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Catalytically generated noncovalent ammonium dienolate:a versatile platform for the development of organocatalytic asymmetric cascade reactions

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Science China Chemistry 2024年第8期67卷 2524-2546页

作者： Jun-Bing Lin Dong-sheng Ji Peng-Fei xu State Key Laboratory of Applied Organic Chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China Shaanxi Key Laboratory of Chemical Reaction Engineering College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China

Organocatalytic cascade reactions represent a powerful strategy for the rapid construction of complex chiral molecules with multiple stereocenters from simple substrates under mild conditions. The intriguing structural feature and diverse reactivity of catalytically generated dienolate species render them competent and versatile intermediates for the development of practical and valuable cascade reactions. Over the past years, a plethora of innovative and pioneering noncovalent ammonium dienolatemediated cascade reactions have been designed and implemented under the catalysis of chiral organocatalysts, making dienolate activation a general, robust, and complementary method for the functionalization of unsaturated carbonyl compounds and related substances. This review illustrates the recent advances in organocatalytic noncovalent ammonium dienolate-mediated cascade reactions(mainly from 2010 to 2023), including the cascade transformations of ammonium dienolates directly generated from unsaturated ketone/aldehyde, ester/lactone/azlactone, amide/lactam/pyrazolone/oxindole, and alkylidene nitrile compounds. The contents are arranged based on the reaction types of the ammonium dienolates, with an emphasis on cascade 2,5-, 3,5-, and 4,5-difunctionalizations of these intermediates. Furthermore, other cascade reactions involving the 1,3-, 2,3-, and even more complex 3,4,5-reactivities of ammonium dienolates were also discussed. The reaction pathway, reaction stereoinduction, and synthetic applications of the ammonium dienolate-mediated cascade reactions were highlighted throughout the article. As a stimulating and ever-growing research area, the organocatalytic noncovalent ammonium dienolate-mediated cascade reactions are expected to continue demonstrating their magic power for constructing chiral targets in the future and further expanding the boundaries of asymmetric catalysis.

关键词： organocatalysis asymmetric catalysis ammonium dienolate cascade reaction difunctionalization

Effect of Mo and cold forging deformation on strength and ductility of cobalt-based alloy L605

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Journal of Iron and Steel Research International 2024年第7期31卷 1811-1823页

作者： Zhong-lin Wang Zhi-hua Gong Quan Li han-sheng Bao School of Materials and Metallurgy Inner Mongolia University of Science and TechnologyBaotou 014017Inner MongoliaChina Institute of Special Steels Central Iron and Steel Research Institute Co.Ltd.Beijing 100081China

Mo element was added to cobalt-based alloy L605,and cold forging deformation was *** effects of the addition and cold forging deformation on the microstructure and mechanical properties of the alloy were studied by thermodynamic calculation,electron backscatter diffraction,transmission electron microscopy,and X-ray *** stacking fault energy(SFE)of the alloy decreased after the addition,and the formation of stacking faults and intersections were promoted to improve the strength and *** tensile strength of the alloy with Mo increased from 1190 to 1702 MPa after 24%cold deformation,producing significant work *** strengthening mechanism is strain-induced martensitic transformation(SIMT)and deformation *** alloy,combined with Mo and after 24%deformation,had both high strength and ductility in comparison with the original cobalt-based alloy *** is attributed to the lower SFE which caused the increase in stacking fault *** the tensile process,theε-hcp phase was easily generated at the stacking fault to reduce the stress concentration and increase the *** SIMT by adjusting the density of stacking faults can improve the mechanical properties of cobalt-based ***ε-hcp phase,the interaction between deformation twins and dislocations,and the interaction between e-hcp phases during cold forging deformation caused local stress concentration,lowering ductility and toughness.

