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Superatomic Ag_(58) nanoclusters incorporating a [MS_(4)@Ag_(12)]^(2+)(M = Mo or W) kernel show aggregation-induced emission

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Chinese Chemical Letters 2024年第10期35卷 452-456页

作者： jun-Jie Fang Zheng Liu yun-Peng Xie Xing Lu State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China

In core-shell silver nanoclusters,the control of core structure presents a more formidable challenge compared to that of the shell ***,we report the successful synthesis and characterization of four distinct silver thiolate nanoclusters[MS_(4)@Ag_(12)@Ag_(46)S_(24)(dppb)_(12)](M=Mo or W),each incorporating a cup-like[MS_(4)@Ag_(12)]^(2+)*** nanoclusters were meticulously prepared using(NH_(4))2Mo S4or(NH_(4))_(2)WS_(4)as both a template and a controlled source of ***,we have observed a unique configuration within these eight-electron superatomic Ag_(58) nanoclusters,where the zerovalent Ag atoms reside exclusively within the inner[MS_(4)@Ag_(12)]^(2+)*** stands in contrast to other superatomic clusters possessing an Ag(0)***,the introduction of phenyl-containing compounds during the synthesis process induced a transformation in the space group symmetry from C_(2)/c to I 4ˉ.This transformative effect was found to originate from the interplay between adjacent 1,4-bis(diphenylphosphino)butane(dppb)ligands,which facilitated enhanced emission through aggregationinduced intermolecular interactions,specifically C-H···π***,our findings contribute substantively to the understanding of the intricate relationship between nanocluster structures and their corresponding properties,shedding light on the crucial roles played by templates and diphosphine ligands in this context.

关键词： Superatom Silver nanocluster Template synthesis Photoluminescence Aggregation-induced emission

Understanding the cooperative effects in the catalysis of homodimeric fluoroacetate dehalogenase

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Science China Chemistry 2024年第7期67卷 2382-2391页

作者： Ke-Wei Chen Jia-Nan Chen jun Zhang Chao Wang Tian-Yu Sun yun-Dong Wu Key Laboratory of Computational Chemistry and Drug Design State Key Laboratory of Chemical OncogenomicSchool of Chemical Biology and BiotechnologyPeking University Shenzhen Graduate SchoolShenzhen 518055China Institute of Chemical Biology Shenzhen Bay LaboratoryShenzhen 518132China College of Chemistry and Molecular Engineering Peking UniversityBeijing 100871China Changping Laboratory Beijing 102200China

Fluoroacetate dehalogenases(FAcD),a homodimeric enzyme,catalyzes the conversion of fluoroacetic acid to glycolic acid(GoA).It has been proved that the enzyme has a half-of-the-site ***,its catalytic(C)subunit converts the first substrate to a covalent intermediate;then,the non-catalytic(NC)subunit binds a second substrate and promotes the conversion of the intermediate in the C subunit into the final *** the release of the product,the C subunit becomes the NC subunit,and the previous NC subunit becomes the C *** elucidate the detailed mechanism behind this cooperative catalysis,we have conducted microsecond-scale MD simulations along the reaction *** simulations indicate that the substrate in the NC subunit induces W185 and Y141 adopting an open conformation in the C *** opening of W185(C)facilitates the entry of catalytic water,enhancing the catalytic activity for product formation,while the opening of Y141(C)creates an unfavorable environment for product binding,promoting its *** interaction network analysis reveals that the substrate in the NC subunit can induce conformational changes through a conserved water chain at the interface.

关键词： enzyme catalysis molecular dynamics cooperative effect pre-reaction state

Application of a concrete thermal pile in cooling the warming permafrost under climate change

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Advances in Climate Change Research 2024年第1期15卷 170-183页

作者： yun-Hu SHANG Fu-jun NIU Guo-Yu LI Jian-Hong FANG Ze-Yong GAO State Key Laboratory of Frozen Soil Engineering Northwest Institute of Eco-Environment and ResourcesChinese Academy of SciencesLanzhou 730000China Da Xing'anling Observation and Research Station of Frozen-Ground Engineering and Environment Northwest Institute of Eco-Environment and ResourcesChinese Academy of SciencesJagdaqi 165000China Qinghai Research Institute of Transportation Xining 810008China

