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Modulation doping of p-type Cu_(12)Sb_(4)S_(13)toward improving thermoelectric performance

Journal of Materials Science & Technology 2024年第4期171卷 71-79页

作者： Khak Ho Lim Mingquan Li Yu Zhang Yue Wu Qimin Zhou Qingyue Wang Xuan Yang Pingwei Liu Wen-Jun Wang Ka Wai Wong Ka Ming Ng Yu Liu Andreu Cabot institute of Zhejiang University-Quzhou Quzhou 324000China College of chemical and Biological Engineering Zhejiang UniversityHangzhou 310007China School of Chemistry and chemical Engineering Hefei University of TechnologyHefei 230009China Materials research institute The Pennsylvania State UniversityUniversity ParkPA 16802USA Ostia Technologies Limited United Kingdom Department of chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayHong KongChina ICREA Pg.Lluis Companys 23Barcelona 08010Spain Catalonia Energy research institute-IREC Sant Adria del BesosBarcelona 08930Spain

The commercial viability of thermoelectric(TE)devices relies heavily on two factors:cost reduction and efficiency enhancement.In this study,we first produce p-type Cu_(12)Sb_(4)S_(16-x)(x=0,3,4)using a low-temperature bottom-up approach and demonstrate Cu_(12)Sb_(4)S_(13)to show the best TE performance among the three tested compositions.Subsequently,the TE energy conversion efficiency of Cu_(12)Sb_(4)S_(13)is further enhanced by optimizing its electronic band structure through the incorporation of small amounts of tel-lurium.At an optimal Te content of 5 mol%,more than a twofold increase in the TE figure of merit(zT)is obtained.To gain insight into the mechanism of improvement on the transport properties of the mate-rial,we compare the interphase transport mechanism by incorporating nanodomains of different metals(Ag and Cu)into the Cu_(12)Sb_(4)S_(13)matrix.The improved electrical conductivity obtained with Cu_(12)Sb_(4)S_(13)-Te nanocomposites is attributed to a charge flooding of the Cu_(12)Sb_(4)S_(13)surface.In contrast,excessive down-ward band-bending at the interphases of Ag/Cu metal-semiconductor drastically reduces the electrical conductivity.Besides,a weighted mobility(μw)analysis shows a dominant thermal activation of carri-ers in Cu_(12)Sb_(4)S_(13)-Te nanocomposites.In this material,a strong decrease in lattice thermal conductivity is also found,which is associated with a phonon-carrier scattering mechanism.Our work shows the impor-tance of proper band-engineering in TE nanocomposites to decouple electrical and thermal transport to enhance TE performance,and the efficacy ofμw for electrical and thermal transport analysis.

关键词： Modulation doping Thermoelectric Interphase transport Charge flooding Phonon-carrier scattering

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Challenges and Opportunities in Preserving Key Structural Features of 3D-Printed Metal/Covalent Organic Framework

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Nano-Micro Letters 2024年第8期16卷 362-381页

作者： Ximeng Liu Dan Zhao John Wang Department of Materials Science and Engineering National University of SingaporeSingapore 117574Singapore Department of chemical and Biomolecular Engineering National University of SingaporeSingapore 117585Singapore National University of Singapore(Chongqing)research institute Chongqing 401123People’s Republic of China

Metal-organic framework(MOF)and covalent organic framework(COF)are a huge group of advanced porous materials exhibiting attractive and tunable microstructural features,such as large surface area,tunable pore size,and functional surfaces,which have significant values in various application areas.The emerging 3D printing technology further provides MOF and COFs(M/COFs)with higher designability of their macrostructure and demonstrates large achievements in their performance by shaping them into advanced 3D monoliths.However,the currently available 3D printing M/COFs strategy faces a major challenge of severe destruction of M/COFs’microstructural features,both during and after 3D printing.It is envisioned that preserving the microstructure of M/COFs in the 3D-printed monolith will bring a great improvement to the related applications.In this overview,the 3D-printed M/COFs are categorized into M/COF-mixed monoliths and M/COF-covered monoliths.Their differences in the properties,applications,and current research states are discussed.The up-to-date advancements in paste/scaffold composition and printing/covering methods to preserve the superior M/COF microstructure during 3D printing are further discussed for the two types of 3D-printed M/COF.Throughout the analysis of the current states of 3D-printed M/COFs,the expected future research direction to achieve a highly preserved microstructure in the 3D monolith is proposed.

