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Enantioselective iridium-catalyzed allylic substitution with a Reformatsky reagent: direct construction of β-stereogenic homoallylic esters

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Science China Chemistry 2024年第11期67卷 3791-3797页

作者： debasis Pal Kirana d.Veeranna Yuk Fai Wong P.Andrew Evans department of Chemistry Queen's University Xiangya School of Pharmaceutical Sciences Central South University

The Reformatsky reagent derived from ethyl bromoacetate circumvents the challenge associated with the direct regio-and enantioselective iridium-catalyzed allylic alkylation with an unstabilized aliphatic ester enolate. Notably, this work represents the first example of using a Reformatsky reagent in a metal-allyl reaction, which permits the direct construction of enantioenriched β-stereogenic homoallylic esters without preactivation of the pronucleophile or post-reaction modification of the product(e.g., thermal decarboxylation of a 1,3-dicarbonyl). Moreover, the process allows the coupling of a broad range of sterically and electronically diverse electrophiles bearing aryl, heteroaryl and alkenyl derivatives, including the significantly more challenging alkyl-substituted allylic carbonates. The versatility of the ester product is exemplified by a series of functional group manipulations and the development of a concise and efficient enantioselective total synthesis of the natural product,(+)-descurainolide A. Finally, mechanistic studies indicate that the zinc enolate behaves as a soft nucleophile that undergoes outer-sphere alkylation.

关键词： allylic substitution asymmetric catalysis mechanistic studies natural product synthesis Reformatsky reagent

Insm1:orchestrating cellular mimicry in the thymus medulla

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Cellular & Molecular Immunology 2024年第4期21卷 414-416页

作者： K.d.James J.E.Cowan UCL Institute of Immunity and Transplantation The Pears BuildingRowland Hill StreetLondonNW32PPUK

The thymus is the primary production site for a functional and self-tolerant T-cell *** establishment of immune tolerance is mediated by the generation and presentation of tissue-restricted self-antigens(TRAs)by medullary thymic epithelial cells(mTECs),which screen T-cell receptors for self-reactivity to eliminate autoreactive T *** studies have extended our understanding of mTEC heterogeneity by examining the mechanisms by which mTECs mimic the peripheral self[1].

关键词： medullary eliminate restricted

Polyhydroxyurethanes from Biobased Monomers and CO_(2):A Bridge between Sustainable Chemistry and CO_(2) Utilization

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Chinese Journal of Chemistry 2024年第6期42卷 652-685页

作者： Tharinee Theerathanagorn Tanika Kessaratikoon Hafeez Ur Rehman Valerio d'Elia daniel Crespy VISTEC Advanced Laboratory for Environment-Related Inorganic and Organic Syntheses Department of Materials Science and EngineeringVidyasirimedhi Institute of Science and Technology21210Wang ChanRayongThailand department of Materials Science and Engineering Vidyasirimedhi Institute of Science and Technology21210Wang ChanRayongThailand

Polyhydroxyurethanes(PHUs)have received considerable attention in the last decade as potential alternatives to traditional phosgene-based polyurethanes(PUs).The development of suitable 5CC(five membered-ring cyclic carbonate)precursors bearing multiple carbonate moieties(multi-5CCs)is a key requisite for preparing PHUs by polyaddition reaction with bis-or *** sustainable PHUs from CO_(2)-based five-membered cyclic carbonates(5CCs)obtained from biobased epoxides is a valuable strategy to bridge CO_(2) utilization and the upcycling of renewable *** this context,while many multi-5CC monomers reported in the literature are oil-based,recent efforts have led to the development of a large variety of multifunctional 5CCs that are produced by the combination of CO_(2) and renewable resources such as fatty acids and vegetable oils,lignin,terpenes,and *** this work,recent crucial advances(2019—2023)on PHUs prepared from bis-and multi-5CCs produced from CO_(2) and(partially/potentially)biobased substrates are reviewed with respect to their synthesis,thermal and mechanical properties,and their recent,emerging applications.

关键词： CO_(2) conversion Polyhydroxyurethanes Cyclic carbonates Biobased compounds Fatty acids Functional polymers Monomers Renewable resources

Simple collective model for nuclear chiral mode

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Frontiers of physics 2024年第2期19卷 1-5页

作者： R.V.Jolos E.A.Kolganova d.R.Khamitova Joint Institute for Nuclear Research 141980 DubnaMoscow regionRussia dubna State University 141982 DubnaMoscow RegionRussia

A simple semi-analytical collective model that takes into account the limitations of the variation interval of the collective variable is suggested to describe the chiral dynamics in triaxial odd−odd nuclei with a fixed particle−hole *** collective Hamiltonian is constructed with the potential energy obtained using the postulated ansatz for the wave function symmetric with respect to chiral *** diagonalizing the collective Hamiltonian the wave functions of the lowest states are obtained and the evolution of the energy splitting of the chiral doublets in transition from chiral vibration to chiral rotation regime is demonstrated.

