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Deliberate design of MOF-based pre-catalyst rationalizing the structural reconstruction toward efficient oxygen evolution reaction

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Science China Chemistry 2025年

作者： Yunhui Chen Meng Tian Zhongqi Zhang Guangzhao Wang Yan guo Jing wu Dawei Qi Zhenhua Yan Xiangyu liu Xi liu State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering College of Chemistry and Chemical EngineeringNingxia University Key Laboratory of Extraordinary Bond Engineering and Advanced Materials Technology of Chongqing School of Electronic Information Engineering Yangtze Normal University Frontiers Science Center for New Organic Matter Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) State Key Laboratory of Advanced Chemical Power Sources College of Chemistry Nankai University School of Chemistry and Chemical Engineering In-situ Center for Physical Sciences Frontiers Science Center for Transformative Molecules Shanghai Jiao Tong University

Metal-organic frameworks （MOFs）,that have emerged as promising electrocatalysts in oxygen evolution reaction （OER）,usually undergo structural reconstruction to form metal hydroxides as active ***,it remains a great challenge to design and synthesize ideal MOF-based pre-catalysts for properly cognizing and utilizing the reconstruction process toward efficient OER ***,the well-defined MOF-808 is post-modified by 2-hydroxyphosphonoacetic acid （HPAA） to form a micro-adsorber that enables to capture of metal ions ***3+and Ni2+ions are synergistically anchored into the microadsorber,developing a Fe/Ni-containing pre-catalyst that can be dynamically electrooxidized to be an active and stable dual-site electrocatalyst denoted by R-MOF-HPAA@FeNi with abundant metal *** a result,R-MOF-HPAA@FeNi exhibits an excellent OER performance with a low overpotential of 272 mV and Tafel slope of 35.9 m V dec-1,as well as long-term stability over 300 h at 10 m A *** and theoretical calculations suggest the resulting catalyst mainly follows a lattice oxygen mechanism （LOM） of dual-metal-site mechanism （DMSM）.Owing to the chelating role of HPAA,the post-synthesized MOF-HPAA behaves as a trap to uniformly and firmly adhere Fe3+and Ni2+ions,leading to a functionalized MOF-based pre-catalyst which can be structurally evolved into atomic level-distributed OER electrocatalysts.

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Deciphering fungal metabolon coupling tandem inverse-electrondemand Diels-Alder reaction and semipinacol rearrangement for the biosynthesis of spiro polycyclic alkaloids

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Science China Chemistry 2025年第1期68卷 288-296页

作者： Shuai liu Wen-Qiang Xu Ying-Tong Di Man-Cheng Tang Ding-Kang Chen Ming-Ming Cao Yao-Wen Chang Hong-Yu Tang Chun-Mao Yuan Jun-Bo Yang Zhi-li Zuo Han guo Zi-Fei Xu Ying Zeng Yun-Dong wu Xiao-Jiang Hao Key Laboratory of Phytochemistry and Natural Medicines (Chinese Academy of Sciences) Kunming Institute of Botany Chinese Academy of Sciences university of Chinese Academy of Sciences Lab of Computational Chemistry and Drug Design State Key Laboratory of Chemical Oncogenomics Peking University Shenzhen Graduate School Shenzhen Bay Laboratory State Key Laboratory of Microbial Metabolism School of Life Sciences & Biotechnology Shanghai Jiao Tong University State Key Laboratory of Functions and Applications of Medicinal Plants Guizhou Medical University Molecular Biology Experimental Center Germplasm Bank of Wild Species in Southwest China Kunming Institute of Botany Chinese Academy of Sciences Yunnan Key Laboratory for Wild Plant Resources Kunming Institute of Botany Chinese Academy of Sciences Research Unit of Chemical Biology of Natural Anti-Virus Products Chinese Academy of Medical Sciences

In the intricate process of natural product biosynthesis, a metabolon can enhance metabolic flux by associating sequential enzymes. A fungal metabolon, comprising of flavin-dependent monooxygenase Spe F and P450 monooxygenase Spe G, is identified in the biosynthesis of spiro polycyclic alkaloids(+)-notoamide B and its diastereomer(+)-versicolamide B. Using notoamide E as a substance, Spe F/Spe G metabolon can control the stereoselectivity of its 2,3-epoxidation, followed by hydrogen atom ion at C-17 to generate reactive epoxide tau-m A with dienyl iminium unit. Subsequently,(+)-notoamide B and(+)-versicolamide B are produced via tandem nonenzymatic inverse-electron-demand Diels-Alder reaction and semipinacol rearrangement. This provides the first example of metabolon in the biosynthesis of spiro-prenylated indole alkaloids.

