect,enhanced kinetic performance,and the inhibition of detrimental phase transitions.This study offers new avenues to the development and design of future low-cost Fe/Mn-based cathodes. 展开更多
关键词 Local electronic Al-doping Low cost Layered oxide cathodes Sodium ion batteries
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Suppressing planar gliding and cation migration in O3-type layered oxide cathode for long-life and wide-temperature sodium-ion batteries 认领 引用
3
作者 Peng Yu Nini Liu +10 位作者 Yizhong Gou Daomin Qin Wen Zhang Lihua Feng Yameng Fan Yu Wang Changhong Wang Jiantao Han Yunhui Huang Jian Peng Chun Fang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第2期789-799,I0017,共11页
Sodium layered oxides stand out as one of the most promising cathodes for sodium-ion batteries due to their high energy density,elemental abundance,and scalability.However,their practical applications are restricted b... Sodium layered oxides stand out as one of the most promising cathodes for sodium-ion batteries due to their high energy density,elemental abundance,and scalability.However,their practical applications are restricted by interplanar gliding,cation migration,and the formation of intragranular microcracks,which collectively lead to rapid structural degradation and capacity loss.Herein,we rationally design an ultrastable O3-type Na0.94Ca0.03Ni1/3Fe1/3Mn1/3O2 cathode,in which Ca2+cations act as pillars within the NaO2slabs,suppressing the irreversible phase transitions and Na/TM cation migration commonly observed in layered oxides.Multiscale in situ and ex situ techniques,combined with post-mortem analysis,reveal that the Ca-pillared pinning effect not only effectively suppresses the interplanar gliding and stress accumulation within the crystal phase but also restrains Na/TM cation migration and surface reconstruction in near-surface regions.Benefiting from the combined effects of structural stabilization,the Ca-pillared cathode exhibits a superior cycling stability,retaining 81.6%of its capacity after 1000 cycles at 2 C within the voltage range of 2.0-4.0 V,along with significantly enhanced wide-temperature(from-40 to 80℃)performance.This work highlights another critical role of Ca pillars in suppressing cation migration and surface structural degradation beyond preventing adverse interplanar gliding,offering valuable insights for designing long-life and wide-temperature layered oxide cathodes. 展开更多
关键词 Layered oxide cathodes Pinning effect Planar gliding Cation migration Sodium-ion batteries
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Electrochemically Induced Local Cation Disorder:A New Paradigm for Stabilizing Layered High-Nickel Oxide Cathodes 认领 引用
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作者 Feng Li Ze-Zhou Lin 《Rare Metals》 SCIE EI CAS CSCD 2026年第7期1-3,共3页
Over the past few decades,the pursuit of higher energy density has driven the development of advanced lithium-ion batteries(LIBs)[1].As the performance-limiting component within the LIBs,the cathode material criticall... Over the past few decades,the pursuit of higher energy density has driven the development of advanced lithium-ion batteries(LIBs)[1].As the performance-limiting component within the LIBs,the cathode material critically determines the upper bound of their energy density through its specific capacity and operating voltage plateau[2,3].Layered high-nickel oxides are primary choices due to their high theoretical capacity and voltage[4,5].When the nickel content exceeds 80%,their reversible capacity reliably surpasses 200 mAh g−1[6]. 展开更多
关键词 electrochemical disorder local cation disorder energy density performance limiting component lithium ion batteries cathode material specific capacity stabilizing layered high nickel oxide cathodes
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Unlocking Iron Redox Depth for High-Energy Layered Sodium Oxide Cathodes 认领 引用
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作者 Yadong Song Wujie Dong +8 位作者 Zhuoran Lv Bingyuan Han Jiaming Li Xin Wang Xinxin Wang Jingjing Chen Chenlong Dong Zhiyong Mao Lianqi Zhang 《Carbon Energy》 SCIE EI CAS CSCD 2026年第3期140-150,共11页
