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NASICONs-type solid-state electrolytes:The history,physicochemical properties,and challenges

Interdisciplinary materials 2023年第1期2卷 91-110页

作者： Lixiao Zhang Yimeng Liu Ya You Ajayan Vinu Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhanChina International School of Materials Science and Engineering Wuhan University of TechnologyWuhanChina Global Innovative Center for Advanced Nanomaterials(GICAN) School of EngineeringCollege of EngineeringScienceand the EnvironmentThe University of NewcastleCallaghanNew South Wales 2308Australia

Solid-state electrolytes are critical for the development of next-generation high-energy and high-safety rechargeable *** all the candidates,sodium(Na)superionic conductors(NASICONs)are highly promising because of their evident advantages in high ionic conductivity and high chemical/electrochemical *** concept of NASICONs was proposed by Hong and Goodenough et *** 1976 by reporting the synthesis and characterization of Na1+xZr2(SixP3−x)O12(0≤x≤3),which has attracted tremendous attention on the NASICONs-type solid-state *** this review,we are committed to describing the development history of NASICONs-type solid-state electrolytes and elucidating the contribution of Goodenough as a tribute to *** summarize the correlations and differences between lithium-based and sodium-based NASICONs electrolytes,such as their preparation methods,structures,ionic conductivities,and the mechanisms of ion *** challenges of NASICONs-structured electrolytes are discussed,and several research directions are proposed to tackle the obstacles toward practical applications.

关键词： electrode/electrolyte interface grain boundary resistance high ionic conductivity NASICONs solid-state electrolyte

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Layer stacked SiO_(x) microparticle with disconnected interstices enables stable interphase and particle integrity for lithium-ion batteries

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Journal of Energy Chemistry 2023年第11期86卷 300-307,I0007页

作者： Yang Ren Xucai Yin Lizhi Xiang Rang Xiao Hua Huo Geping Yin Chunyu Du MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage and Institute of Advanced Chemical Power Sources School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology School of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004GuangxiChina

Severe mechanical fractu re and unstable interphase,associated with the large volumetric expansion/contraction,significantly hinder the application of high-capacity SiO_(x)materials in lithium-ion ***,we report the design and facile synthesis of a layer stacked SiO_(x)microparticle(LS-SiO_(x))material,which presents a stacking structure of SiO_(x)layers with abundant disconnected *** LS-SiO_(x)microparticle can effectively accommodate the volume expansion,while ensuring negligible particle *** importantly,the interstices within SiO_(x)microparticle are disconnected from each other,which efficiently prevent the electrolyte from infiltration into the interior,achieving stable electrode/-electrolyte ***,the LS-SiO_(x)material without any coating delivers ultrahigh average Coulombic efficiency,outstanding cycling stability,and full-cell *** 6 cycles can attain>99.92%Coulombic efficiency and the capacity retention at 0.05 A g^(-1)for 100 cycles exceeds99%.After 800 cycles at 1 A g^(-1),the thickness swelling of LS-SiO_(x)electrode is as low as 0.87%.Moreover,the full cell with pure LS-SiO_(x)anode exhibits capacity retention of 91.2%after 300 cycles at 0.2 *** work provides a novel concept and effective approach to rationally design silicon-based and other electrode materials with huge volume variation for electrochemical energy storage applications.

关键词： Lithium-ion batteries Silicon oxide Layer stacked structure Disconnected interstices Coulombic efficiency

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Effect of content and spin state of iron on electronic properties and floatability of iron-bearing sphalerite:A DFT+U study

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International Journal of Mining Science and technology 2023年第12期33卷 1563-1571页

作者： Yao Feng Zhuofan Li Jianhua Chen Ye Chen State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures School of Chemistry&Chemical EngineeringGuangxi UniversityNanning 530004China MOE Key Laboratory of New Processing Technology for Nonferrous Metals and Materials Guangxi UniversityNanning 530004China School of Resources Environment and MaterialsGuangxi Higher School Key Laboratory of Minerals EngineeringGuangxi UniversityNanning 530004China