关键词： metabolon Diels-Alder reaction semipinacol rearrangement biosynthesis notoamides spiro polycyclic alkaloids

The burden of upper motor neuron involvement is correlated with the bilateral limb involvement interval in patients with amyotrophic lateral sclerosis:a retrospective observational study

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Neural Regeneration Research 2025年第5期20卷 1505-1512页

作者： Jieying wu Shan Ye Xiangyi liu Yingsheng Xu Dongsheng Fan Department of Neurology Peking University Third HospitalBeijingChina Beijing Municipal Key Laboratory of Biomarker and Translational Research in Neurodegenerative Diseases BeijingChina Key Laboratory for Neuroscience National Health Commission/Ministry of EducationPeking UniversityBeijingChina

Amyotrophic lateral sclerosis is a rare neurodegenerative disease characterized by the involvement of both upper and lower motor *** bilateral limb involvement significantly affects patients'daily lives and may lead them to be confined to ***,the effect of upper and lower motor neuron impairment and other risk factors on bilateral limb involvement is *** address this issue,we retrospectively collected data from 586 amyotrophic lateral sclerosis patients with limb onset diagnosed at Peking university Third Hospital between January 2020 and May 2022.A univariate analysis revealed no significant differences in the time intervals of spread in different directions between individuals with upper motor neuron-dominant amyotrophic lateral sclerosis and those with classic amyotrophic lateral *** used causal directed acyclic graphs for risk factor determination and Cox proportional hazards models to investigate the association between the duration of bilateral limb involvement and clinical baseline characteristics in amyotrophic lateral sclerosis *** factor analyses revealed that higher upper motor neuron scores(hazard ratio[HR]=1.05,95%confidence interval[CI]=1.01–1.09,P=0.018),onset in the left limb(HR=0.72,95%CI=0.58–0.89,P=0.002),and a horizontal pattern of progression(HR=0.46,95%CI=0.37–0.58,Plimb *** results demonstrated that a greater degree of upper motor neuron involvement might cause contralateral limb involvement to progress more quickly in limb-onset amyotrophic lateral sclerosis *** findings may improve the management of amyotrophic lateral sclerosis patients with limb onset and the prediction of patient prognosis.

关键词： amyotrophic lateral sclerosis bilateral limb involvement Cox proportional hazards regression model horizontal spread restricted cubic spline analysis time interval upper motor neuron vertical spread

Engineering atomic Rb-N configurations to tune radical pathways for highly selective photocatalytic H2O2 synthesis coupled with biomass valorization

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Journal of Energy Chemistry 2025年第1期100卷 215-225页

作者： Jiaye li Shuang Pan Yihuang Chen Qiong liu College of Chemistry and Materials Engineering Wenzhou University Guangdong Provincial Key Laboratory of Chemical Measurement and Emergency Test Technology (China) Institute of Analysis Guangdong Academy of Sciences (China National Analytical CenterGuangzhou)

Photocatalytic oxygen reduction for hydrogen peroxide （H2O2） synthesis presents a green and costeffective production ***,achieving highly selective H2O2synthesis remains challenging,necessitating precise control over free radical reaction pathways and minimizing undesirable oxidative ***,we report for the visible light-driven simultaneous co-photocatalytic reduction of O2to H2O2and oxidation of biomass using the atomic rubidium-nitride modified carbon nitride（CNRb）.The optimized CNRb catalyst demonstrates a record photoreduction rate of 8.01 mM h-1for H2O2generation and photooxidation rate of 3.75 mM h-1for furfuryl alcohol to furoic acid,achieving a remarkable solar-to-chemical conversion （SCC） efficiency of up to 2.27%.Experimental characterizations and DFT calculation disclosed that the introducing atomic Rb–N configurations allows for the high-selective generation of superoxide radicals while suppressing hydroxyl free radical *** is because the Rb–N serves as the new alternative site to perceive a stronger connection position for O2adsorption and reinforce the capability to extract protons,thereby triggering a high selective redox product *** study holds great potential in precisely regulating reactive radical processes at the atomic level,thereby paving the way for efficient synthesis of H2O2coupled with biomass valorization.

