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Improving discharge voltage and ion storage dynamic in polyaniline via modulation of carrier charge density for magnesiummetal batteries

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Nano Research 2024年第7期17卷 6168-6175页

作者： Ping Luo Feiyang Chao Chunli Zuo Wenwei Zhang Fangyu Xiong Zhen Huang Dongyao Zhu Gongtao Yu Wenhui Zhong Xingbao Chen Han Tang Xiujuan Wei Qinyou An Hubei Provincial Key Laboratory of Green Materials for Light Industry School of Materials and Chemical EngineeringHubei University of TechnologyWuhan 430068China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China College of Materials Science and Engineering Chongqing UniversityChongqing 400044China Institute for Sustainable Transformation School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 510006China

Rechargeable magnesium-metal batteries(RMBs)have gained much attention due to their abundant resources as well as high ***,the high charge density of Mg^(2+)is one of the main reasons for the slow kinetics performance of RMBs,and modulation of the charge density is an important strategy to improve the kinetics and electrochemical performance of ***,we report on the conductive polymer polyaniline(PANI)for RMBs,which is found to have excellent kinetics and high discharge voltage when storing MgCl^(+).In the storage of MgCl^(+),PANI exhibits a high average discharge voltage platform is 2.3 V ***^(2+)/Mg,which is higher than that in storage of Mg^(2+).We demonstrated the reversible intercalation/de-intercalation of MgCl^(+)in PANI accompanying with the reversible transformation between the quinone ring(C–C,–N=)and the benzene ring(C=C,–NH–)during charging and *** functional theory calculation reveals that PANI exhibit higher voltages(2.25 V vs.1.82 V)along with lower diffusion energy barriers(1.27 eV vs.1.55 eV)for MgCl^(+)storage compared to Mg^(2+)*** work refines the storage mechanism of PANI in RMBs and provides new guidelines for the application of PANI in RMBs.

关键词： rechargeable magnesium-metal batteries cathode materials polyaniline MgCl+storage

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How could imperfect device properties influence the performances of spiking neural networks?

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Science China(Information Sciences) 2023年第8期66卷 233-242页

作者： Jingyang CHEN Zhihao WANG Tong WANG Heming HUANG Zheyuan SHAO Zhe WANG Xin GUO State Key Laboratory of Material Processing and Die & Mould Technology School of Materials Science and EngineeringHuazhong University of Science and Technology

Spiking neural networks(SNNs) provide an efficient way to apply artificial intelligence systems on edge devices. Memristive devices with tunable conductance states can be used to emulate the functions of biological neurons and synapses and to build SNNs. In this work, fully-connected SNNs based on various memristive devices are constructed, and a hardware-compatible spike-timing-dependent plasticity(STDP)learning rule is applied to train the SNNs. Strategies are designed to suppress the overfitting problem and improve the performance of the SNNs in the case of a small training set. However, the properties of memristive devices are never perfect. The effects of imperfect device properties, e.g., asymmetric weight update, insufficient number of conductance states, and low on/off ratio, on the performance of the SNNs are elaborated.

关键词： oxides memristive devices device properties spiking neural networks neuromorphic computing

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Selenium-doped cathode materials with polyaniline skeleton for lithium-organosulfur batteries

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Journal of Energy Chemistry 2023年第4期79卷 148-157页

作者： Rong Zou Wenwu Liu Fen Ran State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals School of Materials Science and EngineeringLanzhou University of TechnologyLanzhou 730050GansuChina

Sulfur-containing polymer(SCP)is considered as an outstanding cathode material for lithium-sulfur ***,undesirable soluble polysulfides may shuttle in electrolyte,concluding long-chain Li_(2)S_(n)(n>4)and short-chain Li2Sn(n≤4),as well as the sluggish conversion kinetics are yet to be solved to enhance the performance of lithium-sulfur *** Se-doped sulfurized polyaniline with adjusted sulfur-chain-S_(x)-(x≤6)contribute to ensure the absence of long-chain polysulfides,and the skeleton with quinoid imine can endow strongly adsorption towards short-chain polysulfides by the reversible transition between deprotonated/protonated imine(-NH^(+)=and-N=),which offer double insurance against suppressing“shuttle effect”.Furthermore,Se atoms are doped into sulfurized polysulfides to accelerate the redox conversion and take a frontier orbital theory-oriented view into catalytic ***-doped sulfurized polyaniline as active materials for lithium-organosulfur batteries delivers good electrochemical performance,including high rate,reversible specific capacity(680 mA h g^(-1)at 0.1 A g^(-1)),and lower capacity decay rate only of 0.15%with near 100%coulomb efficiency during long-term *** work provides a valuable guiding ideology and promising solution for the chemistry-oriented structure design and practical application for lithium-organosulfur batteries.