Iron is an impurity widely occurred in sphalerite,and its effect on sphalerite flotation is *** this work,the effects of iron content and spin state on electronic properties and floatability of iron-bearing sphalerite are comprehensively studied using density functional theory Hubbard U(DFT+U)calculations combined with coordination chemistry *** band gap of ideal sphalerite is 3.723 eV,and thus electron transition is difficult to occur,resulting in poor *** results suggest the band gap of sphalerite decreases with increasing iron *** low iron content,the decreased band gap facilitates electron transition;at this case,Fe^(2+)in a high-spin state possesses oneπelectron pair,which can form a weakπ-backbonding with xanthate,causing increasing ***,for medium and high iron-bearing sphalerite,with the further decrease of band gap,Fe^(2+)is oxidized to Fe^(3+)due to electrochemical interaction,and henceπ-backbonding is eliminated,leading to lower floatability of iron-bearing sphalerite,which is consistent with the flotation experimental *** work could give a deeper understanding of how sphalerite flotation behaviors are affected by iron content.

关键词： Sphalerite Iron-bearing sphalerite Iron content Spin state Density functional theory

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Robust architecture of 2D nano Mg-based borohydride on graphene with superior reversible hydrogen storage performance

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Journal of materials Science & technology 2023年第15期146卷 121-130页

作者： Xuancheng Wang Yuxiao Jia Xuezhang Xiao Panpan Zhou Jiapeng Bi Jiacheng Qi Ling Lv Fen Xu Lixian Sun Lixin Chen State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027China Guangxi Collaborative Innovation Center of Structure and Property for New Energy and Materials School of Material Science and EngineeringGuilin University of Electronic TechnologyGuilin 541004China Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province Hangzhou 310013China

Efficient technical strategies to synthesize hydrides with high capacity and favorable reversibility are significant for the development of novel energy ***,nano Mg-based borohydride,Mg(BH_(4))_(2),with robust architecture was designed and prepared by confining on graphene through a solution selfconfinement *** Mg(BH_(4))_(2) confined on graphene displays a wrinkled 2D nano layer morphology within 8.8 nm *** 2D nano Mg(BH_(4))_(2) can start dehydrogenation at 67.9℃ with a high capacity of 12.0 wt.%,which is 190.5℃ lower than pristine Mg(BH_(4))_(2).The isothermal dehydrogenation tests and kinetics fitting results indicate the 2D nano Mg(BH_(4))_(2) possesses much-enhanced dehydrogenation kinetics of 31.3 kJ/mol activation energy,which is only half of pristine Mg(BH_(4))_(2).The thermodynamics of the 2D nano Mg(BH_(4))_(2) is also verified by PCT tests,of which Gibbs free energy value for the confined 2D nano Mg(BH_(4))_(2) is estimated to be-18.01 kJ/mol H_(2),lower than-16.36 kJ/mol H_(2) of pristine Mg(BH_(4))_(2).Importantly,the reversibility of the confined 2D nano Mg(BH_(4))_(2) is significantly enhanced to over 90%capacity retention with relatively kinetics stability during 10 *** mechanism analyses manifest that Mg(BH_(4))_(2) exhibits stable 2D nano morphology during 10 cyclic tests,resulting in the greatly reduced H diffusion path and the improved de/rehydrogenation kinetics of the 2D nano Mg(BH_(4))_(2).Based on theoretical calculations of Mg(BH_(4))_(2) and the intermediate MgB12H12 confined on graphene,the charge transfer status of both samples is modified to facilitate de/rehydrogenation,thus leading to the significant thermodynamic improvements of the reversible hydrogen storage performances for 2D nano Mg(BH_(4))_(2).Such investigation of the Mg-based borohydride will illuminate prospective technical research of energy storage materials.