关键词： Free radical reactions

Multi-layer multi-pass friction rolling additive manufacturing of Al alloy:Toward complex large-scale high-performance components

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 425-438页

作者： Haibin liu Run Hou Chenghao wu Ruishan Xie Shujun Chen College of Mechanical&Energy Engineering Beijing University of TechnologyBeijing 100124China Chongqing Research Institute of Beijing university of Technology Chongqing 401121China

At present,the emerging solid-phase friction-based additive manufacturing technology,including friction rolling additive man-ufacturing(FRAM),can only manufacture simple single-pass *** this study,multi-layer multi-pass FRAM-deposited alumin-um alloy samples were successfully prepared using a non-shoulder tool *** material flow behavior and microstructure of the over-lapped zone between adjacent layers and passes during multi-layer multi-pass FRAM deposition were studied using the hybrid 6061 and 5052 aluminum *** results showed that a mechanical interlocking structure was formed between the adjacent layers and the adja-cent passes in the overlapped center *** friction and rolling of the tool head led to different degrees of lateral flow and plastic deformation of the materials in the overlapped zone,which made the recrystallization degree in the left and right edge zones of the over-lapped zone the highest,followed by the overlapped center zone and the non-overlapped *** tensile strength of the overlapped zone exceeded 90%of that of the single-pass deposition *** is proved that although there are uneven grooves on the surface of the over-lapping area during multi-layer and multi-pass deposition,they can be filled by the flow of materials during the deposition of the next lay-er,thus ensuring the dense microstructure and excellent mechanical properties of the overlapping *** multi-layer multi-pass FRAM deposition overcomes the limitation of deposition width and lays the foundation for the future deposition of large-scale high-performance components.

关键词： aluminum alloy additive manufacturing solid-state friction stir welding multi-layer multi-pass

Atmospheric correction of HJ-1A/B CCD images over Chinese coastal waters using MODIS-Terra aerosol data

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Science China(Technological Sciences) 2010年第S1期53卷 191-195页

作者： TIAN liQiao 1,LU JianZhong 1,CHEN Xiaoling 1,2,3,YU ZhiFeng 1,XIAO JingJing 1,QIU Feng 1 & ZHAO Xi 1 1 State Key Laboratory of Information Engineering in Surveying,Mapping and Remote Sensing,wuhan university,wuhan 430079,China 2Key Laboratory of Poyang Lake Wetland and Watershed Research,Ministry of Education,jiangxi Normal university,nanchang 330022,China 3 The Key Laboratory of Poyang Lake Environment and Resource Utilization,Ministry of Education,nanchang university,nanchang 330031,China State Key Laboratory of Information Engineering in Surveying Mapping and Remote Sensing Wuhan University Wuhan China Key Laboratory of Poyang Lake Wetland and Watershed Research Ministry of Education Jiangxi Normal University Nanchang China The Key Laboratory of Poyang Lake Environment and Resource Utilization Ministry of Education Nanchang University Nanchang China

This paper demonstrates an atmospheric correction method to process HJ-1A/B CCD images over Chinese coastal waters with the aid of MODIS-Terra aerosol *** on the assumption of zero water-leaving radiance at the two near-infrared (NIR)bands or the shortwave infrared(SWIR)bands,the atmospheric aerosol optical depth(AOD)is firstly retrieved from MODIS-Terra with a simple extension of the NIR-SWIR combined atmospheric correction approach embedded in SeaDAS (SeaWiFS data analysis system).Then the"turbid"and"non-turbid"waters are separated by the turbid water *** probability of AOD at 551 nm band is derived based on the NIR information over"non-turbid"waters and FLAASH model is selected to do the atmospheric correction of the HJ-1A/B CCD imagery using the AOD values of highest probabilities as ***,according to the histogram of the AOD distribution at 551 nm band,the studied turbid water area is divided into several blocks and HJ-1A/B CCD imagery is corrected with the corresponding AOD values displayed with the highest frequency in each *** method has been applied to several HJ-1A/B images over Chinese coastal waters and validated by synchronous in-situ *** results have shown that this method is effective in the atmospheric correction process of HJ-1A/B CCD images for ocean color remote sensing study and application in the coastal waters.