Permafrost degradation caused by climate warming is posing a serious threat to the stability of cast-in-place pile foundations in warm permafrost *** cold energy can be effectively utilized by two-phase closed thermosyphons(TPCTs)to cool the ***,we installed TPCTs in a cast-in-place pile foundation to create a unique structure called a thermal pile,which effectively utilizes the TPCTs to regulate ground *** we conducted a case study and numerical simulation to exhibit the cooling performance,and optimize the structure of the thermal *** purpose of this study is to promote the application of thermal piles in unstable permafrost *** on the findings,the thermal pile operated for approximately 53%of the entire year and effectively reduced the deep ground temperature at a rate of at least-0.1℃per ***,it successfully raised the permafrost table that is 0.35 m shallower than the natural ground *** characteristics prove highly beneficial in mitigating the adverse effects of permafrost degradation and enhancing infrastructure *** the length of the condenser section and the diameter of the TPCT in a suitable manner can effectively enhance the cooling capability of the thermal pile and ensure the long-term mechanical stability of the pile foundation even under climate warming.

关键词： Heat transfer Cold energy Warm permafrost Two-phase closed thermosyphons Cast-in-place pile foundation

Universal paradigm of ternary metacomposites with tunable epsilon-negative and epsilon-near-zero response for perfect electromagnetic shielding

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Rare Metals 2024年第2期43卷 796-809页

作者： yun-Peng Qu yun-Lei Zhou Yang Luo Yao Liu jun-Fei Ding Yan-Li Chen Xiu Gong Jing-Liang Yang Qiong Peng Xiao-Si Qi College of Physics Guizhou UniversityGuiyang550025China Hangzhou Institute of Technology Xidian UniversityHangzhou311231China Department of Materials ETH Zurich8093ZurichSwitzerland Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials(Ministry of Education) Shandong UniversityJinan250061China

CaCu_(3)Ti_(4)O_(12)(CCTO)ceramic nanocomposites incorporating graphene–carbon black(GRCB)fillers were fabricated by spark plasma sintering *** percolative effects of conductive GRCB fillers on dielectric response of GRCB/CCTO ternary metacomposites were systematically *** weakly real permittivity(ε′)-negative response(ε′~−1×10^(2))was achieved which originated from weakly low-frequency plasmonic state of free carriers within constructed GRCB *** enhancing three-dimensional GRCB network,the plasma frequency of metacomposites increased while the damping factor ***,theε′-negative values of metacomposites were tuned from−10^(2) to−10^(4) orders of magnitude andε′-near-zero(ENZ)frequencies from~142 to~340 MHz which substantially benefited from the moderate carrier concentration of GRCB dual *** Drude model and equivalent circuit models were adopted to demonstrate dielectric and electrical *** obtained metacomposites show strong EM shielding effect along with enhanced plasmonic oscillation and even better achieving perfect EM shielding effect in ENZ *** work achieves the tunableε′-negative andε′-near-zero response and more importantly clarifies its regulation mechanism in ceramic-based ternary metacomposites,which opens up the possibility of designing high-performance EM shielding materials based on metacomposites.

关键词： Metacomposites Ceramic matrix composites Negative permittivity Epsilon-near-zero Electromagnetic shielding

Metamorphic P-T conditions and ages of garnet-biotite schists in the Dahongshan Group from the southwestern Yangtze Block

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Acta Geochimica 2024年第4期43卷 707-718页

作者： jun-xiao Ma Guang-shu Yang Yong-feng Yan Xiao-Fei Xu yun-hua Ren Hui Zhao Xiao-jun Zheng Yuan Qin Faculty of Land Resources Engineering Kunming University of Science and TechnologyKunming 650093China Geological Team 306 of yunnan Non-Ferrous Metals Geological Bureau Kunming 650217China yunnan Provincial Bureau of Non-Ferrous Geology Kunming 650051China

The Dahongshan Group,situated at the southwestern margin of the Yangtze Block,represents a geological unit characterized by relatively high-grade metamorphism in the *** paper investigates the garnet-biotite schist from the Laochanghe Formation of the Dahongshan Group,employing an integrated approach that includes petrological analysis,phase equilibrium modeling,and zircon U-Pb *** schist is mainly composed of garnet,biotite,plagioclase,quartz,rutile,and *** equilibrium modeling revealed the peak metamorphic conditions of 8-9 kbar and 635-675°*** further integrating the prograde metamorphic profile of garnet and geothermobarometric results,a clockwise P-T metamorphic evolution path is constructed,which includes an increase in temperature and pressure during the prograde ***-ICP-MS zircon U-Pb dating and zircon Ti thermometry constrains the post-peak metamorphic age of 831.2±7.2 *** with previously reported results,it is revealed that the southwestern margin of the Yangtze Block experienced a large-scale regional metamorphism during the Neoproterozoic(890-750 Ma),which is related to the collisional orogenic *** may be associated with the late-stage assembly of the Rodinia supercontinent or with local compression and subduction processes during the breakup of the Rodinia supercontinent.