关键词： Mg(BH_(4))_(2) Nano-confinement Kinetics Thermodynamics Reversible hydrogen storage

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Hierarchical cobalt-molybdenum layered double hydroxide arrays power efficient oxygen evolution reaction

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Nano Research 2024年第6期17卷 5080-5086页

作者： Xinyi Zhu Jiahui Lyu Shanshan Wang Xingchuan Li Xiaoyu Wei Cheng Chen Wanida Kooamornpattana Francis Verpoort Jinsong Wu Zongkui Kou State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya 572000China Nanostructure Research Center Wuhan University of TechnologyWuhan 430070China Department of Chemical Engineering Faculty of EngineeringMahidol UniversityNakhon Pathom 73170Thailand

Transition metal-based layered double hydroxides(LDHs)have been capable of working efficiently as catalysts in the basic oxygen evolution reaction(OER)for sustaining hydrogen production of alkaline water ***,exploring new LDH-based electrocatalysts featuring both remarkable activity and good stability is still in high demand,which is pivotal for comprehensive understanding and impressive improvement of the sluggish OER ***,a series of bimetallic(Co and Mo)LDH arrays were designed and fabricated via a facile and controlled strategy by incorporating a Mo source into presynthesized Co-based metal-organic framework(MOF)arrays on carbon cloth(CC),named as ZIF-67/CC *** found that tuning the Mo content resulted in gradual differences in the structural properties,surface morphology,and chemical states of the resulting catalysts,namely CoMox-LDH/CC(x representing the added weight of the Mo source).Gratifyingly,the best-performing CoMo_(0.20)-LDH/CC electrocatalyst demonstrates a low overpotential of only 226 mV and high stability at a current density of 10 mA·cm^(−2),which is superior to most LDH-based OER catalysts reported ***,it only required 1.611 V voltage to drive the overall water splitting device at the current density of 10 mA·cm^(−2).The present study represents a significant advancement in the development and applications of new OER catalysts.

关键词： layered double hydroxides(LDHs) metal-organic frameworks(MOFs) array catalysts Mo modification electrocatalytic oxygen evolution reaction(OER)

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Inhibiting Voltage Decay in Li-Rich Layered Oxide Cathode:From O3-Type to O2-Type Structural Design

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Nano-Micro Letters 2024年第12期16卷 81-102页

作者： Guohua Zhang Xiaohui Wen Yuheng Gao Renyuan Zhang Yunhui Huang Institute of New Energy for Vehicles Shanghai Key Laboratory for R&D and Application of Metallic Functional MaterialsSchool of Materials Science and EngineeringTongji UniversityShanghai 201804People’s Republic of China Contemporary Amperex Technology Co. LtdNingde 352100People’s Republic of China State Key Laboratory of Material Processing and Die and Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiPeople’s Republic of China

Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox ***,continuous voltage decay during cycling remains the primary obstacle for practical applications,which has yet to be fundamentally *** is widely acknowledged that voltage decay originates from the irreversible migration of transition metal ions,which usually further exacerbates structural evolution and aggravates the irreversible oxygen redox ***,constructing O2-type structure has been considered one of the most promising approaches for inhibiting voltage *** this review,the relationship between voltage decay and structural evolution is systematically *** to suppress voltage decay are systematically ***,the design of O2-type structure and the corresponding mechanism of suppressing voltage decay are comprehensively ***,the reported O2-type LRLO cathodes still exhibit partially disordered structure with extended ***,the factors that may cause the irreversible transition metal migrations in O2-type LRLO materials are also explored,while the perspectives and challenges for designing high-performance O2-type LRLO cathodes without voltage decay are proposed.

