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Selective N-Methylation of N-Methylaniline with CO_(2) and H_(2) over Cu/In_(2)O_(3) Catalyst

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Chinese Journal of Chemistry 2024年第3期42卷 276-282页

作者： Huan zheng Bo Qian Lin He State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhouGansu730000 China University of Chinese Academy of Sciences Beijing100049 China

N-Methylation of amines with CO_(2) and H2 is a potential approach for CO_(2) utilization because N-methylated amines can be used as solvents and organic intermediates. In_(2)O_(3)-supported Cu (Cu/In_(2)O_(3)) acts as an effective heterogeneous catalyst for N-methylation reaction of N-methylaniline (MA) with CO_(2) and H_(2),showing higher N,N-dimethylaniline (DMA) selectivity than other supported Cu catalysts. On one hand,the dispersion of Cu can be improved by the defective In_(2)O_(3) support. On the other hand,In_(2)O_(3) support is active in the dissociative adsorption of CO_(2) through C—O bond breaking. In addition,the H_(2) dissociation ability of In_(2)O_(3) can also be enhanced by Cu. The combination of Cu and In_(2)O_(3) is effective in the activation of CO_(2),the adsorption of intermediate N-methylformanilide (MFA),the hydrogenation of MFA to DMA and the prohibition of C—N bond cleavage side reactions,thereby enhancing the reaction rate of MA conversion and the selectivity to DMA.

关键词： N-Methylation CO_(2) Cu/In_(2)O_(3) Supported catalysts Heterogeneous catalysis

Stereochemical editing:Catalytic racemization of secondary alcohols and amines

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Chinese Chemical Letters 2024年第5期35卷 17-31页

作者： Jun Zhang Zhiyao zheng Can Zhu Department of Chemistry Fudan UniversityShanghai 200438China Department of Organic Chemistry Arrhenius LaboratoryStockholm UniversityStockholm 10691Sweden

Chiral alcohols and amines are important structural units widely existing in pharmaceuticals,agrochemicals,and food *** kinetic resolution(DKR)is an efficient strategy to deliver optically active alcohols and amines from their *** the development of DKR method,racemization catalyst plays as a crucial element with the requirement of compatibility with the kinetic resolution(KR)*** this paper,recent advance in the catalytic racemization of secondary alcohols and amines is summarized based on different types of racemizing intermediates,which are redox racemization via ketone/imine intermediates,racemization via radical intermediates,and racemization via carbocation *** racemization of secondary alcohols and amines is also enclosed.

关键词： Racemization Secondary alcohols Amines Kinetic resolution Dynamic kinetic resolution

Reliability ensemble averaging reduces surface wind speed projection uncertainties in the 21st century over China

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Advances in Climate Change Research 2024年第2期15卷 222-229页

作者： zheng-Tai ZHANG Chang-Ai XU Key Laboratory for Semi-Arid Climate Change of the Ministry of Education College of Atmospheric SciencesLanzhou UniversityLanzhou 730000China

Accurate prediction of future surface wind speed(SWS)changes is the basis of scientific planning for wind *** studies have projected SWS changes in the 21st century over China on the basis of the multi-model ensemble(MME)of the 6th Coupled Model Intercomparison Project(CMIP6).However,the simulation capability for SWS varies greatly in CMIP6 multi-models,so the MME results still have large *** this study,we used the reliability ensemble averaging(REA)method to assign each model different weights according to their performances in simulating historical SWS changes and project the SWS under different shared socioeconomic pathways(SSPs)in *** results indicate that REA considerably improves the SWS simulation capacity of CMIP6,eliminating the overestimation of SWS by the MME and increasing the simulation capacity of spatial *** spatial correlations with observations increased from 0.56 for the MME to 0.85 for ***,REA could eliminate the overestimation of the SWS by 33%in *** for southeastern China,the SWS generally decreases over China in the near term(2020-2049)and later term(2070-2099),particularly under high-emission *** SWS reduction projected by REA is twice as high as that by the MME in the near term,reaching-4%to-3%.REA predicts a larger area of increased SWS in the later term,which expands from southeastern China to eastern *** study helps to reduce the projected SWS uncertainties.

