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nano Research 2024年第4期17卷 2755-2762页

作者： Peiyu Hou Mohan Dong Zhenbo Sun Feng Li School of Physics and Technology University of JinanJinan 250022China

Layered P2-type cathodes with high voltage,large capacity,and easy synthesis show great potential for developing sodium(na)-ion batteries(NIBs).However,the P2–O2 phase transition makes their structural degradation and the na^(+)/vacancy ordering lowers their redox kinetics.Here,we rationally propose a compositionally graded P2-type cathode,where nickel(Ni)and manganese(Mn)fractions decrease gradually,and cobalt(Co)content increases contiguously from the inside to the outside of a secondary particle.Inside these particles,the Ni/Mn-based compound delivers high capacity and high voltage.On the surface of particles,the Co/Mn-based solid solution offers a stable buffer matrix.Benefiting from these synergistic effects,this graded P2-type cathode shows the elimination of P2–O2 transformation even when charged to 4.4 V,which enables good structural stability,maintaining capacity retention reaching~80%within 300 cycles.Moreover,the na^(+)/vacancy ordering superstructure is further suppressed,and the na^(+)diffusion kinetics is significantly improved.The proposed graded structure with optimized chemical composition offers a new perspective for eliminating the unwanted phase transition and thus enhancing the electrochemistry of high-voltage layered cathodes for advanced NIBs.

关键词： na-ion battery P2-type cathode composition regulation phase transition redox stability

Edge Engineering of MoS2 nanoribbons as High Performance Electrode Material for na-ion battery： A First-Principle Study

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Chinese Journal of Chemistry 2017年第6期35卷 896-902页

作者： Jianbin Wang Qing Zhao Jun Chen Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) College of Chemistry Nankai University Tian/in 300071 China Collaborative Innovation Center of Chemical Science and Engineering Nankai University Tianjin 300071 China

Substantial effort has been made to search for electrode materials of na-ion batteries with high energy/power density. The application of S-saturated zigzag MoS2 nanoribbons （MoSzNRs） for na-ion batteries has been explored through density function theory （DFT）. The theoretical maximum specific capacity reaches 386.4 mAh,g t via dou- ble-side and special edge adsorption mode. The electronic structure reveals that there exists charge transfer between na and MoS2NRs. The diffusion barrier on MoS2NRs （0.17 eV） is much lower than that of bulk MoS2 （1.15 eV）, indicating an excellent diffusion kinetics, in addition, the S-edge in MoS2NRs plays a key role. Firstly, the Mo edge was half saturated by S, which helps to stabilize the MoS2NRs as well as offer more intercalation sites for na. On the other hand, na migrates much faster on the S edge route in MoS2NRs. Our computational results show that S-saturated MoSzNRs exhibit a great potential as electrode materials for na-ion batteries with high performance.

关键词： MoS2 nanoribbons na-ion battery S-saturated edge effect density function theory

Tailoring interphase structure to enable high-rate, durable sodium-ion battery cathode

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Journal of Energy Chemistry 2022年第5期31卷 564-571页

作者： na Li Shaofei Wang Enyue Zhao Wen Yin Zhigang Zhang Kang Wu Juping Xu Yoshihiro Kuroiwa Zhongbo Hu Fangwei Wang Jinkui Zhao Xiaoling Xiao College of Materials Science and Opto-electronic Technology Center of Materials Science and Optoelectronics EngineeringUniversity of Chinese Academy of SciencesBeijing 100049China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China Spallation Neutron Source Science Center Dongguan 523803GuangdongChina Songshan Lake Materials Laboratory Dongguan 523808GuangdongChina Department of Physical Science Hiroshima UniversityHigashihiroshimaHiroshima 739-8526Japan Beijing national Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China

na-based layered transition metal oxides with O_(3)-type structure have been considered to be promising cathodes for na-ion batteries. However, the intrinsically limited na-ion conductivity induced by the Otype na-coordinate environment compromises their rate and cycle capability, hindering their practical application. Here, we report an interphase-structure tailoring strategy that improves the electrochemical properties of O_(3)-type layered cathodes achieved through surface coating and doping processes.Specifically, a Zr-doped interphase structure is designed in the model compound naNi_(1/3)Mn_(1/3)Fe_(1/3)O_(2) using the ionic conductor na_(3)Zr_(2)Si_(2)PO_(12) as the surface coating material and Zr-dopant provider. We discover that the modified naNi_(1/3)Mn_(1/3)Fe_(1/3)O_(2)cathode shows a stable na-storage structure as well as an enhanced rate/cycle capability. Combined with theoretical calculations, it is suggested that the superior electrochemical performances originate from the Zr-doped interphase structure, which has an enlarged na layer spacing that forms favorable na-ion diffusion channels. This work highlights a general material interface optimization method which opens a new perspective for fabricating high-performance electrodes for na-ion batteries and beyond.

