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Confined Mn^(2+) enables effective aerobic oxidation catalysis

Science China Chemistry 2024年第5期67卷 1545-1553页

作者： Desheng yuan Sicong Ma Xiao Kong Chi Zhang lin Chen Chengsheng Yang lihua Wang Zhen liu lin ye Yongmei liu Rui Ma Zhi-Pan liu Yifeng Zhu Yong Cao Xinhe Bao Department of Chemical Physics University of Science and Technology of ChinaHefei 230026China Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsCollaborative Innovation Center of Chemistry for Energy MaterialsFudan UniversityShanghai 200438China Key laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Materials and Chemistry University of Shanghai for Science and TechnologyShanghai 200093China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China Institute of Advanced Fluorine-Containing Materials Zhejiang Normal UniversityJinhua 321004China State Key laboratory of Catalysis National Laboratory for Clean EnergyCollaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Effective and mild activation of O_(2) is essential but chall.nging for aerobic oxidation. In heterogeneous catalysis, high-valence manganese oxide(e.g., +4) is known to be active for the oxidation, whereas divalent MnO is ineffective due to its limited capacity to supply surface oxygen and its thermodynamically unstable structure when binding O_(2) in reaction conditions. Inspired by natural enzymes that rely on divalent Mn^(2+), we discovered that confining Mn^(2+) onto the Mn_(2)O_(3) surface through a dedicated calcination process creates highly active catalysts for the aerobic oxidation of 5-hydroxymethylfurfural, benzyl alcohol, and *** Mn_(2)O_(3)-confined Mn^(2+) is undercoordinated and efficiently mediates O_(2) activation, resulting in 2–3 orders of magnitude higher activity than Mn_(2)O_(3) alone. Through low-temperature infrared spectroscopy, we distinguished low-content Mn^(2+) sites at Mn_(2)O_(3) surface, which are difficult to be differentiated by X-ray photoelectron spectroscopy. The combination of in-situ energydispersive X-ray absorption spectroscopy and X-ray diffraction further provides insights into the formation of the newly identified active Mn^(2+) sites. By optimizing the calcination step, we were able to increase the catalytic activity threefold *** finding offers promising frontiers for exploring active oxidation catalysts by utilizing the confinement of Mn^(2+)and oftenignored calcination skills.

关键词： confinement catalysis manganese oxide aerobic oxidation divalent Mn^(2+) operando spectroscopies

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Mechanism of Huanglian Detoxification Soup Relieving Postherpetic Neuralgia by Enhancing Il-2 levels in Rats

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Medicinal Plant 2024年第3期15卷 39-40页

作者： Min ye Fengqin ZHAng Quiping yuan Yong XIAng Department of Pain Treatment Taihe HospitalHubei University of MedicineShiyan 442000China

[Objectives]To explore the mechanism of Huanglian detoxification soup improving pain behavior by affecting serum Il-2 levels in postherpetic neuralgia(post herpes neuralgia,PHN)model rats.[Methods]20 PHN rats were randomly divided into model group(PHN group)and detoxification decoction group(n=10).In the group,10%Huanglian detoxification soup(0.4 ml/0.1 kg)was given once in the morning and evening for 14 *** PHN group was filled with an equal volume of 0.9%sodium chloride *** vein serum inflammatory factor interleukin-2(Il-2),Il-βand Il-6 levels were measured using ElISA kits at 7 and 21 d.[Results]Il-2 increased at 14 and 21 d in Il group,while Il-βand Il-6 decreased compared with the PHN group(Plusions]Huanglian detoxification soup may raise Il-2 levels after VZV infection to promote the differentiation of cells of the immune system,so as to relieve the pain caused by Il-βand Il-6 inflammatory factors.

