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Nano-Micro Letters 2022年第1期14卷 278-294页

作者： Su Hyun Yang Yun Jae Lee Heemin Kang Seung-Keun Park Yun Chan Kang Department of Materials Science and Engineering Korea UniversityAnam-DongSeongbuk-GuSeoul 136-713Republic of Korea Department of Advanced Materials Engineering Chung-Ang University4726 Seodong-daeroDaedeok-myeonAnseong-siGyeonggi-do 17546Republic of Korea

Two-dimensional(2D)MXenes are promising as electrode materials for energy storage,owing to their high electronic conductivity and low diffusion barrier.Unfortunately,similar to most 2D materials,MXene nanosheets easily restack during the electrode preparation,which degrades the electrochemical performance of MXene-based materials.A novel synthetic strategy is proposed for converting MXene into restacking-inhibited three-dimensional(3D)balls coated with iron selenides and carbon.This strategy involves the preparation of Fe_(2)O_(3)@carbon/MXene microspheres via a facile ultrasonic spray pyrolysis and subsequent selenization process.Such 3D structuring effectively prevents interlayer restacking,increases the surface area,and accelerates ion transport,while maintaining the attractive properties of MXene.Furthermore,combining iron selenides and carbon with 3D MXene balls offers many more sites for ion storage and enhances the structural robustness of the composite balls.The resultant 3D structured microspheres exhibit a high reversible capacity of 410 mAh g^(−1) after 200 cycles at 0.1 A g^(−1) in Potassium-ion batteries,corresponding to the capacity retention of 97% as calculated based on 100 cycles.Even at a high current density of 5.0 A g^(−1),the composite exhibits a discharge capacity of 169 mAh g^(−1).

关键词： MXene Spray pyrolysis Iron selenide Potassium-ion batteries 3D structures

SnTe nanoparticles physicochemically encapsulated by double carbon as conversion-alloying anode materials for superior Potassium-ion batteries

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Journal of Materials Science & Technology 2023年第27期158卷 86-95页

作者： Ting Li Yikun Wang Qianwen Zhou Lingling Yuan Shuangyan Qiao Meng Ma Zhengqing Liu Shaokun Chong Frontiers Science Center for Flexible Electronics(FSCFE) Xi’an Institute of Flexible Electronics(IFE)and Xi’an Institute of Biomedical Materials&EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Research&Development Institute of Northwestern Polytechnical University in Shenzhen Shenzhen 518063China

Telluride tin(SnTe)is a promising conversion-alloying anode for Potassium-ion batteries(PIBs)due to its high theoretical specific capacity induced by multi-electron transport reaction and low operating voltage,whereas huge volume expansion and poor kinetics behavior become key scientific bottleneck limiting the battery performances.Herein,SnTe nanoparticles physicochemically wrapped by graphene and nitrogen-doped carbon(SnTe@rGO@NC)are proposed as anode materials for PIBs.The pre-electrostatic interaction urges the formation of Sn-C and Te-C chemical bonds between SnTe and double carbon to strengthen the interfacial stability and electron transfer,and the conductive architecture with hierarchical encapsulation effect is beneficial to maintaining the electrode integrity and electrochemical dynamics.It is demon-strated from first principles calculations and experimental results that SnTe@rGO@NC contributes fast electron transmission,strong K-ion adsorption,and superior K-ion diffusion capability.Ex-situ characteri-zations uncover that SnTe undergoes conversion-alloying dual-mechanism with the products of K_(2)Te and K_(4)Sn_(23)replied on Sn redox site(23SnTe+50K^(+)+50e^(-)↔K_(4)Sn_(23)+23K_(2)Te).Thus,the SnTe@rGO@NC electrode delivers a high initial charge specific capacity of 243.9 mAh g^(-1)at 50 mA g^(-1),superior rate performance(112.6 mAh g^(-1)at 1.0 A g^(-1)),and outstanding cyclic stability at various current densities.

