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Building Li-S batteries with enhanced temperature adaptability via a redox-active COF-based barrier-trapping electrocatalyst

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Journal of Energy Chemistry 2025年第2期101卷 702-712页

作者： Jie Xu Acheng Zhu Zhangyu Zheng Yiming Qi Yuwen Cheng Yongjie Cao Bo Peng Lianbo Ma Yonggang Wang School of materials Science and Engineering Key Laboratory of Efficient Conversion and Solid-state Storage of Hydrogen & Electricity of Anhui Province Key Laboratory of Green Fabrication and Surface Technology of Advanced Metal Materials of Ministry of Education Anhui University of Technology Department of Chemistry and Shanghai Key laboratory of Molecular Catalysis and Innovative materials Institute of New Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Fudan University

Covalent organic frameworks（COFs） are promising materials for mitigating polysulfide shuttling in lithium-sulfur（Li-S） batteries,but enhancing their ability to convert polysulfides across a wide temperature range remains a challenge,Herein,we introduce a redox-active COF（RaCOF） that functions as both a physical barrier and a kinetic enhancer to improve the temperature adaptability of Li-S batteries,The RaCOF constructed from redox-active anthraquinone units accelerates polysulfide conversion kinetics through reversible C=O/C-OLi transformations within a voltage range of 1,7 to 2.8 V（***+/Li）,optimizing sulfur redox reactions in ether-based *** conventional COFs,RaCOF provides bidentate trapping of polysulfides,increasing binding energy and facilitating more effective polysulfide ***-situ XRD and ToF-SIMS analyses confirm that RaCOF enhances polysulfide adsorption and promotes the transformation of lithium sulfide（Li2S）,leading to better sulfur cathode ***,RaCOF-modified Li-S batteries demonstrate low self-discharge（4.0% decay over a 7-day rest）,excellent wide-temperature performance（stable from-10 to+60℃）,and high-rate cycling stability（94% capacity retention over 500 cycles at 5.0 C）.This work offers valuable insights for designing COF structures aimed at achieving temperature-adaptive performance in rechargeable batteries.

关键词： Covalent organic framework Lithium-sulfur batteries Redox-active property Wide-temperature adaptability

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Structure,morphology,and microwave dielectric properties of SmAlO_(3) synthesized by stearic acid route

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Journal of advanced Ceramics 2020年第5期9卷 558-566页

作者： Jiamao LI Chuimin ZHANG Hui LIU Tai QIU Chuangang FAN School of materials Science and Engineering Anhui University of TechnologyMaanshan 243032China bkey laboratory of green fabrication and surface technology of advanced metal materials Ministry of EducationAnhui University of TechnologyMaanshan 243002China College of materials Science and Engineering Nanjing Tech UniversityNanjing 211816China

A rapid and facile approach was developed for the synthesis of ultrafine SmAlO_(3) powders through the combustion of stearic acid *** obtained products were characterized by typical techniques including X-ray diffraction(XRD),Fourier Transform Infrared(FT-IR),thermogravimetric and differential thermal analysis(TG-DTA),scanning electron microscopy(SEM),and transmission electron microscopy(TEM)to analyze the phase composition and *** dielectric characteristics of SmAlO_(3) microwave ceramics,using the as-obtained products as original materials,were also *** with the conventional solid-state reaction method,the synthesis temperature was dramatically reduced to 750℃.The large-size sheet structure was composed of a number of micro/nano-scale crystallites,which were mostly irregular in shape due to the mutual growth and overlapping shapes of adjacent *** SmAlO_(3) ceramics with high density and uniform microstructure were obtained after sintering at 1500℃ for 4 h due to the favorable sintering activity of the as-synthesized *** addition,desired dielectric properties at microwave frequencies(dielectric constant ε_(r)=20.22,quality factor Q·f=74110 GHz,and a temperature coefficient of resonant frequency τ_(f)=-74.6 ppm/℃)were achieved.

关键词： stearic acid precursor process nanoparticle perovskite microwave ceramics

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Influences of substituting of(Ni_(1/3)Nb(2/3))for Ti^(4+)on the phase compositions,microstructures,and dielectric properties of Li_(2)Zn[Ti_(1-x)(Ni_(1/3)Nb_(2/3))_(x)]_(3)O_(8)(0<≤x≤0.3)microwave ceramics

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Journal of advanced Ceramics 2023年第4期12卷 760-777页

作者： Jiamao Li Zexing Wang Yunfeng Guo Songlin Rana School of materials Science and Engineering Anhui University of TechnologyMaanshan 243032China Key laboratory of green fabrication and surface technology of advanced metal materials Ministry of EducationAnhui University of TechnologyMaanshan 243002China