关键词： Metal-organic frameworks Covalent organic frameworks 3D printing Microstructure Monolith

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Electrocatalytic NAD(P)H regeneration for biosynthesis

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Green chemical Engineering 2024年第1期5卷 1-15页

作者： Yaoxuan Li Guanhua Liu Weixi Kong Suoqing Zhang Yuemei Bao Hao Zhao Lihui Wang Liya Zhou Yanjun Jiang National-Local Joint Engineering Laboratory for Energy Conservation in chemical Process Integration and Resources Utilization School of Chemical Engineering and TechnologyHebei University of TechnologyTianjin300401China North China Pharmaceutical Group Corp Shijiazhuang050015China Tianjin Food research institute Tianjin301609China

The highly efficient chemoselectivity,stereoselectivity,and regioselectivity render enzyme catalysis an ideal pathway for the synthesis of various chemicals in broad applications.While the cofactor of an enzyme is necessary but expensive,the conversed state of the cofactor is not beneficial for the positive direction of the reaction.Cofactor regeneration using electrochemical methods has the advantages of simple operation,low cost,easy process monitoring,and easy product separation,and the electrical energy is green and sustainable.Therefore,bioelectrocatalysis has great potential in synthesis by combining electrochemical cofactor regeneration with enzymatic catalysis.In this review,we detail the mechanism of cofactor regeneration and categorize the common electron mediators and enzymes used in cofactor regeneration.The reaction type and the recent progress are summarized in electrochemically coupled enzymatic catalysis.The main challenges of such electroenzymatic catalysis are pointed out and future developments in this field are foreseen.

关键词： Biosynthesis Cofactor regeneration Bioelectrocatalysis NAD(P)H Electron mediator

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Optimal search path planning of UUV in battlefeld ambush scene

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Defence Technology（防务技术） 2024年第2期32卷 541-552页

作者： Wei Feng Yan Ma Heng Li Haixiao Liu Xiangyao Meng Mo Zhou Naval research institute Beijing100161China

Aiming at the practical application of Unmanned Underwater Vehicle(UUV)in underwater combat,this paper proposes a battlefield ambush scene with UUV considering ocean current.Firstly,by establishing these mathematical models of ocean current environment,target movement,and sonar detection,the probability calculation methods of single UUV searching target and multiple UUV cooperatively searching target are given respectively.Then,based on the Hybrid Quantum-behaved Particle Swarm Optimization(HQPSO)algorithm,the path with the highest target search probability is found.Finally,through simulation calculations,the influence of different UUV parameters and target parameters on the target search probability is analyzed,and the minimum number of UUVs that need to be deployed to complete the ambush task is demonstrated,and the optimal search path scheme is obtained.The method proposed in this paper provides a theoretical basis for the practical application of UUV in the future combat.

关键词： Battlefield ambush Optimal search path planning UUV path Planning Probability of cooperative search

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Enhanced electrocatalytic CO_(2)reduction to formic acid using nanocomposites of In_(2)O_(3)@C with graphene

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Nano research 2024年第6期17卷 5031-5039页

作者： Wenxiang Li Shuo Gao Chuanruo Yang Juntao Yang Amjad Nisar Guolei Xiang Junsu Jin Beijing Key Laboratory of Membrane Science and Technology Beijing University of Chemical TechnologyBeijing 100029China Nanomaterials research Group PDPINSTECHIslamabad 44000Pakistan institute of Industrial Chemistry College of ChemistryBeijing University of Chemical TechnologyBeijing 100029China

In_(2)O_(3)is an effective electrocatalyst to convert CO_(2)to formic acid(HCOOH),but its inherent poor electrical conductivity limits the efficient charge transfer during the reaction.Additionally,the tendency of In_(2)O_(3)particles to agglomerate during synthesis further limits the exposure of active sites.Here we address these issues by leveraging the template effect of graphene oxide and employing InBDC as a self-sacrificing template for the pyrolysis synthesis of In_(2)O_(3)@C.The resulting In_(2)O_(3)@C/rGO-600 material features In_(2)O_(3)@C nanocubes uniformly anchored on a support of reduced graphene oxide(rGO),significantly enhancing the active sites exposure.The conductive rGO network facilitates charge transfer during electrocatalysis,and the presence of oxygen vacancies generated during pyrolysis,combined with the strong electron-donating ability of rGO,enhances the adsorption and activation of CO_(2).In performance evaluation,In_(2)O_(3)@C/rGO-600 exhibits a remarkable HCOOH Faradaic efficiency exceeding 94.0%over a broad potential window of−0.7 to−1.0 V(vs.reversible hydrogen electrode(RHE)),with the highest value of 97.9%at−0.9 V(vs.RHE)in a H-cell.Moreover,the material demonstrates an excellent cathodic energy efficiency of 71.6%at−0.7 V(vs.RHE).The study underscores the efficacy of uniformly anchoring metal oxide nanoparticles onto rGO for enhancing the electrocatalytic CO_(2)reduction performance of materials.