High-capacity O3-type layered NiFeMn-based oxides are promising cathodes for sodium-ion batteries,though their practical deployment is constrained by the inherent limitations of Fe redox chemistry.Traditional designs ... High-capacity O3-type layered NiFeMn-based oxides are promising cathodes for sodium-ion batteries,though their practical deployment is constrained by the inherent limitations of Fe redox chemistry.Traditional designs generally enforcing stoichiometric symmetry(Ni=Mn)yield low Fe redox activity.Herein,we propose a valence engineering strategy that breaks conventional Ni/Mn stoichiometry to reconfigure Fe's local chemical environment and unlock unprecedented redox depth.Density functional theory(DFT)calculations reveal that the designed NaNi0.35Fe0.225Mn0.425O2cathode exhibits a reduced Bader charge on Fe(1.598 vs.1.638 in NaNi1/3Fe1/3Mn1/3O2)and elevated Fe 3d orbital energy,signifying enhanced Fe redox activity.This configuration enables an exceptional Fe2.60+/Fe3.88+redox(1.28 e~-per Fe),delivering a reversible capacity of184.3 mAh g-1within 2-4.2 V at 0.2 C,markedly exceeding the benchmark NaNi1/3Fe1/3Mn1/3O2(161.3 mAh g-1)with low reaction depth of Fe3.01+/Fe3.61+.The intensified cationic redox reaction enables an ultrahigh energy density of 596 Whkg-1.The NaNi0.35Fe0.225Mn0.425O2cathode demonstrates robust performance over a broad temperature range from-15℃to 60℃.In situ and ex situ characterizations unveil a reversible O3■P3■OP2 phase transition with minimal volume change(1.88%)that circumvents detrimental deleterious O'3 intermediates and intragranular cracking.This work establishes valence engineering as a paradigm to consolidate cationic redox reaction in high-energy layered sodium oxide cathodes. 展开更多
关键词 layered oxide cathodes phase transition redox depth sodium-ion battery valence engineering
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Insights into chemical-mechanical degradation and modification strategies of layered oxide cathode materials of sodium ion batteries 认领 引用 被引量：5
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作者 Tong Zhang Yuesen Li +4 位作者 Zihao Song Yaohui Huang Fei Li Shaoan Cheng Fujun Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2025年第4期294-315,共22页
Sodium-ion batteries(SIBs)have attracted significant attention in large-scale energy storage system because of their abundant sodium resource and cost-effectiveness.Layered oxide materials are particularly promising a... Sodium-ion batteries(SIBs)have attracted significant attention in large-scale energy storage system because of their abundant sodium resource and cost-effectiveness.Layered oxide materials are particularly promising as SIBs cathodes due to their high theoretical capacities and facile synthesis.However,their practical applications are hindered by the limitations in energy density and cycling stability.The comprehensive understanding of failure mechanisms within bulk structure and at the cathode/electrolyte interface of cathodes is still lacking.In this review,the issues related to bulk phase degradation and surface degradation,such as irreversible phase transitions,cation migration,transition metal dissolution,air/moisture instability,intergranular cracking,interfacial reactions,and reactive oxygen loss,are discussed.The latest advances and strategies to improve the stability of layered oxide cathodes and full cells are provided,as well as our perspectives on the future development of SIBs. 展开更多
关键词 Layered oxide cathode Failure mechanism Intercalation chemistry Sodium-ion batteries Sustainability
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Scientific challenges faced by Mn-based layered oxide cathodes with anionic redox for sodium-ion batteries 认领 引用 被引量：3
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作者 Chao Zheng Shengnan He +7 位作者 Jiantuo Gan Zhijun Wu Liaona She Yong Gao YaXiong Yang Jiatao Lou Zhijin Ju Hongge Pan 《Carbon Energy》 SCIE EI CSCD 2025年第1期188-218,共31页
In the realm of sodium-ion batteries(SIBs),Mn-based layered oxide cathodes have garnered considerable attention owing to their anionic redox reactions(ARRs).Compared to other types of popular sodium-ion cathodes,Mn-ba... In the realm of sodium-ion batteries(SIBs),Mn-based layered oxide cathodes have garnered considerable attention owing to their anionic redox reactions(ARRs).Compared to other types of popular sodium-ion cathodes,Mn-based layered oxide cathodes with ARRs exhibit outstanding specific capacity and energy density,making them promising for SIB applications.However,these cathodes still face some scientific challenges that need to be addressed.This review systematically summarizes the composition,structure,oxygen-redox mechanism,and performance of various types of Mn-based cathodes with ARRs,as well as the main scientific challenges they face,including sluggish ion diffusion,cationic migration,O2 release,and element dissolution.Currently,to resolve these challenges,efforts mainly focus on six aspects:synthesis methods,structural design,doped modification,electrolyte design,and surface engineering.Finally,this review provides new insights for future direction,encompassing both fundamental research,such as novel cathode types,interface optimization,and interdisciplinary research,and considerations from an industrialization perspective,including scalability,stability,and safety. 展开更多