关键词： ocean color remote sensing atmospheric correction turbid coastal waters HJ-1A/B MODIS

Si-C Foam Porous-Medium Combustion Power-Generation System for Low-Calorific-Value Biomass Syngas

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Journal of Thermal Science 2025年第1期34卷 206-222页

作者： YANG Jianwen CHEN Wei CAO Bingwei liu Xinhui li Hang College of Mechanical and Aerospace Engineering Jilin University School of Mechanical and Vehicle Engineering Changchun University

Syngas produced from the gasification of organic feedstocks from biomass is one of the clean and sustainable sources of *** advantages of simple access and renewability of biomass energy can meet the energy needs of temporary power *** study presents a biomass power-generation system for vehicular *** biomass and a free-piston Stirling engine generator（FPSEG） as the primary material and prime mover,respectively,biomass energy is converted into electricity by combusting the syngas to heat the *** and key parameter design for biomass gasification and thermoelectric conversion systems within a power generation system were performed.A porous medium area was constructed using Si-C foam ceramics to obtain an energy-conversion experimental *** effects of bed height,porosity,porous-region diameter,and air-intake conditions on the power-generation performance were investigated,and optimisations were performed for the thermoelectric conversion *** rate of increase during FPSEG power generation first increased and then decreased with increasing bed height,peaking at a bed height of 40 *** increasing porous-region diameter accelerated FPSEG power generation,whereas porosity changes in the porous media did not significantly affect the rate of change during FPSEG power *** increasing air intake,the rate of increase during power generation first increased and then *** maximum change rate and the highest thermoelectric conversion efficiency of the power-generation system occurred at 9.5 m3/h and 6.5 m3/h（～45.1%）air intakes,*** the thermal inertia and combustion structure of the thermoelectric conversion system significantly increased the power-generation rate of the system,with 1.8 W/s being observed at a 9.7 m3/h air intake.

关键词： biomass combined heat and power (CHP) gasification porous media combustion power generation

A SECOND-ORDER MOMENT TURBULENCE MODEL FOR POWER LAW FLUID WITH PARTICLES

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Journal of Hydrodynamics 2007年第5期19卷 607-612页

作者： ZENG Zhuo-xiong PAN Yang ZHONG Chun QIU guo-bin Aeronautic and Mechanical Engineering College Nanchang Hangkong University Nanchang 330063 China School of Civil Engineering and Architecture East China Jiaotong University Nanchang 330013 China

The USM-θ model of power law fluid for dense two-phase turbulent flow was developed, which combines the unified second-order moment model for two-phase turbulence with the particle kinetic theory for the inter-particle collision. This model was used to simulate the turbulent flow of power law fluid single-phase in pipe. It is shown that the USM- θ model has better prediction result than the κf -κf - κ- εp -θ model. The USM-O model was then used to simulate the dense two-phase turbulent up flow of power law fluid with particles. With the increase of the flow exponent, the velocities of power law fluid and particles increase near the pipe centre. Comparison between the two-phase flow of power law fluid-particle and of liquid-particle indicates that the axial fluctuation velocity of fluid phase and particle phase in liquid-particle two-phase flow is smaller than that in the power law fluid two-phase flow, but the two-phase velocities of power law fluid-particle and liquid-particle are close to each other.

关键词： power law fluid two-phase flow second-ordermoment turbulence model

Mesh-supported V2O5-WO3/TiO2 nanosheet array catalysts for efficient removal of NOx

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Tungsten 2025年第1期7卷 100-111页

作者： Zhi-Qi Zhang liu Yang Wen Luo Vladimir An Jing li Bao-Dan liu School of Materials Science and Engineering Northeastern University Foshan Graduate School of Innovation Northeastern University Kizhner Research Center School of Advanced Manufacturing Technologies Tomsk Polytechnic University

The design and synthesis of vanadium-based denitration catalysts with low-temperature activity pose significant challenges in the field of toxic gas *** this study,we have developed a novel approach to fabricate highly efficient V2O5-WO3/TiO2monolithic mesh catalysts for NOxreduction at low ***,TiO2nanosheets with strong adhesion and large surface area were grown on Ti mesh using plasma electrolytic oxidation technology and hydrothermal ***,super-small traces of WO3and V2O5active nano-species were subsequently deposited on TiO2nanosheets using the deposition-precipitation *** to traditional ceramic-based V2O5-WO3/TiO2catalysts,our V2O5-WO3/TiO2monolithic mesh catalyst exhibits superior mechanical performance,excellent thermal conductivity,lower pressure drop,higher utilization of active components,and stronger synergistic ***,the V2O5-WO3/TiO2monolithic mesh catalysts exhibited excellent low-temperature catalytic activity with 98% of NOxconversion at 220℃,and remarkable long-term SO2tolerance and water resistance in the selective catalytic reduction（SCR） of NOxwith *** SCR reaction of tiny V2O5and WO3active species supported on TiO2nanosheets directly demonstrated to follow the Eley-Rideal mechanism by in situ infrared spectra.

关键词： Low temperature activity Monolithic mesh catalysts NH3-SCR SO2 tolerance V2O5-WO3/TiO2