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Journal of Materials Science & Technology 2023年第12期143卷 107-116页

作者： Bao Zhang Baohe Xu Haozhe Qin Liang Cao xing ou Engineering Research Center of the Ministry of Education for Advanced Battery Materials School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083China School of Materials Engineering Changshu Institute of TechnologyChangshu 215500China

The intrinsic poor electrical conductivity,severe dissolution of K x S y intermediates,and inferior conversion reaction reversibility extremely impede the practical application of the transition-metal chalcogenides(TMDs)anode for potassium-ion batteries(PIBs).Herein,a rationally designed Cu_(9)S_(5)/MoS_(2)/C heterostruc-ture hollow nanocage was synthesized with assistance from metal-organic frameworks(MOFs)*** the K-storage process,the homogeneously distributed the sulfiphilic nature of Cu 0 reaction prod-uct could act as a dual-functional catalyst,not only facilitating the rapid charge transfer but also effec-tively anchoring(K x S y)polysulfides,thus boosting K-storage reactions reversibility during the conversion reaction *** applied as an anode for PIBs,the as-prepared heterostructure exhibits excellent reversible capacity and long cycle lifespan(350.5 mAh g^(-1)at 0.1 A g^(-1)and 0.04%per cycle capacity de-cay at 1 A g^(-1)after 1000 cycles).Additionally,the potassium storage mechanism is distinctly revealed by in-situ *** nanoarchitecture designing strategy for the advanced electrode in this work could provide vital guidance for relevant energy storage materials.

关键词： Nanocage hollow structure Metal-organic frameworks Cu_(9)S_(5)-MoS_(2)heterostructure Dual-functional catalyst Potassium-ion batteries

Recycling of spent lithium-ion batteries to resynthesize high-performance cathode materials for sodium-ion storage

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Tungsten 2024年第3期6卷 574-584页

作者： Hai-Qiang Gong xing-Yuan Wang Long Ye Bao Zhang xing ou National Engineering Laboratory for High-Efficiency Recovery of Refractory Nonferrous Metals School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083China

The spent lithium-ion batteries recovery has been brought into focus widely for its environmental imperatives and potential profits from the metal components,such as lithium,cobalt,nickel and ***,the weaker pollution and fewer profits of LiMn_(2)O_(4) cathode dispel the enthusiasm and responsibility of industry ***,a simplified and efncient method to regenerate the sodium-ion cathode materials and separate Li from spent LiMn_(2)O_(4) materials for the profit improvement is *** detail,adjusting the parameters of carbothermal reduction process appropriately,the LiMn_(2)O_(4) spinel structure is destroyed within a short period time and transformed into simple metal *** anticipated,nearly 95 wt.%lithium can be obtained and recovered during the water leaching,while 99 wt.%of manganese can be extracted in acid *** that the leaching residue can return to the carbothermic reduction,leading to a closed-loop economic recycling *** regenerated Na_(0.67)Ni_(0.3)Mn_(0.7)O_(2) cathode displays excellent electrochemical performance with superior cycling stability(the initial capacity reaches 95.9 mAh·g^(-1),and the retention rate reached 98.3%after 100 cycles at 1 C).The delicate strategy of sodium-ion cathode material regenerated from spent LiMn_(2)O_(4) aims to realize lithium separation and material utilization of manganese simultaneously,providing the instructive suggestion to rise up the recycling profits of spent batteries.

关键词： Manganese Spent battery LiMn_(2)O_(4) cathode Recycling Regenerated Na_(0.67)Ni_(0.3)Mn_(0.7)O_(2) Sodium-ion storage

Alleviating the anisotropic microstructural change and boosting the lithium ions diffusion by grain orientation regulation for Ni-rich cathode materials

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Journal of Energy Chemistry 2024年第1期88卷 213-222,I0005页

作者： Xinyou He Shilin Su Bao Zhang Zhiming Xiao Zibo Zhang xing ou Engineering Research Center of the Ministry of Education for Advanced Battery Materials School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083HunanChina Zhejiang Power New Energy Co.Ltd Zhuji 311899ZhejiangChina

Generally,layered Ni-rich cathode materials exhibit the morphology of polycrystalline secondary sphere composed of numerous primary *** the arrangement of primary particles plays a very important role in the properties of Ni-rich *** disordered particle arrangement is harmful to the cyclic performance and structural stability,yet the fundamental understanding of disordered structure on the structural degradation behavior is ***,we have designed three kinds of LiNi_(0.83)Co_(0.06)Mn_(0.11)O_(2) cathode materials with different primary particle orientations by regulating the precursor coprecipitation *** finite element simulation and in-situ characterization,the Li^(+)transport and structure evolution behaviors of different materials are ***,the smooth Li^(+)diffusion minimizes the reaction heterogeneity,homogenizes the phase transition within grains,and mitigates the anisotropic microstructural change,thereby modulating the crack evolution ***,the optimized structure evolution ensures radial tight junctions of the primary particles,enabling enhanced Li^(+)diffusion during dynamic ***-loop bidirectional enhancement mechanism becomes critical for grain orientation regulation to stabilize the cyclic *** precursor engineering with particle orientation regulation provides the useful guidance for the structural design and feature enhancement of Ni-rich layered cathodes.