关键词 anionic redox electrochemistry layered oxide cathodes sodium-ion batteries
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Emerging modification strategies for layered Fe-based oxide cathodes toward high-performance sodium-ion batteries 认领 引用 被引量：3
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作者 Zheng-Xiao Li Yi-Meng Wu +6 位作者 Jun-Wei Yin Peng-Fei Wang Zong-Lin Liu Yan-Xuan Wen Jun-Hong Zhang Yan-Rong Zhu Ting-Feng Yi 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2025年第8期122-147,共26页
Sodium-ion batteries(SIBs)have the advantages of environmental friendliness,cost-effectiveness,and high energy density,which are considered one of the most promising candidates for lithium-ion batteries(LIBs).The cath... Sodium-ion batteries(SIBs)have the advantages of environmental friendliness,cost-effectiveness,and high energy density,which are considered one of the most promising candidates for lithium-ion batteries(LIBs).The cathode materials influence the cost and energy output of SIBs.Therefore,the development of advanced cathode materials is crucial for the practical application of SIBs.Among various cathode materials,layered transition metal oxides(LTMOs)have received widespread attention owing to their straightforward preparation,abundant availability,and cost-competitiveness.Notably,layered Fe-based oxide cathodes are deemed to be one of the most promising candidates for the lowest price and easy-to-improve performance.Nevertheless,the challenges such as severe phase transitions,sluggish diffusion kinetics and interfacial degradation pose significant hurdles in achieving high-performance cathodes for SIBs.This review first briefly outlines the classification of layered structures and the working principle of layered oxides.Then,recent advances in modification strategies employed to address current issues with layered iron-based oxide cathodes are systematically reviewed,including ion doping,biphasic engineering and surface modification.Furthermore,the review not only outlines the prospects and development directions for layered Fe-based oxide cathodes but also provides novel insights and directions for future research endeavors for SIBs. 展开更多
关键词 Layered Fe-based oxide cathodes lon doping Biphasic engineering Surface modification Sodium-ion batteries
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Introducing strong metal–oxygen bonds to suppress the Jahn-Teller effect and enhance the structural stability of Ni/Co-free Mn-based layered oxide cathodes for potassium-ion batteries 认领 引用 被引量：2
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作者 Yicheng Lin Shaohua Luo +5 位作者 Pengyu Li Jun Cong Wei Zhao Lixiong Qian Qi Sun Shengxue Yan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2025年第2期713-722,I0015,共10页
Mn-based layered oxides(KMO)have emerged as one of the promising low-cost cathodes for potassiumion batteries(PIBs).However,due to the multiple-phase transitions and the distortion in the MnO6structure induced by the ... Mn-based layered oxides(KMO)have emerged as one of the promising low-cost cathodes for potassiumion batteries(PIBs).However,due to the multiple-phase transitions and the distortion in the MnO6structure induced by the Jahn-Teller(JT)effect associated with Mn-ion,the cathode exhibits poor structural stability.Herein,we propose a strategy to enhance structural stability by introducing robust metal-oxygen(M-O)bonds,which can realize the pinning effect to constrain the distortion in the transition metal(TM)layer.Concurrently,all the elements employed have exceptionally high crustal abundance.As a proof of concept,the designed K0.5Mn0.9Mg0.025Ti0.025Al0.05O2cathode exhibited a discharge capacity of approximately 100 mA h g-1at 20 mA g-1with 79%capacity retention over 50 cycles,and 73%capacity retention over 200 cycles at 200 mA g-1,showcased much better battery performance than the designed cathode with less robust M-O bonds.The properties of the formed M-O bonds were investigated using theoretical calculations.The enhanced dynamics,mitigated JT effect,and improved structural stability were elucidated through the in-situ X-ray diffractometer(XRD),in-situ electrochemical impedance spectroscopy(EIS)(and distribution of relaxation times(DRT)method),and ex-situ X-ray absorption fine structure(XAFS)tests.This study holds substantial reference value for the future design of costeffective Mn-based layered cathodes for PIBs. 展开更多
关键词 Layered oxide cathodes Potassium-ion batteries Robust M-O bonds Low-cost Jahn-Teller effect
