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Grain-boundary segregation and grain growth in nanocrystalline substitutional solid solution alloys

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Journal of materials Science & Technology 2024年第1期168卷 239-249页

作者： Fawei Tang Chao Hou Hao Lu Zhi Zhao Xiaoyan Song Faculty of materials and Manufacturing Key Laboratory of Advanced Functional MaterialsMinistry of Education of ChinaBeijing University of TechnologyBeijing 100124China

A model for describing solute segregation at grain boundaries has been developed for substitutional solid solution alloys,which integrates multiple factors from atomic to microstructural scales.A concept of mo-lar Gibbs free energy of segregation was introduced to evaluate the segregating capability of the solute elements in a closed system,through which the influences of grain boundary structure,grain size,ma-terial composition,and external conditions were described.Based on the evaluation of various energy forms related to solute segregation and grain growth processes,the nature of the thermal stabilization of nanograin structures by solute segregation was disclosed.A criterion for the destabilization of nanostruc-tures,which is determined by the competition of the change rates between the molar Gibbs free energy of segregation and the total energy of grain boundaries with grain size,has been proposed.This study provided guideline to achieve high-temperature stability of nanograin structures of solid solution alloys even for the weakly segregating nanocrystalline systems.

关键词： Substitutional solid solution Grain boundary segregation Thermal stabilization Solute concentration Grain size

Investigation on UV-curing Reprocessable Thermosets Bearing Hindered Urea Bonds and Their Composites with Modified Zinc Oxide Nanoparticles

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Chinese Journal of Polymer Science 2024年第6期42卷 751-765页

作者： Jun-Hao Zhou Li-Ming Tang key laboratory of advanced materials of ministry of education of china Department of Chemical EngineeringTsinghua UniversityBeijing100084China

In this study,a series of hindered urea bond(HUB)containing polyurethane-urea methacrylate prepolymers and a none HUB containing polyurethane methacrylate prepolymer were prepared using isobornyl methacrylate as the reactive diluent via one-pot procedure.The prepolymers were characterized fully by various techniques.Then,their thermosets were fabricated via UV curing in presence of a photo initiator,and their mechanical property and thermal behavior were investigated and compared.Different from the none HUB containing thermoset,the HUB containing thermosets(defined as PUT)could be recycled and reprocessed by hot press under relatively mild conditions with high recovery ratio of mechanical property.Furthermore,zinc oxide(ZnO)nanoparticles were modified with 3-(trimethoxysilyl)propyl methacrylate and the modified ZnO(defined as ZnO-TPM)was dispersed and polymerized into PUT matrix to prepare their nanocomposites.The influence of ZnO-TPM on the mechanical performance of the composites was evaluated,which indicated that the Young’s modulus and tensile strength increased gradually to the maximum values at ZnO-TPM content of 1 wt%and then decreased.The composites also displayed good reprocessability with improved recovery ratio compared to the pure PUT sample.In addition,the composite materials exhibited strong UV absorption capacity,implying their potential application in the circumstance where UV-shielding was required.

关键词： Polyurethane-urea methacrylate Hindered urea bond ZnO nanoparticles Reprocessing UV curing

Superior piezoelectric performance with high operating temperature in bismuth ferrite-based ternary ceramics

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Journal of materials Science & Technology 2024年第2期169卷 172-181页

作者： Yunyao Huang Leiyang Zhang Ruiyi Jing Yang Yang Vladimir Shur Xiaoyong Wei Li Jin Electronic materials Research laboratory Key Laboratory of the Ministry of EducationSchool of Electronic Science and EngineeringXi’an Jiaotong UniversityXi’an 710049China Faculty of materials and Manufacturing Key Laboratory of Advanced Functional MaterialsEducation Ministry of ChinaBeijing University of TechnologyBeijing 100124China School of Natural Sciences and Mathematics Ural Federal UniversityEkaterinburg620000Russia

Due to the thermal depolarization effect,adequate piezoelectric performance with high operating temperature is regarded to be challenging to accomplish concurrently in piezoceramics for applications in specific piezoelectric devices.In this work,we synthesized(0.8−x)BiFeO_(3)-x PbTi_(3)-0.2Ba(Zr_(0.25)Ti_(0.75))O_(3)(abbreviated as BFO-x PT-BZT)ternary solid solutions with 0.15≤x≤0.30 by conventional solid-state reaction method.The MPB composition with a coexisting state of rhombohedral-tetragonal phases exhibits enhanced electromechanical properties,including Curie temperature of 380℃,large-signal equivalent piezoelectric coefficient d^(∗)_(33)of 395 pm V^(-1),small-signal piezoelectric coefficient d_(33)of 302 pC N^(-1),and electromechanical coupling factor k_(p)of 50.2%,which is comparable to commercial PZT-5A ceramics,indicating potential in high-temperature applications.Furthermore,in-situ X-ray diffraction(XRD)and piezoelectric force microscopic(PFM)techniques demonstrate that multiphase coexistence and complex nanodomains promote piezoelectric response via synergism.The x=0.24 composition exhibits the highest in-situ d_(33)of 577 pC N^(-1)and good temperature stability in 30−280℃,indicating that BZT-modified BFO-PT ceramics are promising candidates for high-temperature piezoelectric devices.