关键词： Ni-rich cathode Grain orientation regulation Anisotropic microstructural change Precursor engineering Li~+-ions diffusion

Understanding the failure mechanism towards developing high-voltage single-crystal Ni-rich Co-free cathodes

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Green Energy & Environment 2024年第6期9卷 1045-1057页

作者： Jixue Shen Bao Zhang Changwang Hao Xiao Li Zhiming Xiao Xinyou He xing ou Engineering Research Center of the Ministry of Education for Advanced Battery Materials School of Metallurgy and EnvironmentCentral South UniversityChangsha410083China Zhejiang Power New Energy Co. Ltd.Zhuji311899China Material Science and Chemistry Engineering College China University of GeosciencesWuhan430074China

Benefited from its high process feasibility and controllable costs,binary-metal layered structured LiNi_(0.8)Mn_(0.2)O_(2)(NM)can effectively alleviate the cobalt supply crisis under the surge of global electric vehicles(EVs)sales,which is considered as the most promising nextgeneration cathode material for lithium-ion batteries(LIBs).However,the lack of deep understanding on the failure mechanism of NM has seriously hindered its application,especially under the harsh condition of high-voltage without sacrifices of reversible ***,singlecrystal LiNi_(0.8)Mn_(0.2)O_(2) is selected and compared with traditional LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM),mainly focusing on the failure mechanism of Cofree cathode and illuminating the significant effect of Co element on the Li/Ni antisite defect and dynamic ***,the presence of high Li/Ni antisite defect in NM cathode easily results in the extremely dramatic H2/H3 phase transition,which exacerbates the distortion of the lattice,mechanical strain changes and exhibits poor electrochemical performance,especially under the high cutoff ***,the reaction kinetic of NM is impaired due to the absence of Co element,especially at the single-crystal ***,the negative influence of Li/Ni antisite defect is controllable at low current densities,owing to the attenuated ***,Co-free NM can exhibit better safety performance than that of NCM *** findings are beneficial for understanding the fundamental reaction mechanism of single-crystal Ni-rich Co-free cathode materials,providing new insights and great encouragements to design and develop the next generation of LIBs with low-cost and high-safety performances.

关键词： Li/Ni antisite defect Dynamic characteristic High-voltage Single-crystal Ni-rich Co-free cathodes Lithium-ion batteries

Effective regeneration of high-performance anode material recycled from the whole electrodes in spent lithium-ion batteries via a simplified approach

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Green Energy & Environment 2021年第5期6卷 725-733页

作者： Long Ye Chunhui Wang Liang Cao Hougui Xiao Jiafeng Zhang Bao Zhang xing ou National Engineering Laboratory for High Efficiency Recovery of Refractory Nonferrous Metals School of Metallurgy and EnvironmentCentral South UniversityChangsha410083China

Along with the extensive application of energy storage devices,the spent lithium-ion batteries(LIBs)are unquestionably classified into the secondary resources due to its high content of several valuable ***,current recycling methods have the main drawback to their tedious process,especially the purification and separation ***,we propose a simplified process to recycle both cathode(LiCoO_(2))and anode(graphite)in the spent LIBs and regenerate newly high-performance anode material,CoO/CoFe2O4/expanded graphite(EG).This process not only has the advantages of succinct procedure and easy control of reaction conditions,but also effectively separates and recycles lithium from transition *** 98.43%of lithium is recovered from leachate when the solid product CoO/CoFe2O4/EG is synthesized as anode material for *** the product exhibits improved cyclic stability(890 mAh g^(-1) at 1 A g^(-1) after 700 cycles)and superior rate capability(208 mAh g^(-1) at 5 A g^(-1)).The merit of this delicate recycling design can be summarized as three aspects:the utilization of Fe impurity in waste LiCoO_(2),the transformation of waste graphite to EG,and the regeneration of anode *** approach properly recycles the valuable components of spent LIBs,which introduces an insight into the future recycling.

