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Boron-doped high-entropy oxide toward high-rate and long-cycle layered cathodes for wide-temperature sodium-ion batteries

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Journal of Energy Chemistry 2024年第8期95卷 577-587页

作者： Yuzhen Dang Zhe Xu Yurong Wu Runguo Zheng Zhiyuan Wang Xiaopin Lin Yanguo Liu Zheng-Yao Li Kai Sun Dongfeng Chen Dan Wang School of materials Science and Engineering Northeastern University School of Resources and materials Northeastern University at Qinhuangdao key laboratory of dielectric and electrolyte functional material hebei province Neutron Scattering laboratory Department of Nuclear Physics China Institute of Atomic Energy

03-type layered metal oxides hold great promise for sodium-ion batteries cathodes owing to their energy density advantage.However,the severe irreversible phase transition and sluggish Na+diffusion kinetics pose significant challenges to achieve high-performance layered cathodes.Herein,a boron-doped03-type high entropy oxide Na(Fe0.2Co0.15Cu0.05Ni0.2Mn0.2Ti0.2)B0.02O2(NFCCNMT-B0.02) is designed and the covalent B-O bonds with high entropy configuration ensure a robust layered structure.The obtained cathode NFCCNMT-B0.02exhibits impressive cycling performance（capacity retention of 95% and 82% after100 cycles and 300 cycles at 1 and 10 C,respectively） and outstanding rate capability(capacity of 83 mAh g-1at 10 C).Furthermore,the NFCCNMT-B0.02demonstrates a superior wide-temperature performance,maintaining the same capacity level(113,4 mAh g-1@-20℃,121 mAh g-1@25℃,and 119 mAh g-1@60℃) and superior cycle stability（90% capacity retention after 100 cycles at 1 C at-20℃）.The high-entropy configuration design with boron doping strategy contributes to the excellent sodium-ion storage performance.The high-entropy configuration design effectively suppresses irreversible phase transitions accompanied by small volume changes（ΔV=0.65 ?3）.B ions doping expands the Na layer distance and enlarges the P3 phase region,thereby enhancing Na+diffusion kinetics.This work offers valuable insights into design of high-performance layered cathodes for sodium-ion batteries operating across a wide temperature.

关键词： Born substitution High entropy oxide Na+ diffusion kinetics Phase transition Sodium-ion batteries

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Tuning interface mechanism of FeCo alloy embedded N,S-codoped carbon substrate for rechargeable Zn-air battery

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Journal of Energy Chemistry 2024年第6期93卷 400-410,I0010页

作者： Hui Chang Lulu Zhao Shan Zhao Zong-Lin Liu Peng-Fei Wang Ying Xie Ting-Feng Yi School of materials Science and Engineering Northeastern UniversityShenyang 110819LiaoningChina key laboratory of functional Inorganic material Chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080HeilongjiangChina key laboratory of dielectric and electrolyte functional material hebei province School of Resources and MaterialsNortheastern University at QinhuangdaoQinhuangdao 066004HebeiChina

The interface mechanism between catalyst and carbon substrate has been the focus of research.In this paper,the FeCo alloy embedded N,S co-doped carbon substrate bifunctional catalyst(FeCo/S-NC)is obtained by a simple one-step pyrolysis strategy.The experimental results and density functional theory(DFT)calculation show that the formation of FeCo alloy is conducive to promoting electron transfer,and the introduction of S atom can enhance the interaction between FeCo alloy and carbon substrate,thus inhibiting the migration and agglomeration of particles on the surface of carbon material.The FeCo/SNC catalysts show outstanding performance for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).FeCo/S-NC shows a high half-wave potential(E_(1/2)=0.8823 V)for ORR and a low overpotential at 10 mA cm^(-2)(E_(j=10)=299 mV)for OER.In addition,compared with Pt/C+RuO_(2) assembled Zn-air battery(ZAB),the FeCo/S-NC assembled ZAB exhibits a larger power density(198.8 mW cm^(-2)),a higher specific capacity(786.1 mA h g_(zn)~(-1)),and ultra-stable cycle performance.These results confirm that the optimized composition and the interfacial interaction between catalyst and carbon substrate synergistically enhance the electrochemical performance.

