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high‑Entropy Layered Oxide Cathode Enabling high‑rate for Solid‑State Sodium‑Ion Batteries

Nano-Micro Letters 2024年第1期16卷 160-171页

作者： Tianxun Cai Mingzhi Cai Jinxiao Mu Siwei Zhao Hui Bi Wei Zhao Wujie Dong Fuqiang Huang State Key Laboratory of high performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050People’s Republic of China State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871People’s Republic of China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049People’s Republic of China Zhongke Institute of Strategic Emerging Materials Yixing 214213JiangsuPeople’s Republic of China

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 Na_(0.95)Li_(0.06)Ni_(0.25)Cu_(0.05)Fe_(0.15)Mn_(0.49)O_(2).This cathode delivers a high reversible capacity(141 mAh g^(−1)at 0.2C),excellent rate capability(111 mAh g^(−1)at 8C,85 mAh g^(−1)even 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^(−1)at 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.

关键词： high-entropy high-rate performance Li-TM interaction Air stability O3 layered oxide cathode

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A double-layer covered architecture with spinel phase induced by LiPP for Co-free Li-rich cathode with high-rate performance and long lifespan

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Nano Research 2023年第5期16卷 6805-6814页

作者： Ruiqi Zhao Manman Wu Peixin Jiao Xueting Wang Jie Zhu Yang Zhao Hongtao Zhang Kai Zhang Chenxi Li Yanfeng Ma Yongsheng Chen The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin 300071China State Key Laboratory of Elemento-Organic Chemistry Nankai UniversityTianjin 300071China Renewable Energy Conversion and Storage Center(RECAST) Nankai UniversityTianjin 300071China Department Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China Engineering Research Center of high-efficiency Energy Storage(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China

Co-free Li-rich Mn-based layered oxides are promising candidates for next-generation lithium-ion batteries(LIBs)due to their high specific capacity,high voltage,low cost.However,their commercialization is hindered by limited cycle life and poor rate performance.Herein,an in-situ simple and low-cost strategy with a nanoscale double-layer architecture of lithium polyphosphate(LiPP)and spinel phase covered on top of the bulk layered phase,is developed for Li_(1.2)Mn_(0.6)Ni_(0.2)O_(2)(LMNO)using Li^(+)-conductor LiPP(denoted as LMNO@S-LiPP).With such a double-layer covered architecture,the half-cell of LMNO@S-LiPP delivers an extremely high capacity of 202.5 mAh·g^(−1)at 1 A·g^(−1)and retains 85.3%of the initial capacity after 300 cycles,so far,the best highrate electrochemical performance of all the previously reported LMNOs.The energy density of the full-cell assembled with commercial graphite reaches 620.9 Wh·kg^(−1)(based on total weight of active materials in cathode and anode).Mechanism studies indicate that the superior electrochemical performance of LMNO@S-LiPP is originated from such a nanoscale double-layer covered architecture,which accelerates Li-ion diffusion,restrains oxygen release,inhibits interfacial side reactions,suppresses structural degradation during cycling.Moreover,this strategy is applicable for other high-energy-density cathodes,such as LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2),Li_(1.2)Ni_(0.13)Co_(0.13)Mn_(0.54)O_(2),LiCoO_(2).Hence,this work presents a simple,cost-effective,scalable strategy for the development of high-performance cathode materials.

关键词： Co-free Li-rich layered oxides double-layer covered architecture lithium polyphosphate high-rate performance long cycle life

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Phosphorus/nitrogen co-doped hollow carbon fibers enabling high-rate potassium storage

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稀有金属:英文版 2023年第8期42卷 2622-2632页

作者： Yu Zhou Shuang Tian Min-Yu Jia Pei-Bo Gao Guang-Chao Yin Xiao-Mei Wang Jing-Lin Mu Jin Zhou Tong Zhou School of Physics and Optoelectronic Engineering Shandong University of TechnologyZibo 255049China School of Chemistry and Chemical Engineering Shandong University of TechnologyZibo 255049China

Potassium-ion hybrid capacitors(PIHCs)reconcile the advantages of batteries and supercapacitors,exhibiting both good energy density and high-power density.However,the low-rate performance and poor cycle stability of battery-type anodes hinder their practical application.Herein,phosphorus/nitrogen co-doped hollow carbon fibers(P-HCNFs)are prepared by a facile template method.The stable grape-like structure with continuous and interconnected cavity structure is an ideal scaffold for shortening the ion transport and relieving volume expansion,while the introduction of P atoms and intrinsic N atoms can create abundant extrinsic/intrinsic defects and additional active sites,reducing the K+diffusion barrier and improving the capacitive-controlled capacity.The P-HCNFs delivers a high specific capacity of 310 mAh·g^(-1)at 0.1 A·g^(-1)with remarkable ultra-high-rate performance(140 mAh·g^(-1)at 50 A·g^(-1))and retains an impressive capacity retention of 87%after 10,000 cycles at 10 A·g^(-1).As expected,the as-assembled PIHCs present a high energy density(115.8 Wh·kg^(-1)at 378.0 W·kg^(-1))and excellent capacity retention of 91%after 20,000 cycles.This work not only shows great potential for utilizing heteroatom-doping and structural design strategies to boost potassium storage,but also paves the way for advancing the practicality of high-energy PIHCs devices.

