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Extending the solid solution range of sodium ferric pyrophosphate:Off‐stoichiometric Na_(3)Fe(2.5)(P_(2)O_(7))_(2)as a novel cathode for sodium‐ion batteries

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Carbon Energy 2024年第4期6卷 128-139页

作者： Xiang jun Pu Kunran Yang Zibing Pan Chunhua Song Yangyang Lai Renjie Li Zheng‐Long Xu Zhongxue Chen yuliang cao Hubei Key Laboratory of Electrochemical Power Sources College of Chemistry and Molecular SciencesWuhan UniversityWuhanChina Key Laboratory of Hydraulic Machinery Transients Ministry of EducationSchool of Power and Mechanical EngineeringWuhan UniversityWuhanChina School of Chemistry and Chemical Engineering Jiangsu University of TechnologyChangzhouJiangsuChina Zonergy Corporation ZigongSichuanChina Department of Industrial and Systems Engineering The Hong Kong Polytechnic UniversityHung HomHong Kong SARChina

Iron‐based pyrophosphates are attractive cathodes for sodium‐ion batteries due to their large framework,cost‐effectiveness,and high energy density.However,the understanding of the crystal structure is scarce and only a limited candidates have been reported so far.In this work,we found for the first time that a continuous solid solution,Na_(4−α)Fe_(2+α)_(2)(P_(2)O_(7))_(2)(0≤α≤1,could be obtained by mutual substitution of cations at center‐symmetric Na3 and Na4 sites while keeping the crystal building blocks of anionic P2O7 unchanged.In particular,a novel off‐stoichiometric Na_(3)Fe(2.5)(P_(2)O_(7))_(2)is thus proposed,and its structure,energy storage mechanism,and electrochemical performance are extensively investigated to unveil the structure–function relationship.The as‐prepared off‐stoichiometric electrode delivers appealing performance with a reversible discharge capacity of 83 mAh g^(−1),a working voltage of 2.9 V(vs.Na^(+)/Na),the retention of 89.2%of the initial capacity after 500 cycles,and enhanced rate capability of 51 mAh g^(−1)at a current density of 1600 mA g^(−1).This research shows that sodium ferric pyrophosphate could form extended solid solution composition and promising phase is concealed in the range of Na_(4−α)Fe_(2+α)_(2)(P_(2)O_(7))_(2),offering more chances for exploration of new cathode materials for the construction of high‐performance SIBs.

关键词： extending solid‐solution range off‐stoichiometric Na_(3)Fe_(2.5)(P_(2)O_(7))_(2) sodium‐ion batteries structure-function relationship

A high-loading and cycle-stable solid-phase conversion sulfur cathode using edible fungus slag-derived microporous carbon as sulfur host

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Nano Research 2023年第6期16卷 8360-8367页

作者： Hui Li Xiangjiang Wu Sijie Jiang Qian Zhang yuliang cao Hanxi Yang Feifei cao Xinping Ai Hubei Key Laboratory of Electrochemical Power Sources College of Chemistry&Molecular ScienceWuhan UniversityWuhan 430072China College of Science Huazhong Agricultural UniversityWuhan 430070China

Developing a high sulfur(S)-loading cathode with high capacity utilization and long term cyclability is a key challenge for commercial implementation of Li-S battery technology.To overcome this challenge,we propose a solid-phase conversion sulfur cathode by using an edible fungus slag-derived porous carbon(CFS)as sulfur host to fabricate the S/CFS composite and meanwhile,utilizing the vinyl carbonate(VC)as co-solvent of the ether-based electrolyte to in-situ form a protective layer on the S/CFS composite surface through its nucleophilic reaction with the freshly generated lithium polysulfides(LiPSs)at the very beginning of initial discharge,thus isolating the interior sulfur from the outer electrolyte and inhibiting the further generation of soluble LiPSs.Benefitting from the ultrahigh specific surface area of>3,000 m^(2)·g^(−1),ideal pore size of2.0 cm^(3)·g^(−1)of the CFS host matrix,the S/CFS cathode even with a high S-loading of 80 wt.%(based on the weight of S/CFS composite)can still operate in a solid-phase conversion manner in the VC-ether co-solvent electrolyte to exhibit a high reversible capacity of 1,557 mAh·g^(−1),a high rate capability with 50%remaining capacity at 2 A·g^(−1)and a high cycling efficiency of 99.9%over 500 cycles.The results presented in this work suggest that a combined action of solid-phase conversion electrochemistry and nanoarchitectured host structure may provide a new path for the design and development of practical lithium-sulfur batteries.