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Entropy tuning and artificial CEI synergistically enhance the stability and kinetics of P2-type layered oxide cathode for high-voltage sodium-ion batteries 认领 引用 被引量：1
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作者 Yingxinjie Wang Ziying Zhang +6 位作者 Kejian Tang Yongchun Li Guohao Li Jie Wang Zhenjun Wu Nan Zhang Xiuqiang Xie 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2025年第8期241-251,共11页
P2-type layered oxide Na2/3Ni1/3Mn2/3O2(NM)is a promising cathode material for sodium-ion batteries(SIBs).However,the severe irreversible phase transition,sluggish Na+diffusion kinetics,and interfacial sid... P2-type layered oxide Na2/3Ni1/3Mn2/3O2(NM)is a promising cathode material for sodium-ion batteries(SIBs).However,the severe irreversible phase transition,sluggish Na+diffusion kinetics,and interfacial side reactions at high-voltage result in grievous capacity degradation and inferior electrochemical performance.Herein,a dual-function strategy of entropy tuning and artificial cathode electrolyte interface(CEI)layer construction is reported to generate a novel P2-type medium-entropy Na0.75Li0.1Mg0.05Ni0.18Mn0.66Ta0.01O2with NaTaO3surface modification(LMNMT)to address the aforementioned issues.In situ X-ray diffraction reveals that LMNMT exhibits a near zero-strain phase transition with a volume change of only 1.4%,which is significantly lower than that of NM(20.9%),indicating that entropy tuning effectively suppresses irreversible phase transitions and enhances ion diffusion.Kinetic analysis and post-cycling interfacial characterization further confirm that the artificial CEI layer promotes the formation of a stable,thin NaF-rich CEI and reduces interfacial side reactions,thereby further enhancing ion transport kinetics and surface/interface stability.Consequently,the LMNMT electrode exhibits outstanding rate capability(46 mA h g−1at 20 C)and cycling stability(89.5%capacity retention after 200 cycles at 2 C)within the voltage range of 2–4.35 V.The LMNMT also exhibits superior all-climate performance and air stability.This study provides a novel path for the design of high-voltage cathode materials for SIBs. 展开更多
关键词 Layered oxide cathodes Entropy tuning Artificial CEl High-voltage Sodium-ion batteries
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Basicity regulation of Ni-rich layered oxide cathodes for all-solid-state Li-ion batteries 认领 引用
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作者 Xiao-Zhong Fan Jin-Hao Zhang +6 位作者 Xiao-He Zhou Jin-Xiu Chen Yan-Qin Shi Gulnur Kalimuldina Fang Wang Ayaulym Belgibayeva Long Kong 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2025年第6期454-460,I0011,共7页
Ni-rich layered oxide cathode materials such as LiNi0.8Mn0.1Co0.1O2(NCM811)face poor interfacial stability and serious side reactions with sulfide solid-state electrolytes.This problem is thought to be exa... Ni-rich layered oxide cathode materials such as LiNi0.8Mn0.1Co0.1O2(NCM811)face poor interfacial stability and serious side reactions with sulfide solid-state electrolytes.This problem is thought to be exacerbated by the gradually accumulated basicity of the surface with the Ni content increasing.Herein,the acidic Li3PO4coating layer on NCM811 particles is introduced by ball-milling approach to neutralize the basicity and aggrandize the interfacial stability.The tailored surface structure and components of NCM811 not only suppress the direct contact of cathode particles with sulfide solid-state electrolyte,but also facilitate electrochemical dynamics by driving the Li+migration across the interface and promoting the electron exchange.Thus,cells with Li3PO4coating layer yield 101.3 mAh g-1specific capacity at 2.0 C and highly reversed discharging capacity after suffering from harsh work conditions.Additionally,the stable coating layer broadens the electrochemical windows of cells,delivering long cycle stability(>100 cycles 0.5 C).This contribution highlights the importance of basicity regulation of Ni-rich layered oxide cathode and offers a low-cost and effective approach to design the interfacial structures for the development of all solid-state batteries. 展开更多
关键词 Basicity regulation Cathode coating Interfacial stability Ni-rich layered oxide cathode All-solid-state lithium battery
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Entropy-mediated layered oxide cathodes:Synergistic channel expansion and strain control for sodium-ion batteries at cryogenic conditions 认领 引用
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作者 Yuzhen Dang Yurong Wu +7 位作者 Zhe Xu Jianxing Wang Runguo Zheng Zhishuang Song Zhiyuan Wang Xiaoping Lin Yanguo Liu Dan Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2025年第10期637-648,共12页