关键词： Cobalt-based alloy-Stacking fault energy Strain-induced martensitic transformation Deformation twin Cold forging deformation

Electrochemical Mono-Deuterodefluorination of Trifluoromethyl Aromatic Compounds with Deuterium Oxide

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CCS Chemistry 2024年第1期6卷 230-240页

作者： Jie sheng xu Cheng Institute of Chemistry and Biomedical Sciences Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023 State Key Laboratory of Elemento-Organic Chemistry Nankai UniversityTianjin 30071

The deuterodifluoromethyl group CF_(2)D combines the structural features of CF_(3) and CD_(3) groups,finding wide applications in diverse pharmaceutical *** this work,the electrochemical monodeuterodefluorination of Ar-CF_(3) to Ar-CF_(2)D is achieved with an unreported deuterium atom transfer-coupled electron transfer pathway using D_(2)O as the only D source for the first time.A series of Ar-CF_(3) substances,including commercial pharmaceuticals,were converted to corresponding CF_(2)D products in up to 91% yield and 97% D-incorporation.A variety of functional groups,including pyridine,pyrrole,furan,thiophene,borate,thio ether,amine,amide,sulfonamide,and halide,are well tolerated in this protocol.t-BuOLi was an essential reagent to achieve chemoselective mono-defluorination.

关键词： electrochemistry C-F activation fluorinecontaining drugs deuterated drugs deuterium oxide

Perception of fundamental science to boost lithium metal anodes toward practical application

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Green Energy & Environment 2024年第3期9卷 454-472页

作者： Jinkun Wang Li Wang Hong xu Li sheng Xiangming He Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing100084China

As a key material for lithium metal batteries(LMBs),lithium metal is one of the most promising anode materials to break the bottleneck of battery energy density and a commonly used active material for reference *** lithium anodes are regarded as the holy grail of lithium batteries,decades of exploration have not led to the successful commercialization of LMBs,due mainly to the challenges related to the inherent properties of lithium *** pave the way for further investigation,herein,a comprehensive review focusing on the fundamental science of lithium are ***,the natures of lithium atoms and their isotopes,lithium clusters and lithium crystals are revisited,especially their structural and energetic ***,the electrochemical properties of lithium metal are *** important concepts and scientific questions,including the electronic structure of lithium,influence of high pressure and low temperature on the properties of lithium,factors influencing lithium deposition,generation of lithium dendrites,and electrode potential of lithium in different electrolytes,are explained and analyzed in *** to improve the performance of lithium anodes and thoughtfulness about the electrode potential in lithium battery research are proposed.

关键词： Lithium Cluster Crystal Physicochemical property Fundamental science

Neighbor Sum Distinguishing Total Choosability of Planar Graphs with Maximum Degree at Least 10

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Acta Mathematicae Applicatae Sinica 2024年第1期40卷 211-224页

作者： Dong-han Zhang You Lu sheng-gui Zhang Li Zhang School of Mathematics and Statistics Northwestern Polytechnical UniversityXi’an710129China School of Mathematics and Computer Application Shangluo UniversityShangluo726000China

A neighbor sum distinguishing(NSD)total coloringφof G is a proper total coloring of G such thatΣz∈EG(u)U{u}φ(z)≠Σz∈EG(v)U{v}φ(z)for each edge uv∈E(G),where EG(u)is the set of edges incident with a vertex *** 2015,Pilśniak and Wozniak conjectured that every graph with maximum degreeΔhas an NSD total(Δ+3)-***,Yang et *** that the conjecture holds for planar graphs withΔ≥10,and Qu et *** that the list version of the conjecture also holds for planar graphs withΔ≥*** this paper,we improve their results and prove that the list version of the conjecture holds for planar graphs withΔ≥10.

关键词： planar graphs neighbor sum distinguishing total choosibility combinatorial nullstellensatz discharging method

Non-Gaussian feature of the output field from a double qubit-cavity ultrastrong coupling system

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Communications in Theoretical Physics 2024年第7期76卷 30-36页

作者： sheng-wen xu Shi-yu Dai Teng Zhao Center for Quantum Science and Technology Jiangxi Normal UniversityNanchang 330022China

We investigate the non-Gaussian feature of radiation in a circuit quantum electrodynamics(QED)system where two qubits are strongly coupled to a single-mode *** the regime of ultrastrong coupling(USC),the rotating-wave approximation is not valid,and the Rabi Hamiltonian contains counter-rotating wave terms,leading to level crossing and avoided crossings in the energy *** further analyze the intensity-amplitude correlation of the output field in these two novel *** the USC regime,the creation and annihilation operators in the correlation function are replaced,allowing for the identification of non-Gaussian features in the output *** findings reveal that despite the absence of squeezing effects in the output light,significant non-Gaussian characteristics are ***,we demonstrate that as the driving or coupling strength increases,the non-Gaussian features of the output field become more *** suggests that USC systems hold broad potential applications in the realms of nonlinear optics and the generation of non-Gaussian states.