关键词： Huanglian detoxification soup Postherpetic neuralgia Serum inflammatory factor

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Transforming liquid flow fuel cells to controllable reactors for highlyefficient oxidation of 5-hydroxymethylfurfural to 2, 5-furandicarboxylic acid at low temperature

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Journal of Energy Chemistry 2024年第3期90卷 621-631,I0014页

作者： ye Qiang Xi liu Denghao Ouyang Zhao Jiang Xuebing Zhao Key laboratory of Industrial Biocatalysis Ministry of EducationTsinghua UniversityBeijing 100084China Institute of Applied Chemistry Department of Chemical EngineeringTsinghua UniversityBeijing 100084China School of Chemical Engineering and Technology Xi'an Jiaotong UniversityXi'an 710049ShaanxiChina

Highly-efficient oxidation of 5-hydroxymethylfurtural(HMF) to 2,5-furandicarboxylic acid(FDCA) at low temperature with air as the oxidant is still ***,inspired by the respirato ry electron transport chain(ETC) of living cells mediated by electron carriers,we constructed artificial ETCs and transformed liquid flow fuel cells(lFFCs) to flexible reactors for efficient oxidation of HMF to produce FDCA under mild *** lFFC reactor employed an electrodeposition modified nickel foam as an anode to promote HMF oxidation and(VO_(2))_(2)SO_(4) as a cathode electron carrier to facilitate the electron transfer to *** reaction rate could be easily controlled by selecting the anode catalyst,adjusting the external loading and changing the cathodic electron carrier or oxidants.A maximal power density of 44.9 mW cm^(-2) at room temperature was achieved,while for FDCA production,short-circuit condition was preferred to achieve quick transfer of *** a single batch operation with 0.1 M initial HMF,FDCA yield reached 97.1%.By fed-batch operation,FDCA concentration reached 144.5 g l^(-1) with a total yield of 96%.Ni^(2+)/Ni^(3+) redox couple was the active species mediating the electron transfer,while both experimental and DFT calculation results indicated that HMFCA pathway was the preferred reaction mechanism.

关键词： 5-Hydroxymethylfurfural 2 5-Furandicarboxylic acid Electrodeposition Electron transport chain liquid flow fuel cell

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Theoretical analysis of the double-differential cross-sections of neutron,proton,deuteron,^(3)He,andαfor the p+^(6) li reaction

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Nuclear Science and Techniques 2024年第3期35卷 181-197页

作者： Fang-lei Zou Xiao-Jun Sun Jing-Shang Zhang Hai-Rui Guo Yin-lu Han Rui-Rui Xu Xi Tao Ji-Min Wang Xiao-Dong Sun yuan Tian Tao ye Yong-li Xu Chun-Tian liang College of Physics Guangxi Normal University541004 GuilinChina Guangxi Key laboratory of Nuclear Physics and Nuclear Technology 541004 GuilinChina China Institute of Atomic Energy P.O.Box 275(41)102413 BeijingChina Institute of Applied Physics and Computational Mathematics 10094 BeijingChina College of Physics and Electronic Shanxi Datong University037009 DatongChina School of Science Tianjin Chengjian University300384 TianjinChina

Based on the unified Hauser–Feshbach and exciton model,which can describe the particle emission processes between discrete energy levels with energy,angular momentum,and parity conservations,a statistical theory of light nucleus reaction(STlN)is developed to calculate the double-differential cross-sections of the outgoing neutron and light charged particles for the proton-induced^(6) li reaction.A significant difference is observed between the p+^(6) li and p+^(7) li reactions owing to the discrepancies in the energy-level structures of the *** reaction channels,including sequential and simultaneous emission processes,are analyzed in *** the double-differential cross-sections of the outgoing proton as an example,the influence of contaminations(such as^(1) H,^(7)li,^(12)C,and^(16)O)on the target is identified in terms of the kinetic energy of the first emitted *** optical potential parameters of the proton are obtained by fitting the elastic scattering differential *** calculated total double-differential cross-sections of the outgoing proton and deuteron at E_(p)=14 MeV agree well with the experimental data for different outgoing ***,the mixed double differential cross-sections of^(3) He andαare in good agreement with the *** agreement between the measured data and calculated results indicates that the two-body and three-body breakup reactions need to be considered,and the pre-equilibrium reaction mechanism dominates the reaction *** on the STlN model,a PlUNF code for the p+^(6) li reaction is developed to obtain an ENDF-6-formatted file of the double-differential cross-sections of the nucleon and light composite charged particles.