关键词： FeCo alloy N S co-doped carbon DFT calculation Zn-air batteries Interfacial interaction

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Double-confined nanoheterostructure Sb/Sb2S3@Ti3C2Tx@C toward ultra-stable Li-/Na-ion batteries

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Rare Metals 2024年第5期43卷 2067-2079页

作者： Dan Wang Qun Ma Huan He Zhi-Yuan Wang Run-Guo Zheng Hong-Yu Sun Yan-Guo Liu Chun-Li Liu School of materials Science and Engineering Northeastern University School of Resources and materials Northeastern University at Qinhuangdao key laboratory of dielectric and electrolyte functional material hebei province Department of Physics and Oxide Research Center Hankuk University of Foreign Studies

Antimony-based materials with high capacities and moderate potentials are promising anodes for lithium-/-sodium-ion batteries.However,their tremendous volume expansion and inferior conductivity lead to poor structural stability and sluggish reaction kinetics.Herein,a doubleconfined nanoheterostructure Sb/Sb2S3@Ti3C2Tx@C has been fabricated through a solvothermal method followed by low-temperature heat treatment.The dual protection of‘‘MXene’’and‘‘carbon’’can better accommodate the volume expansion of Sb/Sb2S3.The strong covalent bond （Ti–S,Ti–O–Sb,C–O–Sb） can firmly integrate Sb-based material with Ti3C2Txand carbon,which significantly improves the structure stability.In addition,the carbon layer can restrain the oxidation of MXenes,and the nano-Sb/Sb2S3can facilitate electron/ion transport and suppress the restacking of MXenes.The heterogeneous interface between Sb and Sb2S3can further promote interfacial charge transfer.The MXene-Sb/Sb2S3@C-1 with the optimal Sb content shows high specific capacities,comparable rate properties and ultra-stable cycling performances (250 m Ah·g-1after 2500 cycles at 1 A·g-1for sodium-ion batteries).Ex situ X-ray diffractometer （XRD）test reveals the storage mechanism including the conversion and alloying process of MXene-Sb/Sb2S3@C-1.Cyclic voltammetry （CV） test results demonstrate that the pseudocapacitance behavior is dominant in MXene-Sb/Sb2S3@C-1,especially at large current.This design paves the way for exploring high-performance alloy-based/conversion-type anode for energy storage devices.

关键词： Sb/Sb 2 S 3 MXene Carbon Anode Lithium-ion batteries Sodium-ion batteries

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Unraveling magnetic properties and martensitic transformation in Mn-rich Ni-Mn-Sn alloys:first-principles calculations and experiments

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Rare Metals 2024年第4期43卷 1769-1785页

作者： Yu Zhang Jing Bai Ke-Liang Guo Jia-Xin Xu Jiang-Long Gu Nicola Morley Qui-Zhi Gao Yu-Dong Zhang Claude Esling Xiang Zhao Liang Zuo key laboratory for Anisotropy and Texture of materials (Ministry of Education) School of Material Science and EngineeringNortheastern University key laboratory of dielectric and electrolyte functional material hebei province School of Resources and Materials Northeastern University at Qinhuangdao Department of material Science and Engineering University of Sheffield State key laboratory of Metastable materials Science and Technology Yanshan University Laboratoire d'Etude des Microstructures Et de Mecanique des Materiaux University of Lorraine

We have investigated the phase stability,magnetic properties,and martensitic transformation thermodynamics/kinetics of the Ni24-xMn18+x+ySn6-y(x,y=0,1,2) system by combining the first-principles calculations and experiments.The calculation results show that the optimized lattice parameters are consistent with the experimental data.Respectively,we obtain the relation equation for the austenite formation energy(Eform-A) and Mn content(XMn):Eform-A=507.358XMn-274.126,as well as for the six-layer modulated(6M) martensite formation energy(Eform-6M) and Ni content(XNi):Eform-6M=-728.484XNi+264.374.The ternary phase diagram of the total magnetic moment was established.The excess Mn will reduce the total magnetic moment of 6M(Mag6M) and non-modulated(NM)(MagNM) martensites,with the following equations relating the total magnetic moment and Mn content:Mag6M=-15.905XMn+7.902and MagNM=-14.781XMn+7.411,while the effect on austenite is complex.The variation of total magnetic moment is mainly dominated by the Mn atomic magnetic moment.The 3d electrons of MnSn(Mn at Sn sublattice)play an important role in magnetic properties from the perspective of the electronic density of states.Based on the thermodynamics of martensitic transformation,the alloys will likely undergo austenite?6M?NM transformation sequence.Combining the thermodynamic and kinetic results,the martensitic transformation temperature decreases with x increasing and increases with y increasing.These results are expected to provide reference for predicting the phase stability and magnetic properties of NiMn-Sn alloys.

