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Pressure-induced cation and vacancy disorder-order transition and near-zero τ_f in deficient hexagonal perovskite Ba8ZnTa6O24 dielectrics

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Science China Chemistry 2025年

作者： Bin Zheng Ruiwen Ji Cécile Genevois Wenda Zhang Xing Ming Qiang Zhang Mathieu Allix Congling Yin Xiaojun Kuang Xianran Xing MOE Key Laboratory of New Processing Technology for Nonferrous Metal and Materials Guangxi Key Laboratory of Optical and Electronic Materials and Devices College of Materials Science and Engineering Guilin University of Technology Centre National de la Recherche Scientifique (CNRS) CEMHTI UPR3079 Université d'Orléans College of Physics and Electronic Information Engineering Guilin University of Technology Neutron Scattering Division Oak Ridge National Laboratory Collaborative Innovation Center for Exploration of Nonferrous Metal Deposits and Efficient Utilization of Resources Guilin University of Technology Guangxi Key Laboratory of Electrochemical and Magnetochemical Functional Materials College of Chemistry and BioengineeringGuilin University of Technology Beijing Advanced Innovation Center for Materials Genome Engineering and Institute of Solid-State Chemistry University of Science and Technology Beijing

Pressure applications can enable the tuning of atomic/defect ordering and provide access to new functional materials. Here, we report that pressure-induced structural transformation featuring disorder-order transition of both cations and vacancies in the 8-layer deficient hexagonal perovskite tantalate dielectrics Ba8ZnTa6O24, which transformed the structure from twin to shift and remarkably lowered the temperature coefficient of resonant frequency τ_f down to near zero（～0.56 ppm/°C） from 38 ppm/°C for the twinned precursor. The atomic scale STEM-HAADF and EDS results confirm the ordering of Zn in the Ta host at the nanometer scale in the shifted material featuring well-ordered Ba8ZnTa6O24slabs intergrown with Ba3ZnTa2O9and Ba5Ta4O15monolayers and anti-phase grain boundaries as planar defects. The pressure-induced twin-shift structural transformation of Ba8ZnTa6O24features the rare constant concentration of the hexagonal stacked layers, which is allowed by the vacancy ordering at the central layers of face-shared octahedral（FSO） trimers avoiding the FSO B-B repulsion, and remarkably the faster cationic ordering kinetics compared with the 2:1 ordered complex perovskites. Although the inclusion of numerous planar defects and the oxidizable atomic defects led to significant p-type conduction and inhomogeneous electrical microstructures, resulting in an extraordinarily high extrinsic dielectric loss for the high-pressure shifted Ba8ZnTa6O24pellet, the intrinsically near-zero τ_fcould make the shifted Ba8ZnTa6O24perovskite an ideal microwave dielectric resonator candidate if the defects could be eliminated.

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Atomically dispersed Zn-Co-N-C catalyst boosting efficient and robust oxygen reduction catalysis in acid via stabilizing Co-N bonds

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Fundamental Research 2023年第6期3卷 909-917页

作者： Feng Ma Xuan Liu Xiaoming Wang Jiashun Liang Jianyu Huang Cameron Priest Jinjia Liu Shuhong Jiao Tanyuan Wang Gang Wu Yunhui Huang Qing Li State Key Laboratory of Material Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanHubei 430074China State Key Laboratory of Refractories and Metallurgy Institute of Advanced Materials and NanotechnologyKey Laboratory of Hubei Province for Coal Conversion and New Carbon MaterialsSchool of Chemistry and Chemical EngineeringWuhan University of Science and TechnologyWuhan 430081China Clean Nano Energy Center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066004China Department of Chemical and Biological Engineering University at BuffaloThe State University of New YorkBuffaloNY 14260United States State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China National Energy Center for Coal to Clean Fuels Synfuels China Co.LtdHuairou DistrictBeijing 101400China Department of Materials Science and Engineering Key Laboratory of Materials for Energy Conversion Chinese Academy of Science(CAS)University of Science and Technology of ChinaHefei 230026China Department of Chemistry and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province Shantou UniversityShantou 515063China