关键词： na-ion battery naNi_(1/3)Mn_(1/3)Fe_(1/3)O_(2)cathode Interphase structure Zr doping Surface interface modification

P2-na_(2/3)Ni_(2/3)Te_(1/3)O_(2)Cathode for na-ion Batteries with High Voltage and Excellent Stability

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Energy & Environmental Materials 2023年第2期6卷 54-61页

作者： Wenhui Wang Jiaolong Zhang Chaolin Li Xiaohang Kou Baohua Li Denis Y.W.Yu School of Civil and Environmental Engineering Harbin Institute of TechnologyShenzhen 518055China School of Energy and Environment City University of Hong KongHong Kong China School of Materials Science and Engineering Dongguan University of TechnologyDongguan 523808China Shenzhen Key Laboratory on Power battery Safety Research and Shenzhen Geim Graphene Center Tsinghua Shenzhen International Graduate SchoolShenzhen 518055China

Air-stable layered structured cathodes with high voltage and good cycling stability are highly desired for the practical application of na-ion batteries.Herein,we report a P2-na_(2/3)Ni_(2/3)Te_(1/3)O_(2) cathode that is stable in ambient air with an average operating voltage of~3.8 V,demonstrating excellent cycling stability with a capacity retention of more than 92.7%after 500 cycles at 20 mA g^(-1) and good rate capability with 91.9%capacity utilization at 500 mA g^(-1) with respect to capacity at 5 mA g^(-1) between 2.0 and 4.0 V.When the upper cutoff voltage is increased to 4.4 V,P2-na_(2/3)Ni_(2/3)Te_(1/3)O_(2) delivers a reversible capacity of 71.9 mAh g^(-1) and retains 91.8%of the capacity after 100 cycles at 20 mA g^(-1).The charge compensation during charge/discharge is mainly due to the redox couple of Ni^(2+)/Ni^(3+)in the host with a small amount of contribution from oxygen.The stable structure of the material without phase transformation and with small volume change during charge-discharge allows it to give excellent cycle performance especially when the upper cutoff voltage is not higher than 4.2 V.

关键词： air stability cathode na_(2)Ni_(2)TeO_(6) na-ion battery oxygen redox reaction P2 structure

Tuning anionic redox activity to boost high-performance sodium-storage in low-cost na_(0.67)Fe_(0.5)Mn_(0.5)O_(2) cathode

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Journal of Energy Chemistry 2022年第10期31卷 214-222,I0005页

作者： Jianyue Jiao Kang Wu na Li Enyue Zhao Wen Yin Zhongbo Hu Fangwei Wang Jinkui Zhao Xiaoling Xiao College of Materials Science and Opto-electronic Technology Center of Materials Science and Optoelectronics EngineeringUniversity of Chinese Academy of SciencesBeijing 100049China Songshan Lake Materials Laboratory Dongguan 523808GuangdongChina Spallation Neutron Source Science Center Dongguan 523803GuangdongChina Beijing national Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China

na-based layered iron-manganese oxide na_(0.67)Fe_(0.5)Mn_(0.5)O_(2) containing only low-cost elements is a promising cathode for na-ion batteries used in large-scale energy storage systems.However,the poor cycle stability restricts its practical application.The capacity decay of na_(0.67)Fe_(0.6)Mn_(0.5)O_(2) mainly originates from the irreversible anionic redox reaction charge compensation due to the high-level hybridization between oxygen and iron.Herein,we rationally design a surface Ti doping strategy to tune the anionic redox reaction activity of na_(0.67)Fe_(0.5)Mn_(0.5)O_(2) and improve its na-storage properties.The doped Ti ions not only enlarge the na migration spacing layer but also improve the structure stability thanks to the strong Ti-O bond.More importantly,the d0-shell electronic structure of Ti^(4+) can suppress the charge transfer from the oxidized anions to cations,thus reducing the anionic redox reaction activity and enhancing the reversibility of charge compensation.The modified na_(0.67)Fe_(0.5)Mn_(0.5)O_(2) cathode shows a reversible capacity of 198 mA h g^(-1) and an increased capacity retention from 15% to 73% after about1 month of cycling.Meanwhile,a superior na-ion diffusion kinetics and rate capability are also observed.This work advances the commercialization process of na-based layered iron-manganese oxide cathodes;on the other hand,the proposed modification strategy paves the way for the design of high-performance electrode materials relying on anionic redox reactions.

