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Converting intercalation-type cathode in spent lithium-ion batteries into conversion-type cathode

nano Research 2024年第5期17卷 4602-4609页

作者： Dingding Zhu Yong Su Jingzhao Chen Xiangze Ou Xuedong Zhang Wen Xie Yuyan Zhou Yunna Guo Qiushi Dai Peng Jia Jitong Yan Lin Geng Baiyu Guo Liqiang Zhang Yongfu Tang Qiao Huang Jianyu Huang School of materials science and Engineering Xiangtan UniversityXiangtan 411105China clean nano energy center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066000China

The widespread applications of lithium-ion batteries(LIBs)generate tons of spent LIBs.Therefore,recycling LIBs is of paramount importance in protecting the environment and saving the resources.Current commercialized LIBs mostly adopt layered oxides such as LiCoO_(2)(LCO)or LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)(NMC)as the cathode materials.Converting the intercalation-type spent oxides into conversion-type cathodes(such as metal fluorides(MFs))offers a valid recycling strategy and provides substantially improved energy densities for LIBs.Herein,two typical Co-based cathodes,LCO and LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NMC622),in spent LIBs were successfully converted to CoF_(2) and(Ni_(x)Co_(y)Mn_(z))F_(2) cathodes by a reduction and fluorination technique.The as converted CoF_(2) and(Ni_(x)Co_(y)Mn_(z))F_(2) delivered cell energy densities of 650 and 700 Wh/kg,respectively.Advanced atomic-level electron microscopy revealed that the used LCO and NMC622 were converted to highly phase pure Co metal and Ni_(0.6)Co_(0.2)Mn_(0.2) alloys in the used graphite-assisted reduction roasting,simultaneously producing the important product of Li_(2)CO_(3) using only environment friendly solvent.Our study provided a versatile strategy to convert the intercalation-type Co-based cathode in the spent LIBs into conversion-type MFs cathodes,which offers a new avenue to recycle the spent LIBs and substantially increase the energy densities of next generation LIBs.

关键词： spent lithium-ion batteries recycling energy densities conversion-type cathode

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In situ observation of the electrochemical behavior of Li–CO_(2)/O_(2)batteries in an environmental transmission electron microscope

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Carbon energy 2024年第4期6卷 244-255页

作者： Peng Jia Yunna Guo Dongliang Chen Jingming Yao Xuedong Zhang Jianguo Lu Yuqing Qiao Liqiang Zhang Hebei key laboratory of Applied Chemistry College of Environmental and Chemical EngineeringYanshan UniversityQinhuangdaoChina state key laboratory of metastable materials science and technology Clean Nano Energy CenterYanshan UniversityQinhuangdaoChina state key laboratory of Silicon and Advanced Semiconductor materials School of Materials Science and EngineeringZhejiang UniversityHangzhouChina key laboratory of Low Dimensional materials and Application technology of Ministry of Education School of Materials Science and EngineeringXiangtan UniversityXiangtanChina

Li–CO_(2)/O_(2)batteries,a promising energy storage technology,not only provide ultrahigh discharge capacity but also capture CO_(2)and turn it into renewable energy.Their electrochemical reaction pathways'ambiguity,however,creates a hurdle for their practical application.This study used copper selenide(CuSe)nanosheets as the air cathode medium in an environmental transmission electron microscope to in situ study Li–CO_(2)/O_(2)(mix CO_(2)as well as O_(2)at a volume ratio of 1:1)and Li–O_(2)batteries as well as Li–CO_(2)batteries.Primary discharge reactions take place successively in the Li–CO_(2)/O_(2)–CuSe nanobattery:(I)4Li^(+)+O_(2)+4e^(−)→2Li_(2)O;(II)Li_(2)O+CO_(2)→Li_(2)CO_(3).The charge reaction proceeded via(III)2Li_(2)CO_(3)→4Li^(+)+2CO_(2)+O_(2)+4e^(−).However,Li–O_(2)and Li–CO_(2)nanobatteries showed poor cycling stability,suggesting the difficulty in the direct decomposition of the discharge product.The fluctuations of the Li–CO_(2)/O_(2)battery's electrochemistry were also shown to depend heavily on O_(2).The CuSe‐based Li–CO_(2)/O_(2)battery showed exceptional electrochemical performance.The Li^–CO_(2)/O_(2)battery offered a discharge capacity apex of 15,492 mAh g^(−1) and stable cycling 60 times at 100 mA g^(−1).Our research offers crucial insight into the electrochemical behavior of Li–CO_(2)/O_(2),Li–O_(2),and Li–CO_(2)nanobatteries,which may help the creation of high‐performance Li–CO_(2)/O_(2)batteries for energy storage applications.