关键词： Southwestern Yangtze Block Dahongshan Group Phase equilibrium modeling Zircon U-Pb dating Neoproterozoic metamorphism

Synthesis and characterization of iron clusters with an icosahedral [Fe@Fe12]16+ Core

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National Science Review 2024年第4期11卷 123-129页

作者： Gan Xu yun-Shu Cui Xue-Lian Jiang Cong-Qiao Xu jun Li Xu-Dong Chen Jiangsu Collaborative Innovation Center of Biomedical Functional Materials and Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials Science Nanjing Normal University Department of Chemistry and Guangdong Provincial Key Laboratory of Catalytic Chemistry Southern University of Science and Technology Department of Chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education Tsinghua University State Key Laboratory of Coordination Chemistry Nanjing University

Iron-metal clusters are crucial in a variety of critical biological and material systems,including metalloenzymes,catalysts,and magnetic storage ***,a synthetic high-nuclear iron cluster has been absent due to the extreme difficulty in stabilizing species with direct iron-iron *** this work,we have synthesized,crystallized,and characterized a（Tp*）4W4S12(Fe@Fe12) cluster(Tp*=tris（3,5-dimethyl-1-pyrazolyl）borate（1-）),which features a rare trideca-nuclear,icosahedral[Fe@Fe12] cluster core with direct multicenter iron-iron bonding between the interstitial iron（Fei） and peripheral irons（Fep）,as well as Fep…Fepferromagnetic *** chemistry studies reveal that the stability of the cluster arises from the 18-electron shell-closing of the [Fe@Fe12]16+core,assisted by its bonding interactions with the peripheral tridentate [（Tp*）WS3]4-ligands which possess both S→Fe donation and spin-polarized Fe-Wσ *** ground-state electron spin is theoretically predicted to be S=32/2 for the *** existence of low oxidation-state（OS～+1.23） iron in this compound may find interesting applications in magnetic storage,spintronics,redox chemistry,and cluster catalysis.

关键词： Fe13 cluster iron-sulfur cluster low-valence iron iron−iron bond high spin complex

Preparation of tungsten-particle-reinforced Zr-based bulk metallic glass composites by two-step spark plasma sintering:microstructure evolution,densification mechanism and mechanical properties

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Rare Metals 2024年第4期43卷 1793-1808页

作者： yun-Fei Ma Pan Gong Mao Zhang Hui-EHu Zhen Peng Xiao Xu Xin Wang Mehdi Malekan Xue-Feng Tang Lei Deng jun-Song Jin Xin-yun Wang State Key Laboratory of Materials Processing and Die and Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan430074China Research Institute of Huazhong University of Science and Technology in Shenzhen Shenzhen518057China Department of Chemistry and Materials Naval University of EngineeringWuhan430032China School of Materials Science and Engineering Jiangsu UniversityZhenjiang212013China College of Machine Shanghai Dianji UniversityShanghai201306China School of Metallurgy and Materials Engineering College of EngineeringUniversity of TehranTehran 11155-4563Iran

A new two-step spark plasma sintering(TSS)process with low-temperature pre-sintering and high-temperature final sintering has been successfully applied to prepare the tungsten-particle(Wp)-reinforced bulk metallic glass composites(Wp/BMGCs).Compared to normal spark plasma sintering(NS),the densification rate and relative density of Wp/BMGCs can be improved by selecting TSS with appropriate sintering pressure in the low temperature pre-sintering ***,the compressive strength and plastic strain of 30%Wp/BMGCs prepared by TSS are both higher than those of the samples prepared by *** TSS process can significantly enhance the compressive strength of 30%Wp/BMGCs by 12%and remarkably increase the plastic strain by 50%,while the trend is completely opposite for 50%Wp/***-in situ experiments and finite element simulations reveal that uneven temperature distribution among particles during low-temperature pre-sintering causes local overheating at contact points between particles,accelerating formation of sintering neck between particles and plastic deformation of *** the volume fraction of Wp is low,TSS can improve the interface bonding between particles by increasing the number of sintering *** makes the fracture mode of Wp/BMGCs being predominantly transgranular ***,as the volume fraction of Wp increases,the adverse effects of Wp plastic deformation are becoming more and more *** aggregated Wp tends to form a solid"cage structure"that hinders the bonding between particles at the interface;correspondingly,the fracture behavior of Wp/BMGCs is mainly dominated by intergranular ***,reducing the sintering pressure during the low-temperature pre-sintering stage of TSS has been shown to effectively decrease plastic deformation in Wp,resulting in a higher degree of densification and better mechanical properties.