关键词： Statistical theory of light nucleus reaction p+^(6)li reaction light composite charged particle Double-differential cross-sections Two-body breakup Three-body breakup

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Modulated noble metal/2D MOF heterostructures for improved hydrogen storage of MgH_(2)

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Rare Metals 2024年第4期43卷 1672-1685页

作者： Zeng-Yi li li-Xian Sun Fen Xu Yu-Mei luo Yong-Peng Xia Sheng Wei Chen-Chen Zhang Ri-Guang Cheng Chao-Feng ye Meng-yuan liu Ju-lan Zeng Zhong Cao Hong-Ge Pan School of Material Science and Engineering Guilin University of Electronic TechnologyGuilin541004China School of Chemistry and Chemical Engineering Changsha University of Science and TechnologyChangsha410114China Institute of Science and Technology for New Energy Xi’an Technological UniversityXi’an710021China

The conjugation of external species with twodimensional(2D)materials has broad application *** this study,we have explored the potential of noble metal/2D MOF heterostructures in hydrogen ***,the MgH_(2)-Ni-MOF@Pd system has shown remarkable hydrogen desorption/sorption performances,starting to liberate hydrogen at 1810C,which is 2300C lower than that of pristine *** the catalytic effect of Ni-MOF@Pd,the dehydrogenation apparent activation energy of MgH2 is noticeably decreased from(133.5±17.5)to(34.58±1.87)kJ·mol^(-1),and the hydrogenation apparent activation energy is reduced from(70.41±7.43)to(25.78±4.64)kJ·mol^(-1),which is lowered by 63.4%.The fully-dehydrogenated MgH2-NiMOF@Pd composite rapidly uptakes hydrogen,with 2.62wt%at 100℃and 6.06 wt%at 150℃within 300 s,*** mechanism analysis of MgH2 catalyzed by Ni-MOF@Pd has revealed that the transformation of Mg_2Ni and Mg_2NiH_4 could act as a"hydrogen pump",providing numerous channels for fast diffusion and transport of hydrogen ***,in the dehydrogenation process,the element Pd reacts with MgH_(2)to form the MgPd alloy phase,which makes MgH_(2)take precedence to decompose through the Mg-Pd alloy rather than self-decomposition,further reducing thermal stability and improving de/hydrogenation *** synergistic effect of Mg-Pd,Mg_2Ni,and the special ultra-thin 2D sheet structure of the additive is the main reason for the good hydrogen storage property of MgH_(2)-Ni-MOF@*** findings provide inspiration for designing efficient multifunctional additives with unique morphologies to optimize the hydrogen desorption/sorption behaviors of hydrogen storage materials.

关键词： Hydrogen storage Magnesium hydride 2D metal-organic framework nanosheets Ni/Pd Synergistic catalysis

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转向架腹板结构对高速列车气动噪声的影响

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铁道科学与工程学报 2024年第3期21卷 924-935页

作者：袁野杨明智中南大学轨道交通安全教育部重点实验室湖南长沙410075 轨道交通安全关键技术国际合作联合实验室湖南长沙410075 轨道交通列车安全保障技术国家地方联合工程研究中心湖南长沙410075

随着列车运行速度的不断提高,气动噪声问题日益突出,需要有效控制高速列车的气动噪声。为降低高速列车转向架区域的气动噪声,基于IDDES模型与FW-H声学方程,建立转向架不安装腹板及安装腹板的1:8缩比模型,通过数值仿真探究400 km时速下,... 详细信息