关键词： High-temperature piezoelectrics Morphotropic phase boundary In-situ technique Domain structure BFO

Rationally construction of atomic-precise interfacial charge transfer channel and strong build-in electric field in nanocluster-based Zscheme heterojunctions with enhanced photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 5002-5010页

作者： Qingtao Zhu Honglei Shen Chao Han Liu Huang Yanting Zhou Yuanxin Du Xi Kang Manzhou Zhu Department of materials Science and Engineering Centre for Atomic Engineering of Advanced MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationKey Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui UniversityHefei 230601China

The lack of effective charge transfer driving force and channel limits the electron directional migration in nanoclusters(NC)-based heterostructures,resulting in poor photocatalytic performance.Herein,a Z-scheme NC-based heterojunction(Pt1Ag28-BTT/CoP,BTT=1,3,5-benzenetrithiol)with strong internal electric field is constructed via interfacial Co-S bond,which exhibits an absolutely superiority in photocatalytic performance with 24.89 mmol·h^(−1)·g−1 H_(2)production rate,25.77%apparent quantum yield at 420 nm,and~100%activity retention in stability,compared with Pt1Ag28-BDT/CoP(BDT=1,3-benzenedithiol),Ag29-BDT/CoP,and CoP.The enhanced catalytic performance is contributed by the dual modulation strategy of inner core and outer shell of NC,wherein,the center Pt single atom doping regulates the band structure of NC to match well with CoP,builds internal electric field,and then drives photogenerated electrons steering;the accurate surface S modification promotes the formation of Co-S atomic-precise interface channel for further high-efficient Z-scheme charge directional migration.This work opens a new avenue for designing NC-based heterojunction with matchable band structure and valid interfacial charge transfer.

关键词： atomically precise metal nanocluster Z-scheme heterojunction interfacial charge transfer build-in electric field photocatalytic hydrogen production

Multiscale confinement nitridation in molybdenum carbide for efficient hydrogen production

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Journal of Energy Chemistry 2024年第7期94卷 61-69页

作者： Liming Dai Chenchen Fang Xiaoyuan Zhang Xuefeng Xu Xuanxuan Chen Xinyue Zong Xueming Hu Wenyao Zhang Liang Xue Pan Xiong Yongsheng Fu Jingwen Sun Junwu Zhu key laboratory for Soft Chemistry and functional materials Ministry of EducationNanjing University of Science and TechnologyNanjing 210094JiangsuChina

The molybdenum carbide(Mo_(2)C)has been regarded as one of the most cost-efficient and stable electrocatalyst for the hydrogen evolution reaction(HER)by the virtue of its Pt-like electronic structures.However,the inherent limitation of high density of empty valence band significantly reduces its catalytic reactivity by reason of strong hydrogen desorption resistance.Herein,we propose a multiscale confinement synthesis method to design the nitrogen-rich Mo_(2)C for modulating the band structure via decomposing the pre-coordination bonded polymer in a pressure-tight tube sealing system.Pre-bonded c/N-Mo in the coordination precursor constructs a micro-confinement space,enabling the homogeneous nitrogenization in-situ happened during the formation of Mo_(2)C.Simultaneously,the evolved gases from the precursor decomposition in tube sealing system establish a macro-confinement environment,preventing the lattice N escape and further endowing a continuous nitridation.Combining the multiscale confinement effects,the nitrogen-rich Mo2C displays as high as 25%N-Mo concentration in carbide lattice,leading to a satisfactory band structure.Accordingly,the constructed nitrogen-rich Mo_(2)C reveals an adorable catalytic activity for HER in both alkaline and acid solution.It is anticipated that the multiscale confinement synthesis strategy presents guideline for the rational design of electrocatalysts and beyond.

关键词： Molybdenum carbide Hydrogen evolution reaction Multiscale confinement synthesis Valence band modulation Nitrogen doping

Rheological Behaviors of Polymers with Nanoparticles Tethered at Each End

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Chinese Journal of Polymer Science 2024年第3期42卷 400-406,I0009页

作者： Song-Qi Zhang Wen-Qing Wang Jia-Ping Lin Li-Quan Wang Shanghai key laboratory of advanced Polymeric materials Key Laboratory for Ultrafine Materials of Ministry of EducationSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China

The polymer with nanoparticles tethered at each end is a unique model for unraveling the effect of chain ends on the polymer dynamics. We investigated the rheological behavior of this kind of polymer by using nonequilibrium molecular dynamics simulation. The effect of polymer lengths and nanoparticle radii on the complex moduli and viscosity was examined. The dependence of complex moduli on the frequency becomes less pronounced as the polymer is short or the nanoparticle is large. The shear thinning behavior was revealed for these systems, and the scaling exponent of complex viscosity with respect to the frequency was found to change from-1/2 to-3/4 as the polymer shortens or the nanoparticle enlarges. The rheological behavior was further explained by analyzing the mean square distance of nanoparticles. The simulation results were compared with the existing experimental finding, showing an agreement. The work provides information for understanding the chain end effect on polymer rheology.