关键词： ultrastrong coupling non-Gaussian intensity-amplitude correlation

Sustainable and practical semi-heterogeneous photosynthesis of 5-amino-1,2,4-thiadiazoles over WS_(2)/TEMPO

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Chinese Chemical Letters 2024年第8期35卷 250-253页

作者： Jia-Cheng Hou Hong-Tao Ji Yu-han Lu Jia-sheng Wang Yao-Dan xu Yan-Yan Zeng Wei-Min He School of Chemistry and Chemical Engineering University of South ChinaHengyang 421001China

An eco-friendly and practical method for the clean preparation of 5-amino-1,2,4-thiadiazoles was *** WS_(2)as the semiconductor photocatalyst,both TEMPO and O_(2)(in air)as the redox catalysts,a variety of thiadiazoles were semi-heterogeneously formed in high to quantitative yields and could be easily collected by CPME extraction and ***,the catalytic system can be reusable for at least 5 reaction runs.

关键词： Green chemistry Thiadiazoles Heterogeneous catalyst Redox catalyst Extraction

Experimental investigation on coal pore-fracture variation and fractal characteristics synergistically affected by solvents for improving clean gas extraction

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International Journal of Mining Science and Technology 2024年第3期34卷 413-425页

作者： Feilin han sheng xue Chunshan Zheng Zhongwei Chen Guofu Li Bingyou Jiang Key Laboratory of Safe and Effective Coal Mining of Ministry of Education Anhui University of Science and TechnologyHuainan 232001China School of Safety Science and Engineering Anhui University of Science and TechnologyHuainan 232001China School of Mechanical and Mining Engineering University of QueenslandQLD 4072Australia State Key Laboratory of Coal and Coalbed Methane Co-Mining Jincheng 048012China

Chemical solvents instead of pure water being as hydraulic fracturing fluid could effectively increase permeability and improve clean methane extraction ***,pore-fracture variation features of lean coal synergistically affected by solvents have not been fully *** testing,nuclear magnetic resonance analysis,liquid phase mass spectrometry was adopted to comprehensively analyze pore-fracture change characteristics of lean coal treated by combined solvent(NMP and CS_(2)).Meanwhile,quantitative characterization of above changing properties was conducted using geometric fractal *** model between permeability,fractal dimension and porosity were *** indicate that the end face fractures of coal are well developed after CS2and combined solvent treatments,of which,end face box-counting fractal dimensions range from 1.1227 to *** decreases in ultrasonic longitudinal wave velocity of coal affected by NMP,CS_(2)and combined solvent are 2.700%,20.521%,22.454%,*** treatments could lead to increasing amount of both mesopores and *** ratio of fractal dimension Dsis 0.259%–2.159%,while permeability increases ratio of NMR ranges from 0.1904 to ***,combined solvent could dissolve coal polar and non-polar small molecules and expand flow *** could provide reference for solvent selection and parameter optimization of permeability-enhancement technology.

关键词： Clean gas extraction Chemical solvent Experimental investigation Fractal characteristics Pore fracture

Neural Circuitry Involving Substance P in Male Sexual Behavior

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Neuroscience Bulletin 2024年第4期40卷 544-546页

作者： Xinrong Wang Junqiang Zheng han xu Department of Neurobiology and Department of Neurology of the Second Affiliated Hospital and School of Brain Science and Brain Medicine Zhejiang University School of MedicineHangzhou310058China Nanhu Brain-Computer Interface Institute Hangzhou311100China Liangzhu Laboratory MOE Frontier Science Center for Brain Science and Brain-machine IntegrationState Key Laboratory of Brain-Machine IntelligenceZhejiang UniversityHangzhou311121China NHC and CAMS Key Laboratory of Medical Neurobiology Zhejiang UniversityHangzhou310058China Lingang Laboratory Shanghai200031China

Male sexual behavior is an innate social behavior crucial for reproduction[1].Previous studies have identified several brain regions crucial for the control of both sexual and aggressive behaviors in ***,molecularly specified neural circuits that specifically control male sexual behavior remain *** with the inherently rewarding nature of sexual behavior,previous research has implicated the role of the dopamine system in regulating sexual desire[2].However,the interaction between reward and copulation at the circuit level remains largely ***,it is unclear if the associated neural pathways are specific in modulating sexual reward.

关键词： behavior neural specified