关键词： Potassium-ion batteries Anode materials Tin telluride Chemical bonding Conversion-alloying mechanism

Tungsten chalcogenides as anodes for Potassium-ion batteries

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Tungsten 2024年第2期6卷 278-292页

作者： Yu-Han Wu Wei-Hao Xia Yun-Zhuo Liu Peng-Fei Wang Yu-Hang Zhang Jin-Ru Huang Yang Xu De-Ping Li Li-Jie Ci School of Environmental and Chemical Engineering Shenyang University of TechnologyShenyang 110870China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China State Key Laboratory of Advanced Welding and Joining School of Materials Science and EngineeringHarbin Institute of Technology(Shenzhen)Shenzhen 518055China Department of Chemistry University College LondonLondon WC1H 0AJUnited Kingdom

Potassium-ion batteries(PIBs)by virtue of their strong cost competitiveness and similar electrochemical properties to lithiumion batteries have been deemed to be a promising electrochemical energy storage technology.To promote the application in the commercial market,developing electrode materials with high specifi c capacities,superior cycling stability,and reliable safety is of great importance.Anode materials as an important component of PIBs play a decisive role,among which twodimensional transition metal chalcogenides(2D TMCs)have attracted wide attention owing to their unique material and electrochemical properties.In the 2D TMCs’family,molybdenum chalcogenides as fl agship are the most studied materials and demonstrated the potential as anodes.With the deepening of research on 2D TMCs,another shining member that possesses similar properties to molybdenum chalcogenides,tungsten chalcogenides(WS_(2),WSe_(2),and WTe_(2)),has aroused tremendous attention.Despite many inspiring results,various challenges remain to be further addressed;meanwhile,some results are still unclear and disputed.Herein,this review fi rst introduces their material properties and electrochemical storage mechanisms.Then,we systematically overview the research progress and put forward promoting improvement strategies.Finally,challenges and opportunities that would be future research directions are discussed.

关键词： Electrochemical energy storage Potassium-ion batteries Anodes Tungsten chalcogenides

Reversible Oxygen-Rich Functional Groups Grafted 3D Honeycomb-Like Carbon Anode for Super-Long potassium ion batteries

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Nano-Micro Letters 2022年第9期14卷 132-146页

作者： Na Cheng Wang Zhou Jilei Liu Zhigang Liu Bingan Lu School of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082People’s Republic of China School of Materials Science and Engineering Hunan UniversityChangsha 410082People’s Republic of China School of Physics and Electronics Hunan UniversityChangsha 410082People’s Republic of China

Studies have found that oxygen-rich-containing functional groups in carbon-based materials can be used as active sites for the storage performance of K^(+),but the basic storage mechanism is still unclear.Herein,we construct and optimize 3D honeycomb-like carbon grafted with plentiful COOH/C=O functional groups(OFGC)as anodes for potassium ion batteries.The OFGC electrode with steady structure and rich functional groups can effectively contribute to the capacity enhancement and the formation of stable solid electrolyte interphase(SEI)film,achieving a high reversible capacity of 230 mAh g^(-1) at 3000 mA g^(-1) after 10,000 cycles(almost no capacity decay)and an ultra-long cycle time over 18 months at 100 mA g^(-1).The study results revealed the reversible storage mechanism between K^(+)and COOH/C=O functional groups by forming C-O-K compounds.Meanwhile,the in situ electrochemical impedance spectroscopy proved the highly reversible and rapid de/intercalation kinetics of K+in the OFGC electrode,and the growth process of SEI films.In particular,the full cells assembled by Prussian blue cathode exhibit a high energy density of 113 Wh kg^(-1) after 800 cycles(calculated by the total mass of anode and cathode),and get the light-emitting diodes lamp and ear thermometer running.

关键词： Honeycomb-like Super-long Carbon anode Potassium-ion batteries

Hierarchical Bimetallic Selenides CoSe_(2)–MoSe_(2)/rGO for Sodium/Potassium-ion batteries Anode: Insights into the Intercalation and Conversion Mechanism

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Energy & Environmental Materials 2022年第2期5卷 627-636页

作者： Yanan Xu Xiaofeng Liu Hang Su Shan Jiang Jianmin Zhang Dan Li College of Chemistry Zhengzhou UniversityZhengzhou 450001China Green Catalysis CenterCollege of ChemistryZhengzhou UniversityZhengzhou 450001China