关键词： Potassium-ion hybrid capacitors(PIHCs) Hollow carbon anodes Phosphorus/nitrogen cooping high-rate performance

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Synergetic effect of lattice distortion and oxygen vacancies on high-rate lithium-ion storage in high-entropy perovskite oxides

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Journal of Advanced Ceramics 2023年第6期12卷 1214-1227页

作者： Yanggang Jia Shijie Chen Xia Shao Jie Chen Dao-Lai Fang Saisai Li Aiqin Mao Canhua Li aSchool of Materials Science and Engineering Anhui University of TechnologyMa'anshan 243032China Key Laboratory of Green Fabrication and Surface Technology of Advanced Metal Materials Ministry of EducationAnhui University of TechnologyMa'anshan 243002China School of Metallurgical Engineering Anhui University of TechnologyMa'anshan 243032China

high-entropy oxides(HEOs)have gained great attention as an emerging kind of highperformance anode materials for lithium-ion batteries(LIBs)due to the entropy stabilization and multi-principal synergistic effect.Herein,the porous perovskite-type RE(Co_(0.2)Cr_(0.2)Fe_(0.2)Mn_(0.2)Ni_(0.2))O_(3)(RE(=La,Sm,and Gd)is the abbreviation of rare earth)HEOs were successfully synthesized by a solution combustion synthesis(SCS)method.Owing to the synergistic effect of lattice distortion and oxygen vacancies(Ov),the Gd(Co_(0.2)Cr_(0.2)Fe_(0.2)Mn_(0.2)Ni_(0.2))O_(3) electrode exhibits superior high-rate lithium-ion storage performance and excellent cycling stability.A reversible capacity of 403 mAh·g^(-1) at a current rate of 0.2 A·g^(-1) after 500 cycles and a superior high-rate capacity of 394 mAh·g^(-1)even at 1.0 A·g^(-1)after 500 cycles are achieved.Meanwhile,the Gd(Co_(0.2)Cr_(0.2)Fe_(0.2)Mn_(0.2)Ni_(0.2))O_(3) electrode also exhibits a pronounced pseudo-capacitive behavior,contributing to an additional capacity.By adjusting and balancing the lattice distortion and oxygen vacancies of the electrode materials,the lithium-ion storage performance can be further regulated.

关键词： high-entropy anode perovskite oxides lattice distortion oxygen vacancies(Ov) pseudocapacitance high-rate performance

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Tuning dual-atom mediator toward high-rate bidirectional polysulfide conversion in Li-S batteries

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Journal of Energy Chemistry 2023年第12期87卷 462-472,I0012页

作者： Yifan Ding Zhongti Sun Jianghua Wu Tianran Yan Lin Shen Zixiong Shi Yuhan Wu Xiaoqing Pan Liang Zhang Qiang Zhang Jingyu Sun College of Energy Soochow Institute for Energy and Materials InnovationsKey Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006JiangsuChina School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina National Laboratory of Solid-State Microstructures Jiangsu Key Laboratory of Artificial Functional MaterialsCollege of Engineering and Applied Sciences and Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210093JiangsuChina Institute of Functional Nano&Soft Materials Jiangsu Provincial Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215006JiangsuChina Department of Chemical Engineering Tsinghua UniversityBeijing 100084China

An emerging practice in the realm of Li-S batteries lies in the employment of single-atom catalysts(SACs)as effective mediators to promote polysulfide conversion,but monometallic SACs affording isolated geometric dispersion and sole electronic configuration limit the catalytic benefits and curtail the cell performance.Here,we propose a class of dual-atom catalytic moieties comprising hetero-or homo-atomic pairs anchored on N-doped graphene(NG)to unlock the liquid–solid redox puzzle of sulfur,readily realizing Li-S full cell under high-rate-charging conditions.As for Fe-Ni-NG,in-depth experimental and theoretical analysis reveal that the hetero-atomic orbital coupling leads to altered energy levels,unique electronic structures,and varied Fe oxidation states in comparison with homo-atomic structures(FeFe-NG or Ni-Ni-NG).This would weaken the bonding energy of polysulfide intermediates and thus enable facile electrochemical kinetics to gain rapid liquid-solid Li_(2)S_(4)?Li_(2)S conversion.Encouragingly,a Li-S battery based on the S@Fe-Ni-NG cathode demonstrates unprecedented fast-charging capability,documenting impressive rate performance(542.7 mA h g^(-1)at 10.0 C)and favorable cyclic stability(a capacity decay of 0.016%per cycle over 3000 cycles at 10.0 C).This finding offers insights to the rational design and application of dual-atom mediators for Li-S batteries.