关键词： Spent lithium ion battery Regenerating Anode material Succinct procedure High-added value

Van der Waals heterostructure engineering by 2D space-confinement for advanced potassium-ion storage

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Nano Research 2021年第11期14卷 3854-3863页

作者： Bi Luo Peng Wu Jiafeng Zhang Liang Cao Chunhui Wang Bin Lu Bao Zhang xing ou National Engineering Laboratory for High Efficiency Recovery of Refractory Nonferrous Metals School of Metallurgy and EnvironmentCentral South UniversityChangsha410083China Key Laboratory on Fuel Cell Technology of Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou510641China Institute of Advanced Magnetic Materials College of Materials&Environmental EngineeringHangzhou Dianzi UniversityHangzhou310018China

Molybdenum disulfide (MoS_(2)) has received enormous attentions in the electrochemical energy storage due to its unique two-dimensional layered structure and relatively high reversible capacity. However, the application of MoS_(2) in potassium-ion batteries (PIBs) is restricted by poor rate capability and cyclability, which are associated with the sluggish reaction kinetics and the huge volume expansion during K+ intercalation. Herein, we propose a two-dimensional (2D) space confined strategy to construct van der Waals heterostructure for superior PIB anode, in which the MoS_(2) nanosheets can be well dispersed on reduced graphene oxide nanosheets by leveraging the confinement effect within the graphene layers and amorphous carbon. The strong synergistic effects in 2D van der Waals heterostructure can extremely promote the electron transportation and ions diffusion during K+ insertion/extraction. More significantly, the 2D space-confinement effect and van der Waals force inhibit polysulfide conversion product dissolution into the electrolyte, which significantly strengthens the structural durability during the long-term cycling process. As anticipated, the as-synthesized the “face-to-face” C/MoS_(2)/G anode delivers remarkable K-storage performance, especially for high reversible capacity (362.5 mAh·g^(-1) at 0.1 A·g^(-1)), excellent rate capability (195.4 mAh·g^(-1) at 10 Ag^(-1)) and superior ultrahigh-rate long-cycling stability (126.4 mAh·g^(-1) after 4000 cycles at high rate of 5 A·g^(-1)). This work presents a promise strategy of structure designing and composition optimization for 2D layered materials in advanced energy storage application.

关键词： van der Waals heterostructure space confinement molybdenum disulfide anode materials potassium-ion batteries

A flexible carbon nanotube@V_(2)O_(5) film as a high-capacity and durable cathode for zinc ion batteries

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Journal of Energy Chemistry 2021年第8期30卷 126-133,I0004页

作者： Xiaowei Wang Liqun Wang Bao Zhang Jianmin Feng Jiafeng Zhang xing ou Feng Hou Ji Liang School of Metallurgy and Environment Central South UniversityChangsha 410083China College of Physics and Materials Science Tianjin Normal University300387 TianjinChina Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and EngineeringTianjin University300072 TianjinChina Institute for Superconducting&Electronic Materials(ISEM) Australian Institute of Innovative Materials(AIIM)Innovation CampusSquires WayUniversity of Wollongong2522 Australia

Aqueous zinc-ion batteries(ZIBs)are receiving a continuously increasing attention for mobile devices,especially for the flexible and wearable electronics,due to their non-toxicity,non-flammability,and low-cost *** the significant progress in achieving higher capacities for electrode materials of ZIBs,to endow them with high flexibility and economic feasibility is,however,still a significant challenge remaining ***,we present a highly flexible composite film composed of carbon nanotube film and V_(2)O_(5)(CNTF@V_(2)O_(5))with high strength and high conductivity,which is prepared by simply impregnating a porous CNT film with an aqueous V_(2)O_(5)sol under *** this material,intimate incorporation between V_(2)O_(5)and CNTs has been achieved,successfully integrating the high zinc ion storage capability with high mechanical *** a result,this CNTF@V_(2)O_(5)film delivers a high capacity of 356.6 m Ah g^(-1)at 0.4 A g^(-1)and excellent cycling stability with 80.1%capacity retention after 500 cycles at 2.0 A g^(-1).The novel strategy and the outstanding battery performance presented in this work should shed light on the development of high-performance and flexible ZIBs.

关键词： Zinc-ion batteries Carbon nanotube films Flexible cathode Wearable devices

Boosting High-Voltage and Ultralong-Cycling Performance of Single-Crystal LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) Cathode Materials via Three-in-One Modification

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Energy & Environmental Materials 2023年第1期6卷 207-217页

作者： Bao Zhang Jixue Shen Qi Wang Changqing Hu Bi Luo Yun Liu Zhiming Xiao xing ou Engineering Research Center of the Ministry of Education for Advanced Battery Materials School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083China Zhejiang Power New Energy Co.Ltd. Zhuji 311899China Beijing Key Laboratory of Environmental Science and Engineering School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China

LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) is extensively researched as one of the most widely used commercially materials for Li-ion batteries at ***,the poor high-voltage performance(≥4.3 V)with low reversible capacity limits its replacement for LiCoO_(2) in high-end digital ***,three-in-one modification,Na-doping and Al_(2)O_(3)@Li_(3)BO_(3) dual-coating simultaneously,is explored for single-crystalline LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(N-NCM@AB),which exhibits excellent high-voltage performance.N-NCM@AB displays a discharge-specific capacity of 201.8 mAh g^(−1) at 0.2 C with a high upper voltage of 4.6 V and maintains 158.9 mAh g^(−1) discharge capacity at 1 C over 200 cycles with the corresponding capacity retention of 87.8%.Remarkably,the N-NCM@AB||graphite pouch-type full cell retains 81.2% of its initial capacity with high working voltage of 4.4 V over 1600 *** importantly,the fundamental understandings of three-in-one modification on surface morphology,crystal structure,and phase transformation of N-NCM@AB are clearly *** Na+doped into the Li–O slab can enhance the bond energy,stabilize the crystal structure,and facilitate Li+***,the interior surface layer of Li^(+)-ions conductor Li_(3)BO_(3) relieves the charge transfer resistance with surface coating,whereas the outer surface Al_(2)O_(3) coating layer is beneficial for reducing the active materials loss and alleviating the electrode/electrolyte parasite *** three-in-one strategy provides a reference for the further research on the performance attenuation mechanism of NCM,paving a new avenue to boost the high-voltage performance of NCM cathode in Li-ion batteries.

关键词： Al_(2)O_(3)/Li_(3)BO_(3)dual-coating Li-ion batteries Na doping single-crystal cathode three-in-one modification

Enhanced rate capability and mitigated capacity decay of ultrahigh-nickel cobalt-free LiNi_(0.9)Mn_(0.1)O_(2) cathode at high-voltage by selective tungsten substitution

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Chinese Chemical Letters 2023年第7期34卷 354-359页

作者： xingyuan Wang Bao Zhang Zhiming Xiao Lei Ming Minghuang Li Lei Cheng xing ou Engineering Research Center of the Ministry of Education for Advanced Battery Materials School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083China

Owing to the further requirement for electric vehicle market, it is appropriate to lower the cost and improve the energy density of lithium-ion batteries by adopting the Co-free and Ni-rich layered ***, their practical application is severely limited by structural instability and slow kinetics. Herein,ultrahigh-nickel cobalt-free LiNi_(0.9)Mn_(0.1)O_(2) cathode is elaborate designed via in-situ trace substitution of tungsten by a wet co-precipitation method following by high-temperature sintering. It is revealed that the in-situ doping strategy of high valence W^(6+) can effectively improve the structure stability by reducing irreversible phase transition and suppressing the formation of microcracks. Moreover, the transformed fine particles determined by W-doping can facilitate the kinetic characteristics by shortening Li^(+) diffusion paths. As expected, 0.3 mol% W-doped LiNi_(0.9)Mn_(0.1)O_(2) cathode exhibits a high specific capacity of 143.5 mAh/g after 200 cycles at high rate of 5 C in the wide potential range of 2.8-4.5 V, representing a potential next-generation cathode with low-cost, high energy-density and fast-charging capabilities.

关键词： Lithium-ion batteries Ultrahigh-nickel cobalt-free cathode In-situ tungsten doping High cut-off voltage Rapid charge performance

Degradation analysis and doping modification optimization for high-voltage P-type layered cathode in sodium-ion batteries

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Journal of Energy Chemistry 2024年第2期89卷 1-9,I0002页

作者： Bao Zhang Yi Zhao Minghuang Li Qi Wang Lei Cheng Lei Ming xing ou Xiaowei Wang National Engineering Laboratory for High-Efficiency Recovery of Refractory Nonferrous Metals School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083HunanChina Zhejiang Power New Energy Co. LTDZhuji 311800ZhejiangChina

Advancing high-voltage stability of layered sodium-ion oxides represents a pivotal avenue for their progress in energy storage *** this,a comprehensive understanding of the mechanisms underpinning their structural deterioration at elevated voltages remains insufficiently *** this study,we unveil a layer delamination phenomenon of Na_(0.67)Ni_(0.3)Mn_(0.7)O_(2)(NNM)within the 2.0-4.3 V voltage,attributed to considerable volumetric fluctuations along the c-axis and lattice oxygen reactions induced by the simultaneous Ni^(3+)/Ni^(4+)and anion redox *** introducing Mg doping to diminished Ni-O antibonding,the anion oxidation-reduction reactions are effectively mitigated,and the structural integrity of the P2 phase remains firmly intact,safeguarding active sites and precluding the formation of novel *** Na_(0.67)Mg_(0.05)Ni_(0.25)Mn_(0.7)O_(2)(NMNM-5)exhibits a specific capacity of100.7 mA h g^(-1),signifying an 83%improvement compared to the NNM material within the voltage of2.0-4.3 *** investigation underscores the intricate interplay between high-voltage stability and structural degradation mechanisms in layered sodium-ion oxides.

关键词： Soidum ion batteries Layer cathode materials P-type High-voltage performance Degradation analysis