As anode materials for high-performance sodium-ion batteries and Potassium-ion batteries,bimetallic selenides have attracted great concern due to their relatively high electrical conductivity and electrochemical activity.However,the formidable challenge in the reaction process is the large volume change,leading to the structural collapse of material,and eventually the decline in electrochemical performance.Herein,a composite of hierarchical CoSe_(2)–MoSe_(2) tubes anchored on reduced graphene oxide nanosheets(CoSe_(2)–MoSe_(2)/rGO)is designed by an in situ hydrothermal selenization treatment.Benefiting from the synergistic effects between CoSe_(2) and MoSe_(2),unique hierarchical structure,and effective reduced graphene oxide coating,the CoSe_(2)–MoSe_(2)/rGO exhibited improved reaction kinetics and structural stability,and thus good electrochemical properties.A combination mechanism of intercalation and conversion of CoSe_(2)–MoSe_(2)/rGO by forming NaxCoSe_(2) and Mo_(15)Se_(19) as intermediate states is put forward on the basis of in situ and ex situ XRD analyses.

关键词： CoSe_(2) hierarchical structure MoSe_(2) Potassium-ion batteries sodium-ion batteries

Rational design of ultrafine FeSe_(2) nanocrystals emb e dde d within hollow mesoporous carbon bowls for Potassium-ion batteries with long-term cycling stability and high volumetric capacity

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Journal of Materials Science & Technology 2023年第12期143卷 129-139页

作者： Yu Jin Jang Hong Geun Oh Seung-Keun Park Department of Advanced Materials Engineering Chung-Ang University4726Seodong-daeroDaedeok-myeonAnseong-siGyeonggi-do 17546Republic of Korea

Hollow structures are commonly used to alleviate the mechanical stress on electrode materials and to provide more active sites in Potassium-ion batteries(KIBs).Nevertheless,the excessive internal voids within these structures significantly reduce the packing density of particles,resulting in a relatively low volumetric energy density of the fabricated electrodes,which is undesirable for practical use.We designed a hollow mesoporous carbon bowl embedded with ultrafine bis(selanylidene)iron(FeSe 2)nanocrystals(FeSe 2@HMCB)via a controllable impregnation method and subsequent selenization pro-cess for high-performance KIBs.The as-obtained FeSe 2@HMCB can inherit the advantages of conventional hollow carbon-based composites,such as alleviation of volume variation in active materials,abundant ion storage sites,and high electrical conductivity.Simultaneously,the bowl structure has a higher pack-ing density than the conventional hollow structure,resulting in a significant increase in the volumet-ric energy density of the fabricated electrodes.Because of these advantages,the FeSe 2@HMCB exhibits a high,stable reversible capacity of 326 mA h g^(-1) even after 1000 cycles at 0.5 A g^(-1),and excellent rate capacities(182 mA h g^(-1) at 3.0 A g^(-1)).Compared with the hollow structured counterpart,the vol-umetric capacity(mA h cm−3)of FeSe 2@HMCB increased by 60%.Furthermore,a full cell consisting of FeSe 2@HMCB//Prussian blue(PB)exhibits excellent electrochemical performance(99 mA h g^(-1) after 100 cycles at 0.1 A g^(-1)).

关键词： Potassium-ion batteries Iron selenide Bowl-like structure Mesoporous carbon Anode material

Cocoon-shaped P3-type K0.5Mn0.7Ni0.3O2 as an advanced cathode material for Potassium-ion batteries

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Journal of Energy Chemistry 2023年第1期76卷 332-338,I0008页

作者： Liping Duan Jianzhi Xu Yifan Xu Ruiqi Tian Yingying Sun Chuannan Zhu Xiangyin Mo Xiaosi Zhou Jiangsu Key Laboratory of New Power batteries Jiangsu Collaborative Innovation Center of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023JiangsuChina