关键词： lithium-sulfur batteries solid-phase conversion high sulfur loading cathode edible fungus slag-derived carbon nucleophilic reaction

Understanding of the sodium storage mechanism in hard carbon anodes

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Carbon Energy 2022年第6期4卷 1133-1150页

作者： Xiaoyang Chen Changyu Liu Yongjin Fang Xinping Ai Faping Zhong Hanxi Yang yuliang cao Hubei Key Laboratory of Electrochemical Power Sources College of Chemistry and Molecular SciencesWuhan UniversityWuhanChina Shenzhen National Engineering Research Center of Advanced Energy Storage Materials ShenzhenChina

Hard carbon has been regarded as the most promising anode material for sodiumion batteries(SIBs)due to its low cost,high reversible capacity,and low working potential.However,the uncertain sodium storage mechanism hinders the rational design and synthesis of high-performance hard carbon anode materials for practical SIBs.During the past decades,tremendous efforts have been put to stimulate the development of hard carbon materials.In this review,we discuss the recent progress of the study on the sodium storage mechanism of hard carbon anodes,and the effective strategies to improve their sodium storage performance have been summarized.It is anticipated that hard carbon anodes with high electrochemical properties will be inspired and fabricated for large-scale energy storage applications.

关键词： anode electrochemical energy storage hard carbon sodium-ion batteries sodium storage mechanism

Boosting the sodium storage performance of Prussian blue analogues via effective etching

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Science China Chemistry 2023年第11期66卷 3154-3160页

作者： Yanan Zhao Jian Peng Kean Chen Laibing Luo Hui Chen Hang Zhang Shulei Chou Xiangmin Feng Weihua Chen Ruoyu cao Xinping Ai Yongjin Fang yuliang cao Hubei Key Laboratory of Electrochemical Power Sources College of Chemistry and Molecular SciencesWuhan UniversityWuhan 430072China Institute for Superconducting and Electronic Materials Australian Institute for Innovative MaterialsUniversity of WollongongInnovation CampusSquires WayNorth Wollongong 2522Australia Institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China College of Chemistry and Molecular Engineering Zhengzhou UniversityZhengzhou 450001China

Prussian blue analogues(PBAs)have gained significant popularity as cathode materials for sodium-ion batteries(SIBs)due to their remarkable features such as high capacity and convenient synthesis.However,PBAs usually suffer from kinetic problems during the electrochemical reactions due to sluggish Na~+diffusion in the large crystals,resulting in low-capacity utilization and inferior rate capability.In this study,we present a facile etching method aiming at activating the sodium storage sites and accelerating the Na~+transport of Na_2NiFe(CN)_6(denoted as NaNiHCF)by precisely controlling its morphologies.A progressive corner passivation phenomenon occurred in NaNiHCF during the etching process,which led to a substantial augmentation of the specific surface area as the morphology transitioned from a standard cube to a dice shape.Notably,by controlling the etching time,the obtained NaNiHCF-3 electrode exhibited boosted electrochemical performance with high reversible capacity of 83.5mAh g~(-1)(98.2%of its theoretical capacity),superior rate capability(71.2 mAh g~(-1)at 10 C),and stable cycling life-span at different temperatures.Both experimental and computational methods reveal the remarkably reversible structural evolution process and improved Na~+diffusion coefficient.We believe that this work can serve as an indispensable reference to tailor the structure of PBAs to obtain improved electrochemical performance.