关键词： na-ion battery P2-na_(0.67)Fe_(0.5)Mn_(0.5)O_(2) Anionic redox reaction Surface Ti doping

Understanding voltage hysteresis and decay during anionic redox reaction in layered transition metal oxide cathodes:A critical review

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nano Research 2023年第3期16卷 3766-3780页

作者： Wei Zheng Gemeng Liang Shilin Zhang Kenneth Davey Zaiping Guo School of Chemical Engineering&Advanced Materials The University of AdelaideAdelaideSA 5005Australia

The emergence of anionic redox reactions in layered transition metal oxide cathodes provides practical opportunity to boost the energy density of rechargeable batteries.However,the activation of anionic redox reaction in layered oxides has significant voltage hysteresis and decay that reduce battery performance and limit commercialization.Here,we critically review the up-todate development of anionic redox reaction in layered oxide cathodes,summarize the proposed reaction mechanism,and unveil their connection to voltage hysteresis and decay based on the state-of-the-art progress.In addition,advances associated with various modification approaches to mitigate the voltage hysteresis/decay in layered transition metal oxide cathodes are also included.Finally,we conclude with an appraisal of further research directions including rational design of high-performance layered oxide cathodes with reversible anionic redox reactions and suppressed voltage hysteresis/decay.Findings will be of immediate benefit to the development of layered oxide cathodes for high performance rechargeable batteries.

关键词： anionic redox reaction voltage hysteresis voltage decay layered transition metal oxides Li-ion battery na-ion battery

ionic covalent organic frameworks with tailored anionic redox chemistry and selective ion transport for high-performance na-ion cathodes

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Journal of Energy Chemistry 2022年第12期75卷 441-447,I0012页

作者： Zhongqiu Tong Hui Wang Tianxing Kang Yan Wu Zhiqiang Guan Fan Zhang Yongbing Tang Chun-Sing Lee Faculty of Metallurgical and Energy Engineering Kunming University of Science and TechnologyKunming 650093YunnanChina Department of Chemistry City University of Hong KongHong Kong 999077China Center of Super-Diamond and Advanced Films(COSDAF) City University of Hong KongHong Kong 999077China Key Laboratory of Material Physics of Ministry of Education School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou 450052HenanChina Shenzhen Institutes of Advanced Technology Chinese Academy of SciencesShenzhen 518055GuangdongChina

Employing cathode materials with multiple redox couples and electrolytes with efficient cation transport kinetics are two effective approaches to improving the electrochemical performance of batteries.In this work,for the first time,we present a design strategy of simultaneously realizing reversible cationic and anionic redox chemistries as well as selective anion/cation transport in the viologen-based COFs(BAVCOF:X,coordinated anions of X=Cl^(-),Br^(-),I^(-),and ClO_(4)^(-))for high-performance na-ion cathodes.Besides the cationic redox of viologen segments,the different redox activities of anions effectively tune the total capacities of the COFs.Meanwhile,electrochemical analysis and ab-initial molecular dynamics(AIMD)calculation illustrate that the anion/cation transport kinetics of electrolytes caged in the COFs'channels can be selectively tuned by the coordinated anions.As a result,combining high-potential Br-/Br_(2)redox couple,cationic redox of viologen segments,and enhanced na+transport kinetics,the BAV-COF:Brdemonstrates stable performance with energy densities of 358.7 and 145.2 Wh kg^(-1)at power densities of 116.5 and 2124.1 W kg^(-1),respectively.This study offers new insight into the fabrication of organic cathodes with anionic redox and the advantages of COFs electrode materials in anion/cation transport selectivity for energy storage applications.

关键词： Cationic and anionic redox chemistries Selective anion/cation transport ionic COFs Organic cathode na-ion battery

A solvothermal pre-oxidation strategy converting pitch from soft carbon to hard carbon for enhanced sodium storage

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Chinese Chemical Letters 2023年第4期34卷 580-583页

作者： Jing Wang Lei Yan Binhua Liu Qingjuan Ren Linlin Fan Zhiqiang Shi Qingyin Zhang Tianjin Key Laboratory of Advanced Fibers and Energy Storage School of Materials Science and EngineeringTiangong UniversityTianjin 300387China School of Chemical Engineering and Technology Tiangong UniversityTianjin 300387China