Transition metal supported N-doped carbon(M-N-C)catalysts for oxygen reduction reaction(ORR)are viewed as the promising candidate to replace Pt-group metal(PGM)for proton exchange membrane fuel cells(PEMFCs).However,the stability of M-N-C is extremely challenging due to the demetalation,H_(2)O_(2)attack,*** the strongly oxidative conditions of *** this study,we demonstrate the universal effect of Zn on promoting the stability of atomically dispersed M-Nx/C(M=Co,Fe,Mn)catalysts and the enhancement mechanism is unveiled for the first *** best-performing dual-metal-site Zn-Co-N-C catalyst exhibits a high half-wave potential(E1/2)value of 0.81 V *** hydrogen electrode(RHE)in acid and outstanding durability with no activity decay after 15,000 accelerated degradation test(ADT)cycles at 60℃,surpassing most reported Co-based PGM-free catalysts in acid *** comparison,the Co-N-C in the absence of Zn suffers from a rapid degradation after ADT due to the demetalation and higher H_(2)O_(2)yield.X-ray adsorption spectroscopy(XAS)and density functional theory(DFT)calculations suggest the more negative formation energy(by 1.2 eV)and increased charge transfer of Zn-Co dual-site structure compared to Co-N-C could strength the Co-N bonds against the demetalation and the optimized d-band center accounts for the improved ORR kinetics.

关键词： Electrocatalysis Oxygen reduction reaction Non-noble metal catalysts Metal-nitrogen carbon catalysts Demetalation Structural stability

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Surface-engineered caterpillar-like silica nanocomposites for enhanced interparticle friction and interlock in shear thickening suspension

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Journal of Molecular Liquids 2024年 414卷

作者： Wang, Xiaobing Wang, Lujie Zhou, Yi Lu, Ying Liu, Jing Zhu, Lanyan Ding, Zhao Zhou, Yang School of Textile Science and Engineering / State Key Laboratory of New Textile Materials and Advanced Processing Technology Wuhan Textile University Wuhan430200 China School of Electronics and Electrical Engineering Wuhan Textile University Wuhan430200 China College of Materials Science and Engineering / National Engineering Research Center for Magnesium Alloys Chongqing University Chongqing400044 China

This study presents a novel method for fabricating surface-engineered caterpillar-like silica nanocomposites by combining rod-like nanorods with spherical nanoparticles to control aspect ratios and surface functionalization. This unique design facilitates functional assembly at the nanoscale. Additionally, we developed an innovative composite by encapsulating polyurethane elastomers within shear thickening fluid (STF)-impregnated Kevlar, significantly enhancing the flexibility and durability of the resulting STF/Kevlar/PU composite. Microstructural and chemical modifications were characterized, and detailed rheological analysis revealed a 165 % increase in viscosity and a substantial rise in storage modulus from 91.56 to 18,640 Pa, indicating improved surface morphology and roughness. These enhancements promoted stronger interparticle friction and rotational motion during flow. Impact resistance tests further demonstrated a 314 % increase in peak impact force, driven by frictional interactions between the dispersed caterpillar-like particles. The results confirmed that surface roughness and adhesive forces play a critical role in activating stress-dependent frictional contacts, a key mechanism behind the improved performance. These findings highlight the potential of these composites for mitigating penetration injuries and offer precise control over the shear-thickening transition in engineering applications, making them promising candidates for lightweight protective materials. © 2024 Elsevier B.V.