关键词： Surface wind speed Uncertainty Multi-model ensemble Reliability ensemble averaging CMIP6

A microphysical investigation of different convective cells during the precipitation event with sustained high-resolution observations

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Frontiers of Earth Science 2024年第2期18卷 279-295页

作者： Ziheng HUANG zheng RUAN Debin SU State Key Laboratory of Severe Weather Chinese Academy of Meteorological SciencesBeijing 100081China College of Electronic Engineering Chengdu University of Information TechnologyChengdu 610225China Key Laboratory of Atmospheric Sounding China Meteorological AdministrationChengdu 610225China

The growth and breakup processes of raindrops within a cloud influence the rain intensity and the sizes of raindrops on the *** Doppler velocity spectrum acquired by a vertically pointing radar(VPR)contains information on atmospheric turbulence and the size classification of falling *** this study,the four types of Convective Cells(CC)during precipitation events with more than 700 mm of precipitation in southern China are *** characteristics of four types of CCs correspond to the isolated convection,the early stage,the mature stage,and the decline stage of organizational convection,in that *** analysis using retrieval of vertical air motion(Vair)and raindrop evolution in clouds from Doppler velocity spectra collected by C-band VPR revealed the growth and breakup of falling raindrops with dynamic *** raindrops appear in the early stages and are accompanied by ice particles,which are impacted by the falling path᾽s *** aggregation,which is primarily related to the alternation of updraft and downdraft,accounts for the mature stage᾽s high efficiency of surface *** CCs in the decline stage originate from the shallow uplift in the weak and broad downdraft under conditions of enough water *** updraft dominates the stage of isolated *** of convective cells could be more accurately represented in model evaluations.

关键词： cloud microphysics convective systems convective cell vertically pointing radar observations Doppler velocity spectrum

π-conjugated chromophore functionalized high-nuclearity titanium-oxo clusters containing structural unit of anatase for photocatalytic selective oxidation of sulfides

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Rare Metals 2024年第4期43卷 1736-1746页

作者： Ling-Rong Liao Dong-Chun zheng Pin-Xi Ou Qi-Xin Zhao Wei-Min Xuan Qi zheng State Key Laboratory for Modification of Chemical Fibers and Polymer Materials&College of Materials Science and Engineering Donghua UniversityShanghai201620China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials and College of Chemistry and Chemical Engineering Donghua UniversityShanghai 201620China

N-doping has significant influence in manipulating the properties of TiO_(2),and this has stimulated the development of N-donor-functionalized titanium-oxo clusters(TOCs)as molecular models to study the structure-property ***,the structural type and photoresponsive application are still limited for such TOCs,especially regarding the high-nuclearity TOCs that contain structure unit of TiO_(2)for ***,we showed the synthesis of a series of high-nuclearity TOCs 1-3 compounds usingπ-conjugated 1,10-phenanthroline(phen)as chromophore and N-donor functional *** 1 features cocrystal structure composed of one[Ti_(26)]~(2+)and half[Ti_(22)]~(2+),which renders it as the first cocrystallized TOC containing two positively charged species and phen-functionalized TOC showing the highest nuclearity up to 37 Ti *** adjusting the synthetic conditions,the individual{Ti_(22)}and{Ti_(26)}clusters can also be isolated as Compounds 2 and 3,*** core structure of{Ti_(22)}is mainly constructed from four lacunary{Ti_(4)}derived from pentagonal{Ti(Ti)_5}unit,while{Ti_(26)}is built from four complete{Ti(Ti)_5}***,a{Ti_8O_(14)}structure unit of anatase TiO_(2)can be identified in{Ti_(26)}.Based on the unique structural features and proper photophysical and photochemical properties of Compounds 1-3,they are applied for photocatalytic *** to the presence of anatase structure unit in{Ti_(26)}and the synergistic effect from{Ti_(22)}and{Ti_(26)},the catalytic performance presents in the order of Compound 1>Compound 3>Compound *** work provides excellent models to understand the structureproperty relationship from the perspective of cocrystallization and Ti-O binding model and will further promote the application of TOCs as functional catalysts for organic transformation.

关键词： Titanium-oxo cluster Molecular model of anatase TiO_(2) High nuclearity π-conjugated chromophore Photocatalytic sulfoxidation

HetNets Under Decoupled Uplink and Downlink Access with UE Random Discontinuous Transmission: Local Delay and Energy Efficiency

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China Communications 2024年第3期21卷 205-216页

作者： Zhang Yue zheng Fuchun Luo Jingjing School of Electronic and Information Engineering Harbin Institute of Technology(Shenzhen)Shenzhen 518055China

Due to the limited uplink capability in heterogeneousnetworks (HetNets), the decoupled uplinkand downlink access (DUDA) mode has recently beenproposed to improve the uplink performance. In thispaper, the random discontinuous transmission (DTX)at user equipment (UE) is adopted to reduce the interferencecorrelation across different time slots. By utilizingstochastic geometry, we analytically derive themean local delay and energy efficiency (EE) of an uplinkHetNet with UE random DTX scheme under theDUDA mode. These expressions are further approximatedas closed forms under reasonable *** results reveal that under the DUDA mode, there isan optimal EE with respect to mute probability underthe finite local delay constraint. In addition, with thesame finite mean local delay as under the coupled uplinkand downlink access (CUDA) mode, the HetNetsunder the DUDA mode can achieve a higher EE witha lower mute probability.