关键词： Lithium-organosulfur batteries Selenium-doped Cathode materials Sulfur-containing polymer Frontier orbital theory

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Generation and Suppression of Pendant Droplet Oscillation in Electron Beam Directed Energy Deposition

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Engineering 2024年第6期37卷 215-229页

作者： Zhiyue Liang Zhenyu Liao Haoyu Zhang Zixiang Li Li Wang Baohua Chang Dong Du Department of Mechanical Engineering Tsinghua UniversityBeijing 100084China Key Laboratory for Advanced Materials Processing Technology Ministry of EducationTsinghua UniversityBeijing 100084China

Electron beam–directed energy deposition(EB–DED)has emerged as a promising wire-based metal additive manufacturing ***,the effects of EBs on pendant droplets at wire tips have not yet been *** aim of this study is to enhance the understanding of this action by analyzing the mechanism of droplet *** pendant droplet oscillation phenomenon hinders the stable transfer of droplets to the molten pool and limits the feasibility of manufacturing complex lattice structures by EB–***,another aim of this study is to create an oscillation suppression *** escalating asymmetric amplitude is the main characteristic of droplet *** primary oscillationinducing force is the recoil force generated from the EB-acted local surface of the *** physical mechanism of this force is the rapid increase and uneven distribution of the local surface temperature caused by the partial action of the *** prerequisites for droplet oscillation include vacuum conditions,high power densities,and bypass wire feeding *** proposed EB–dynamic surrounding melting(DSM)method can be applied to conveniently and effectively suppress oscillations,enable the accurate transfer of droplets to the molten pool,and achieve stable processes for preparing the strut elements of lattice *** the temperature and improving the uniformity of its distribution are the mechanisms of oscillation suppression in EB–*** this study,the physical basis for interpreting the mechanism by which EBs act on droplets and the technical basis for using EB–DED to prepare complex lattice structure parts are provided.

关键词： Additive manufacturing Electron beam freeform fabrication In situ monitoring Pendant droplet

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Probing the Nucleation and Growth Kinetics of Bismuth Nanoparticles via In-situ Transmission Electron Microscopy

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Journal of Wuhan University of technology(materials Science) 2024年第4期39卷 877-887页

作者：王浪李超凡 RAN Maojin YUAN Manman 胡执一 LI Yu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Nanostructure Research Centre(NRC) Wuhan University of TechnologyWuhan 430070China Institute of Chemistry Henan Academy of SciencesZhengzhou 450002China Henan Academy of Sciences Zhengzhou 450046China

The nucleation and growth mechanism of nanoparticles is an important theory,which can guide the preparation of ***,it is still lacking in direct observation on the details of the evolution of intermediate state structure during nucleation and *** this work,the evolution process of bismuth nanoparticles induced by electron beam was revealed by in-situ transmission electron microscopy(TEM)at atomic *** experimental results demonstrate that the size,stable surface and crystallographic defect have important influences on the growth of Bi *** non-classical growth paths including single crystal growth and polycrystalline combined growth,as well as,corresponding layer-by-layer growth mechanism along{012}stable crystal plane of Bi nanoparticles with dodecahedron structure were revealed by in-situ TEM *** results provide important guidance and a new approach for in-depth understanding of the nucleation and growth kinetics of nanoparticles.