关键词： Ni–Mn–Sn First-principles calculations Martensitic transformation Magnetic property Kinetics

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Boosting overall saline water splitting by constructing a strain-engineered high-entropy electrocatalyst

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Carbon Energy 2024年第2期6卷 154-166页

作者： Ateer Bao Yaohang Gu Yuxuan Zhang Bowen Zhang Juncheng Wu Bo Ni Xiaoyan Zhang Haijun Pan Xiwei Qi School of materials Science and Engineering Northeastern UniversityShenyangChina School of Resources and materials Northeastern University at QinhuangdaoQinhuangdaoChina key laboratory of dielectric and electrolyte functional material hebei province Northeastern University at QinhuangdaoQinhuangdaoChina College of Metallurgy and Energy North China University of Science and TechnologyTangshanChina

High-entropy materials(HEMs),which are newly manufactured compounds that contain five or more metal cations,can be a platform with desired properties,including improved electrocatalytic performance owing to the inherent complexity.Here,a strain engineering methodology is proposed to design transition-metal-based HEM by Li manipulation(LiTM)with tunable lattice strain,thus tailoring the electronic structure and boosting electrocatalytic performance.As confirmed by the experiments and calculation results,tensile strain in the LiTM after Li manipulation can optimize the d-band center and increase the electrical conductivity.Accordingly,the asprepared LiTM-25 demonstrates optimized oxygen evolution reaction and hydrogen evolution reaction activity in alkaline saline water,requiring ultralow overpotentials of 265 and 42 mV at 10 mA cm−2,respectively.More strikingly,LiTM-25 retains 94.6%activity after 80 h of a durability test when assembled as an anion-exchange membrane water electrolyzer.Finally,in order to show the general efficacy of strain engineering,we incorporate Li into electrocatalysts with higher entropies as well.

关键词： d-band center electrical conductivity high-entropy electrocatalyst lattice-strain engineering saline/alkaline water splitting

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Progress,challenges,and prospects of spent lithium-ion batteries recycling:A review

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Journal of Energy Chemistry 2024年第2期89卷 144-171,I0005页

作者： Pengwei Li Shaohua Luo Lin Zhang Qiuyue Liu Yikai Wang Yicheng Lin Can Xu Jia Guo Peam Cheali Xiaoning Xia School of materials Science and Engineering Northeastern UniversityShenyang 110819LiaoningChina School of Resources and materials Northeastern University at QinhuangdaoQinhuangdao 066004HebeiChina Department of Chemistry and Bioscience Aalborg UniversityAalborg 9220Denmark key laboratory of dielectric and electrolyte functional material hebei province Qinhuangdao 066004HebeiChina Department of materials and Production Aalborg UniversityAalborg 9220Denmark School of Metallurgy Northeastern UniversityShenyang 110819LiaoningChina

The recycling and reutilization of spent lithium-ion batteries(LIBs)have become an important measure to alleviate problems like resource scarcity and environmental pollution.Although some progress has been made,battery recycling technology still faces challenges in terms of efficiency,effectiveness and environmental sustainability.This review aims to systematically review and analyze the current status of spent LIB recycling,and conduct a detailed comparison and evaluation of different recycling processes.In addition,this review introduces emerging recycling techniques,including deep eutectic solvents,molten salt roasting,and direct regeneration,with the intent of enhancing recycling efficiency and diminishing environmental repercussions.Furthermore,to increase the added value of recycled materials,this review proposes the concept of upgrading recycled materials into high value-added functional materials,such as catalysts,adsorbents,and graphene.Through life cycle assessment,the paper also explores the economic and environmental impacts of current battery recycling and highlights the importance that future recycling technologies should achieve a balance between recycling efficiency,economics and environmental benefits.Finally,this review outlines the opportunities and challenges of recycling key materials for next-generation batteries,and proposes relevant policy recommendations to promote the green and sustainable development of batteries,circular economy,and ecological civilization.