关键词： CuSe nanosheets electrochemical reaction in situ environmental transmission electron microscopy Li-CO_(2)battery Li-CO_(2)/O_(2)battery Li-O_(2)battery

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The dynamic surface evolution of halide perovskites induced by external energy stimulation

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National science Review 2024年第4期11卷 185-194页

作者： Feiyu Cheng Pengdong Wang Chenzhe Xu Qingliang Liao Suicai Zhang Haochun Sun Wenqiang Fan Guodong Liu Zhiyun Li Yaping Kong Li Wang Fangsen Li Zhuo Kang Yue Zhang Academy for Advanced Interdisciplinary science and technology State Key Laboratory for Advanced Metals and Materials University of Science and Technology Beijing Beijing key laboratory for Advanced energy materials and Technologies Key Laboratory of Advanced Materials and Devices for Post-Moore ChipsMinistry of EducationBeijing Advanced Innovation Center for Materials Genome Engineering School of Materials Science and EngineeringUniversity of Science and Technology Beijing Vacuum Interconnected nanotech Workstation(nano-X) Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of Sciences Beijing National laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences

Tracking the dynamic surface evolution of metal halide perovskite is crucial for understanding the corresponding fundamental principles of photoelectric properties and intrinsic instability. However, due to the volatility elements and soft lattice nature of perovskites, several important dynamic behaviors remain unclear. Here, an ultra-high vacuum（UHV） interconnection system integrated by surface-sensitive probing techniques has been developed to investigate the freshly cleaved surface of CH3NH3PbBr3in situ under given energy stimulation. On this basis, the detailed three-step chemical decomposition pathway of perovskites has been clarified. Meanwhile, the evolution of crystal structure from cubic phase to tetragonal phase on the perovskite surface has been revealed under energy stimulation. Accompanied by chemical composition and crystal structure evolution, electronic structure changes including energy level position,hole effective mass, and Rashba splitting have also been accurately determined. These findings provide a clear perspective on the physical origin of optoelectronic properties and the decomposition mechanism of perovskites.

关键词： metal halide perovskite external energy stimulation surface dynamic evolution surface electronic structure ultra-high vacuum interconnection system

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In-situ imaging electrocatalysis in a solid-state Li-O_(2) battery with CuSe nanosheets as air cathode

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Chinese Chemical Letters 2024年第5期35卷 466-470页

作者： Peng Jia Yunna Guo Dongliang Chen Xuedong Zhang Jingming Yao Jianguo Lu Liqiang Zhang Hebei key laboratory of Applied Chemistry College of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004China clean nano energy center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066004China state key laboratory of Silicon and Advanced Semiconductor materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310058China key laboratory of Low Dimensional materials and Application technology of Ministry of Education School of Materials Science and EngineeringXiangtan UniversityXiangtan 411105China