关键词： Bulk metallic glass composites Tungsten particle Two-step spark plasma sintering Densification mechanism Mechanical properties

Enhancing the Interaction of Carbon Nanotubes by Metal-Organic Decomposition with Improved Mechanical Strength and Ultra-Broadband EMI Shielding Performance

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Nano-Micro Letters 2024年第7期16卷 281-294页

作者： Yu-Ying Shi Si-Yuan Liao Qiao-Feng Wang Xin-yun Xu Xiao-yun Wang Xin-Yin Gu You-Gen Hu Peng-Li Zhu Rong Sun Yan-jun Wan Shenzhen Institute of Advanced Electronic Materials Shenzhen Institutes of Advanced TechnologyChinese Academy of SciencesShenzhen 518055People’s Republic of China Southern University of Science and Technology Shenzhen 518055People’s Republic of China National Key Laboratory of Materials for Integrated Circuits Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai 200050People’s Republic of China

The remarkable properties of carbon nanotubes(CNTs)have led to promising applications in the field of electromagnetic inter-ference(EMI)***,for macroscopic CNT assemblies,such as CNT film,achieving high electrical and mechanical properties remains challenging,which heavily depends on the tube-tube interac-tions of ***,we develop a novel strategy based on metal-organic decomposition(MOD)to fabricate a flexible silver-carbon nanotube(Ag-CNT)*** Ag particles are introduced in situ into the CNT film through annealing of MOD,leading to enhanced tube-tube *** a result,the electrical conductivity of Ag-CNT film is up to 6.82×10^(5) S m^(-1),and the EMI shielding effectiveness of Ag-CNT film with a thickness of~7.8μm exceeds 66 dB in the ultra-broad frequency range(3-40 GHz).The tensile strength and Young’s modulus of Ag-CNT film increase from 30.09±3.14 to 76.06±6.20 MPa(~253%)and from 1.12±0.33 to 8.90±0.97 GPa(~795%),***,the Ag-CNT film exhibits excellent near-field shield-ing performance,which can effectively block wireless *** innovative approach provides an effective route to further apply macroscopic CNT assemblies to future portable and wearable electronic devices.

关键词： EMI shielding Mechanical strength Carbon nanotubes Metal-organic decomposition Flexibility

Monte Carlo method for evaluation of surface emission rate measurement uncertainty

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Nuclear Science and Techniques 2024年第7期35卷 126-136页

作者： Yuan-Qiao Li Min Lin Li-jun Xu Rui Luo Yu-He Zhang Qian-Xi Ni yun-Tao Liu China Institute of Atomic Energy Beijing102413China National Key Laboratory for Metrology and Calibration Techniques Beijing102413China Department of Radiation Oncology Hunan Cancer HospitalChangsha410031China The Affiliated Cancer Hospital of Xiangya School of Medicine Central South UniversityChangsha410031China

The aim of this study is to evaluate the uncertainty of 2πα and 2πβ surface emission rates using the windowless multiwire proportional counter *** study used the Monte Carlo method (MCM) to validate the conventional Guide to the Expression of Uncertainty in Measurement (GUM) method.A dead time measurement model for the two-source method was established based on the characteristics of a single-channel measurement system,and the voltage threshold correction factor measurement function was indirectly obtained by fitting the threshold correction *** uncertainty in the surface emission rate was calculated using the GUM method and the law of propagation of *** MCM provided clear definitions for each input quantity and its uncertainty distribution,and the simulation training was realized with a complete and complex mathematical *** results of the surface emission rate uncertainty evaluation for four radioactive plane sources using both methods showed the uncertainty’s consistency E_(n)<0.070 for the comparison of each source,and the uncertainty results of the GUM were all lower than those of the ***,the MCM has a more objective evaluation process and can serve as a validation tool for GUM results.

关键词： Surface emission rate Monte Carlo method Metrology Probability distribution function Dead time Low-energy loss correction Least-squares method