Due to its low cost and easy availability, the pitch is considered a promising precursor for soft carbon anodes. However, pitch-derived soft carbon shows a high graphitization degree and small interlayer spacing, resulting in its much lower sodium storage performance than hard carbon. We propose a novel preoxidation strategy to introduce additional oxygen atoms into the low-cost soft carbon precursor pitch to fabricate a defect-rich and large-interlayer spacing hard carbon anode(HPP-1100). Compared with the direct pyrolysis of pitch carbon, the sodium storage capacity of HPP-1100 is significantly improved from 120.3 m Ah/g to 306.7 m Ah/g, with an excellent rate and cycling capability(116.5 m Ah/g at 10 C). Moreover, when assorted with an O_(3)-na(NiFeMn)1/3O_(2)cathode, the full cell delivers a high reversible capacity of 274.0 m Ah/g at 0.1 C with superb cycle life. This work provides a new solution for realizing the application of low-cost pitch anodes in na-ion batteries.

关键词： Soft carbon Hard carbon Solvothermal pre-oxidation na-ion battery Pitch

Interwoven scaffolded porous titanium oxide nanocubes/carbon nanotubes framework for high-performance sodium-ion battery

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Journal of Energy Chemistry 2021年第8期30卷 38-46,I0002页

作者： Wen-Bei Yu Wen-Da Dong Chao-Fan Li nasiruddin Macadam Jiu-Xiang Yang Guo-Bin Zhang Zhi-Yi Hu Tien-Chun Wu Yu Li Tawfique Hasan Li-Hua Chen Li-Qiang Mai Bao-Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Cambridge Graphene Centre University of Cambridge9 JJ Thomson AvenueCB30FA CambridgeUnited Kingdom nanostructure Research Centre(NRC) Wuhan University of TechnologyWuhan 430070China Laboratory of Inorganic Materials Chemistry(CMI) University of Namur61 rue de Bruxelles5000 NamurBelgium

Supercapacitor-like na-ion batteries have attracted much attention due to the high energy density of batteries and power density of capacitors.Titanium dioxide(TiO_(2)),is a promising anode material.Its performance is however seriously hindered by its low electrical conductivity and the sluggish diffusion of sodium ions(na^(+))in the TiO_(2)matrix.Herein,this work combines porous TiO_(2)nanocubes with carbon nanotubes(CNTs)to enhance the electrical conductivity and accelerate na^(+)diffusivity for na-ion batteries(NIBs).In this composite,an interwoven scaffolded TiO_(2)/CNTs framework is formed to provide abundant channels and shorter diffusion pathways for electrons and ions.The in-situ X-ray diffraction and cyclic voltammetry confirm the low strain and superior transport kinetics in na^(+)intercalation/extraction processes.In addition,the chemically bonded TiO_(2)/CNTs hybrid provides a more feasible channel for na^(+)insertion/extraction with a much lower energy barrier.Consequently,the TiO_(2)/CNTs composite exhibits excellent electrochemical performance with a capacity of 223.4 m Ah g^(-1)at 1 C and a capacity of 142.8 m Ah g^(-1)at 10 C(3.35 A g^(-1)).The work here reveals that the combination of active materials with CNTs can largely improve the utilization efficiency and enhance their sodium storage.

关键词： Supercapacitor-like Interwoven scaffold na-ion battery TiO_(2) Carbon nanotubes

Growth of SnO_2 nanoflowers on N-doped Carbon nanofibers as Anode for Li-and na-ion Batteries

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nano-Micro Letters 2018年第2期10卷 21-29页

作者： Jiaojiao Liang Chaochun Yuan Huanhuan Li Kai Fan Zengxi Wei Hanqi Sun Jianmin Ma School of Physics and Electronics Hunan University Automotive Engineering Research Institute Jiangsu University Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University

It is urgent to solve the problems of the dramatic volume expansion and pulverization of SnO_2 anodes during cycling process in battery systems. To address this issue, we design a hybrid structure of N-doped carbon fibers@SnO_2 nanoflowers(NC@SnO_2) to overcome it in this work. The hybrid NC@SnO_2 is synthesized through the hydrothermal growth of SnO_2 nanoflowers on the surface of N-doped carbon fibers obtained by electrospinning. The NC is introduced not only to provide a support framework in guiding the growth of the SnO_2 nanoflowers and prevent the flower-like structures from agglomeration, but also serve as a conductive network to accelerate electronic transmission along one-dimensional structure effectively. When the hybrid NC@SnO_2 was served as anode, it exhibits a high discharge capacity of 750 Ah g^(-1) at 1 A g^(-1) after 100 cycles in Li-ion battery and 270 mAh g^(-1) at 100 mA g^(-1) for 100 cycles in na-ion battery, respectively.

关键词： SnO2 nanostructures Anode Li-ion battery na-ion battery