关键词： Prussian blue analogues Na_2NiFe(CN)_6 cathode materials etching sodium-ion batteries

Boosting rate and cycling performance of K-doped Na_(3)V_(2)(PO_(4))_(2)F_(3) cathode for high-energy-density sodium-ion batteries

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Green Energy & Environment 2022年第6期7卷 1253-1262页

作者： Jiexin Zhang YangYang Lai Peng Li Yanxia Wang Faping Zhong Xiangming Feng Weihua Chen Jianjun Liu Xinping Ai Hanxi Yang yuliang cao Engineering Research Center of Organosilicon Compounds&Materials of Ministry of Education College of Chemistry and Molecular SciencesWuhan UniversityWuhan430072China National Engineering Research Center of Advanced Energy Storage Materials Hunan410205China College of Chemistry and Molecular Engineering Zhengzhou UniversityZhengzhou450001China State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of Sciences1295 Dingxi RoadShanghai200050China

As a promising cathode material,Na_(3)V_(2)(PO_(4))_(2)F_(3)(NVPF)has attracted wide attention for sodium-ion batteries(SIBs)because of its high operating voltage and high structural stability.However,the low intrinsic electronic conductivity and insufficient Na ion mobility of NVPF limit its development.Herein,K-doping NVPF is prepared through a facile ball-milling combined calcination method.The effects of K-doping on the crystal structure,kinetic properties and electrochemical performance are investigated.The results demonstrate that the Na_(2.90)K_(0.10)V_(2)(PO_(4))_(3)F_(3)(K0.10-NVPF)exhibits a high capacity(120.8 mAh g^(-1) at 0.1 C),high rate capability(66 mAh g^(-1) at 30 C)and excellent cycling performance(a capacity retention of 97.5%at 1 C over 500 cycles).Also,the occupation site of K ions in the lattice,electronic band structure and Na-ion transport kinetic property in K-doped NVPF are investigated by density functional theory(DFT)calculations,which reveals that the K-doped NVPF exhibits improved electronic and ionic conductivities,and located K^(+) ions in the lattice to contribute to high reversible capacity,rate capability and cycling stability.Therefore,the K-doped NVPF serves as a promising cathode material for high-energy and high-power SIBs.

关键词： Potassium doping Na_(3)V_(2)(PO_(4))_(2)F_(3) Cathode materials Sodium ion batteries Long-term stability

Mixed polyanion cathode materials:Toward stable and high-energy sodium-ion batteries

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Journal of Energy Chemistry 2021年第9期30卷 635-648页

作者： Along Zhao Yongjin Fang Xinping Ai Hanxi Yang yuliang cao Engineering Research Center of Organosilicon Compounds and Materials of Ministry of Education College of Chemistry and Molecular SciencesWuhan UniversityWuhan 430072HubeiChina

Sodium-ion batteries(SIBs)are considered as one of the most fascinating alternatives to lithium-ion batteries for grid-scale energy storage applications because of the low cost and wide abundance of sodium resources.Among various cathode materials,mixed polyanion compounds come into the spotlight as promising electrode materials due to their superior electrochemical properties,such as high working voltage,long cycling stability,and facile reaction kinetics.In this review,we summarize the recent development in the exploration of different mixed polyanion cathode materials for SIBs.We provide a comprehensive understanding of the structure-composition-performance relationship of mixed polyanion cathode materials together with the discussion of their sodium storage mechanisms.It is anticipated that further innovative works on the material design of advanced cathode materials for batteries can be inspired.

