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Synergistic silver-mediated and palladium-catalyzed nondirected olefination of aryl C–H bond: quick access to multi-substituted aryl olefins

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Science China Chemistry 2024年第3期67卷 882-889页

作者： Jian yao Lili Shao Xiaohong Huo Xiaoming wang Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Frontiers Science Center for Transformative MoleculesSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Organometallic Chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 20032China School of Chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China

Transition metal-catalyzed olefination of aryl C-H bond is a powerful tool for the synthesis of alkenes. While the Pd-catalyzed oxidative C-H olefination of arenes, also known as Fujiwara-Moritani reaction, has been established as one of the most efficient methods, the substrates are largely limited to terminal olefins with electron-withdrawing group(s). Herein, we report a synergistic silver-mediated and palladium-catalyzed non-directed C-H olefination of arenes with vinyl(pseudo)halides, which offers a complementary strategy to the typical Fujiwara-Moritani reaction. The reactions proceeded well for a variety of halogenated arenes, heteroarenes, and olefin substrates, providing an efficient access to various multi-substituted aryl olefins, including trisubstituted/tetrasubstituted olefins and several complex olefins derived from medicines or natural products. Mechanistic studies indicated a bimetallic Pd/Ag cooperation is operative in the catalysis, i.e., the reaction is initiated by aryl C-H bond cleavage via ligation with phosphine/Ag species, followed by transferring of the aryl moiety to a vinyl palladium intermediate,which is in turn formed by oxidative addition of vinyl(pseudo)halide to a Pd complex. This method enables the synthesis of a wide range of challenging multi-substituted vinyl products from simple arenes(directing-group free) in a streamlined and controllable fashion.

关键词： direct C–H olefination multi-substituted aryl alkenes bimetallic Pd/Ag cooperation C–H functionalization

Ignition and Lean Blowout Characteristics of a Reverse-Flow Combustor for an Ultra-Compact Gas Turbine Engine

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Journal of Thermal Science 2024年第5期33卷 1897-1906页

作者： JIN Yi HUANG Yakun yao Kanghong ZHANG Kai wang Yunbiao wang Donghao College of Energy and Power Engineering Nanjing University of Aeronautics and AstronauticsNanjing 210016China National Key Laboratory of Transient Physics Nanjing University of Science and TechnologyNanjing 210094China Low-carbon Aerospace Power Engineering Research Center of Ministry of Education Nanjing 210016China

The flame stability limit and propagation characteristics of a reverse-flow combustor without any flame-stabilized device were experimentally investigated under room temperature and *** results indicate that it is feasible to stabilize the flame in the recirculation zones constructed by the impact jet flow from the primary holes and dilution *** flame projected area is mainly distributed in the recirculation zone upstream of the primary holes,whose presence and absence mark the ignition and *** the ignition process,the growth rate and value of the flame projected area first increase and then decrease with the inlet velocity increasing from 9.4 m/s to 42.1 m/s.A rapid reduction followed by a slow reduction of ignition and lean blowout equivalence ratios is achieved by the increased inlet *** the non-reacting fluid structure in three sections was measured,and detailed velocity profiles were analyzed to improve the understanding of the flame stabilization *** results are conducive to the design of an ultra-compact combustor.

关键词： ultra-compact combustor gas turbine reverse-flow combustor ignition lean blowout

Steady-state Voltage Security-constrained Optimal Frequency Control for Weak HVDC Sending-end AC Power Systems

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Journal of Modern Power Systems and Clean Energy 2024年第2期12卷 658-669页

作者： Qiangqiang wang Liangzhong yao Jian Xu Yuping Zheng Wei Li Wei wang School of Electrical Engineering and Automation Wuhan UniversityWuhan 430072China Hubei Engineering and Technology Research Center for AC/DC Intelligent Distribution Network(Wuhan University) Wuhan 430072China State Key Laboratory of Smart Grid Protection and Control NARI Group Corporation(State Grid Electric Power Research Institute)Nanjing 211106China

Due to the fact that a high share of renewable energy sources(RESs)are connected to high-voltage direct current(HVDC)sending-end AC power systems,the voltage and frequency regulation capabilities of HVDC sending-end AC power systems have *** has resulted in potential system operating problems such as overvoltage and overfrequency,which occur simultaneously when block faults exist in the HVDC *** this study,a steady-state voltage security-constrained optimal frequency control method for weak HVDC sending-end AC power systems is *** integrated virtual inertia control of RESs is employed for system frequency *** dynamic reactive power compensation devices are utilized to control the voltage of all nodes meet voltage security ***,an optimization model that simultaneously considers the frequency and steady-state voltage security constraints for weak HVDC sending-end AC power systems is *** optimal control scheme with the minimum total cost of generation tripping and additional dynamic reactive power compensation required is obtained through the optimization *** are conducted on a modified IEEE 9-bus test system and practical Qing-Yu line commutated converter based HVDC(LCC-HVDC)sending-end AC power system to verify the effectiveness of the proposed method.