关键词： collective model nuclear chiral

design of Resilient Sensor Networks Balancing Resilience and Efficiency

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International Journal of disaster Risk Science 2024年第1期15卷 107-115页

作者： Sergey N.Vecherin Kiril d.Ratmanski Luke Hogewood Igor Linkov Cold Regions Research and Engineering Laboratory Engineering Research and Development CenterHanoverNH 03755USA Environmental Laboratory Engineering Research and Development CenterVicksburgMS 39180USA

In recent years,the notion of resilience has been developed and applied in many technical areas,becoming exceptionally pertinent to disaster risk *** a disaster situation,accurate sensing information is the key to efficient recovery *** general,resilience aims to minimize the impact of disruptions to systems through the fast recovery of critical functionality,but resilient design may require redundancy and could increase *** this article,we describe a method based on binary linear programming for sensor network design balancing efficiency with *** application of the developed framework is demonstrated for the case of interior building surveillance utilizing infrared sensors in both twoand three-dimensional *** method provides optimal sensor placement,taking into account critical functionality and a desired level of resilience and considering sensor type and *** problem formulation,resilience requirements,and application of the optimization algorithm are described in *** of sensor locations with and without resilience requirements shows that resilient configuration requires redundancy in number of sensors and their intelligent *** tasks are successfully solved by the described method,which can be applied to strengthen the resilience of sensor networks by *** proposed methodology is suitable for large-scale optimization problems with many sensors and extensive coverage areas.

关键词： Binary linear programming Optimal sensor placement Redundant networks Resilience and efciency Resilient sensor networks

Radioisotope production using lasers:From basic science to applications

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Matter and Radiation at Extremes 2024年第3期9卷 31-44页

作者： M.R.d.Rodrigues A.Bonasera M.Scisciò J.A.Pérez-Hernández M.Ehret F.Filippi P.L.Andreoli M.Huault H.Larreur d.Singappuli d.Molloy d.Raffestin M.Alonzo G.G.Rapisarda d.Lattuada G.L.Guardo C.Verona Fe.Consoli G.Petringa A.McNamee M.La Cognata S.Palmerini T.Carriere M.Cipriani G.di Giorgio G.Cristofari R.de Angelis G.A.P.Cirrone d.Margarone L.Giuffrida d.Batani P.Nicolai K.Batani R.Lera L.Volpe d.Giulietti S.Agarwal M.Krupka S.Singh Fa.Consoli Cyclotron Institute Texas A&M UniversityCollege StationTexas 77840USA Laboratori Nazionali del Sud Istituto Nazionale di Fisica Nucleare(LNS-INFN)CataniaItaly ENEA Fusion and Technologies for Nuclear Safety and Security Department-CFrascatiItaly Centro de Láseres Pulsados(clpu) VillamayorSpain Universidad de Salamanca SalamancaSpain Centre Lasers Intenses et Applications(CELIA) Universitéde BordeauxCNRSCEATalenceFrance HB11 Energy Holdings Pty FreshwaterNew South WalesAustralia School of Mathematics and Physics Queen’s University BelfastBelfastUnited Kingdom dipartimento di Fisica e Astronomia“E.Majorana ”Università di CataniaCataniaItaly Facoltàdi Ingegneria e Architettura Universitàdegli Studi di Enna“Kore”EnnaItaly dipartimento di Ingegneria Industriale Universitàdi Roma“Tor Vergata”RomaItaly dipartimento di Fisica e Geologia Universitàdegli Studi di PerugiaPerugiaItaly Istituto Nazionale di Fisica Nucleare Sezione di PerugiaPerugiaItaly ELI Beamlines Facility the Extreme Light Infrastructure ERICDolni BrezanyCzech Republic ETSIA Universidad Politécnica de MadridMadridSpain dipartimento Fisica “E.Fermi”Universitàdi Pisa and INFNPisaItaly FZU–Institute of Physics of Czech Academy of Sciences PragueCzech Republic Institute of Plasma Physics of Czech Academy of Sciences PragueCzech Republic

The discovery of chirped pulse amplification has led to great improvements in laser technology,enabling energetic laser beams to be compressed to pulse durations of tens of femtoseconds and focused to a few *** with energies of tens of MeV can be accelerated using,for instance,target normal sheath acceleration and focused on secondary *** such conditions,nuclear reactions can occur,with the production of radioisotopes suitable for medical *** use of high-repetition lasers to produce such isotopes is competitive with conventional methods mostly based on *** this paper,we study the production of^(67)Cu,^(63)Zn,^(18)F,and^(11)C,which are currently used in positron emission tomography and other *** the same time,we study the reactions^(10)B(p,α)^(7)Be and^(70)Zn(p,4n)^(67)Ga to put further constraints on the proton distributions at different angles,as well as the reaction^(11)B(p,α)^(8)Be relevant for energy *** experiment was performed at the 1 PW laser facility at VegaⅢin Salamanca,*** distributions of radioisotopes in the forward(with respect to the laser direction)and backward directions were measured using a high purity germanium *** results are in reasonable agreement with numerical estimates obtained following the approach of Kimura and Bonasera[*** ***.,Sect.A 637,164–170(2011)].