关键词： Nanorods

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Ultra-Stable and Durable Piezoelectric Nanogenerator with All-Weather Service Capability Based on N Doped 4H-SiC Nanohole Arrays

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Nano-Micro Letters 2022年第2期14卷 151-160页

作者： Linlin Zhou Laipan Zhu Tao Yang Xinmei Hou Zhengtao Du Sheng Cao Hailong Wang Kuo-Chih Chou Zhong Lin Wang Beijing Advanced Innovation Center for Materials Genome Engineering Collaborative Innovation Center of Steel TechnologyUniversity of Science and Technology BeijingBeijing 100083People’s Republic of China Beijing Institute of Nanoenergy and Nanosystems Chinese Academy of SciencesBeijing 100083People’s Republic of China MOE Key Laboratory of New Processing Technology for Non‑Ferrous Metals and Materials Guangxi Key Laboratory of Processing for Non‑Ferrous Metals and Featured MaterialsGuangxi UniversityNanning 530004People’s Republic of China School of Materials Science Engineering Zhengzhou UniversityZhengzhou 450001People’s Republic of China

Ultra-stable piezoelectric nanogenerator(PENG)driven by environmental actuation sources with all-weather service capability is highly ***,the PENG based on N doped 4H-SiC nanohole arrays(NHAs)is proposed to harvest ambient energy under low/high temperature and relative humidity(RH)*** element method simulation of N doped 4H-SiC NHAs in compression mode is developed to evaluate the relationship between nanohole diameter and piezoelectric *** density of short circuit current of the assembled PENG reaches 313 nA cm^(-2),which is 1.57 times the output of PENG based on N doped 4H-SiC nanowire *** enhancement can be attributed to the existence of nanohole sidewalls in ***-weather service capability of the PENG is verified after being treated at-80/80℃and 0%/100%RH for 50 *** PENG is promising to be widely used in practice worldwide to harvest biomechanical energy and mechanical energy.

关键词： Piezoelectric nanogenerators N doped 4H-SiC nanohole arrays Environmental actuation sources All-weather service capability Enhanced short circuit current density

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Revealing ionically isolated Li loss in practical rechargeable Li metal pouch cells

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Science Bulletin 2025年第6期70卷 914-922页

作者： Xiangrui Duan Yuanjian Li Kai Huang Shuibin Tu Guocheng Li Wenyu Wang Hongyu Luo Zihe Chen Chunhao Li Kai Cheng Xin-Xin Wang Li Wang Yongming Sun Wuhan National Laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074China State Key Laboratory of Material Processing and Die&Mold Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China State Key Laboratory of Material Processing and Die&Mold Technology Department of MechanicsSchool of Aerospace EngineeringHuazhong University of Science and TechnologyWuhan 430074China Institute of Nuclear&New Energy Technology Tsinghua UniversityBeijing 100084China

The degradation of rechargeable lithium(Li)metal batteries is primarily attributed to active Li loss,encompassing isolated Li,also known as“dead Li”,and solid electrolyte interphase(SEI-Li).Comprehending the formation of dead Li is pivotal for devising strategies to mitigate Li ***,we reveal the existence of an alternative form of dead Li,termed ionically isolated Li(I-iLi),which diverges from the traditionally recognized electronically isolated Li(E-iLi).This phenomenon is elucidated through a quantitative analysis of electrolyte-dependent capacity recovery at a specific state of health(SOH)in high-energy pouch cells,which originates from disconnections within the Li-ion percolation network induced by electrolyte ***,we propose the electrolyte infilling ratio(EFR),contingent upon the porosity of Li deposits and electrolyte retention,as a criterion to evaluate electrode *** uphold a high EFR environment,we introduce stress modulation to compact the anode structure and mitigate electrolyte degradation,significantly reducing the I-iLi content from 21%at 0.1 MPa to 1%at 1 *** these insights,a prototype anode-free LiNi_(0.95)Mn_(0.03)Co_(0.02)O_(2)||Cu pouch cell(1.4 Ah)achieves an extraordinary cell-level energy density of 551 Wh kg^(−1)and maintains 70%capacity after 100 cycles at 0.2 C.