Complex ion substitution is gaining more attention as an appealing method of modifying the structure and performance of microwave *** this work,Li_(2)Zn[Ti_(1-x)(Ni_(1/3)Nb_(2/3))_(x)]_(3)O_(8),0≤x≤0.3ceramics were designed based on the complex ion substitution strategy,following the substitution rule of radius and valence to investigate the relationship among phase compositions(containing oxygen vacancies and Ti^(3+)ions),microstructures,and microwave dielectric characteristics of the LZTNNx *** samples maintained a single Li_(2)ZnTi_(3)O_(8)solid solution phase as x≤0.2,whereas the sample of x=0.3 produced a second phase with the LiNbO_(3)*** appropriate amount of(Ni_(1/3)Nb_(2/3))^(4+)substitution could slightly improve the densification of the LZTNNx ceramics due to the formation of the LiZnTi_(3)O_(8)solid solution accompanied by a decrease in the average grain *** presence of a new Aig Raman active band at about 848 cm^(-1)indicated that local symmetry changed,affecting atomic interactions of the LZTNNx *** variation of the relative dielectric constant(εr)was closely related to the molar volume ionic polarizability(α_(D)^(T)),and the temperature coefficient of the resonant frequency(τ_(f))was related to the bond valence(V_(1))of *** increase in density,the absence of the Ti3+ions and oxygen vacancies,and the reduction in damping behavior were responsible for the decreased dielectric *** LZTNNO.2 ceramics sintered at 1120℃exhibited favorable microwave dielectric properties:εr=22.13,quality factor(Q×f)=97,350 GHz,andτ_(f)=-18.60 ppm/C,which might be a promising candidate for wireless communication applications in highly selective electronics.

关键词： Li_(2)ZnTi_(3)O_(8)ceramics microwave dielectric properties microstructure Raman spectroscopy X-ray photoclcctron spectroscopy(XPS)

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Energy band and charge-carrier engineering in skutterudite thermoelectric materials

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Chinese Physics B 2022年第10期31卷 208-219页

作者： Zhiyuan Liu Ting Yang Yonggui Wang Ailin Xia Lianbo Ma Key laboratory of green fabrication and surface technology of advanced metal materials(Ministry of Education) Anhui University of TechnologyMaanshan 243002China School of materials Science and Engineering Anhui University of TechnologyMaanshan 243002China

The binary CoSb_(3) skutterudite thermoelectric material has high thermal conductivity due to the covalent bond between Co and Sb, and the thermoelectric figure of merit, ZT, is very low. The thermal conductivity of CoSb_(3) materials can be significantly reduced through phonon engineering, such as low-dimensional structure, the introduction of nano second phases,nanointerfaces or nanopores, which greatly improves their ZT values. The phonon engineering can optimize significantly the thermal transport properties of CoSb_(3)-based materials. However, the improvement of the electronic transport properties is not obvious, or even worse. Energy band and charge-carrier engineering can significantly improve the electronic transport properties of CoSb_(3)-based materials while optimizing the thermal transport properties. Therefore, the decoupling of thermal and electronic transport properties of CoSb_(3)-based materials can be realized by energy band and charge-carrier engineering. This review summarizes some methods of optimizing synergistically the electronic and thermal transport properties of CoSb_(3) materials through the energy band and charge-carrier engineering strategies. Energy band engineering strategies include band convergence or resonant energy levels caused by doping/filling. The charge-carrier engineering strategy includes the optimization of carrier concentration and mobility caused by doping/filling, forming modulation doped structures or introducing nano second phase. These strategies are effective means to improve performance of thermoelectric materials and provide new research ideas of development of high-efficiency thermoelectric materials.

关键词： CoSb_(3)-based skutterudite materials energy band engineering charge-carrier engineering thermoelectric properties

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Ageing Hardening Mechanism and Corrosion Resistance in the Fe65Cr13Cu3(CoMnMoNiAlTi)19 Medium-Entropy Stainless Alloy

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Acta metallurgica Sinica(English Letters) 2021年第11期34卷 1601-1608页

作者： Ben-Qi Xu Hui Zhang Dong Ma Qun-Shuang Ma Li-Zhai Pei Key laboratory of green fabrication and surface technology of advanced metal materials(Ministry of Education) Anhui University of Technology243002Ma'anshanChina School of materials Science and Engineering Anhui University of TechnologyMa'anshan 243002China

The ageing hardening mechanism of a newly designed Fe65Cr13Cu3(CoMnMoNiAlTi)19 medium-entropy stainless alloy(ME-SA)with a simple bcc solid solution matrix was *** kind of ME-SA possessed a higher ageing hardness of approximately 584 HV and higher compressive stress and corrosion resistance than those of the conventional precipitation hardening stainless steel 17-4 PH(Cr17Ni4Cu4 Nb),which has comparable compressive *** well-dispersed B2-ordered phase in the cast state transformed to a D03 crystal structure with a higher ordering degree and reduced the precipitate size after ageing at 500℃,thus promoting a great ageing hardening effect.