potassium ion batteries(PIBs)are emerging as potential next-generation energy storage systems on account of their low cost and high theoretical energy density.Nevertheless,they also face challenges of low specific capacity and suboptimal cycling stability.Herein,we synthesize a cocoon-like P3-type K_(0.5)Mn_(0.7)Ni_(0.3)O_(2)(KMNO)cathode material by a self-template method.The KMNO cocoons possess a hierarchical layered architecture composed of nanoparticle stacking,which can accelerate the transport kinetics of potassium ions,mitigate the stress caused by K^(+)intercalation and deintercalation,and improve structural stability.In addition,Ni can not only alleviate the Jahn-Teller distortion and suppress the phase transition to stabilize the structure,but also act as an electrochemically active element,providing the capacity of two electrons from Ni2+to Ni4+.Combining the advantages of structure and nickel substitution,the P3-type KMNO cocoons are used for electrochemical performance testing of PIB cathodes,delivering an excellent rate capability of 57.1 m A h g^(-1)at 500 m A g^(-1)and a remarkable cycling stability of 77.0%over 300 cycles at 100 m A g^(-1).Impressively,the KMNO cocoons//pitch-derived soft carbon assembled full battery exhibits superior electrochemical performance with a reversible capacity of 79.7 m A h g^(-1)at 50 m A g^(-1).Moreover,ex-situ XRD also further reveals a solid solution phase reaction with a volume change of only 1.46%.This work furnishes a suitable approach to fabricating highperformance layered oxide cathodes for PIBs with outstanding cycling stability and rate capability.

关键词： Layered metal oxides Cathode Potassium-ion batteries Cocoons Ex-situ XRD

KVPO_(4)F/carbon nanocomposite with highly accessible active sites and robust chemical bonds for advanced Potassium-ion batteries

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Green Energy & Environment 2023年第5期8卷 1469-1478页

作者： Jianzhi Xu Liping Duan Jiaying Liao Haowei Tang Jun Lin Xiaosi Zhou School of Chemistry and Materials Science Nanjing Normal UniversityNanjing210023China

KVPO_(4)F(KVPF)has been extensively investigated as the potential cathode material for Potassium-ion batteries(PIBs)owing to its high theoretical capacity,superior operating voltage,and three-dimensional Kt conduction pathway.Nevertheless,the electrochemical behavior of KVPF is limited by the inherent poor electronic conductivity of the phosphate framework and unstable electrode/electrolyte interface.To address the above issues,this work proposes an infiltration-calcination method to confine the in-situ grown KVPF into the mesoporous carbon CMK-3(denoted KVPF@CMK-3).The assembled KVPF@CMK-3 nanocomposite features three-dimensional interconnected carbon channels,which not only offer abundant active sites and significantly accelerate K t/electron transport,but also prevent the growth of KVPF nanoparticle agglomerates,hence stabilizing the structure of the material.Additionally,V–F–C bonds are created at the interface of KVPF and CMK-3,which reduce the loss of F and stabilize the electrode interface.Thus,when tested as a cathode material for PIBs,the KVPF@CMK-3 nanocomposite delivers superior reversible capacitiy(103.2 mAh g^(-1) at 0.2 C),outstanding rate performance(90.1 mAh g^(-1) at 20 C),and steady cycling performance(92.2 mAh g^(-1) at 10 C and with the retention of 88.2%after 500 cycles).Moreover,its potassium storage mechanism is further examined by ex-situ XRD and ex-situ XPS techniques.The above synthetic strategy demonstrates the potential of KVPF@CMK-3 to be applied as the cathode for PIBs.

关键词： Potassium-ion batteries Cathode KVPO_(4)F CMK-3 V–F–C bond

Regulating solid electrolyte interphases on phosphorus/carbon anodes via localized high-concentration electrolytes for Potassium-ion batteries

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Journal of Energy Chemistry 2023年第3期78卷 589-605,I0016页

作者： Wei Xiao Peiyi Shi Zhengkui Li Chong Xie Jian Qin Huijuan Yang Jingjing Wang Wenbin Li Jiujun Zhang Xifei Li Key Laboratory of Advanced batteries Materials for Electric Vehicles of China Petroleum and Chemical Industry Federation Institute of Advanced Electrochemical Energy&School of Materials Science and EngineeringXi’an University of TechnologyXi’an 710048ShaanxiChina Engineering Research Center of Conducting Materials and Composite Technology Ministry of EducationXi’an 710048ShaanxiChina School of Materials Science and Engineering Fuzhou UniversityFuzhou 350108FujianChina Center for International Cooperation on Designer Low-carbon&Environmental Materials(CDLCEM) Zhengzhou UniversityZhengzhou 450001HenanChina