O3-type layered oxide cathodes for sodium-ion batteries are promising owing to high theoretical capacity and broad temperature adaptability,yet hindered by structural degradation and sluggish Na+diffusion kinetics.... O3-type layered oxide cathodes for sodium-ion batteries are promising owing to high theoretical capacity and broad temperature adaptability,yet hindered by structural degradation and sluggish Na+diffusion kinetics.Herein,we present a sodium-deficient high-entropy layered oxide cathode(Na0.85Ni0.3Mn0.3Fe0.1Co0.15Ti0.1Cu0.05B0.02O2,denoted as Na0.85-HEO),combining sodium content optimization and high-entropy composition design.Incorporating six transition metals and light element boron creates a unique high-entropy configuration,effectively mitigating local lattice distortion and internal strain through chemical disorder effects,thereby enabling highly reversible phase transitions(O3-P3-O3)and smaller volume change(0.6A3)during the initial cycle.The sodium-deficient high-entropy design effectively increases the sodium interlayer spacing to 0.322 nm,facilitating the Na+diffusion kinetics.Moreover,this high-entropy strategy enables the cathode to have a completely solid solution charge curve and significantly reduces the proportion of(O2)n-,thereby suppressing gas release during the cycling process.The resultant cathode demonstrates exceptional cyclability(80% capacity retention after 400 cycles at 100 mA g-1in a full cell),and remarkable low-temperature performance(108.6 mAh g-1at -40℃).This work guides the design of high-entropy electrode materials with tailored ionic transport channels for extreme-temperature energy storage applications. 展开更多
关键词 Sodium-ion batteries Layered oxide cathodes High-entropy Low-temperature performance
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New Insights in the Electrochemical Stability of Various Solid Polymer Electrolytes/Layered Positive Metal-Oxide Electrode Interfaces in Solid-State Lithium-Ion Battery 认领 引用
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作者 Alexandre Roelens Ashish Raj +7 位作者 Meron D.Tuemay Lieven Bekaert Xinhua Zhu Mats Meeusen Frank De Proft Jean-François Gohy Annick Hubin Mesfin H.Mamme 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2026年第3期58-72,共15页
All-solid-state battery is a promising solution to make lithium batteries safer while boosting their energy density.Solid polymer electrolytes offer a cheaper alternative to inorganic solid electrolyte.Solid polymer e... All-solid-state battery is a promising solution to make lithium batteries safer while boosting their energy density.Solid polymer electrolytes offer a cheaper alternative to inorganic solid electrolyte.Solid polymer electrolytes even outperform inorganic solid electrolytes in some domains;for example,they are less prone to mechanical failure or to contact loss with electrodes upon cycles.However,there are still a couple of challenges to address,including the solid electrolyte/positive electrode interface degradation.The interface between solid polymer electrolyte and the positive electrode is largely overlooked in favor of that of the negative electrode.Ab initio molecular dynamics was combined with relative bond length change analysis and X-ray photoelectron spectroscopy to study the compatibility of a broad selection of functional groups with two grades of Ni-rich NMC cathode(NMC622,NMC811).The results emphasize the relative reactivity of NMC811 compared to NMC622.It was observed that Li is mostly responsible for triggering chemical degradation by interacting with negatively charged atoms from functional groups.Results revealed that hydroxyl or amine deprotonation is a major mechanism of interface degradation that leads to capacity fading.The role of the electric field during cycling was also investigated,showing how it affects functional group orientation and interactions with the NMC electrode. 展开更多
关键词 ab initio molecular dynamics all-solid-state battery cathode/electrolyte interface layered oxide cathode proton intercalation solid polymer electrolyte
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Medium-entropy configuration enabling reversible P2-OP4 phase transition in layered oxides for high-rate sodium-ion batteries 认领 引用 被引量：3
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作者 Fei-Fei Hong Xin Zhou +9 位作者 Hao Liu Gui-Lin Feng Xiao-Hong Liu Heng Zhang Wei-Feng Fan Bin Zhang Mei-Hua Zuo Wang-Yan Xing Ping Zhang Wei Xiang 《Rare Metals》 SCIE EI CAS CSCD 2025年第5期2997-3007,共11页