关键词： bismuth nanoparticles crystal growth transmission electron microscopy in-situ electron microscopy

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A new thiol-sulfur click chemistry for lithium-organosulfide batteries

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The Innovation 2025年第2期6卷 42-48,41页

作者： Rong Zou Wenwu Liu Fen Ran State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals Department of Polymeric Materials EngineeringSchool of Materials Science and EngineeringLanzhou University of TechnologyLanzhou 730050China

Click chemistry is a rapid,reliable,and powerful function and a highly selective organic reaction that facilitates the efficient synthesis of various molecules by joining small *** approach has found widespread applications in fields such as drug development,chemical synthesis,and molecular *** recent years,the reaction of alkali-catalyzed polymerization of thiol and sulfur has been employed to prepare various sulfur-containing polymers,which are applied as electrochemical active electrode materials in the pursuit of good *** this study,it is surprising to find that the reaction mechanism exhibits characteristics of both the alkali-catalyzed sulfhydryl Micheal addition reaction and thiol-epoxy click chemistry;for the first time,thiol-sulfur click chemistry is defined in detail,providing a comprehensive description of its underlying scientific *** introduction of this new reaction pathway holds significant potential for advancing research and the development of sulfur-containing *** on this novel click chemistry,a new sulfur-containing polymer,polydivinylthioether hexasulfide,has been designed and successfully applied as a cathode material in lithium-organosulfide *** material demonstrates excellent electrochemical performance,achieving an initial capacity that reaches 790.5 mAh g−1(82.6%of theoretical capacity),and in a long-term cycle test,the capacity decay rate is only 0.063%after 1,000 cycles.

关键词： electrochemical active electrode mater thiol sulfur click chemistry molecular biologyin lithium organosulfide batteries synthesis various molecules organic reaction click chemistry joining small unitsthis

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Exploring the Core-shell Structure of BaTiO3-based Dielectric Ceramics Using Machine Learning Models and Interpretability Analysis

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Journal of Wuhan University of technology(materials Science) 2024年第3期39卷 561-569页

作者：孙家乐 XIONG Peifeng 郝华 LIU Hanxing State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Material Science and EngineeringInternational School of Material Science and EngineeringWuhan University of TechnologyWuhan 430070China Sanya Science and Education Innovation Park Wuhan University of TechnologySanya 572000China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshan 528200China

A machine learning(ML)-based random forest(RF)classification model algorithm was employed to investigate the main factors affecting the formation of the core-shell structure of BaTiO_(3)-based ceramics and their interpretability was analyzed by using Shapley additive explanations(SHAP).An F1-score changed from 0.8795 to 0.9310,accuracy from 0.8450 to 0.9070,precision from 0.8714 to 0.9000,recall from 0.8929 to 0.9643,and ROC/AUC value of 0.97±0.03 was achieved by the RF classification with the optimal set of features containing only 5 features,demonstrating the high accuracy of our model and its high *** the interpretability analysis of the model,it was found that the electronegativity,melting point,and sintering temperature of the dopant contribute highly to the formation of the core-shell structure,and based on these characteristics,specific ranges were delineated and twelve elements were finally obtained that met all the requirements,namely Si,Sc,Mn,Fe,Co,Ni,Pd,Er,Tm,Lu,Pa,and *** the process of exploring the structure of the core-shell,the doping elements can be effectively localized to be selected by choosing the range of features.

关键词： machine learning BaTiO_(3) core-shell structure random forest classifier

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Single-atom Cu anchored on N-doped graphene/carbon nitride heterojunction for enhanced photocatalytic H_(2)O_(2) production

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Journal of materials Science & technology 2023年第30期161卷 192-200页

作者： Han Li Bicheng Zhu Bei Cheng Guoqiang Luo Jingsan Xu Shaowen Cao State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430078China School of Chemistry and Physics Queensland University of TechnologyBrisbaneQLD 4000Australia

Photocatalytic production of H_(2)O_(2) by polymeric carbon nitride has been regarded as a promising ap-proach for the conversion of solar energy into valuable ***,the efficiency of pristine car-bon nitride is limited by the rapid charge recombination and the lack of suitable active ***,we introduce single-atom Cu anchored on N-doped graphene(Cu-NG)as a cocatalyst coupled with carbon nitride via covalent bonding to enhance photocatalytic H_(2)O_(2) *** Cu-NG/carbon nitride could broaden the light absorption from UV to near-infrared region,contributing to the photocatalytic ***,NG containing electron-rich N atoms could serve as anchoring sites for stabilizing single-atom ***,the single-atom Cu acts not only as an electron sink to steer the interfacial charge sep-aration but also as an active site for molecular oxygen adsorption and *** the synergistic effect of the enhanced interfacial charge separation and suitable active sites,Cu-NG/carbon nitride ex-hibits improved photocatalytic performance with an H_(2)O_(2) generation rate of 2856μmol g^(−1)h^(−1),which is 2.6 times that of pristine carbon *** work provides a protocol for high-performance photocat-alytic H_(2)O_(2) production using a single-atom cocatalyst.