The resourceful and inexpensive red phosphorus has emerged as a promising anode material of Potassium-ion batteries(PIBs) for its large theoretical capacities and low redox potentials in the multielectron alloying/dealloying reactions,yet chronically suffering from the huge volume expansion/shrinkage with a sluggish reaction kinetics and an unsatisfactory interfacial stability against volatile electrolytes.Herein,we systematically developed a series of localized high-concentration electrolytes(LHCE) through diluting high-concentration ether electrolytes with a non-solvating fluorinated ether to regulate the formation/evolution of solid electrolyte interphases(SEI) on phosphorus/carbon(P/C) anodes for PIBs.Benefitting from the improved mechanical strength and structural stability of a robust/uniform SEI thin layer derived from a composition-optimized LHCE featured with a unique solvation structure and a superior K+migration capability,the P/C anode with noticeable pseudocapacitive behaviors could achieve a large reversible capacity of 760 mA h g^(-1)at 100 mA g^(-1),a remarkable capacity retention rate of 92.6% over 200 cycles at 800 mA g^(-1),and an exceptional rate capability of 334 mA h g^(-1)at8000 mA g^(-1).Critically,a suppressed reduction of ether solvents with a preferential decomposition of potassium salts in anion-derived interfacial reactions on P/C anode for LHCE could enable a rational construction of an outer organic-rich and inner inorganic-dominant SEI thin film with remarkable mechanical strength/flexibility to buffer huge volume variations and abundant K+diffusion channels to accelerate reaction kinetics.Additionally,the highly reversible/durable full PIBs coupling P/C anodes with annealed organic cathodes further verified an excellent practical applicability of LHCE.This encouraging work on electrolytes regulating SEI formation/evolution would advance the development of P/C anodes for high-performance PIBs.

关键词： Potassium-ion batteries Phosphorus/carbon anodes Localized high-concentration electrolytes Solid electrolyte interphases Interfacial stability

具有共价键特征的金属-有机基团促进高性能钾离子电池

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Science China Materials 2023年第10期66卷 3827-3836页

作者：贾鑫鑫李胜阳陈嵩王磊邓弘立袁艺智孙洪涛符立才朱建鲁兵安 College of Materials Science and Engineering College of Chemistry and Chemical EngineeringCollege of Physics and ElectronicsHunan UniversityChangsha 410082China MOE Key Laboratory of Low-grade Energy Utilization Technologies and Systems School of Energy&Power EngineeringChongqing UniversityChongqing 400044China The Harold&Inge Marcus Department of Industrial&Manufacturing Engineering Materials Research Institute(MRI)The Pennsylvania State UniversityUniversity ParkPennsylvania 16802USA

钾离子电池(PIBs)面临的一个关键问题是设计具有先进结构的负极材料,以实现快速电荷传输以提高钾的存储性能.采用碳二亚胺铁(FeNCN)作为阳极,由于其含有一定数量的共价键且在分子水平上具有稳定的结构,使得储钾系统能够实现优异的电化... 详细信息

钾离子电池(PIBs)面临的一个关键问题是设计具有先进结构的负极材料,以实现快速电荷传输以提高钾的存储性能.采用碳二亚胺铁(FeNCN)作为阳极,由于其含有一定数量的共价键且在分子水平上具有稳定的结构,使得储钾系统能够实现优异的电化学性能.FeNCN阳极具有高导电性,带隙接近0 eV,并且由于其共价键结构具有良好的结构稳定性.此外,无定形反应产物也为离子扩散提供了多种途径.因此,FeNCN阳极表现出高可逆比容量(在50 mA g^(-1)电流密度下具有600 mA h g^(-1)比容量),显著的倍率性能和长寿命循环(电流密度为500 mA g^(-1)时拥有400 mA h g^(-1)比容量且超过300次循环).通过理论模拟、X射线原位衍射分析和X射线光电子能谱分析揭示了Fe^(2+)和K^(+)之间的转化反应机理.此外,将FeNCN负极与苝-3,4,9,10-四羧酸二酐正极材料匹配,组装成的全电池在198.6 Wkg^(-1)的功率密度下实现了184.7 W h kg^(-1)的超高能量密度,明显高于以往所有铁基负极的PIBs或钾离子混合电容器.

关键词： Potassium-ion batteries metal-organic group anodes covalent bond