关键词： Medium-entropy stainless alloy Ordered phase transition Aging hardening Corrosion resistance

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Boosting high-rate Li-ion storage properties by La(Ⅲ)ion doping in spinel(Co_(0.2)Cr_(0.2)Fe_(0.2)Mn_(0.2)Ni_(0.2))_(3)O_(4)high-entropy oxide anode

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Journal of advanced Ceramics 2024年第6期13卷 769-779页

作者： Shijie Chen Mengfan Bao Yanggang Jia Pengpeng Wang Dan Wei Yuhuan Guo Jie Tan Aiqin Mao advanced Ceramics Research Center School of Materials Science and EngineeringAnhui University of TechnologyMa’anshan 243032China Key laboratory of green fabrication and surface technology of advanced metal materials(Anhui University of technology) Ministry of EducationMa’anshan 243032China

The present work aims to create lattice distortion and optimize the surface oxygen vacancy(OV)concentration in a model spinel(Co_(0.2)Cr_(0.2)Fe_(0.2)Mn_(0.2)Ni_(0.2))_(3)O_(4)high-entropy oxide(HEO)through a heteroatom La^(3+)doping *** demonstrated,La^(3+)with a large radius can be doped successfully into the spinel lattice of(Co_(0.2)Cr_(0.2)Fe_(0.2)Mn_(0.2)Ni_(0.2))_(3)O_(4),thereby not only causing lattice distortion to increase oxygen vacancies but also refining crystalline grains and improving the specific *** with the(Co_(0.2)Cr_(0.2)Fe_(0.2)Mn_(0.2)Ni_(0.2))_(3)O_(4)anode,the(La_(0.01)CoCrFeMnNi)_(3/5.01)O_(4) anode with moderate doping exhibits excellent cycling performance(1228 mAh·g^(−1)after 400 cycles at 0.2 A·g^(−1))and yields an increase of 75%rate capability at 3 A·g^(−1)(420 mAh·g^(−1)at 3 A·g^(−1)).The desirable kinetic transport of electrons and diffusion of Li+within the moderately La^(3+)-doped anode and the synergistic interfacial pseudocapacitive behavior satisfy the redox reaction at a high rate,thus increasing rate capability.

关键词： lithium-ion battery(LIB) anode lattice distortion high-entropy oxide(HEO) high-rate performance La^(3+)doping oxygen vacancy(OV)

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Research progress of p-type Fe-based skutterudite thermoelectric materials

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Frontiers of materials Science 2021年第3期15卷 317-333页

作者： Xin TONG Zhiyuan LIU Jianglong ZHU Ting YANG Yonggui WANG Ailin XIA Key laboratory of green fabrication and surface technology of advanced metal materials(Ministry of Education) Anhui University of TechnologyMaanshan 243002China School of materials Science and Engineering Anhui University of TechnologyMaanshan 243002China

Filled skutterudite is currently one of the most promising intermediate-temperature thermoelectric(TE)materials,having good thermoelectric transport performance and excellent mechanical *** the preparation of high-efficiency filled skutterudite TE devices,it is important to have p-and n-type filled skutterudite TE materials with matching ***,the current TE properties of p-type Fe-based filled skutterudite materials are worse than n-type filled skutterudite ***,how to obtain high-performance p-type Fe-based filled skutterudite materials is the key to preparation of high-efficiency skutterudite-based TE *** review summarizes some methods for optimizing the thermal transport performance of p-type filled skutterudite materials at the atomic-molecular and nano-mesoscopic scale that have been used in recent *** methods include doping,multi-atom filling,and use of low-dimensional structure and of *** addition,the synergistic optimization methods of the electrical and thermal transport parameters and advanced preparation technologies of p-type filled skutterudite materials in recent years are also briefly *** optimizational methods and advanced preparation technologies can significantly improve the TE properties of p-type Fe-based filled skutterudite materials.