关键词： Polymer rheology Modulus Viscosity Molecular dynamics

Reconfigurable logic and in-sensor encryption operations in an asymmetrically tunable van der Waals heterostructure

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Nano Research 2024年第4期17卷 3113-3119页

作者： Fan Gong Wenjie Deng Yi Wu Fengming Liu Yihao Guo Zelin Che Jingjie Li Jingzhen Li Yang Chai Yongzhe Zhang key laboratory of Optoelectronics Technology of education ministry of china Faculty of Information TechnologyBeijing University of TechnologyBeijing 100124China key laboratory of advanced functional materials Ministry of EducationFaculty of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China Department of Applied Physics Hong Kong Polytechnic UniversityKowloonHong KongChina

Reconfigurable devices can be used to achieve multiple logic operation and intelligent optical sensing with low power consumption,which is promising candidates for new generation electronic and optoelectronic integrated circuits.However,the versatility is still limited and need to be extended by the device architectures design.Here,we report an asymmetrically gate two-dimensional(2D)van der Waals heterostructure with hybrid dielectric layer SiO_(2)/hexagonal boron nitride(h-BN),which enable rich function including reconfigurable logic operation and in-sensor information encryption enabled by both volatile and non-volatile optoelectrical modulation.When the partial gate is grounded,the non-volatile light assisted electrostatic doping endowed partially reconfigurable doping between n-type and p-type,which allow the switching of logic XOR and not implication(NIMP).When the global gate is grounded,additionally taking the optical signal as another input signal,logic AND and OR is realized by combined regulation of the light and localized gate voltage.Depending on the high on/off current ratio approaching 105 and reliable&switchable logic gate,in-sensor information encryption and decryption is demonstrated by manipulating the logic output.Hence,these results provide strong extension for current reconfigurable electronic and optoelectronic devices.

关键词： in-sensor encryption reconfigurable logic van der Waals heterostructure asymmetrical tunable architecture

Phosphine-catalyzed acyl-transfer of heteroaryl ketones for the construction of N-fused heterocycles

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Chinese Chemical Letters 2024年第3期35卷 252-256页

作者： Yu Zhang De-Rui Han Dan Ye Hong Lu Hao Wei key laboratory of Synthetic and Natural functional Molecule of the ministry of education College of Chemistry&Materials ScienceNorthwest UniversityXi'an 710069China

An inexpensive phosphine catalyst was used effectively for a transition-metal-free acyl-transfer of N-containing heteroaryl ketones for the rapid synthesis of N-fused heterocycles.The key pre-aromatic spirocyclic intermediate initialized by the single electron transfer(SET)process of Togni's reagentⅡpromoted by the tertiary phosphine resulted in an intriguing and alternative tactic for the cleavage of C–C bonds.By using inexpensive tertiary phosphine as the catalyst,this skeleton-reorganizing approach of N-containing heteroaryl ketones allows a streamlined assembly of complex N-fused heterocycles with broad functional group tolerance.

关键词： Phosphine catalysis Acyl-transfer N-Fused heterocycles C–C bond activation Aromatization

Theoretical screening of cooperative N-bridged dual-atom sites for efficient electrocatalytic nitrogen reduction with remolding insight

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Nano Research 2024年第4期17卷 3413-3422页

作者： Huimei Chen Yan Yang Chi Jiao Zhiwen Zhuo Junjie Mao Yan Liu key laboratory of functional Molecular Solids Ministry of EducationCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China

The electrocatalytic nitrogen reduction reaction(e-NRR)is a promising alternative method for the Haber–Bosch process.However,it still faces many challenges in searching for high activity,stability,and selectivity catalysts and ascertaining the catalytic mechanism with complete insight.Here,a series of graphene-based N-bridged dual-atom catalysts(M1-N-M2/NC)are systematically investigated via first-principle calculation and a high-throughput screening strategy.The result unveils that N_(2) adsorption on M1-N-M2/NC in bridge-on adsorption mode can effectively break the scaling relationship on single-atom catalysts(SACs).Moreover,V-N-Ru/NC and V-N-Os/NC are systematically screened out as promising e-NRR catalysts,with extremely low limiting potentials of-0.20 and-0.18 V,respectively.Furthermore,the adsorption site competition between*N_(2) and*H,as well as the competitive twin reactions of hydrogen evolution reaction(HER)on intermediates(N_(n)H_(m))during the e-NRR process,is systematically evaluated to form a remodeling insight for the reactions in mechanism,and the e-NRR of new proposed dual-atom catalysts(DACs)is strategically optimized for its high-efficiency performance potential via our remolding insight in e-NRR mechanism.This work provides new ideas and insights for the design and mechanism of e-NRR catalysts and an effective strategy for rapidly screening highly efficient e-NRR catalysts.

关键词： nitrogen reduction dual-atom catalysts high-throughput screening hydrogen evolution reaction density functional theory calculations