关键词： Lithium-ion batteries Li-rich layered oxide Voltage decay Migration of transition metal ions O2-type structural design

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Synthesis and mechanical and elevated temperature tribological properties of a novel high-entropy(TiVNbMoW)C_(4.375) with carbon stoichiometry deviation

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Journal of advanced Ceramics 2023年第2期12卷 242-257页

作者： Jicheng LI Yanchun ZHOU Yunfeng SU Shuna CHEN Qiuan SUN Hengzhong FAN Junjie SONG Litian HU Yongsheng ZHANG State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Science and Technology on Advanced Functional Composite Laboratory Aerospace Research Institute of Materials&Processing TechnologyBeijing 100076China

High-entropy carbides are a nascent group of ceramics that are promising for high-temperature applications due to the combination of good stability,high hardness(H),high strength,and superior creep resistance that they *** to high melting points and low lattice diffusion coefficients,however,the high-entropy carbides are usually difficult to consolidate to a nearly full *** cope with this challenge,herein,binary carbides including TiC,V_(8)C_(7),NbC,Mo_(2)C,and WC with different carbon stoichiometry were used to prepare dense high-entropy(TiVNbMoW)C_(4.375),and the influence of carbon vacancy on formation ability and mechanical properties of carbon-deficient high-entropy(TiVNbMoW)C_(4.375) were ***,although the starting binary carbides have different crystal structures and carbon stoichiometry,the as-prepared high-entropy material showed a rock-salt structure with a relatively high density(98.1%)and good mechanical properties with hardness of 19.4±0.4 GPa and fracture toughness(KIC)of 4.02 MPa·m^(1/2).More importantly,the high-entropy(TiVNbMoW)C_(4.375) exhibited low coefficient of friction(COF)at room temperature(RT)and 800℃.Wear rate(W)gradually increased with the temperature rising,which were attributed to the formation of low-hardness oxidation films at high temperatures to aggravate *** 800℃,lubricating films formed from sufficient oxidation products of V_(2)O_(5) and MoO_(3) effectively improved tribological behavior of the high-entropy(TiVNbMoW)C_(4.375).Wear mechanisms were mainly abrasive wear resulting from grain pullout and brittle fracture as well as oxidation wear generated from high-temperature *** results are useful as valuable guidance and reference to the synthesis of high-entropy ceramics(HECs)for sliding parts under high-temperature serving conditions.

关键词： high-entropy ceramics(HECs) transition metal(TM)carbides carbon stoichiometry deviation tribological performances wear

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Strain engineering of Pt-based electrocatalysts for oxygen reaction reduction

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Frontiers in Energy 2024年第2期18卷 241-262页

作者： Zeyu WANG Yanru LIU Shun CHEN Yun ZHENG Xiaogang FU Yan ZHANG Wanglei WANG State Key Laboratory of Solidification Processing Atomic Control and Catalysis Engineering LaboratorySchool of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China State Key Laboratory of Oral and Maxillofacial Reconstruction and Regeneration National Clinical Research Center for Oral DiseasesShaanxi Key Laboratory of StomatologyDepartment of Dental MaterialsSchool of StomatologyThe Fourth Military Medical UniversityXi’an 710032China Institute of New Energy Materials and Engineering School of Materials Science and EngineeringFuzhou UniversityFuzhou 350108China Key Laboratory of Marine Chemistry Theory and Technology(Ministry of Education) College of Chemistry and Chemical EngineeringOcean University of ChinaQingdao 266100China

Proton exchange membrane fuel cells(PEMFCs)are playing irreplaceable roles in the construction of the future sustainable energy ***,the insufficient performance of platinum(Pt)-based electrocatalysts for oxygen reduction reaction(ORR)hinders the overall efficiency of *** the surface strain of catalysts is considered an effective way to tune their electronic structures and therefore optimize catalytic *** this paper,insights into strain engineering for improving Pt-based catalysts toward ORR are elaborated in ***,recent advances in understanding the strain effects on ORR catalysts are comprehensively ***,strain engineering methodologies for adjusting Ptbased catalysts are comprehensively ***,further information on the various challenges and potential prospects for strain modulation of Pt-based catalysts is provided.