随着列车运行速度的不断提高,气动噪声问题日益突出,需要有效控制高速列车的气动噪声。为降低高速列车转向架区域的气动噪声,基于IDDES模型与FW-H声学方程,建立转向架不安装腹板及安装腹板的1:8缩比模型,通过数值仿真探究400 km时速下,转向架区域安装腹板后流场特性、噪声源强度、远场辐射噪声频谱特性和声压级幅值的变化,分析腹板对整车及转向架区域气动噪声的影响。研究结果表明:转向架区域底部安装腹板后,腹板的导流作用减缓了转向架部位的流体冲击和流体相互作用,抑制了转向架区域涡的形成,各频率下,转向架前、后轮对及构架的脉动压力级明显减小,有效降低了转向架区域气动噪声源的强度;转向架安装腹板后,各测点在200~1 000 Hz以及2 000 Hz以上频段的声压级幅值下降,其远场辐射噪声总声压级幅值也有所降低,其中,整车远场辐射噪声总声压级平均值降低2.33 dB(A),转向架辐射噪声总声压级平均值降低4.03 dB(A),转向架辐射噪声能量占整车辐射噪声能量的比例从53.2%下降到27.8%,转向架区域气动噪声得到有效控制;头车一位端转向架的降噪效果最好,辐射噪声总声压级平均值下降了5.88 dB(A),腹板对转向架辐射噪声的控制主要体现在对前、后轮对及构架等部件辐射噪声的控制。研究结果可为进一步优化高速列车气动噪声提供一定参考。

关键词：气动噪声高速列车转向架腹板流场降噪

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Origin of the Disparity between the Stability of Transmutated Mix-Cation and Mix-Anion Compounds

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Chinese Physics letters 2024年第5期41卷 53-60页

作者：野仕伟耿松源梁汉普张燮魏苏淮 Beijing Computational Science Research Center Beijing 100193China Advanced Materials Thrust Function HubHong Kong University of Science and TechnologyGuangzhou 511458China School of Materials Science and Engineering Northwestern Polytechnical UniversityXi’an 710072China

Transmutation is an efficient approach for material design. For example, ternary compound CuGaSe_(2) in chalcopyrite structure is a promising material for novel optoelectronic and thermoelectric device applications. It can be considered as formed from the binary host compound ZnSe in zinc-blende structure by cation transmutation(i.e., replacing two Zn atoms by one Cu and one Ga). While cation-transmutated materials are common, aniontransmutated ternary materials are rare, for example, Zn_(2)As Br(i.e., replacing two Se atoms by one As and one Br)is not reported. The physical origin for this puzzl.ng disparity is unclear. In this work, we employ first-principles calculations to address this issue, and find that the distinct differences in stability between cation-transmutated(mix-cation) and anion-transmutated(mix-anion) compounds originate from their different trends of ionic radii as functions of their ionic state, i.e., for cations, the radius decreases with the increasing ionic state, whereas for anions, the radius increases with the increasing absolute ionic state. Therefore, for mix-cation compounds,the strain energy and Coulomb energy can be simultaneously optimized to make these materials stable. In contrast, for mix-anion systems, minimization of Coulomb energy will increase the strain energy, thus the system becomes unstable or less stable. Thus, the trend of decreasing strain energy and Coulomb energy is consistent in mix-cation compounds, while it is opposite in mix-anion compounds. Furthermore, the study suggests that the stability strategy for mix-anion compounds can be controlled by the ratio of ionic radii r3/r1, with a smaller ratio indicating greater stability. Our work, thus, elucidates the intrinsic stability trend of transmutated materials and provides guidelines for the design of novel ternary materials for various device applications.

关键词： stability stability ternary

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Model.ng l.ng- and Short-Term Service Recommendations with a Deep Multi-Interest Network for Edge Computing

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Tsinghua Science and Technology 2024年第1期29卷 86-98页

作者： Rui yuan Shunmei Meng Ruihan Dou Xinna Wang Department of Computer Science and Engineering Nanjing University of Science and TechnologyNanjing 210056China Faculty of Mathematics University of WaterlooWaterloo N2L 3G1Canada

Edge computing platforms enable application developers and content providers to provide context-aware services(such as service recommendations)using real-time wireless access network *** to recommend the most suitable candidate from these numerous available services is an urgent ***-through rate(CTR)prediction is a core task of traditional service ***,many existing service recommender systems do not exploit user mobility for prediction,particularly in an edge computing *** this paper,we propose a model named l.ng and short-term user preferences model.ng with a multi-interest network based on user *** uses a logarithmic network to capture multiple interests in different fields,enriching the representations of user short-term *** terms of l.ng-term preferences,users'comprehensive preferences are extracted in different periods and are fused using a nonlocal *** experiments on three datasets demonstrate that our model relying on user mobility can substantially improve the accuracy of service recommendation in edge computing compared with the state-of-the-art models.