关键词： In_(2)O_(3)@C nanocomposite electrochemical CO_(2)reduction reduced graphene oxide oxygen vacancy

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Combined Treatment with Bojungikgi-tang(Buzhong Yiqi Decoction) and Riluzole Attenuates Cell Death in TDP-43-Expressing Cells

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Chinese Journal of Integrative Medicine 2024年第7期30卷 616-622页

作者： Eun Jin Yang Department of KM Science research Korea Institute of Oriental Medicine

Objective: To examine the effect of combined treatment with Bojungikgi-tang(BJIGT, Buzhong Yiqi Decoction) and riluzole(RZ) in transactive response DNA-binding protein 43(TDP-43) stress granule(SG) cells, a amyotrophic lateral sclerosis(ALS) cell line using transcriptomic and molecular techniques. Methods: TDP-43 SG cells were pretreated with BJIGT(100 μg/mL), RZ(50 μmol/L), and combined BJIGT(100 μg/mL)/RZ(50 μmol/L) for 6 h before treatment with lipopolysaccharide(LPS, 200 μmol/L). Cell viability assay was performed to elucidate cell toxicity in TDP-43 SC cells using a cell-counting kit-8(CCK8) assay kit. The expression levels of cell death-related proteins, including Bax, caspase 1, cleaved caspase 3 and DJ1 in TDP-43 SG cells were examined by Western blot analysis. The autophagy-related proteins, including pmTOR/mTOR, LC3b, P62, ATG7 and Bcl-2-associated athanogene 3(Bag3) were investigated using immunofluorescence and immunoblotting assays. Results: Cell viability assay and Western blot analysis showed that combined treatment with BJIGT and RZ suppressed LPS-induced cell death and expression of cell death-related proteins, including Bax, caspase 1, and DJ1(P<0.05 or P<0.01). Immunofluorescence and immunoblotting assays showed that combined treatment with BJIGT and RZ reduced LPS-induced formation of TDP-43 aggregates and regulated autophagy-related protein levels, including p62, light chain 3b, Bag3, and ATG7, in TDP-43-expressing cells(P<0.05 or P<0.01). Conclusion: The combined treatment of BJIGT and RZ might reduce inflammation and regulate autophagy dysfunction in TDP-43-induced ALS.

关键词： Bojungikgi-tang Buzhong Yiqi Decoction transactive response DNA-binding protein 43 autophagy oxidative stress amyotrophic lateral sclerosis

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Plasma-etching on monolithic MOFs-based MIM filter boosted chemical sensing

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Nano research 2024年第4期17卷 2800-2807页

作者： Jianxi Liu Li Feng Zhihuan Li Yang Wu Feng Zhou Yadong Xu research&Development institute Northwestern Polytechnical University in ShenzhenShenzhen 518057China State Key Laboratory of Solidification Processing Center of Advanced Lubrication and Seal MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Yantai Zhongke research institute of Advanced Materials and Green chemical Engineering Shandong Laboratory of Advanced Materials and Green Manufacturing at YantaiYantai 264006China State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China

Metal-insulator-metal(MIM)cavity as a lithography-free structure to control light transmission and reflection has great potential in the field of optical sensing.However,the dense top metal layer of the MIM prohibits any external medium from entering the dielectric insulation layer,which limits the application of the cavity in the sensing field.Herein,we demonstrate a series of monolithic metal-organic frameworks(MOFs)based MIM cavities,which are treated by plasma etching to provide channels for chemical diffusion and to advance sensing.We modulate the bandwidth of the MIM filters by controlling the MOF thickness as insulator layers.Oxygen plasma-etching is applied to build channels on the top metal layer without altering their saturation and brightness for chemical sensing performance.The etching time regulates the number and size of channels on the top metal layer.Sensing behavior is demonstrated on the plasma-etched MOFs-based MIM cavity when external chemicals diffuse in the cavity.In addition,we generate patterned structure of the MOFs-based MIM cavity via plasma-mask method,which can transfer to different substrates and produce a controllable structure color change for chemical sensing.Our MIM cavity may promote the advancement and applications of structural color in security imaging,color display,information anticounterfeiting,and color printing.