关键词： Dead Li Ionically isolated Li Electrolyte infilling ratio Li metal batteries Lean electrolyte conditions

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Sustainable Generation of Sulfate Radicals and Decontamination of Micropollutants via Sequential Electrochemistry

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Engineering 2023年第11期30卷 144-152页

作者： Wentian Zheng Shijie You Yuan Yao Nanqi Ren Bin Ding Fang Li Yanbiao Liu College of Environmental Science and Engineering Donghua UniversityShanghai 201620China State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150080China Innovation Center for Textile Science and Technology College of TextilesDonghua UniversityShanghai 200051China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

The removal of emerging micropollutants in the aquatic environment remains a global *** routes are often chemically,energetically,and operationally intensive,which decreases their sustainability during ***,we develop an advanced chemical-free strategy for micropollutants decontamination that is solely based on sequential electrochemistry involving ubiquitous sulfate anions in natural and engineered *** can be achieved via a chain reaction initiated by electrocatalytic anodic sulfate(SO_(4)^(2-))oxidation to produce persulfate(S_(2)O_(8)^(2-))and followed by a cathodic persulfate reduction to produce sulfate radicals(SO_(4)^(·-)).These SO_(4)^(·-)are powerful reactive species that enable the unselective degradation of micropollutants and yield SO_(4)^(2-)again in the treated *** proposed flow-through electrochemical system achieves the efficient degradation(100.0%)and total organic carbon removal(65.0%)of aniline under optimized conditions with a single-pass *** also reveal the effectiveness of the proposed system for the degradation of a wide array of emerging micropollutants over a broad pH range and in complex *** work provides the first proof-ofconcept demonstration using ubiquitous sulfate for micropollutants decontamination,making water purification more sustainable and more economical.

关键词： advanced oxidation Chain reaction Sulfate radical Micropollutants Sequential electrochemistry

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Multidisciplinary and multiscale nanoscience research roadmap based on large scientific facilities

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Science China Chemistry 2024年第8期67卷 2497-2523页

作者： Yuan Zeng Shuhan Zhang Yuecong Guo Yalin Cong Xu Ding Peihua Li Yunxiang Lin Wenzhi Ren Hui Su Weigang Sun Liuxin Xu Guikai Zhang Shihua Chen Yu Chen Weiren Cheng Shengqi Chu Yong Guan Jinru Han Jie Lin Hengjie Liu Zheyi Liu Pan Luo Fanchun Meng Sicong Qiao Zongyin Song Ying Wang Zhao Wu Chenyu Yang Meng Yang Shirui Yang Zi Yin Zhibin Yin Pengjun Zhang Hongyu Zhang Pingping Zheng Jia Zhou Wanlin Zhou Pengfei An He Cheng Chunhai Fan Xingjiu Huang Yong Lei Lina Li Mu Li Qinghua Liu Shuming Peng Li Song Zhihu Sun Yangchao Tian Fangjun Wang Lihua Wang Liming Wang Shiqiang Wei Aiguo Wu Chunlei Xiao Xueming Yang Panchao Yin Jing Zhang Mingxin Zhang Yaling Wang Chunying Chen CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety New Cornerstone Science LaboratoryNational Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China Institute of Solid State Physics Hefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031China Institutes of Physical Science and Information Technology Anhui UniversityHefei 230601China Ningbo Key Laboratory of Biomedical Imaging Probe Materials and Technology Zhejiang International Cooperation Base of Biomedical Materials Technology and ApplicationCAS Key Laboratory of Magnetic Materials and DevicesNingbo Cixi Institute of Biomedical EngineeringZhejiang Engineering Research Center for Biomedical MaterialsNingbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201China Advanced Energy Science and Technology Guangdong Laboratory Huizhou 516000China College of Chemistry and Chemical Engineering Hunan Normal UniversityChangsha 410081China State Key Laboratory of Luminescent Materials and Devices South China Advanced Institute for Soft Matter Science and TechnologySouth China University of TechnologyGuangzhou 510640China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China CAS Key Laboratory of Separation Sciences for Analytical Chemistry Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China State Key Laboratory of Molecular Reaction Dynamics Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Institute of Advanced Science Facilities Shenzhen 518107China State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China State Key Laboratory of Particle Detection and Electronics Institute of High Energy PhysicsChinese Acade