关键词： Renewable energy source(RES) high-voltage direct current(HVDC) AC power system optimal frequency control steady-state voltage security dynamic reactive power compensation

Solubility determination and comparison ofβ-HMX and RDX in two binary mixed solvents(acetonitrile+water,nitric acid+water)

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Chinese Journal of Chemical Engineering 2024年第5期69卷 238-249页

作者： Yuehua yao Fan wang Yinguang Xu Zishuai Xu Lizhen Chen Jianlong wang School of Chemistry and Chemical Engineering North University of ChinaTaiyuan 030051China Gansu Yinguang Chemical Industry Group Co.Ltd. Baiyin 730900China

In order to remove hexahydro-1,3,5-trinitro-1,3,5-triazine(RDX),the main impurity,in process of polymorphic transformation of octrahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine(HMX),the solubility ofβ-HMX and RDX in acetonitrile(ACN)+water in the temperature range of 288.15-333.15 K and in nitric acid(HNO_(3))+water in the temperature range of 298.15-333.15 K were measured by laser dynamic *** results showed that the solubility of bothβ-HMX and RDX in binary mixed solvents increased monotonously as the temperature increase at a given solvent composition or with increasing of mole fraction of solvent(ACN and nitric acid).Solubility data were well correlated by the modified Apelblat equation,Jouyban-Acree model,Yaws equation and van't Hoff equation,and the Yaws equation achieved the best fitting results according to the relative error and the mean square error ***,the solubility ofβ-HMX and RDX in binary mixed solvent was compared,based on the solubility difference and the solvent's own properties,the best separation degree ofβ-HMX and RDX was found when the mole fraction of nitric acid was 0.22 at room temperature,which provided data support for HMX crystallization in mixed *** solubility differences between RDX andβ-HMX in mixed solvents were explained from the formation of intermolecular and intramolecular hydrogen bonds.

关键词： Solubility Octrahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine Hexahydro-1,3,5-trinitro-1,3,5-triazine Separation Model Hydrogen bond

Synthesis of betanin by expression of the core betalain biosynthetic pathway in carrot

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Horticultural Plant Journal 2024年第3期10卷 732-742页

作者： Bo wang Yahui wang Yuanjie Deng Quanhong yao Aisheng Xiong State Key Laboratory of Crop Genetics and Germplasm Enhancement College of HorticultureNanjing Agricultural UniversityNanjingJiangsu 210095China Shanghai Key Laboratory of Agricultural Genetics and Breeding Biotechnology Research Institute of Shanghai Academy of Agricultural ScienceShanghai 201106China

Betalain has received increased attention because of its high nutritional value and crucial physiological *** on the elucidation of its core biosynthetic pathway,betalain can be produced in additional plants by metabolic *** of betalain in carrot(Daucus carota L.)can improve its nutritional quality and economic value by extracting betalain from the fleshy root,non-edible part,and processing residue of *** this study,two different constructs,namely,pYB:mCD(AomelOS,BvCYP76AD1S,and BvDODA1S)and p YB:CDD(BvCYP76AD1S,BvDODA1S,and MjcDOPA5GTS),were introduced into carrot for betanin synthesis by Agrobacterium-mediated *** can be synthetized in both transgenic calli,and p YB:m CD-transgenic callus can be used to produce betacyanin by suspension ***,pYB:mCD-transgenic seedlings can synthetize betanin only by tyrosine *** p YB:CDD-transgenic lines can synthetize betanin in whole *** betanin content in fleshy root of pYB:CDD-transgenic carrot was(63.4±9)μg·g^(-1)fresh weight according to quantitative *** betanin-producing carrot plant materials can be used to synthesize betanin for industrial application or consumption as dietary sources.