关键词： metal-organic frameworks(MOFs) spin-coating metal-insulator-metal filter patterns sensing

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Stabilization and detection of labile reaction intermediates in supramolecular containers

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Chinese chemical Letters 2024年第6期35卷 47-52页

作者： Rui Wang Yang Liang Julius Rebek Jr. Yang Yu Center for Supramolecular Chemistry&Catalysis and Department of Chemistry College of ScienceShanghai UniversityShanghai 200444China Skaggs institute for chemical Biology and Department of Chemistry The Scripps Research InstituteLa JollaCA 92037United States

Detection and observation of reactive intermediates is an essential step in investigation of reaction pathways.However,most reactive intermediates are unstable and present at low concentrations;their short lifetimes make them difficult to detect and characterize.Supramolecular containers offer opportunities for the stabilization and characterization of those labile species,through isolation from the media and protection inside the cavity of the host.In this review,we summarize the examples of labile reaction intermediates that are stabilized and characterized with the help of supramolecular containers.The container compounds include carcerands,deep cavitands and amide naphthotubes.We focus on unstable guest species-cyclobutadiene,benzocyclopropenone,o-benzyne,1,2,4,6-cycloheptatetraene,anti-Bredt's olefin,fluorophenoxycarbene,O-acylisoamide,and hemiaminalthat act as intermediates in certain organic reactions.

关键词： Supramolecular containers Reaction intermediates Labile species stabilization Short-lived species detection Supramolecular chemistry

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Slope stability of reclaimed coal mines through a new water filling index

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Journal of Rock Mechanics and Geotechnical Engineering 2024年第3期16卷 828-839页

作者： Antonios Mikroutsikos Alexandros I.Theocharis Nikolaos C.Koukouzas Ioannis E.Zevgolis chemical Process&Energy Resources institute Centre for Research&Technology HellasAthensGreece School of Mining and Metallurgical Engineering National Technical University of AthensAthensGreece

A common reclamation practice for closed coal surface mines is filling them with water to form pit lakes.The creation and sustainability of these lakes are significantly affected by the stability of the corresponding slopes.The present study provides a general framework for analyzing the water filling’s effect on slope stability based on a new water filling index,which can indirectly consider the factors affecting the process and efficiently quantify the filling speed’s influence.The assumptions of the proposed approach are thoroughly discussed,and the range of the water filling index is identified.Furthermore,the safety factor is calculated using the finite element method with the shear strength reduction technique during the filling process for various conditions(soil properties,slope geometry,hydraulic conditions,and water filling speed).Results are presented as normalized stability charts for practical use.During the water filling,the stability gradually decreases until the reservoir reaches a critical level of 10%e40%of the total height;it then increases to even more stable conditions than the initial one.Overall,the present analysis allows for the preliminary stability evaluation of a coal mine during the formation of a pit lake and the appropriate quantification of the water filling’s effect.

关键词： Post-coal era Open-pit flooding Stability charts Critical level

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Hyperbranched polymer hollow-fiber-composite membranes for pervaporation separation of aromatic/aliphatic hydrocarbon mixtures

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Chinese Journal of chemical Engineering 2024年第5期69卷 13-22页

作者： Tong Liu Hao Sun Xiangqiong Wang Jie Li Zhanquan Zhang Pei Wu Naixin Wang Quanfu An Beijing Key Laboratory for Green Catalysis and Separation Department of Chemical EngineeringCollege of Materials Science and EngineeringBeijing University of TechnologyBeijing 100124China Petrochemical research institute CNPCBeijing 102206China

The separation of aromatic/aliphatic hydrocarbon mixtures is crucial in the petrochemical industry.Pervaporation is regarded as a promising approach for the separation of aromatic compounds from alkanes. Developing membrane materials with efficient separation performance is still the main task since the membrane should provide chemical stability, high permeation flux, and selectivity. In this study, the hyperbranched polymer(HBP) was deposited on the outer surface of a polyvinylidene fluoride(PVDF)hollow-fiber ultrafiltration membrane by a facile dip-coating method. The dip-coating rate, HBP concentration, and thermal cross-linking temperature were regulated to optimize the membrane structure.The obtained HBP/PVDF hollow-fiber-composite membrane had a good separation performance for aromatic/aliphatic hydrocarbon mixtures. For the 50%/50%(mass) toluene/n-heptane mixture, the permeation flux of optimized composite membranes could reach 1766 g·m^(-2)·h^(-1), with a separation factor of 4.1 at 60℃. Therefore, the HBP/PVDF hollow-fiber-composite membrane has great application prospects in the pervaporation separation of aromatic/aliphatic hydrocarbon mixtures.

关键词： Aromatic/aliphatic hydrocarbons Hyperbranched polymer Pervaporation Hollow fiber membrane Dip-coating

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