With the advancement of modern science and technology, large scientific facilities are increasingly oriented toward demand and application, and can be used for basic research as well as serving multiple disciplines. Developing large scientific facilities and related analytical technologies enhances understanding of large scientific facilities and popularizes their application in research across multiple disciplines. The combination of light or neutron sources from large scientific facilities and advanced analytical technologies can be achieved for materials structure information, dynamics study of chemical reactions, high dissociation of biomolecules, 3D visualization of energy materials or biological samples, etc. We first introduce the progress of domestic large scientific facilities of synchrotron radiation(SR) and free electron lasers(FELs) with different wavelengths and neutron *** further discuss the comparison between Chinese and typical foreign facilities in X-ray radiation from X-ray tubes, synchrotrons, X-ray FELs, and neutron sources based on physical parameters of light and neutron sources. In addition, we focus on the technological progress and perspectives combined with advanced X-ray radiation and neutron sources of large scientific facilities in China, especially in the nanoscience fields of energy catalysis and biological science. We hope that this roadmap will provide references on technology and methods to experimental users, as well as prospects for future development of technologies based on large research infrastructure facilities. Comprehensive studies and guidelines for basic research to practical application in various disciplines can be made with the assistance of large scientific facilities.

关键词： large scientific facilities synchrotron radiation FEL light sources neutron sources spectroscopic analysis methods X-ray imaging techniques structural information chemical dynamics

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The integral role of high-entropy alloys in advancing solid-state hydrogen storage

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Interdisciplinary materials 2025年第1期4卷 75-108页

作者： Zhao Ding Yuting Li Han Jiang Yang Zhou Haiyi Wan Junqi Qiu Fangning Jiang Jun Tan Wenjia Du Yu'an Chen Leon L.Shaw Fusheng Pan College of Materials Science and Engineering National Engineering Research Center for Magnesium AlloysNational Innovation Center for Industry-Education Integration of Energy Storage TechnologyChongqing UniversityChongqingChina State Key Laboratory of New Textile Materials and Advanced Processing Technology School of Textile Science and EngineeringWuhan Textile UniversityWuhanChina Department of Engineering Science University of OxfordOxfordUK Department of Mechanical Materials and Aerospace EngineeringIllinois Institute of TechnologyChicagoIllinoisUSA

High-entropy alloys(HEAs)have emerged as a groundbreaking class of ma-terials poised to revolutionize solid-state hydrogen storage *** comprehensive review delves into the intricate interplay between the unique compositional and structural attributes of HEAs and their remarkable hydrogen storage *** meticulously exploring the design strategies and synthesis techniques,encompassing experimental procedures,thermo-dynamic calculations,and machine learning approaches,this work illumi-nates the vast potential of HEAs in surmounting the challenges faced by conventional hydrogen storage *** review underscores the pivotal role of HEAs'diverse elemental landscape and phase dynamics in tailoring their hydrogen storage *** elucidates the complex mechanisms governing hydrogen absorption,diffusion,and desorption within these novel alloys,offering insights into enhancing their reversibility,cycling stability,and safety ***,it highlights the transformative impact of advanced characterization techniques and computational modeling in un-raveling the structure–property relationships and guiding the rational design of high-performance HEAs for hydrogen storage *** bridging the gap between fundamental science and practical implementation,this review sets the stage for the development of next-generation solid-state hydrogen storage *** identifies key research directions and strategies to accelerate the deployment of HEAs in hydrogen storage systems,including the optimization of synthesis routes,the integration of multiscale characterization,and the harnessing of data-driven ***,this comprehensive analysis serves as a roadmap for the scientific community,paving the way for the widespread adoption of HEAs as a disruptive tech-nology in the pursuit of sustainable and efficient hydrogen storage for a clean energy future.