关键词： Single-atom catalysis Interfacial charge separation Photocatalytic H_(2)O_(2)production

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Transformation of Undesired Li_(2)CO_(3)into Lithiophilic Layer Via Double Replacement Reaction for Garnet Electrolyte Engineering

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Energy & Environmental materials 2022年第3期5卷 962-968页

作者： Jiaxu Zhang Ruohan Yu Jun Li Huiyu Zhai Gangjian Tan Xinfeng Tang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China International School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070China

Garnet-type solid-state electrolytes(SSEs)are a remarkable Li-ion electrolyte for the realization of next-generation all-solid-state lithium batteries due to their excellent stability against Li metal as well as high ionic conductivities at room ***,garnet electrolytes always contain undesired and hardly removable Li_(2)CO_(3) contaminations that have persistently large resistance and unstable interface contact with Li *** is a critical bottleneck for the practical application of garnet ***,we design a novel strategy to completely root out Li_(2)CO_(3) both inside and on the surface of *** is achieved by a so-called double replacement reaction between Li_(2)CO_(3) and SiO_(2) during one-step hot press process for garnet electrolyte *** leads to in-situ transformation of LixSiOy(LSO)mostly locating around the grain boundaries of *** to the higher ion conductivity and better electrochemistry stability of LSO than Li_(2)CO_(3),the modified garnet electrolyte shows much improved electrochemical ***,the wettability between modified garnet electrolyte and lithium metals was significantly enhanced in the absence of surface Li_(2)CO_(3).As a proof of concept,an assembled Li symmetric cell with modified garnet electrolyte displays a high critical current density(CCD)of 0.7 mA cm^(-2)and a low interfacial impedance(5Ωcm^(2))at 25℃.These results indicate that the upcycling of Li_(2)CO_(3)is a promising strategy to well-address the degradation and interfacial issue associated with garnet electrolytes.

关键词： double replacement reaction garnet electrolytes lithiophilic layer solid-state lithium batteries

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ZnIn_(2)S_(4)/MOF S-scheme photocatalyst for H_(2)production and its femtosecond transient absorption mechanism

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Journal of materials Science & technology 2024年第30期197卷 183-193页

作者： Jiajie Cai Bowen Liu Shumin Zhang Linxi Wang Zhen Wu Jianjun Zhang Bei Cheng State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Hunan Key Laboratory of Applied Environmental Photocatalysis Changsha UniversityChangsha 410022China Laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of Geosciences68 Jincheng StreetWuhan 430078China Department of Chemical Engineering Ordos Institute of TechnologyOrdos 017000China

Photocatalytic water splitting is a popular pathway for H_(2)evolution,but the slow water oxidation greatly hampers the overall *** harness photogenerated holes in an efficient and lucrative way,the wa-ter oxidation reaction is replaced by selective oxidation of organic compounds to achieve simultaneous production of H_(2)and value-added ***,an alternative tactic is reported where an organic compound(benzylamine,BA)not only serves as the precursor for N-benzylidene-benzylamine(NBBA)production but also provides hydrogen sources for H_(2)evolution,achieving the goal under anhydrous *** process is realized using an S-scheme photocatalyst composed of ZnIn_(2)S_(4)and the UiO-66-NH_(2)(U6N)metal-organic framework(MOF).The S-scheme carrier transfer mechanism was validated by in-situ irradiated X-ray photoelectron spectroscopy(ISI-XPS)and femtosecond transient absorption(fs-TA)*** increased carrier efficiency and reinforced redox power endowed by the S-scheme heterojunction,the composite performed better than ZnIn2 S4 and *** performance was further ameliorated by Pt-cocatalyst modification,achieving an H_(2)production rate of 5275μmol h^(-1)g^(-1)as well as BA conversion of 94.3%with 99.3%NBBA *** studies reveal that BA is ini-tially oxidized to carbon-centered radicals and further to imines along with the release of *** imine reacts with another BA molecule to form NBBA,while the protons are reduced to H_(2).This work provides new insights into concurrent photocatalytic H_(2)production and selective organic oxidation from organic amines using S-scheme photocatalysts.

关键词： Photocatalysis S-scheme heterojunction Hydrogen production Selective oxidation Benzylamine Femtosecond transient absorption

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