The development of highly efficient catalysts in the cathodes of rechargeable Li-O_(2) batteries is a considerable challenge.To enhance the electrochemical performance of the Li-O_(2) battery,it is essential to choose a suitable catalyst material.Copper selenide(CuSe)is considered as a more promising cathode catalyst material for Li-O_(2) battery due to its better conductivity and rich electrochemical active sites.However,its electrochemical reaction and fundamental catalytic mechanism remain unclear till now.Herein,in-situ environmental transmission electron microscopy technique was used to study the catalysis mechanism of the CuSe nanosheets in Li-O_(2) batteries during discharge and charge processes.It is found that Li_(2)O was formed and decomposed around the ultrafine-grained Cu during the discharge and charge processes,respectively,demonstrating excellent cycling.This indicate that the freshly formed ultrafine-grained Cu in the conversion reaction catalyzed the latter four-electron-transfer oxygen reduction reaction,leading to the formation of Li_(2)O.Our study provides important understanding of the electrochemistry of the LiO_(2) nanobatteries,which will aid the development of high-performance Li-O_(2) batteries for energy storage applications.

关键词： In-situ environmental transmission electron microscopy Lithium oxygen batteries CuSe nanosheets Oxygen reduction reaction Oxygen evolution reaction

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Enhanced electrochemical performance of nanoscale single crystal NMC811 modification by coating LiNbO_(3)

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Chinese Chemical Letters 2024年第5期35卷 514-518页

作者： Fengyu Zhang Yali Liang Zhangran Ye Lei Deng Yunna Guo Ping Qiu Peng Jia Qiaobao Zhang Liqiang Zhang clean nano energy center state key laboratory of metastable materials science and technology Yanshan UniversityQinhuangdao 066004China School of New energy and materials China University of Petroleum BeijingBeijing 102249China Hebei key laboratory of Applied Chemistry College of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004China state key laboratory of Physical Chemistry of Solid Surfaces College of MaterialsXiamen UniversityXiamen 361005China

Single crystallization is an important strategy to resolve intergranular cracks and unnecessary side reactions with electrolytes in layered transition metal oxide cathodes LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811).Due to the limitations of high-temperature sintering and multi-step calcination,single crystal NMC811 generally shows irregular particles with a size of 2-3μm.However,the prolonged Li-ion diffusion pathway and the stress generated by the uneven de-/intercalation sluggish Li-ion diffusion kinetics,what is more,cause structural damage such as intragranular cracks.A slow Li extraction rate or particle size reduction will ameliorate the structural damage and improve the cycling stability.As the most promising cathodes for next-generation power batteries,NMC811 required fast charge performance and cycle stability.Particle size reduction appears to be the displacement option.nanonization is an effective strategy to mitigate intragranular cracks of single crystal NMC811.However,the serious aggregation and increased specific surface area become new challenges.In this article,we synthesized monodisperse nanoscale single crystal NMC811 by molten salt method and modified the surface by LiNbO3 coating.The electrochemical performance shows that nanoscale single crystal NMC811 has faster kinetic and higher capacity retention,so the strategy of combining nanonization and surface coating is an alternative way to prepare high specific capacity and cycle stable single crystal NMC811.

关键词： Ni-rich NMC811 Molten salt method nanonization Surface coating Micron cracks

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An intermittent lithium deposition model based on CuMnbimetallic MOF derivatives for composite lithium anode with ultrahigh areal capacity and current densities

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nano Research 2024年第4期17卷 2763-2769页

作者： Tao Wei Yanyan Zhou Cheng Sun Xingtong Guo Shoudong Xu Daifen Chen Yongfu Tang School of energy and Power Jiangsu University of Science and TechnologyZhenjiang 212003China state key laboratory of metastable materials science and technology(MMST) Hebei Key Laboratory of Applied ChemistryYanshan UniversityQinhuangdao 066004China College of materials science and Engineering Taiyuan University of TechnologyTaiyuan 030024China