关键词： compositional influence designstrategies high-entropy alloys solid-state hydrogenstorage structural characteristics

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Influence mechanism of different elements and alloy phases on the corrosion resistance of Zn-Al-Mg coated steel in the atmospheric environment: A review

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Corrosion Communications 2024年第1期13卷 49-59页

作者： Xin He Xun Zhou Ting Shang Wuhua Liu Guangrui Jiang Chao Liu Xuequn Cheng Xin Zhang Xiaogang Li Institute of Advanced Materials&Technology University of Science and Technology Beijing National Materials Corrosion and Protection Data Center University of Science and Technology Beijing Technology Research Institute Shougang Group Co.Ltd. Beijing Key Laboratory of Green Recyclable Process for Iron&steel Production Technology Shougang Jingtang United Iron&Steel Co. Ltd. Institute of New Energy Technology State Power Investment Corporation Central Research Institute

Sacrificial metallic coatings are an effective strategy for mitigating corrosion in steel operating in industrial environments. This review article focuses on examining the protection mechanism of zinc-aluminum-magnesium(Zn-Al-Mg) coatings on steel substrates. Specifically, it investigates the effects of various elements and their corrosion products on the corrosion resistance of Zn-Al-Mg coatings. Furthermore, this review summarizes the formation mechanisms of various specialized corrosion modes that occur following the corrosion of Zn-Al-Mg coatings, based on previous experimental findings. It also includes suggestions for further research areas that could contribute to the development of highly corrosion-resistant and long-lasting coatings. These suggestions are based on published laboratory and field test results available in literature.

关键词： Zn-Al-Mg coated steel Corrosion resistance Corrosion products Black rust Filiform corrosion

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Flower-like superstructure of boron carbon nitride nanosheets with adjustable band gaps for photocatalytic hydrogen peroxide production

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Journal of materials Science & technology 2024年第16期183卷 23-31页

作者： Dehong Yang Yang Li Ruihua Chen Xiangjian Wang Zhi Li Tao Xing Lei Wei Sheng Xu Pengcheng Dai Mingbo Wu College of New Energy State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum(East China)Qingdao 266580China National Engineering Research Center of Coal Gasification and Coal-based Advanced Materials Shandong Energy Group Co.Ltd.Jining 273500China Qinghai Salt Lake Industry Co. Ltd.Haixi Mongolian and Tibetan Autonomous PrefectureQinghai 850099China

The self-assembly of two-dimensional(2D)semiconductor nanosheets into three-dimensional(3D)ordered superstructures represents an ingenious way to avoid aggregation,expose massive available active sites and benefit the mass transfer,which maximizes the advantages of the 2D nanostructures in ***,a flower-like superstructure of ternary semiconducting boron carbon nitride nanosheets(FS-BCNNSs)was synthesized through the morphology-preserved thermal transformation of a flower-like superstructure of boron-containing metal-organic framework nanosheets(FS-MOFNSs).Taking advantage of this functional superstructure,FS-BCNNSs was employed for the pioneering application in the field of photocatalytic hydrogen peroxide(H_(2)O_(2))production and exhibited excellent photocatalytic performance,yielding an impressive rate of 1415.9μmol g^(−1)h^(−1)for the production of H_(2)O_(2).The results of this work offer not just a promising catalyst for photocatalytic H_(2)O_(2)production but also a facile strategy to fabricate unique superstructures constructed from 2D nanosheets for catalysis,energy conversion,and other related fields.

关键词： Photocatalysis Boron carbon nitride Flower-like superstructure Metal-organic framework Hydrogen peroxide production

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