关键词： recommender system logarithmic network nonlocal network

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MAPK9 as a therapeutic target:unveil.ng ferroptosis in localized prostate cancer progression

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BIOCEll 2024年第5期48卷 771-792页

作者： CHEng-GOng lUO JIAO ZHAng YUN-ZHAO AN XUAN lIU SHUAI-JIE lI WEI ZHAng KAI lI XU ZHAO DOng-BO yuan l.ng-YUE AN WEI CHEN ye TIAN BIN XU Department of Urology Guizhou Provincial People’s HospitalGuiyangChina Department of Urology First Affiliated Hospital of Sun Yat-sen UniversityGuangzhouChina

Background:Ferroptosis,a lipid peroxidation-mediated programmed cell death,is closely linked to tumor development,including prostate cancer(PCa).Despite established connections between ferroptosis and PCa,a comprehensive investigation is essential for understanding its impact on patient ***:A risk model incorporating four ferroptosis-related genes was developed and *** risk scores correlated with an increased likelihood of biochemical recurrence(BCR),diminished immune infiltration,and adverse clinicopathological *** corroborate these results,we performed validation analyses utilizing datasets from both the Cancer Genome Atlas Cohort(TCGA)and the Gene Expression Synthesis Cohort(GEO).Moreover,we conducted further investigations into the pivotal gene identified in our model to explore its impact on tumor characteristics through cell proliferation and invasion assays,as well as animal studies conducted in ***,we conducted further experiments involving ferroptosis-related analysis to validate its association with ***:The risk model demonstrated exceptional predictive capabilities for prognosis and therapeutic outcomes in PCa ***-activated protein kinase 9(MAPK9)emerged as a crucial gene within the *** vivo and in vitro experiments explored MAPK9’s role in ferroptosis and its influence on tumor migration and ***:The findings provide a novel perspective for advancing ferroptosis exploration in PCa,bridging basic research and clinical applications.

关键词： Ferroptosis Biochemical recurrence Prostate cancer TCGA GEO MAPK9

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Basic Survey Schedul.ng for the Wide Field Survey Telescope(WFST)

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Research in Astronomy and Astrophysics 2024年第1期24卷 59-69页

作者： Yan-Peng Chen Ji-An Jiang Wen-Tao luo Xian-Zhong Zheng Min Fang Chao Yang yuan-Yu Hong Zong-Fei lü Purple Mountain Observatory Chinese Academy of SciencesNanjing 210023China School of Astronomy and Space Science University of Science and Technology of ChinaHefei 230026China Department of Astronomy University of Science and Technology of ChinaHefei 230026China National Astronomical Observatory of Japan National Institutes of Natural Sciences2-21-1 OsawaMitakaTokyo 181-8588Japan Institute of Deep Space Sciences Deep Space Exploration LaboratoryHefei 230026China

Aiming at improving the survey efficiency of the Wide Field Survey Telescope, we have developed a basic schedul.ng strategy that takes into account the telescope characteristics, observing conditions, and weather conditions at the l.nghu site. The sky area is divided into rectangular regions, referred to as “tiles,” with a size of2°. 577 × 2°. 634 slightly smaller than the focal area of the mosaic CCDs. These tiles are continuously filled in annulars parallel to the equator. The brightness of the sky background, which varies with the moon phase and distance from the moon, plays a significant role in determining the accessible survey fields. Approximately 50connected tiles are grouped into one block for observation. To optimize the survey schedule, we perform simulations by taking into account the l.ngth of exposures, data readout, telescope slewing, and all relevant observing conditions. We utilize the Greedy Algorithm for schedul.ng optimization. Additionally, we propose a dedicated dithering pattern to cover the gaps between CCDs and the four corners of the mosaic CCD array, which are located outside of the 3° field of view. This dithering pattern helps to achieve relatively uniform exposure maps for the final survey outputs.

关键词： telescopes surveys Moon

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