Recently,three-dimensional(3D)conductive frameworks have been chosen as the host for composite lithium(Li)metal anode because of their exceptional electrical conductivity and remarkable thermal and electrochemical stability.However,Li tends to accumulate on the top of the 3D frameworks with homogenous lithiophilicity and Li dendrite still growth.This work firstly designed a bimetallic metal-organic framework(MOF)(CuMn-MOF)derived Cu_(2)O and Mn_(3)O_(4) nanoparticles decorated carbon cloth(CC)substrates(CC@Cu_(2)O/Mn_(3)O_(4))to fabricate a composite Li anode.Thanks to the synergistic effects of lithiophilic Cu_(2)O and Mn_(3)O_(4),the CC@Cu_(2)O/Mn_(3)O_(4)@Li symmetrical cell can afford a prolonged cycling lifespan(1400 h)under an ultrahigh current density and areal capacity(6 mA·cm^(-2)/6 mAh·cm^(-2)).When coupled with the LiFePO_(4)(LFP)cathode,the LFP||CC@Cu_(2)O/Mn_(3)O_(4)@Li full cell demonstrated a superior performance of 89.7 mAh·g^(-1) even at an extremely high current density(10 C).Furthermore,it can also be matched well with LiNi_(0.5)Co^(0).2Mn_(0.3)O_(2)(NCM523)cathode.Importantly,to explain the excellent performances of the CC@Cu_(2)O/Mn_(3)O_(4)@Li composite anode,an intermittent model was also proposed.This study offers a novel model that can enhance our comprehension of the Li deposition behavior and pave the way to attain stable and safe Li metal anodes by employing bimetallic MOF-derived materials to construct 3D frameworks.

关键词： lithium metal anode(LMA) three-dimensional(3D)frameworks intermittent lithiophilic model high areal capacity bimetallic metal-organic frameworks(MOFs)

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Conceptual transition from molecular to atomic: unleashing a new era in hydrogen therapy for chronic disease

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National science Review 2024年第4期11卷 17-18页

作者： Zhigang Zou Eco-materials and Renewable energy Research center (ERERC) Jiangsu Key Laboratory for Nano Technology National Laboratory of Solid State Microstructures and Department of PhysicsNanjing University

The dysregulated overexpression of reactive oxygen and nitrogen species (RONS)intricately links to the occurrence and development of diverse chronic diseases[1–3]. Hydrogen therapy stands out as a promising treatment methodology recognized for effectively mitigating RONS and maintaining intracellular redox equilibrium, thereby yielding therapeutic benefits [4,5].

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Static recrystallization behaviors and mechanisms of 7Mo super-austenitic stainless steel with undissolved sigma precipitates during double-stage hot deformation

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Journal of Iron and Steel Research(International) 2024年第2期31卷 475-487页

作者： Shi-guang Xu Jin-shan He Run-ze Zhang Fu-cheng Zhang Xi-tao Wang Collaborative Innovation center of Steel technology University of Science and Technology BeijingBeijing100083China state key laboratory of metastable materials science and technology Yanshan UniversityQinhuangdao066004HebeiChina Shandong Provincial key laboratory for High Strength Lightweight Metallic materials Advanced Materials InstituteQilu University of Technology(Shandong Academy of Science)Jinan250353ShandongChina

Static recrystallization(SRX)behaviors and corresponding recrystallization mechanisms of 7Mo super-austenitic stainless steel were studied under different deformation conditions.The order of influence of deformation parameters on static recrystallization behaviors,from high to low,is followed by temperature,first-stage strain and strain rate.Meanwhile,the effect of holding time on static recrystallization behaviors is significantly controlled by temperature.In addition,with the increase in temperature from 1000 to 1200°C,the static recrystallization mechanism evolves from discontinuous static recrystallization and continuous static recrystallization(cSRX)to metadynamic recrystallization and cSRX,and finally to cSRX.The cSRX exists at all temperatures.This is because high stacking fault energy(56 mJ m−2)promotes the movement of dislocations,making the deformation mechanism of this steel is dominated by planar slip of dislocation.Large undissolved sigma precipitates promote static recrystallization through particle-stimulated nucleation.However,small strain-induced precipitates at grain boundaries hinder the nucleation of conventional SRX and the growth of recrystallized grains,while the hindering effect decreases with the increase in temperature.