关键词： Daucus carota L. Betanin Biosynthesis Metabolic engineering Biofortification

Decline in tree-ring growth of Picea mongolica and its intra-annual eco-physiological responses to drought and CO_(2) enrichment in semi-arid China

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Journal of Forestry Research 2024年第4期35卷 89-101页

作者： Xiaomin Zeng Ping Ni Xiaohong Liu Wenzhi wang yao Li Wenchao wang School of Geography and Tourism Shaanxi Normal UniversityXi’an 710119People’s Republic of China The Key Laboratory of Mountain Environment Evolution and Regulation Institute of Mountain Hazards and EnvironmentChinese Academy of SciencesChengdu 610041People’s Republic of China CAS Key Laboratory of Forest Ecology and Management Institute of Applied EcologyChinese Academy of SciencesShenyang 110016People’s Republic of China University of Chinese Academy of Sciences Beijing 100049People’s Republic of China

Episodes of drought-induced decline in tree growth and mortality are becoming more frequent as a result of climate warming and enhanced water stress in semi-arid ***,the ecophysiological mechanisms under-lying the impact of drought on tree growth remains *** this study,earlywood and latewood tree-ring growth,δ^(13)C,andδ^(18)O chronologies of Picea mongolica from 1900 to 2013 were developed to clarify the intra-and inter-annual tree-ring growth responses to increasingly fre-quent *** results indicate that annual basal area increment residuals(BAI_(res)),which removed tree age and size effects,have significantly decreased since ***-ever,the decreasing trend of earlywood BAI_(res) was higher than that of *** response analysis suggests that the dominant parameters for earlywood and latewood proxies(BAI_(res),δ^(13)C andδ^(18)O)were drought-related climate variables(Palmer drought severity index,temperature,rela-tive humidity,and vapor pressure deficit).The most signifi-cant period of earlywood and latewood proxies’responses to climate variables were focused on June-July and July-August,***_(res),andδ^(13)C were significantly affected by temperature and moisture conditions,whereasδ^(18)O was slightly *** stomatal conduct-ance due to drought outweighed the influence of increasing CO_(2) on intrinsic water use efficiency(iWUE),and ultimately led to a decline in BAI_(res).Compared to latewood,the faster decreasing BAI_(res) and smaller increasing iWUE of early-wood suggested trees were more vulnerable to water stress in the early growing *** study provides insights into the inter-and intra-annual mechanisms of tree-ring growth in semi-arid regions under rising CO_(2) and climate change.

关键词： Tree growth Drought Water-use efficiency Seasonal differences Stable isotopes

Accelerating the Screening of Modified MA_(2)Z_(4)Catalysts for Hydrogen Evolution Reaction by Deep Learning-Based Local Geometric Analysis

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Energy & Environmental Materials 2024年第6期7卷 290-302页

作者： Jingnan Zheng Shibin wang Shengwei Deng Zihao yao Junhua Hu Jianguo wang Institute of Industrial Catalysis State Key Laboratory Breeding Base of Green-Chemical Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310032China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China School of Materials Science and Engineering State Center for International Cooperation on Designer Low-Carbon&Environmental Materials(CDLCEM)Zhengzhou UniversityZhengzhou 450001China

Machine learning(ML)integrated with density functional theory(DFT)calculations have recently been used to accelerate the design and discovery of single-atom catalysts(SACs)by establishing deep structure–activity *** traditional ML models are always difficult to identify the structural differences among the single-atom systems with different modification methods,leading to the limitation of the potential application *** to the structural properties of several typical two-dimensional MA_(2)Z_(4)-based single-atom systems(bare MA_(2)Z_(4)and metal single-atom doped/supported MA_(2)Z_(4)),an improved crystal graph convolutional neural network(CGCNN)classification model was employed,instead of the traditional machine learning regression model,to address the challenge of incompatibility in the studied *** CGCNN model was optimized using crystal graph representation in which the geometric configuration was divided into active layer,surface layer,and bulk layer(ASB-GCNN).Through ML and DFT calculations,five potential single-atom hydrogen evolution reaction(HER)catalysts were screened from chemical space of 600 MA_(2)Z_(4)-based materials,especially V_(1)/HfSn_(2)N_(4)(S)with high stability and activity(Δ_(GH*)is 0.06 eV).Further projected density of states(pDOS)analysis in combination with the wave function analysis of the SAC-H bond revealed that the SAC-dz^(2)orbital coincided with the H-s orbital around the energy level of−2.50 eV,and orbital analysis confirmed the formation ofσ*** study provides an efficient multistep screening design framework of metal single-atom catalyst for HER systems with similar two-dimensional supports but different geometric configurations.

