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Role of catalyst surface-active sites in the hydrogenation ofα,β-unsaturated aldehyde

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Frontiers of Chemical Science and Engineering 2024年第6期18卷 41-69页

作者： Haixiang Shi Tongming su Zuzeng qin Hongbing Ji School of Chemistry and Chemical Engineering Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification TechnologyGuangxi UniversityNanning 530004China Zhejiang Green Petrochemical and Light Hydrocarbon Transformation Research Institute Zhejiang University of TechnologyHangzhou 310014China

As an important technology in fine chemical production,the selective hydrogenation ofα,β-unsaturated aldehydes has attracted much attention in recent *** the process ofα,β-unsaturated aldehyde hydrogenation,a conjugated system is formed between>C=CC=O,leading to hydrogenation at both ends of the conjugated system,which competes with each other and results in more complex ***,improving the reaction selectivity is also difficult in industrial ***,many researchers have reported that surface-active sites on catalysts play a crucial role inα,β-unsaturated aldehyde *** review attempts to summarize recent advances in understanding the effects of surface-active sites(SASs)over metal catalysts for enhancing the process of *** construction strategies and roles of SASs for hydrogenation catalysts are *** attention has been given to the adsorption configuration and transformation mechanism ofα,β-unsaturated aldehydes on catalysts,which contributes to understanding the relationship between SASs and hydrogenation *** addition,recent advances in metal-supported catalysts for the selective hydrogenation ofα,β-unsaturated aldehydes to understand the role of SASs in hydrogenation are briefly ***,the opportunities and challenges will be highlighted for the future development of the precise construction of SASs.

关键词： α,β-unsaturatedd aldehydes hydrogenation active site cinnamaldehyde

Experimental and numerical investigation of the impacts of rotor tip-rake on excitation forces of pump-jet propulsors

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Journal of Hydrodynamics 2024年第1期36卷 142-157页

作者： Xue-qin Ji xiao-song Zhang Chen-jun Yang xiao-qian Dong State Key Laboratory of Ocean Engineering Marine Numerical Experiment CentreSchool of Naval ArchitectureOcean and Civil EngineeringShanghai Jiao Tong UniversityShanghai200240China CSSC Shanghai Marine Energy Saving Technology Co. Ltd.Shanghai200011China China Ship Scientific Research Center Shanghai Branch Shanghai200011China

The tip-clearance flow in a pump-jet propulsor exerts great impacts on the fluctuating pressures and resultant unsteady forces,which are important sources of structural vibrations and radiated noise *** blade geometry close to the tip is an important factor determining the vortex strength in the tip-clearance *** the open-water condition,the effects of raking the rotor tips on the duct-surface fluctuating pressures and the resultant unsteady forces acting on different components of the propulsor are investigated via physical model experiments and the numerical solution of Reynolds-averaged Navier-Stokes(RANS)equations coupled with the SST k-ωturbulence *** measured and simulated results of hydrodynamic pressures are consistent to each other,and the simulated flows help better understand why the fluctuating pressures change with the tip *** strong fluctuations of duct-surface pressures are caused by intensive tip separation *** duct-surface pressure fluctuations are effectively reduced by using the rake distribution near the tip towards blade back side and,for the combination of the five-bladed rotor and the seven-bladed stator,the resultant unsteady horizontal(and vertical)forces acting on the duct and stator are also reduced;while increasing rake leads to negative effect on pressure fluctuations and unsteady horizontal(and vertical)forces acting on all the components of the propulsor.