关键词： Spent li-ion batteries Recycle Direct regeneration High-value conversion functional materials

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Defect engineered nickel hydroxide nanosheets for advanced pseudocapacitor electrodes

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Nano Research 2024年第6期17卷 5233-5242页

作者： Yaohang Gu Yuxuan Zhang Xuanyu Wang Ateer Bao Bo Ni Haijun Pan Xiaoyan Zhang Xiwei Qi School of materials Science and Engineering Northeastern UniversityShenyang 110189China College of Metallurgy and Energy North China University of Science and TechnologyTangshan 063210China key laboratory of dielectric and electrolyte functional material hebei province School of Resources and MaterialsNortheastern University at QinhuangdaoQinhuangdao 066004China School of Resources and materials Northeastern University at QinhuangdaoQinhuangdao 066004China

While the past years have witnessed great achievement in pseudocapacitors,the inauguration of electrode materials of high-performance still remains a formidable challenge.Moreover,the capacity and rate capability of the electrode depends largely on its electrical conductivity,which ensures fast charge transfer kinetics in both the grain bulk and grain boundaries.Here,nickel hydroxides with oxygen vacancies are facilely fabricated via a hydrothermal method.The active materials exhibit a high specific capacitance of 3250 F·g^(−1)and a high areal of capacitance of 14.98 F·cm^(−2)at 4.6 mA·cm^(−2).The asymmetric supercapacitor device based on our material delivers a high energy density of~71.6 Wh·kg^(−1)and a power density of~17,300 W·kg^(−1)and could retain~95%of their initial capacitance even after 30,000 cycles.In addition,the defect-rich hydroxides demonstrate higher electrical conductivity as well as dielectric constant,which is responsible for the superior pseudocapacitive performance.Our new scientific strategy in terms of taking the advantages of oxygen vacancies might open up new opportunities for qualified pseudocapacitive materials of overall high performances not only for nickel hydroxides but also for other metal hydroxides/oxides.

关键词： pseudocapacitors nickel hydroxides oxygen vacancies electrical conductivity

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Mechanism of interfacial effects in sodium-ion storage devices

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Nano Research 2024年第3期17卷 1313-1326页

作者： Yifan Wei Lingxing Zan Huicong Xia Wenfu Yan Jia-Nan Zhang College of materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China key laboratory of Advanced Energy Catalytic and functional material Preparation of Zhengzhou City Zhengzhou 450001China key laboratory of Chemical Reaction Engineering of Shaanxi province College of Chemistry&Chemical EngineeringYan’an UniversityYan’an 716000China State key laboratory of Inorganic Synthesis and Preparative Chemistry and College of Chemistry Jilin UniversityChangchun 130012China

Rechargeable sodium-ion batteries(SIBs)are considered as the next-generation secondary batteries.The performance of SIB is determined by the behavior of its electrode surface and the electrode–electrolyte interface during charging and discharging.Thus,the characteristics of these surfaces and interfaces should be analyzed to realize large-scale energy storage systems with high energy density and long-cycle stability.Although various studies have investigated the properties of electrode materials,few studies have focused on the construction of stable and efficient SIB interfaces,and even fewer have explored the mechanisms of interfacial effects;however,the strategies of regulating interfacial effects are yet to be completely developed.Moreover,the results obtained thus far are insufficient to draw systematic conclusions.The present study reviews the literature on the mechanism of interfacial effects in Na+storage devices.The interfaces in a sodium-ion storage device include a heterogeneous interface between electrode materials,a solid electrolyte interphase,and a cathode electrolyte interphase.The interfacial effects during the intercalation,transformation,and alloy reactions and the resulting overall battery performance were theoretically analyzed.In this review,we aim to provide a theoretical basis for optimizing the structures of electrode surface and electrode–electrolyte interface to optimize the performance of SIBs.In addition,the challenges of investigating interfacial effects and several possible helpful methods and opportunities for studying the mechanisms of interfacial effects in SIBs will be presented.