关键词： Li-S batteries Reaction kinetics Dual-atom rate-determining step high-rate performance

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二维材料TiNCl用于类电容式锂离子储能

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Science China Materials 2022年第11期65卷 2942-2948页

作者：樊灵刚张绍宁董武杰徐吉健车相立李睿哲毕辉黄富强 State Key Laboratory of high performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

本研究利用结构设计理念将TiNCl应用于高倍率锂离子电池,并解释其储能机理.由于Ti-N层的高导电性,它可作为电子导电单元.由Cl层构成的多面体通道有助于锂离子的传输,并作为离子传输单元.此外,由于TiNCl中的Cl带负电的特性,负极材料在1 m... 详细信息

本研究利用结构设计理念将TiNCl应用于高倍率锂离子电池,并解释其储能机理.由于Ti-N层的高导电性,它可作为电子导电单元.由Cl层构成的多面体通道有助于锂离子的传输,并作为离子传输单元.此外,由于TiNCl中的Cl带负电的特性,负极材料在1 mV s^(-1)下的赝电容贡献率高达99.5%.而在50 C的高倍率下,经过1000次循环后,它依旧保持极高的可逆比容量(202 mA h g^(-1)).这种基于结构单元的设计理念对于研发高性能新型电极材料具有指导意义.

关键词： lithium-ion battery high-rate performance TiNCl titanium-based anode

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Development of a roll-to-roll high-speed laser micro processing machine for preparing through-holed anodes and cathodes of lithium-ion batteries

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International Journal of Extreme Manufacturing 2023年第3期5卷 534-546页

作者： Mitsuru Yamada Naohiko Soma Masaya Tsuta Susumu Nakamura Nobuo Ando Futoshi Matsumoto Department of Materials and Life Chemistry Kanagawa University3-27-1RokkakubashiKanagawa-kuYokohamaKanagawa221-8686Japan Wired Co. Ltd2-4-15kitashinboSanjoNiigata955-0861Japan Department of Electrical and Electronic Systems Engineering National Institute of TechnologyNagaoka College888NishikatakaiNagaokaNiigata940-8532Japan Research Institute for Engineering Kanagawa University3-27-1RokkakubashiKanagawa-kuYokohamaKanagawa221-8686Japan

Aiming to improve the battery performance of lithium-ion batteries(LIBs),modification of the cathodes and anodes of LIBs using laser beams to prepare through-holes,non-through-holes or ditches arranged in grid and line patterns has been proposed by many researchers and engineers.In this study,a laser processing system attached to rollers,which realizes this modification without large changes in the present mass-production system,was developed.The laser system apparatus comprises roll-to-roll equipment and laser equipment.The roll-to-roll equipment mainly consists of a hollow cylinder with openings on its circumferential surface.Cathode and anode electrodes for LIBs are wound around the cylinder in the longitudinal direction of the electrodes.A pulsed beam reflected from the central axis of the cylinder can continuously open a large number of through-holes in the thin electrodes.Through-holes were formed at a rate of 100000 holes per second on lithium iron phosphate cathodes and graphite anodes with this system.The through-holed cathodes and anodes prepared with this system exhibited higher C-rate performance than nontreated cathodes and anodes.

关键词： lithium-ionbatteries laser processingsystem roll-to-roll system through-holing structure high-rate performance

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Review of the structure and performance of through-holed anodes and cathodes prepared with a picosecond pulsed laser for lithium-ion batteries

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International Journal of Extreme Manufacturing 2023年第1期5卷 1-20页

作者： Futoshi Matsumoto Mitsuru Yamada Masaya Tsuta Susumu Nakamura Nobuo Ando Naohiko Soma Department of Material and Life Chemistry Faculty of EngineeringKanagawa University3-27-1 Rokkakubashikanagawa-kuYokohama 221-8686Japan Department of Electrical and Electronic Systems Engineering National Institute of TechnologyNagaoka College888 NishikatakaiNagaokaNiigata 940-8532Japan Research Institute for Engineering Kanagawa University3-27-1RokkakubashiKanagawa-kuYokohamaKanagawa 221-8686Japan Wired Co. Ltd1628 Hitotsuyashiki ShindenSanjoNiigata 959-1152Japan

To move the performance of lithium-ion batteries into the next stage,the modification of the structure of cells is the only choice except for the development of materials exhibiting higher performance.In this review paper,the employment of through-holing structures of anodes and cathodes prepared with a picosecond pulsed laser has been proposed.The laser system and the structure for improving the battery performance were introduced.The performance of laminated cells constructed with through-holed anodes and cathodes was reviewed from the viewpoints of the improvement of high-rate performance and energy density,removal of unbalanced capacities on both sides of the current collector,even greater high-rate performance by hybridizing cathode materials and removal of irreversible capacity.In conclusion,the points that should be examined and the problem for the through-holed structure to be in practical use are summarized.