关键词： decoupled uplink and downlink access(DUDA) heterogeneous networks(HetNets) random discontinuous transmission(DTX) stochastic geometry

A Possible γ-Ray Pulsation from PSR J1740-5340B in the Globular Cluster NGC 6397

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Research in Astronomy and Astrophysics 2024年第1期24卷 285-291页

作者： Jiao zheng Pengfei Zhang Li Zhang Department of Astronomy School of Physics and AstronomyKey Laboratory of Astroparticle Physics of Yunnan ProvinceYunnan UniversityKunming 650091China

Recently, a new radio millisecond pulsar(MSP) J1740-5340B, hosted in the globular cluster(GC) NGC 6397,was reported with a 5.78 ms spin period in an eclipsing binary system with a 1.97 days orbital period. Based on a modified radio ephemeris updated by tool tempo2, we analyze the ~15 yr γ-ray data obtained from the Large Area Telescope on board the Fermi Gamma-ray Space Telescope and detect PSR J1740-5340B's γ-ray pulsation at a confidence level of ~4σ with a weighted H-test value of ~26. By performing a phase-resolved analysis, the γ-ray luminosity in on-pulse interval of PSR J1740-5340B is L_(γ)~ 3.8 × 10^(33) erg s^(-1) using NGC 6397's distance of 2.48 kpc. And γ-rays from the on-pulse part of PSR J1740-5340B contribute ~90% of the total observed γ-ray emissions from NGC 6397. No significant γ-ray pulsation of another MSP J1740-5340A in the GC is *** that the previous four cases of MSPs in GCs, more data in γ-ray, X-ray, and radio are encouraged to finally confirm the γ-ray emissions from MSP J1740-5340B, especially starving for a precise ephemeris.

关键词： gamma-rays:galaxies (stars:)pulsars:individual(PSR J1740-5340B) (Galaxy:)globular clusters:individual(NGC 6397)

Experimental observation of spontaneous symmetry breaking in a quantum phase transition

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Science China(Physics,Mechanics & Astronomy) 2024年第2期67卷 34-39页

作者： Wen Ning Ri-Hua zheng Jia-Hao Lu Fan Wu Zhen-Biao Yang Shi-Biao zheng Fujian Key Laboratory of Quantum Information and Quantum Optics College of Physics and Information EngineeringFuzhou UniversityFuzhou 350108China Hefei National Laboratory Hefei 230088China

Spontaneous symmetry breaking(SSB)plays a central role in understanding a large variety of phenomena associated with phase transitions,such as superfluid and *** far,the transition from a symmetric vacuum to a macroscopically ordered phase has been substantially *** process bridging these two distinct phases is critical to understanding how a classical world emerges from a quantum phase transition,but so far remains unexplored in *** here report an experimental demonstration of such a process with a quantum Rabi model engineered with a superconducting *** move the system from the normal phase to the superradiant phase featuring two symmetry-breaking field components,one of which is observed to emerge as the classical *** results demonstrate that the environment-induced decoherence plays a critical role in the SSB.

关键词： quantum phase transition Rabi model spontaneous symmetry breaking superconducting circuit Schrodinger cat states

Detection of Increasingγ-Ray Emissions from 4FGL J1718.5+4237 with Fermi-LAT

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Research in Astronomy and Astrophysics 2024年第8期24卷 169-174页

作者： Jiao zheng Pengfei Zhang Li Zhang Department of Astronomy School of Physics and AstronomyKey Laboratory of Astroparticle Physics of Yunnan ProvinceYunnan UniversityKunming 650091China School of Physics and Engineering Technology Xingyi Normal University for NationalitiesXingyi 562400China

We report a gradual brighteningγ-ray source,4FGL J1718.5+4237,in 0.1-500.0 GeV,which may be associated with a blazar NVSS J171822+423948 with a redshift of~*** analyzed 15.25 yr ofγ-ray data recorded by the Large Area Telescope on board the Fermi Gamma-ray Space Telescope and detected significantγ-ray emissions in the direction of the blazar with a test statistic(TS)of~*** on timing analysis using a 1 yr time bin,we have observed a gradual brightening inγ-ray emissions from the *** our analysis,we categorize them into two states:Quiet(TS~0)and Loud(TS~226)states,with the distinction occurring in 2016 August(MJD57602.69).From the Quiet state to the brightest period(the last data point),theγ-ray flux in 0.1-500.0 GeV increased by more than 12-fold from<0.2×10^(-8)photons cm^(-1)s^(-1)to 2.6×10^(-8)photons cm^(-1)s^(-1).Additionally,we studied the spectral properties in detail for the Loud state and the overall *** no significant variation was detected,both exhibited a spectral indexΓof~*** origin of the brighteningγ-ray emissions from the target is not yet *** long-term multi-wavelength observations and studies will provide insight into the astrophysical mechanisms of the target.

关键词： galaxies active-blazars individual(4FGL J1718.5+4237)