关键词： Mixed polyanion compounds Cathode materials Polyanions Energy storage Sodium-ion batteries

A green route to synthesize low-cost and high-performance hard carbon as promising sodium-ion battery anodes from sorghum stalk waste

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Green Energy & Environment 2017年第3期2卷 310-315页

作者： Xiaoming Zhu Xiaoyu Jiang Xiaoling Liu Lifen Xiao yuliang cao Hubei Collaboration Innovation Center of Non-power Nuclear Technology School of Nuclear Technology & Chemistry and Biology Hubei University of Science and Technology Hubei Key Lab.of Electrochemical Power Sources College of Chemistry and Molecular Sciences Wuhan University College of Chemistry Central China Normal University

Sodium-ion batteries(SIBs) have been considered to be potential candidates for next-generation low-cost energy storage systems due to the low-cost and abundance of Na resources. However, it is a big challenge to find suitable anode materials with low-cost and good performance for the application of SIBs. Hard carbon could be a promising anode material due to high capacity and expectable low-cost if originating from biomass. Herein, we report a hard carbon material derived from abundant and abandoned biomass of sorghum stalk through a simple carbonization method. The effects of carbonization temperature on microstructure and electrochemical performance are investigated. The hard carbon carbonized at 1300 ℃ delivers the best rate capability(172 mAh g^(-1) at 200 mA g^(-1)) and good cycling performance(245 mAh g^(-1) after 50 cycles at 20 mA g^(-1),96% capacity retention). This contribution provides a green route for transforming sorghum stalk waste into "treasure"of promising low-cost anode material for SIBs.

关键词： Sorghum stalk Hard carbon Anode Sodium-ion battery Carbonization

LiOH: A "double-edged" effect toward electrochemical oxidation of Li2O2

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Journal of Energy Chemistry 2021年第6期57卷 401-405页

作者： Qinghua Cui Lipo Ma Peng Zhang yuliang cao Jiawei Wang State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences Institute of Materials Engineering Beijing Institute of Collaborative Innovation Laboratory of Advanced Spectro-electrochemistry and Lithium-ion Batteries Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences Department of Materials Science & Engineering Academy for Advanced Interdisciplinary Studies Shenzhen Key Laboratory of Solid State Batteries Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Southern University of Science and Technology College of Chemistry and Molecular Sciences Engineering Research Center of Organosilicon Compounds & Materials of Ministry of Education Wuhan University

The aprotic lithium-oxygen battery(Li-O2battery) has attracted much attraction for the future advanced battery technologies due to its ultra-high theoretical energy density that can well meet the ever-growing energy d... 详细信息

关键词： Lithium-oxygen batteries LiOH-doped Li2O2 Li2O2 oxidation Differential electrochemical mass spectrometer Isotope-labelling

A polyethylene microsphere-coated separator with rapid thermal shutdown function for lithium-ion batteries

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Journal of Energy Chemistry 2020年第5期29卷 33-40页

作者： Chongrong Zhang Hui Li Shixuan Wang yuliang cao Hanxi Yang Xinping Ai Faping Zhong Hubei Key Lab of Electrochemical Power Sources College of Chemistry&Molecular ScienceWuhan UniversityWuhan 430072HubeiChina National Engineering Research Center of Advanced Energy Storage Materials Changsha 410205HunanChina

Thermal runaway is the main factor contributing to the unsafe behaviors of lithium-ion batteries(LIBs)in practical applications.The application of separators for the thermal shutdown has been proven as an effective approach to protecting LIBs from thermal runaway.In this work,we developed a thermal shutdown separator by coating a thin layer of low-density polyethylene microspheres(PM)onto a commercial porous polypropylene(PP)membrane and investigated the thermal response behaviors of the as-prepared PM/PP separator in LIBs.The structural and thermal analysis results revealed that the coated PM layer had a porous structure,which facilitated the occurrence of normal charge-discharge reactions at ambient temperature,although it could melt completely and fuse together within very short time periods:3 s at 110℃and 1 s at 120℃,to block off the pores of the PP substrate,thereby cutting off the ion transportation between the electrodes and interrupting the battery reaction.Consequently,the PM/PP separator exhibits very similar electrochemical performance to that of a conventional separator at ambient temperature.However,it performs a rapid thermal shutdown at an elevated temperature of^110℃,thus controlling the temperature rise and maintaining the cell in a safe status.Due to its synthetic simplicity and low cost,this separator shows promise for possible application in building safe LIBs.

关键词： Thermal shutdown Separator Safety Lithium-ion battery