关键词： Pump-jet tip-clearance tip-rake fluctuating pressures excitation forces

Semi-quantitative analysis of the structural evolution of mesophase pitch-based carbon foams by Raman and FTIR spectroscopy

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新型炭材料（中英文） 2024年第4期39卷 668-680页

作者： LIU Yue CHANG Sheng-kai su Zhan-peng HUANG Zu-jian qin Ji YANG Jian-xiao Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology College of Materials Science and EngineeringHunan UniversityChangsha410082China

Graphitized carbon foams(GFms)were prepared using mesophase pitch(MP)as a raw material by foaming(450℃),pre-oxidation(320℃),carbonization(1000℃)and graphitization(2800℃).The differences in structure and properties of GFms prepared from different MP precursors pretreated by ball milling or liquid phase extraction were investigated and compared,and semi-quantitative calculations were conducted on the Raman and FTIR spectra of samples at each preparation ***-quantitat-ive spectroscopic analysis provided detailed information on the structure and chemical composition changes of the MP and GFm de-rived from *** with microscopic observations,the change from precursor to GFm was *** results showed that ball milling concentrated the distribution of aromatic molecules in the pitch,which contributed to uniform foaming to give a GFm with a uniform pore distribution and good *** phase extraction helped remove light components while retaining large aromatics to form graphitic planes with the largest average size during post-treatment to produce a GFm with the highest degree of graphitization and the fewest open pores,giving the best compression resistance(2.47 MPa),the highest thermal conductivity(64.47 W/(m·K))and the lowest electrical resistance(13.02μΩ·m).Characterization combining semi-quantitative spectroscopic ana-lysis with microscopic observations allowed us to control the preparation of the MP-derived GFms.

关键词： Mesophase pitch Carbon foams Raman FTIR Graphitization

Cumulative effects of excess high-normal alanine aminotransferase levels in relation to new-onset metabolic dysfunction-associated fatty liver disease in China

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World Journal of Gastroenterology 2024年第10期30卷 1346-1357页

作者： Jing-Feng Chen Zhuo-qing Wu Hao-Shuang Liu su Yan You-Xiang Wang Miao Xing xiao-qin Song su-Ying Ding Health Management Center The First Affiliated Hospital of Zhengzhou UniversityZhengzhou 450052Henan ProvinceChina Institute of Systems Engineering Dalian University of TechnologyDalian 116024Liaoning ProvinceChina College of Public Health Zhengzhou UniversityZhengzhou 450001Henan ProvinceChina School of Basic Medicine and Forensic Medicine Henan University of Science and TechnologyLuoyang 471003Henan ProvinceChina

BACKGROUND Within the normal range,elevated alanine aminotransferase(ALT)levels are associated with an increased risk of metabolic dysfunction-associated fatty liver disease(MAFLD).AIM To investigate the associations between repeated high-normal ALT measurements and the risk of new-onset MAFLD *** A cohort of 3553 participants followed for four consecutive health examinations over 4 years was *** incidence rate,cumulative times,and equally and unequally weighted cumulative effects of excess high-normal ALT levels(ehALT)were *** proportional hazards regression was used to analyse the association between the cumulative effects of ehALT and the risk of new-onset *** A total of 83.13%of participants with MAFLD had normal ALT *** incidence rate of MAFLD showed a linear increasing trend in the cumulative ehALT *** with those in the low-normal ALT group,the multivariate adjusted hazard ratios of the equally and unequally weighted cumulative effects of ehALT were 1.651[95%confidence interval(CI):1.199-2.273]and 1.535(95%CI:1.119-2.106)in the third quartile and 1.616(95%CI:1.162-2.246)and 1.580(95%CI:1.155-2.162)in the fourth quartile,*** Most participants with MAFLD had normal ALT ***-term high-normal ALT levels were associated with a cumulative increased risk of new-onset MAFLD.

关键词： Metabolic dysfunction-associated fatty liver disease High-normal alanine aminotransferase level Cumulative effect Cox proportional hazards regression Cohort study

Control of fine particulate nitrate during severe winter haze in“2+26”cities

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Journal of Environmental Sciences 2024年第2期136卷 261-269页

作者： Chuang qin xiao Fu Tao Wang Jian Gao Jiaqi Wang Institute of Environment and Ecology Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China Department of Civil and Environmental Engineering Hong Kong Polytechnic UniversityHong Kong 99907China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 10084China