Layered transition metal oxides have emerged as promising cathode materials for sodium ion batteries.However,irreversible phase transitions cause structural distortion and cation rearrangement,leading to sluggish Na+d... Layered transition metal oxides have emerged as promising cathode materials for sodium ion batteries.However,irreversible phase transitions cause structural distortion and cation rearrangement,leading to sluggish Na+dynamics and rapid capacity decay.In this study,we propose a medium-entropy cathode by simultaneously introducing Fe,Mg,and Li dopants into a typical P2-type Na0.75Ni0.25Mn0.75O2cathode.The modified Na0.75Ni0.2125Mn0.6375Fe0.05Mg0.05Li0.05O2cathode predominantly exhibits a main P2 phase(93.5%)with a minor O3 phase(6.5%).Through spectroscopy techniques and electrochemical investigations,we elucidate the redox mechanisms of Ni2+/3+/4+,Mn3+/4+,Fe3+/4+,and O2-/O2n-during charging/discharging.The medium-entropy doping mitigates the detrimental P2-O2phase transition at high-voltage,replacing it with a moderate and reversible structural evolution(P2-OP4),thereby enhancing structural stability.Consequently,the modified cathode exhibits a remarkable rate capacity of 108.4 mAh·g-1at 10C,with a capacity retention of 99.0%after 200 cycles at 1C,82.5%after 500 cycles at 5C,and 76.7%after 600 cycles at 10C.Furthermore,it also demonstrates superior electrochemical performance at high cutoff voltage of 4.5 V and extreme temperature(55 and 0℃).This work offers solutions to critical challenges in sodium ion batteries cathode materials. 展开更多
关键词 Layered oxide cathode Sodium ion batteries Phase transition Medium-entropy P2/O3 biphasic structure
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High‑Entropy Layered Oxide Cathode Enabling High‑Rate for Solid‑State Sodium‑Ion Batteries 认领 引用 被引量：22
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作者 Tianxun Cai Mingzhi Cai +5 位作者 Jinxiao Mu Siwei Zhao Hui Bi Wei Zhao Wujie Dong Fuqiang Huang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第1期160-171,共12页
Na-ion O3-type layered oxides are prospective cathodes for Na-ion batteries due to high energy density and low-cost.Nevertheless,such cathodes usually suffer from phase transitions,sluggish kinetics and air instabilit... Na-ion O3-type layered oxides are prospective cathodes for Na-ion batteries due to high energy density and low-cost.Nevertheless,such cathodes usually suffer from phase transitions,sluggish kinetics and air instability,making it difficult to achieve high performance solid-state sodium-ion batteries.Herein,the high-entropy design and Li doping strategy alleviate lattice stress and enhance ionic conductivity,achieving high-rate performance,air stability and electrochemically thermal stability for Na0.95Li0.06Ni0.25Cu0.05Fe0.15Mn0.49O2.This cathode delivers a high reversible capacity(141 mAh g−1at 0.2C),excellent rate capability(111 mAh g−1at 8C,85 mAh g−1even at 20C),and long-term stability(over 85%capacity retention after 1000 cycles),which is attributed to a rapid and reversible O3–P3 phase transition in regions of low voltage and suppresses phase transition.Moreover,the compound remains unchanged over seven days and keeps thermal stability until 279℃.Remarkably,the polymer solid-state sodium battery assembled by this cathode provides a capacity of 92 mAh g−1at 5C and keeps retention of 96%after 400 cycles.This strategy inspires more rational designs and could be applied to a series of O3 cathodes to improve the performance of solid-state Na-ion batteries. 展开更多
关键词 High-entropy High-rate performance Li-TM interaction Air stability O3 layered oxide cathode
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Recent progress on electrolyte functional additives for protection of nickel-rich layered oxide cathode materials 认领 引用 被引量：7
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作者 Longshan Li Dingming Wang +7 位作者 Gaojie Xu Qian Zhou Jun Ma Jianjun Zhang Aobing Du Zili Cui Xinhong Zhou Guanglei Cui 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第2期280-292,共13页
In advantages of their high capacity and high operating voltage,the nickel(Ni)-rich layered transition metal oxide cathode materials(LiNixCoyMnzO2(NCMxyz,x+y+z=1,x≥0.5)and LiNi0.8Co0.15Al0.05O_(2... In advantages of their high capacity and high operating voltage,the nickel(Ni)-rich layered transition metal oxide cathode materials(LiNixCoyMnzO2(NCMxyz,x+y+z=1,x≥0.5)and LiNi0.8Co0.15Al0.05O2(NCA))have been arousing great interests to improve the energy density of LIBs.However,these Nirich cathodes always suffer from rapid capacity degradation induced by unstable cathode-electrolyte interphase(CEI)layer and destruction of bulk crystal structure.Therefore,varied electrode/electrolyte interface engineering strategies(such as electrolyte formulation,material coating or doping)have been developed for Ni-rich cathodes protection.Among them,developing electrolyte functional additives has been proven to be a simple,effective,and economic method to improve the cycling stability of Nirich cathodes.This is achieved by removing unfavorable species(such as HF,H2O)or constructing a stable and protective CEI layer against unfavorable reactive species(such as HF,H2O).Herein,this review mainly introduces the varied classes of electrolyte functional additives and their working mechanism for interfacial engineering of Ni-rich cathodes.Especially,key favorable species for stabilizing CEI layer are summarized.More importantly,we put forward perspectives for screening and customizing ideal functional additives for high performance Ni-rich cathodes based LIBs. 