关键词： p-type Fe-based filled skutterudite lattice thermal conductivity synergistic optimization preparation technology thermoelectric property

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A review of CoSb_(3)-based skutterudite thermoelectric materials

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Journal of advanced Ceramics 2020年第6期9卷 647-673页

作者： Zhi-Yuan LIU Jiang-Long ZHU Xin TONG Shuo NIU Wen-Yu ZHAO School of materials Science and Engineering Anhui University of TechnologyMaanshan 243002China Key laboratory of green fabrication and surface technology of advanced metal materials Ministry of EducationAnhui University of TechnologyMaanshan 243002China State Key laboratory of advanced technology for materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

The binary skutterudite CoSb_(3) is a narrow bandgap semiconductor thermoelectric(TE)material with a relatively flat band structure and excellent electrical ***,thermal conductivity is very high because of the covalent bond between Co and Sb,resulting in a very low ZT ***,researchers have been trying to reduce its thermal conductivity by the different optimization *** addition,the synergistic optimization of the electrical and thermal transport parameters is also a key to improve the ZT value of CoSb_(3) material because the electrical and thermal transport parameters of TE materials are closely related to each other by the band structure and scattering *** review summarizes the main research progress in recent years to reduce the thermal conductivity of CoSb_(3)-based materials at atomic-molecular scale and nano-mesoscopic *** also provide a simple summary of achievements made in recent studies on the non-equilibrium preparation technologies of CoSb_(3)-based materials and synergistic optimization of the electrical and thermal transport *** addition,the research progress of CoSb_(3)-based TE devices in recent years is also briefly discussed.

关键词： skutterudite CoSb_(3)-based materials lattice thermal conductivity synergistic optimization thermoelectric properties thermoelectric devices

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Effects of Magnetization on Thermoelectric Transport Properties of CoSb_(3)Material

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Journal of Wuhan University of technology(materials Science) 2021年第3期36卷 353-357页

作者： ZHU Jianglong TONG Xin NIU Shuo LIU Zhiyuan XU Dong Key laboratory of green fabrication and surface technology of advanced metal materials Ministry of EducationAnhui University of TechnologyMaanshan 243002China School of materials Science and Engineering Anhui University of TechnologyMaanshan 243002China

The effects of magnetization on the phase composition,microstructure and thermoelectric transport properties of CoSb_(3)were studied *** magnetic properties of CoSb_(3)material were also measured at room temperature in order to confirm its magnetic *** results of XRD and FESEM analysis indicated that the phase composition and microstructure of the CoSb_(3)were not affected by *** results of thermoelectric transport measurement showed that the electrical and thermal transport properties of materials were also not affected by *** results were mainly attributed to the diamagnetism of the CoSb_(3)material,which were consistent with the results of the magnetic properties *** study is expected to provide a special research perspective for studying the effects of the external conditions on the structure and properties of thermoelectric materials.

关键词： CoSb_(3)materials magnetization thermoelectric properties thermoelectric materials

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Alloying engineering for thermoelectric performance enhancement in p-type skutterudites with synergistic carrier concentration optimization and thermal conductivity reduction

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Journal of advanced Ceramics 2023年第3期12卷 539-552页

作者： Zhiyuan Liu Yonggui Wang Ting Yang Zuju Ma Huiyan Zhang Hailing Li Ailin Xia Key laboratory of green fabrication and surface technology of advanced metal materials Ministry of EducationAnhui University of TechnologyMaanshan 243002China School of materials Science and Engineering Anhui University of TechnologyMaanshan 243002China School of Environmental and materials Engineering Yantai UniversityYantai 264005China

The enhancements in thermoelectric(TE)performances of p-type skutterudites are usually limited due to the relatively low Seebeck coefficients owing to the higher carrier concentration and more impurity phases induced by inherent structural instability of a Fe-based *** shown in this study,alloying engineering of Ni doping at Fe sites in a p-type CeFe_(3.8)Co_(0.2)Sb_(12)skutterudite can not only reduce the impurity phases with high thermal conductivity but also regulate the carrier concentration,and thus significantly increase the Seebeck *** thermal conductivity was largely suppressed due to the enhanced point defect phonon scattering and decreased hole *** a result,a TE figure of merit ZT of the CeFe_(3.5)Ni_(0.3)Co_(0.2)Sb_(12)sample reached 0.8,which is approximately 50%higher than that of a Ni-free *** Ni doping can maintain a high ZT at a high temperature by controlling the reduction in a band ***,a high average ZT close to 0.8 at 650–800 K for CeFe_(3.5)Ni_(0.3)Co_(0.2)Sb_(12)was obtained,which was comparable to or even higher than those of the reported Ce-filled Fe-based skutterudites due to the synergistic optimization of electrical and thermal *** study provides a strategy to synergistically optimize electrical–thermal performances of the p-type skutterudites by alloying engineering.

关键词： p-type skutterudite materials Ni doping synergistic optimization thermoelectric(TE)properties

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