关键词： purity estimates backward

Assessing the biennial conference on science and technology(BICOST IX)2023 technical output on renewable energy,energy storage,and green hydrogen in line with UN SdG commitments

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Clean Energy 2024年第2期8卷 85-88页

作者： S.K.B.d.Silva K.G.d.Piyumali Rasitha Thilini Suranjana Perera K.d.K.G.Kaluarachchi Thilini Munagamage R.M.R.Ahammed C.S.P.Piyankarage Seyed Shahmy Veranja Karunaratne National Science and Technology Commission of Sri Lanka ColomboSri Lanka Sri Lanka Technological Campus(SLTC) PadukkaSri Lanka University of Peradeniya PeradeniyaSri Lanka

The development,production and utilization of renewable energy,energy storage and green hydrogen and the associated technologies in Sri Lanka have great potential to contribute to the United Nations’Sustainable development Goals(SdGs).The island aims to achieve 70%electricity generation from renewable energy sources by 2030(within the target of 40%utilization of renewable energy sources for the entire energy generation of the country by 2030).The power sector has to invest US$11 billion from 2023 to 2030 to contribute to reaching this *** commentary aims to provide a critical perspective on the recommendations of the report from the National Science and Technology Commission’s 9th biennial conference in 2023 on science and technology,the sub-thematic technical report on clean energy,energy storage and green hydrogen in line with the SdGs in the Sri Lankan *** technical report provides insightful recommendations for Sri Lanka’s energy sector under three main sections:renewable energy,energy storage and green ***,it explores the potential of various renewable energy sources,energy storage systems and green hydrogen as sustainable solutions to address the country’s energy challenges while emphasizing the spillover effects of them,which could contribute to the enterprise’s job creation and uplift the economy.

关键词： renewable energy energy storage green hydrogen sustainable development goals Sri Lanka social economic environmental sustainable affordable

Uncovering Microstructure-Property Relationship in Ni-Alloyed Fe-Mn-Al-C Low-density Steel Treated by Hot-Rolling and Air-Cooling Process

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Acta Metallurgica Sinica(English Letters) 2024年第4期37卷 713-725页

作者： Xiaoliang Jia Guhui Gao Xiaolu Gui Chun Feng R.d.K.Misra Bingzhe Bai School of Mechanical Electronicand Control EngineeringBeijing Jiaotong UniversityBeijing100044China CNPC Tubular Goods Research Institute Xi’an710077China Laboratory for Excellence in Advanced Steel Research University of Texas at El PasoEl PasoTX79968-0521USA School of Material Science and Engineering Key Laboratory of Advanced Materials of Ministry of EducationTsinghua UniversityBeijing100084China

This paper focuses on the relationship between the microstructure and tensile properties of Fe-Mn-Al-C low-density high-strength steel processes by hot-rolling and air-cooling process. The microstructure analysis reveals that the combination of hot-rolling and air-cooling results in the formation of heterogeneous structures comprising different-sized γ and B_(2) phases in the low-density steel with the addition of nickel (Ni). The addition of Ni promotes the formation of the B_(2) phase and induces the pinning of B_(2) phase particles at the γ grain boundaries. This pinning effect effectively hinders the growth of the γ grains, leading to grain refinement. The tensile test results demonstrate that LdS-5Ni (low-density steel, LdS) exhibits excellent high strength and ductility combination, e.g., a tensile strength of 1535 MPa, yield strength of 1482 MPa, and elongation of 23.3%. These remarkable mechanical properties are primarily attributed to the combined strengthening contributions of grain refinement and duplex nano-sized second-phase precipitation hardening.

关键词： Low-density steel Microstructure B_(2)phase κ-Carbide Tensile properties

Charting the course to solid-state dual-ion batteries

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Carbon Energy 2024年第3期6卷 132-177页

作者： Habtom d.Asfaw Antonia Kotronia Nuria Garcia-Araez Kristina Edström daniel Brandell department of Chemistry Ångström LaboratoryUppsala UniversityUppsalaSweden department of Chemistry University of SouthamptonSouthamptonUK

An electrolyte destined for use in a dual-ion battery(dIB)must be stable at the inherently high potential required for anion intercalation in the graphite electrode,while also protecting the Al current collector from anodic dissolution.A higher salt concentration is needed in the electrolyte,in comparison to typical battery electrolytes,to maximize energy density,while ensuring acceptable ionic conductivity and operational *** recent years,studies have demonstrated that highly concentrated organic electrolytes,ionic liquids,gel polymer electrolytes(GPEs),ionogels,and water-in-salt electrolytes can potentially be used in *** can help reduce the use of solvents and thus lead to a substantial change in the Coulombic efficiency,energy density,and long-term cycle life of ***,GPEs are suited to manufacture compact dIB designs without separators by virtue of their mechanical strength and electrical *** this review,we highlight the latest advances in the application of different electrolytes in dIBs,with particular emphasis on GPEs.

关键词： anion intercalation concentrated electrolytes dual-ion battery graphite ionic liquids polymer electrolyte