展开更多
关键词 Nickel-rich layered oxide cathode Electrolyte additive Functional group Working mechanism Cathode-electrolyte interphase(CEI)
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In/ex-situ Raman spectra combined with EIS for observing interface reactions between Ni-rich layered oxide cathode and sulfide electrolyte 认领 引用 被引量：3
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作者 Xuelei Li Huilan Guan +7 位作者 Zhijie Ma Ming Liang Dawei Song Hongzhou Zhang Xixi Shi Chunliang Li Lifang Jiao Lianqi Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第9期195-202,I0006,共8页
The interfacial instability between Ni-rich layered oxide cathodes and sulfide electrolytes is a serious problem,leading to poor electrochemical properties of all-solid-state lithium batteries(ASSLB).The chemical/elec... The interfacial instability between Ni-rich layered oxide cathodes and sulfide electrolytes is a serious problem,leading to poor electrochemical properties of all-solid-state lithium batteries(ASSLB).The chemical/electrochemical side reactions are considered to be the origin of the interfacial deterioration.However,the influence of chemical and electrochemical side reactions on the interfacial deterioration is rarely studied specifically.In this work,the deterioration mechanism of the interface between LiNi0.85-xCo0.15AlxO2 and Li10GeP2S12 is investigated in detail by combining in/ex-situ Raman spectra and Electrochemical Impedance Spectroscopy(EIS).It can be determined that chemical side reaction between LiNi0.8Co0.15Al0.05O2 and Li10GeP2S12 will occur immediately once contacted,and the interfacial deterioration becomes more serious after charge-discharge process under the dual effects of chemical and electrochemical side reactions.Moreover,our research reveals that the interfacial stability and the cycle performance of ASSLB can be greatly enhanced by increasing Al-substitution for Ni in LiNi0.85-xCo0.15AlxO2.In particular,the capacity retention of LiNi0.6Co0.15Al0.25O2 cathode after 200 cycles can reach 81.9%,much higher than that of LiNi0.8Co0.15Al0.05O2 cathode(12.5%@200 cycles).This work gives an insight to study the interfacial issues between Ni-rich layered oxide cathode and sulfide electrolyte for ASSLBs. 展开更多
关键词 All-solid-state lithium batteries Ni-rich layered oxide cathode Sulfide electrolytes Interfacial stability Chemical/electrochemical reactions
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Lowering Sodium-Storage Lattice Strains of Layered Oxide Cathodes by Pushing Charge Transfer on Anions 认领 引用 被引量：3
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作者 Na Li Wen Yin +4 位作者 Baotian Wang Fangwei Wang Xiaoling Xiao Jinkui Zhao Enyue Zhao 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第4期99-106,共8页
Due to a high energy density,layered transition-metal oxides have gained much attention as the promising sodium-ion batteries cathodes.However,they readily suffer from multiple phase transitions during the Na extracti... Due to a high energy density,layered transition-metal oxides have gained much attention as the promising sodium-ion batteries cathodes.However,they readily suffer from multiple phase transitions during the Na extraction process,resulting in large lattice strains which are the origin of cycledstructure degradations.Here,we demonstrate that the Na-storage lattice strains of layered oxides can be reduced by pushing charge transfer on anions(O2-).Specifically,the designed O3-type Ru-based model compound,which shows an increased charge transfer on anions,displays retarded O3-P3-O1 multiple phase transitions and obviously reduced lattice strains upon cycling as directly revealed by a combination of ex situ X-ray absorption spectroscopy,in situ X-ray diffraction and geometric phase analysis.Meanwhile,the stable Na-storage lattice structure leads to a superior cycling stability with an excellent capacity retention of 84%and ultralow voltage decay of 0.2 mV/cycle after 300 cycles.More broadly,our work highlights an intrinsically structure-regulation strategy to enable a stable cycling structure of layered oxides meanwhile increasing the materials’redox activity and Nadiffusion kinetics. 展开更多