The“2+26”cities,suffering the most severe winter haze pollution,have been the key region for air quality improvement in *** prominent nitrate pollution is one of the most challenging environmental issues in this region,necessitating development of an effective control ***,we use observations,and state-of-the-art model simulations with scenario analysis and process analysis to quantify the effectiveness of the future SO_(2)-NO_(X)-VOC-NH_(3) emission control on nitrate pollution mitigation in“2+26”*** on a serious winter haze episode,we find that limited NO_(X)emission reduction alone in the short-term period is a less effective choice than VOC or NH_3emission reduction alone to decrease nitrate concentrations,due to the accelerated NO_(X)-HNO_(3)conversion by atmospheric oxidants and the enhanced HNO_(3)to NO_(3)^(-)partition by ammonia,although deep NO_(X)emission reduction is essential in the long-term *** synergistic NH_(3) and VOC emission control is strongly recommended,which can counteract the adverse effects of nonlinear photochemistry and aerosol chemical feedback to decrease nitrate *** extra benefits will be reduced if the synergistic NH_(3) and VOC reduction is delayed,and thus reducing emission of multiple precursors is urgently required for the effective control of increasingly severe winter nitrate pollution in“2+26”cities.

关键词： Nitrate Winter haze pollution Emission reduction “2+26”cities

Construction of electron rich Fe active sites by FeCu alloy anchoring on carbon nitride for photocatalytic nitrogen reduction

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Rare Metals 2024年第4期43卷 1570-1579页

作者： Gang Dong Cong Huang Fei-Yang Chen Xue-qin Liu Zhen Li xiao-Li su Tao Zeng Yun-Xia Chen Yi-Huang Chen Yang Wang School of Materials Science and Engineering Jingdezhen Ceramic UniversityJingdezhen333403China Faculty of Materials Science and Chemistry China University of GeosciencesWuhan430074China College of Chemistry and Materials Engineering Wenzhou UniversityWenzhou325035China

Given the clean and inexhaustible solar energy from solar light,photocatalytic ammonia synthesis is extremely ***,high electron-hole recombination rates and insufficient active sites severely limited N2 photoreaction ***,we designed and fabricated FeCu alloy nanoparticles anchored on carbon nitride nanosheets with excellent photocatalyt ic ammonia synthesis *** a coupler between Fe and carbon nitride,Cu promotes the separation of photogenerated charge carriers in carbon nitride under solar light irradiation,and renters the semiconductor a forceful electron donor for the Fe active *** accumulated electrons at Fe sites furtherly facilitated the adsorption and activation of the molecular ***,the uniform dispersed FeCu alloy nanoparticles were on carbon nitride nanosheets enhanced the stability of photocataly tic nitrogen reduction reaction,making the artificial photocataly tic ammonia synthesis more sustainable for *** work highlights that a direct electron transfer channel can be used to regulate the photochemical nitrogen fixation network.

关键词： Photocatalytic N_2 fixation Carbon nitride FeCu alloy Active sites Hydrogenation pathway

Anthropogenic Influence on Decadal Changes in Concurrent Hot and Dry Events over China around the Mid-1990s

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Advances in Atmospheric Sciences 2024年第2期41卷 233-246页

作者： qin su Buwen DONG Fangxing TIAN Nicholas P.KLINGAMAN Yunnan Key Laboratory of Meteorological Disasters and Climate Resources in the Great Mekong subregion Yunnan UniversityKunming 650500China Department of Atmospheric Sciences Yunnan UniversityKunming 650500China National Centre for Atmospheric Science Department of MeteorologyUniversity of ReadingReadingRG66BBUK Geofysisk Institut University of BergenBergen 5007Norway Citadel Investment Group Moor House120 London WallLondonRG66BBUK