关键词： graph convolutional neural network hydrogen evolution reaction modified MA_(2)Z_(4)substrate single atom catalyst

Simultaneous improving luminescence intensity and stability of CsPbBr_(3):SCN−@Eu/Zr-Uio-66-NH_(2) with tunable emissions from blue to green and applications in indoor photovoltaics

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Nano Research 2024年第8期17卷 6879-6887页

作者： Minze Li yao Sun Honglai Lu Peifen Zhu Ruihong wang Guofeng wang Key Laboratory of Functional Inorganic Material Chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China Department of Electrical Engineering and Computer Science University of MissouriColumbiaMO 65211USA

The construction of stable and efficient materials that emit blue and green light remains a *** the blue light materials reported,metal-organic framework(MOF)materials are rarely reported as blue phosphors due to their weak luminescence *** on the construction of CsPbBr_(3)@MOF(CPB@MOF),an innovative idea was proposed to simultaneously enhance the green luminescence of CPB and the blue luminescence of MOF through the interaction between CPB and MOF for the first *** expected,the blue luminescence from CPB:7%SCN−@0.5%MOF:Eu as well as the green luminescence from 5%CPB:7%SCN−@MOF:Eu was sufficient to construct high-performance light-emitting diode(LED)devices and further excite solar cells to generate stable photoelectric *** white LED(WLED)device with excellent color quality(color rendering index(CRI)=96.2)and correlated color temperature(CCT=9688 K)can be constructed by using the obtained blue-emitting CPB:7%SCN-@0.5%MOF:Eu,green-emitting 5%CPB:7%SCN−@MOF:Eu,and red-emitting PPB:30%Mn^(2+).The density functional theory(DFT)theoretical calculation results indicate that the p orbital of Pb plays the major role in the conduction band,and the p orbital of Br plays the major role in the valance band of CPB and CPB:SCN−.While the p orbital of O plays the major role in both the conduction band and valance band of *** heat capacity of CPB and CPB:SCN−separately reaches the Dulong–Petit limit at 200 and 400 K,indicating that the thermal stability of CsPbBr_(3)increases after SCN−doping.

关键词： CsPbBr_(3):SCN−@Uio-66-NH_(2) composites luminescence stability white light-emitting diodes(WLEDs) indoor photovoltaics density functional theory(DFT)calculation

A Quick Calculation Method for Radiation Pattern of Submillimeter Telescope with Deformation and Displacement

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Research in Astronomy and Astrophysics 2024年第3期24卷 249-265页

作者： Jia You Yi-Wei yao Zheng wang School of Automation Southeast UniversityNanjing 210096China

Radiation pattern captures the electromagnetic performance of reflector antennas,which is significantly affected by the deformation of the primary reflector due to gravity and the displacement of the secondary *** the design process of large reflector antennas,a substantial amount of time is often dedicated to iteratively adjusting structural parameters and validating electromagnetic *** improve the efficiency of the design process,we first propose an approximate calculation method of optical path difference(OPD)for the deformation of the primary reflector under gravity and the displacement of the secondary *** an OPD fitting function based on the modified Zernike polynomials is proposed to capture the phase difference of radiation over the aperture plane,based on which the radiation pattern will be obtained quickly by the aperture field integration *** experiments demonstrate the effectiveness of the proposed quick calculation method for analyzing the radiation pattern of a 10.4 m submillimeter telescope antenna at its highest operating frequency of 856 *** comparison with the numerical simulation method based on GRASP(which is an antenna electromagnetic analysis tool combining physical optics(PO)and physical theory of diffraction(PTD)),the quick calculation method reduces the time for radiation pattern analysis from more than one hour to less than two ***,the quick calculation method exhibits excellent accuracy for the figure of merit(FOM)of the radiation ***,the proposed quick calculation method can obtain the radiation pattern with high speed and *** to the time-consuming numerical simulation method(PO and PTD),it can be employed for quick analysis of the radiation pattern for the lateral displacement of the secondary reflector and the deformation of the primary reflector under gravity in the design process of a reflector antenna.

关键词： instrumentation high angular resolution-methods data analysis-methods analytical