关键词 anionic redox reaction lattice strains layered oxide cathodes phase transitions sodium-ion battery
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Cationic ordering transition in oxygen-redox layered oxide cathodes 认领 引用 被引量：2
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作者 Xinyan Li Ang Gao +10 位作者 Qinghua Zhang Hao Yu Pengxiang Ji Dongdong Xiao Xuefeng Wang Dong Su Xiaohui Rong Xiqian Yu Hong Li Yong-Sheng Hu Lin Gu 《Carbon Energy》 SCIE EI CAS CSCD 2024年第1期197-206,共10页
Understanding the structural origin of the competition between oxygen 2p and transition-metal 3d orbitals in oxygen-redox(OR)layered oxides is eminently desirable for exploring reversible and high-energy-density Li/Na... Understanding the structural origin of the competition between oxygen 2p and transition-metal 3d orbitals in oxygen-redox(OR)layered oxides is eminently desirable for exploring reversible and high-energy-density Li/Na-ion cathodes.Here,we reveal the correlation between cationic ordering transition and OR degradation in ribbon-ordered P3-Na0.6Li0.2Mn0.8O2 via in situ structural analysis.Comparing two different voltage windows,the OR capacity can be improved approximately twofold when suppressing the in-plane cationic ordering transition.We find that the intralayer cationic migration is promoted by electrochemical reduction from Mn4+to Jahn–Teller Mn3+and the concomitant NaO6 stacking transformation from triangular prisms to octahedra,resulting in the loss of ribbon ordering and electrochemical decay.First-principles calculations reveal that Mn4+/Mn3+charge ordering and alignment of the degenerate eg orbital induce lattice-level collective Jahn–Teller distortion,which favors intralayer Mn-ion migration and thereby accelerates OR degradation.These findings unravel the relationship between in-plane cationic ordering and OR reversibility and highlight the importance of superstructure protection for the rational design of reversible OR-active layered oxide cathodes. 展开更多
关键词 cationic ordering layered oxide cathodes oxygen redox sodium-ion batteries
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Synergistic regulation of lattice strain and electronic structure toward a high-rate and long-cycle O3-NaNi1/3Fe1/3Mn1/3O2 cathode material for sodium-ion batteries 认领 引用
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作者 Yuqi Meng Ying Yang +6 位作者 Rui Wang Yong Ji Yiqi Guo Gaoqiang Mao Wanjing Yu Qinghua Tian Hui Tong 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第8期939-948,I0021,共10页
O3-type NaNi1/3Fe1/3Mn1/3O2is regarded as a highly promising cathode material for sodium-ion batteries(SIBs),benefiting from its high theoretical capacity and cost advantages.However,its practical applicat... O3-type NaNi1/3Fe1/3Mn1/3O2is regarded as a highly promising cathode material for sodium-ion batteries(SIBs),benefiting from its high theoretical capacity and cost advantages.However,its practical application is impeded by structural degradation during cycling and sluggish reaction kinetics.Herein,an in situ coprecipitation doping strategy is proposed to synergistically regulate lattice strain and electronic structure,endowing the cathode material with superior electrochemical performance.Characterizations confirm that Ho3+ions are effectively incorporated into the crystal lattice,preferentially substituting Ni sites and forming robust Ho–O covalent bonds.These bonds function as pinning centers within the structure,thereby enhancing the lattice stability.Meanwhile,the hybridization of Ho-4f orbitals with O-2p and TM-3d orbitals not only strengthens the transition metal–oxygen bonds but also optimizes the electronic structure near the Fermi level.These effects simultaneously boost both the structural stability and the intrinsic electronic conductivity.In situ X-ray diffraction coupled with geometric phase analysis demonstrates that Ho3+doping effectively mitigates extreme lattice variations and homogenizes the lattice strain distribution within the particles,thereby suppressing microcrack generation.Consequently,the obtained cathode delivered a reversible capacity of 147.5 mA h g-1 at 0.1C and maintained 91.2%capacity retention after 300 cycles at5C.This work provides an innovative material design strategy and provides fresh theoretical insights for developing high-stability,high-rate layered oxide cathodes in SIBs. 展开更多
关键词 Ho3+ion doping Co-precipitation method Lattice strain Electronic structure Layered oxide cathode material
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