关键词： sodium-ion storage interfacial effects solid electrolyte interphase cathode electrolyte interphase

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Bifunctional TiO_(2-x)nanofibers enhanced gel polymer electrolyte for high performance lithium metal batteries

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Journal of Energy Chemistry 2024年第2期89卷 437-448,I0011页

作者： Yixin Wu Zhen Chen Yang Wang Yu Li Chunxing Zhang Yihui Zhu Ziyu Yue Xin Liu Minghua Chen key laboratory of Engineering dielectric and Applications(Ministry of Education) School of Electrical and Electronic EngineeringHarbin University of Science and TechnologyHarbin 150080HeilongjiangChina

Exploration of advanced gel polymer electrolytes(GPEs)represents a viable strategy for mitigating dendritic lithium(Li)growth,which is crucial in ensuring the safe operation of high energy density Li metal batteries(LMBs).Despite this,the application of GPEs is still hindered by inadequate ionic conductivity,low Li^(+)transference number,and subpar physicochemical properties.Herein,Ti O_(2-x)nanofibers(NF)with oxygen vacancy defects were synthesized by a one-step process as inorganic fillers to enhance the thermal/mechanical/ionic-transportation performances of composite GPEs.Various characterizations and theoretical calculations reveal that the oxygen vacancies on the surface of Ti O_(2-x)NF accelerate the dissociation of Li PF_6,promote the rapid transfer of free Li^(+),and influence the formation of Li F-enriched solid electrolyte interphase.Consequently,the composite GPEs demonstrate enhanced ionic conductivity(1.90m S cm^(-1)at room temperature),higher lithium-ion transference number(0.70),wider electrochemical stability window(5.50 V),superior mechanical strength,excellent thermal stability(210℃),and improved compatibility with lithium,resulting in superior cycling stability and rate performance in both Li||Li,Li||Li Fe PO_(4),and Li||Li Ni_(0.8)Co_(0.1)Mn_(0.1)O_(2)cells.Overall,the synergistic influence of nanofiber morphology and enriched oxygen vacancy structure of fillers on electrochemical properties of composite GPEs is comprehensively investigated,thus,it is anticipated to shed new light on designing high-performance GPEs LMBs.

关键词： Nanofibers fillers Oxygen vacancies Gel polymer electrolytes Lithium metal batteries

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Enhanced cycling stability and rate performance of Co-doped and La_(2)O_(3)-coated LiNi_(0.9)Mn_(0.1)O_(2) toward power battery

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Rare Metals 2024年第2期43卷 658-670页

作者： Jia-Qi Peng Yuan-Yuan Wei Dong-Ming Liu Yun Li Bin Hu Bin Huang Jian-Wen Yang Shun-Hua Xiao Ren-Heng Wang Guangxi key laboratory of Electrochemical and Magneto-Chemical functional materials College of Chemistry and BioengineeringGuilin University of TechnologyGuilin541004China key laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong province College of Physics and Optoelectronic EngineeringShenzhen UniversityShenzhen518060China

Ultra-high nickel layered oxide cathode material with high energy density is the most promising material to improve the electrochemical performance of lithium-ion batteries(LIBs).However,the poor structural stability and severe surface/interface side reactions of the material lead to poor rate performance and cyclic stability,which limits its application in practice.In this paper,the dual-modification strategy of Co doping and La_(2)O_(3) coating is used to meet the above challenges.Co doping can effectively widen layer spacing and reduce Li^(+)/Ni^(2+) mixing,and La_(2)O_(3) coating can effectively eliminate the residual alkali on the surface of active material,inhibit the thickening of cathode electrolyte interphase(CEI)film and reduce surface/interface side reactions.Therefore,the modified material(NM90-CL)with excellent electrochemical properties is achieved through the synergistic enhancement of Co doping and La_(2)O_(3) coating.Its capacity retention rate can reach 77.9%after 200 cycles at 1.0℃ and 75.7%after 200 cycles at 5.0℃.Its reversible capacity can up to 153.5 mAh·g^(–1) at 10.0℃.This dual-modification strategy will provide theoretical guidance and technical support for the synthesis of other high-performance electrode materials.

关键词： High nickel cathode material Co doping La_(2)O_(3) coating Electrochemical performance Electrochemical mechanism

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