关键词： lithium-ionbattery picosecond pulsedlaser through-holed structure high-rate performance energydensity prelithiation

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Phosphorus-doped lithium- and manganese-rich layered oxide cathode material for fast charging lithium-ion batteries

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Journal of Energy Chemistry 2021年第11期30卷 538-545,I0012页

作者： Yuqiong Kang Xingang Guo Zhiwu Guo Jiangang Li Yunan Zhou Zheng Liang Cuiping Han Xiangming He Yun Zhao Naser Tavajohi Baohua Li School of Chemical Engineering Beijing Institute of Petrochemical TechnologyBeijing 102617China Engineering Laboratory for Next Generation Power and Energy Storage Batteries Graduate School at ShenzhenTsinghua UniversityShenzhen 518055GuangdongChina School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai 200240China Institute of Nuclear&New Energy Technology Tsinghua UniversityBeijing 100084China Department of Chemistry Chemical-Biological CentreUmeåUniversityUmeå90187Sweden Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology Beijing 102617China

Owing to their high theoretical specific capacity and low cost, lithium- and manganese-rich layered oxide (LMR) cathode materials are receiving increasing attention for application in lithium-ion batteries. However, poor lithium ion and electron transport kinetics plus side effects of anion and cation redox reactions hamper power performance and stability of the LMRs. In this study, LMR Li_(1.2)Mn_(0.6)Ni_(0.2)O_(2) was modified by phosphorus (P)-doping to increase Li+ conductivity in the bulk material. This was achieved by increasing the interlayer spacing of the lithium layer, electron transport and structural stability, resulting in improvement of the rate and safety performance. P^(5+) doping increased the distance between the (003) crystal planes from ~0.474 nm to 0.488 nm and enhanced the structural stability by forming strong covalent bonds with oxygen atoms, resulting in an improved rate performance (capacity retention from 38% to 50% at 0.05 C to 5 C) and thermal stability (50% heat release compared with pristine material). First-principles calculations showed the P-doping makes the transfer of excited electrons from the valence band to conduction band easier and P can form a strong covalent bond helping to stabilize material structure. Furthermore, the solid-state electrolyte modified P5+ doped LMR showed an improved cycle performance for up to 200 cycles with capacity retention of 90.5% and enhanced initial coulombic efficiency from 68.5% (pristine) or 81.7% (P-doped LMR) to 88.7%.

关键词： Lithium-ion battery Lithium-and manganese-rich layered oxide Phosphorus doping high-rate performance

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highly Efficient Na+ Storage in Uniform Thorn Ball-Like α-MnSe/C Nanospheres

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Acta Metallurgica Sinica(English Letters) 2021年第3期34卷 373-382页

作者： Zhenzhe Li Shuhao Xiao Jiawei Liu Xiaobin Niu Yong Xiang Tingshuai Li Jun Song Chen School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 610054China Center for Applied Chemistry University of Electronic Science and Technology of ChinaChengdu 611731China

Because of its high theoretical capacity,MnSe has been identified as a promising candidate as the anode material for sodiumion batteries.However,its fast capacity deterioration due to the huge volume change during the intercalation/deintercalation of sodium ions severely hinders its practical application.Moreover,the sodium storage mechanism of MnSe is still under discussion and requires in-depth investigations.Herein,the unique thorn ball-likeα-MnSe/C nanospheres have been prepared using manganese-containing metal organic framework(Mn-MOF)as a precursor followed by in situ gas-phase selenization at an elevated temperature.When serving as the anode material for sodium-ion battery,the as-preparedα-MnSe/C exhibits enhanced sodium storage capabilities of 416 and 405 mAh g^(-1)at 0.2 and 0.5 A g^(-1)after 100 cycles,respectively.It also shows a superior capacity retention of 275 mA h g^(-1)at 10 A g^(-1)after 2000 cycles,and a rate performance of 279 mA h g^(-1)at 20 A g^(-1).Such sodium storage properties could be attributed to the unique structure offering a highly efficient Na+diffusion kinetics with a diffusion coefficient between 1×10^(-11) and 3×10^(-10) cm^(2) s-1.The density functional theory calculation indicates that the fast Na+diffusion mainly takes place on the(100)plane of MnSe along a V-shaped path because of a relatively low diffusion energy barrier of 0.15 eV.

关键词： MnSe Sodium storage mechanism high-rate performance Long-term stability Uniform nanospheres

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