关键词： strain engineering Pt-based catalysts oxygen reduction reaction(ORR) catalytic performance proton exchange membrane fuel cells(PEMFCs)

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Carbon composite support improving catalytic effect of NbC nanoparticles on the low-temperature hydrogen storage performance of MgH_(2)

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Journal of materials Science & technology 2023年第19期150卷 65-74页

作者： Yuxiao Jia Xuancheng Wang Leijie Hu Xuezhang Xiao Shuoqing Zhang Jiahuan He Jiacheng Qi Ling Lv Fen Xu Lixian Sun Lixin Chen State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027China Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province Hangzhou 310013China Guangxi Collaborative Innovation Center of Structure and Property for New Energy and Materials School of Material Science and EngineeringGuilin University of Electronic TechnologyGuilin 541004China

Ultrafine carbon-based transition metal compounds have been widely investigated as efficient catalysts for enhancing the hydrogen storage performance of magnesium *** this work,the carbon ther-mal shock method is applied to synthesize the ultrafine carbon-encapsulated NbC nanoparticles with an average grain size of 17.3 *** MgH_(2)-10 wt%NbC/C composites show excellent low-temperature hy-drogen storage performance with the onset dehydrogenation temperature of 196.1℃,which is 92.2℃ and 98℃ lower than that of MgH_(2)-10 wt%NbC and undoped MgH_(2),***,MgH_(2)-10 wt%NbC/C can absorb 6.71 wt%H_(2) at 100℃ within 30 min around and retain almost 100%reversible hydrogen desorption capacity after 10 *** the catalytic mechanism,the electron transfer process between multi-valence Nb cations of in-situ formed NbH x and Mg,H atoms can greatly improve the cyclic de/rehydrogenation kinetics of MgH_(2)-NbC/***,the enhancement of dehydrogenation kinetics can also be ascribed to MgH_(2) particle refinement by NbC nanoparticles,and destabilization of the Mg-H bond caused by carbon *** investigation not only proves that carbon-encapsulated NbC nanoparti-cles can greatly enhance the hydrogen storage performance of MgH_(2) but provides an idea of preparing carbon-based transition metal carbides as effective catalysts for magnesium-based hydrogen storage ma-terials.

关键词： MgH_(2) Carbon-encapsulated Nanoparticles Catalyst Kinetics

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Building a Highly Stable Ultrathin Nanoporous Layer Assisted by Glucose for Desalination

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Engineering 2022年第9期16卷 247-255页

作者： Yanqiu Zhang Fan Yang Hongguang Sun Yongping Bai Songwei Li Lu Shao MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage&State Key Laboratory of Urban Water Resource and Environment School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China MOE Key Laboratory of Materials Processing and Molding&National Engineering Research Center for Advanced Polymer Processing Technology Zhengzhou UniversityZhengzhou 450002China

Although nanoporous membranes are of great interest in desalination,it is still challenging to construct highly permeable nanoporous membranes with excellent rejections for an efficient desalination *** this work,highly permeable nanoporous membranes were built from renewable resources,assisted by the versatile functions of glucose and dopamine,with coupling reactive groups via interfacial reaction with 1,3,5-benzenetricarbonyl trichloride(TMC).The small molecules(0.66 nm)of glucose,which have high hydrophilicity,can diffuse into the membrane for an effective reaction to ensure structural *** novel ultrathin(~44 nm)nanofiltration(NF)membrane exhibits ultra-high Na_(2)SO_(4)flux and excellent rejection of Na_(2)SO_(4)(66.5 L·m^(-2)·h^(-1),97.3%)and MgSO4(63.0 L·m^(-2)·h^(-1),92.1%)under a pressure of 5 bar(1 bar=10^(5)Pa)which is much superior to the performance of natural-product NF *** membrane demonstrates excellent long-term stability,as well as tremendous acid-base and alkali-base stability and high anti-pollution *** designed membrane materials and architecture open a new door to biopolymer-based separation membranes beyond existing membrane materials.

关键词： Nanoporous membrane Renewable resources Nanofiltration Desalination Glucose

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