关键词： 7Mo super-austenitic stainless steel Double-stage hot deformation Conventional static recrystallization Metadynamic recrystallization Strain-induced precipitation

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Simple preparation of C(CS)/g-C_(3)N_(4)/Co carbon aerogel and its catalytic performance for ammonium perchlorate

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Defence technology（防务技术） 2024年第3期33卷 186-196页

作者： Yujie Yan Bo Jin Rufang Peng state key laboratory of Environment-friendly energy materials School of Materials Science and EngineeringSouthwest University of Science and TechnologyMianyang621010China

Biomass chitosan(CS)was used as a template,graphitic phase carbon nitride(g-C_(3)N_(4))with high nitrogen content and certain catalytic activity was used as a dopant,and nano-transition metal cobalt(Co)was used as a catalytic center point.The carbon aerogel(C(CS)/g-C_(3)N_(4)/Co)with a three-dimensional network-like structure was prepared by assembling the three materials through experimental operations such as freeze-drying and high-temperature carbonization.It was demonstrated by scanning and transmission characterization that the CS in the carbon aerogel could provide more active sites for the cobalt nanoparticles,and the doping of graphite-phase carbon nitride as a template dispersed the cobalt nanoparticles and changed the conductivity of the CS.To investigate the catalytic effect of carbon aerogel on ammonium perchlorate(AP),it was investigated by differential thermal analyzer and TG thermal analysis.This carbon aerogel was very effective in catalyzing AP,and the 10 wt% content of the catalyst reduced the AP pyrolysis peak from 703.9 to 595.5 K.And to further investigate the synergistic effect of the three materials,further carbon aerogels such as C(CS)/Co,g-C_(3)N_(4)/Co were prepared and applied to catalyze AP,and the same ratio reduced the AP pyrolysis peak by 98.1℃ and 97.7℃.This result indicates a synergistic effect of the assembly of the three materials.

关键词： g-C_(3)N_(4) Chitosan Co Ammonium perchlorate Pyrolysis kinetics

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Kinetically and thermodynamically expediting elementary steps via high-valence Cr-incorporated of nickel selenide for water electrolysis

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nano Research 2024年第3期17卷 1199-1208页

作者： Huafeng Fan Dongxu Jiao Jinchang Fan Dewen Wang Bilal Zaman Wei Zhang Lei Zhang Weitao Zheng Xiaoqiang Cui state key laboratory of Automotive Simulation and Control School of Materials Science and EngineeringKey Laboratory of Automobile Materials of MOEJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy CenterJilin UniversityChangchun 130012China College of Chemistry Jilin UniversityChangchun 130012China

Designing high-performance electrocatalysts toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is essential to reduce the activation barrier and optimize free adsorption energy of reactive intermediates.Herein,we report that incorporating high-valence Cr into NiSe_(2)(Cr_(x)Ni_(1-x)Se_(2))kinetically and thermodynamically expedites elementary steps of both HER and OER.The as-prepared Cr_(0.05)Ni_(0.95)Se_(2) catalyst displays excellent HER and OER activities,with low overpotentials of 89 and 272 mV at the current density of 10 mA·cm^(-2)(j10),respectively,and remains stable during operation for 30 h.A low cell voltage of only 1.59 V is required to drive j10 in alkaline media.In situ Raman spectroscopy reveals that Cr incorporation facilitates the formation of NiOOH active species during the OER process.Meanwhile,theoretical explorations demonstrate that high-valence Cr incorporation efficiently accelerates water dissociation kinetics and improves H*adsorption during HER process,lowering the activation barrier of OER and optimizing the adsorption energy of oxygen-based intermediate,thus kinetically and thermodynamically enhancing the intrinsic performance of NiSe_(2) for over water splitting.This strategy provides a new horizon to design transition metal based electrocatalysts in the clean energy field.

关键词： nickel selenide electrocatalytic water splitting high-valence Cr density functional theory(DFT)calculation

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