The frequency and duration of observed concurrent hot and dry events(HDEs) over China during the growing season(April–September) exhibit significant decadal changes across the mid-1990s. These changes are characterized by increases in HDE frequency and duration over most of China, with relatively large increases over southeastern China(SEC), northern China(NC), and northeastern China(NEC). The frequency of HDEs averaged over China in the present day(PD,1994–2011) is double that in the early period(EP, 1964–81);the duration of HDEs increases by 60%. Climate experiments with the Met Office Unified Model(MetUM-GOML2) are used to estimate the contributions of anthropogenic forcing to HDE decadal changes over China. Anthropogenic forcing changes can explain 60%–70% of the observed decadal changes,suggesting an important anthropogenic influence on HDE changes over China across the mid-1990s. Single-forcing experiments indicate that the increase in greenhouse gas(GHG) concentrations dominates the simulated decadal changes,increasing the frequency and duration of HDEs throughout China. The change in anthropogenic aerosol(AA) emissions significantly decreases the frequency and duration of HDEs over SEC and NC, but the magnitude of the decrease is much smaller than the increase induced by GHGs. The changes in HDEs in response to anthropogenic forcing are mainly due to the response of climatological mean surface air temperatures. The contributions from changes in variability and changes in climatological mean soil moisture and evapotranspiration are relatively small. The physical processes associated with the response of HDEs to GHG and AA changes are also revealed.

关键词： concurrent hot and dry events decadal variation greenhouse gases aerosol emissions

Manipulating fast Li_(2)S redox via carbon confinement and oxygen defect engineering of In_(2)O_(3)for lithium-sulfur batteries

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Nano Research 2024年第6期17卷 5179-5187页

作者： Jinlei qin Rui Wang Zilong Yuan Pei xiao Deli Wang Key Laboratory of Material Chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Lithium-sulfur(Li-S)batteries have been considered as promising energy storage systems due to the merits of high energy density and low ***,the lithium polysulfides(LiPSs)diffusion and sluggish redox kinetics hamper the battery *** this work,low-bandgap indium oxide(In_(2)O_(3))with dense oxygen vacancies(In_(2)O_(3−x),0sulfur electrodes exhibit a stable cycling over 550 cycles at 1.0 C and splendid rate capability up to 4.0 *** significantly,when the sulfur-loading reaches as high as 5.5 mg·cm^(−2),the cathodes achieve an areal capacity of 5.12 mAh·cm^(−2)at 0.1 *** strategy of NC confined catalyst with rich defects engineering demonstrates great promise in the development of practical Li-S batteries.

关键词： Li-S batteries nitrogen-doped carbon confinement oxygen vacancies bidirectional Li_(2)S redox

Ligand-controlled electrochemiluminescence generation from CdSe/CdS/ZnS core/shell/shell quantum dots

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Nano Research 2024年第8期17卷 7776-7785页

作者： Hui sun Zhiyuan Cao Haiyan qin xiaogang Peng Bin su Key Laboratory of Excited-State Materials of Zhejiang Province Department of ChemistryZhejiang UniversityHangzhou 310058China

The CdSe/CdS/ZnS core/shell/shell quantum dots(QDs)with strong exciton confinement have manifested themselves as competitive light-emitting materials in electrochemiluminescence(ECL).However,cathodic ECL generation by these QDs requires the injection of electron and hole from solid electrode and electrogenerated radicals(for example SO_(4)•^(−)),which is inevitably influenced by not only the inorganic structure of QDs but also the organic ligands on the *** this work we aimed at studying the impact of surface organic ligands on ECL performance of CdSe/CdS/ZnS *** changing the surface ligand from oleate to acetate,we phenomenologically observed the positive shift of ECL onset potential by ca.200 mV and the increase of ECL intensity by~100 times,suggesting that a short ligand is more favorable for ECL *** further comprehend the ligand effect,we measured the charge injection kinetics using potential-modulated,time-resolved photoluminescence,and thinlayer spectroelectrochemistry *** electron and hole injection into QDs were found to be accelerated by 2–20 times if shortening the ligand from oleate to acetate,confirming the significant impact of surface ligands on ECL performance of *** study is expected to provide guidance on how to design surface functionalized QDs for specific applications such as ECL immunodiagnosis,photocatalysis,and photovoltaics.

关键词： electrochemiluminescence quantum dots spectroelectrochemistry surface ligands charge injection charge transfer