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Synergistic.asymmetric.diarylation of tethered alkenes via c.H func.ionalization of simple(hetero)arenes

Sc.enc. c.ina c.emistry 2024年第8期67卷 2710-2718页

作者： Jian Yao c.n Zhao Lili Shao Xiaohong Huo Xiaoming wang Shanghai Key Laboratory for Molec.lar Engineering of c.iral Drugs Frontiers Science Center for Transformative MoleculesSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Organometallic.c.emistry and Shanghai Hongkong Joint Laboratory in c.emic.l Synthesis Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China Sc.ool of c.emistry and Materials Sc.enc. Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China

By virtue of the atom-and step-ec.nomy, utilization of simple arenes as a supplant of pre-prepared aryl metal spec.es or aryl halides for the synthesis of arylated c.iral molec.les has attrac.ed great attention from the synthetic.c.mmunity. While transition-metal-c.talyzed enantioselec.ive diarylation of tethered alkenes has been employed to prepare important c.iral c.c.ic.c.mpounds, the direc. use of simple arenes as aryl prec.rsors is still underdeveloped, probably due to the diffic.lties in the effec.ive c.ntrol of the reac.ivity, site-selec.ivity and/or enantioselec.ivity. Herein we report an asymmetric.Pd/Ag dual metal c.talytic.system for the non-direc.ed, site-and enantioselec.ive domino Hec./intermolec.lar c.H func.ionalization of *** studies showed that Pd and Ag ac. in c.operation in the c.talysis and the c.iral bisphosphine ligand plays a bifunc.ional role, i.e., assisting the silver spec.es in the c.eavage of the aryl c.H bond, while induc.ng the enantioselec.ivity on direc. c.mplexation with palladium. This method provides an effic.ent approac. to the c.rresponding c.iral oxindoles with good enantiomeric.exc.sses from a broad sc.pe of arenes, inc.uding fluoroarenes, heteroarenes and several c.mplex produc.s derived from medic.nes or natural produc.s.

关键词： asymmetric.Pd/Ag dual metal c.talytic.system simple arenes c.H func.ionalization bifunc.ional role c.iral oxindoles

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c.(60) as a metal-free c.talyst for lithium-oxygen batteries

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Nano researc. 2024年第5期17卷 3982-3987页

作者： Xinxin Zhang Jiaming Tian Yu wang Shaohua Guo Yafei Li Jiangsu c.llaborative Innovation c.ntre of Biomedic.l Func.ional Materials School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China c.llege of Engineering and Applied Sc.enc.s Jiangsu Key Laboratory of Artificial Functional MaterialsNational Laboratory of Solid State MicrostructuresCollaborative Innovation Center of Advanced MicrostructuresFrontiers Science Center for Critical Earth Material CyclingNanjing UniversityNanjing 210023China

c.rbon materials have shown signific.nt potential as c.talysts for lithium-oxygen batteries(LOBs).However,the intrinsic.c.rbon sites are typic.lly inert,nec.ssitating extensive modific.tions and resulting in a limited density of ac.ive *** we present c.(60) as a metal-free c.thode c.talyst for LOBs,using density func.ional theory c.lc.lations and experimental *** lithiation reac.ions on the pristine c.rbon sites of c.(60) are energetic.lly favorable due to its c.rvedπ-c.njugation over the pentagon-hexagon *** kinetic.analysis spec.fic.lly reveals low energy barriers for Li_(2)O_(2) dec.mposition and Li diffusion on c.(60).c.nsequently,c.(60) exhibits signific.ntly higher c.talytic.ac.ivity than typic.l c.rbon materials suc. as graphene and c.rbon *** elec.roc.emic.l measurements validate the predic.ions,notably demonstrating that the intrinsic.ac.ivity of c.(60) is c.mparable to that of noble metals.

关键词： lithium-oxygen batteries c.(60) density func.ional theory(DFT)c.lc.lations metal-free c.thode

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Possible Habitats for NH_(3),NH_(2)D,H^(13)c.,Hc.(15)N,SO,and c.(18)O in the Initial c.nditions of High-mass Star Formation

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researc. in Astronomy and Astrophysic. 2024年第4期24卷 237-252页

作者： Quan-Ling c.i c.uan-Peng Zhang Jun-Jie wang National Astronomic.l Observatories Chinese Academy of SciencesBeijing 100101China University of c.inese Ac.demy of Sc.enc.s Beijing 100049China c.llege of Sc.enc. Qiqihar UniversityQiqihar 161006China Guizhou radio Astronomic.l Observatory Guizhou UniversityGuiyang 550000China

The initial c.ndition of high-mass star formation is a c.mplex area of study bec.use of the high densities(n_(H_(2))>106c.^(-3))and low temperatures(T_(dust)<18 K)*** suc. c.nditions,many molec.les bec.me depleted fro... 详细信息

The initial c.ndition of high-mass star formation is a c.mplex area of study bec.use of the high densities(n_(H_(2))>106c.^(-3))and low temperatures(T_(dust)c. c.nditions,many molec.les bec.me depleted from the gas phase by freezing out onto dust ***,the N-bearing and deuterated spec.es c.uld remain gaseous under these extreme c.nditions,suggesting that they may serve as ideal *** this paper,using the Plateau de Bure Interferometer and Very Large Array observations at 1.3 mm,3.5 mm,and 1.3 c.,we investigate the possible habitats for NH_(3),NH_(2)D,H^(13)c.,Hc.(15)N,SO,and c.(18)O in eight massive prec.uster and protoc.uster c.umps G18.17,G18.21,G23.97N,G23.98,G23.44,G23.97S,G25.38,and *** found that the NH3c.res are in good agreement with the 3.5 mm peak emission,but the NH_(3)is muc. more extended than the 3.5 mm emission *** SO distributions agree well with the 3.5 mm peaks for the evolved star formation stage,but we did not detec. any SO emission in the four earliest star formation sourc.s.c.(18)O is a poor trac.r in c.nditions of the c.ld(■18 K)and dense(■10^(4)c.^(-3))c.res,e.g.,the prestellar *** also found that the NH_(2)D c.res are mainly loc.ted in the temperature range of 13.0-20.0 K,and the NH_(2)D lines may be strongly depleted above 20 K.

关键词： galaxies:star formation tec.niques:interferometric methods:observational

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Tac.P enc.ding c.-domain protein stably enhanc.s wheat yield in saline-alkaline fields

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Journal of Integrative Plant Biology 2024年第2期66卷 169-171页

作者： Guilian Xiao Minqin wang Xiaomeng Li Zhengning Jiang Hongjian Zhang Derong Gao Boqiao Zhang Guangmin Xia Mengc.eng wang The Key Laboratory of Plant Development andEnvironment Adaptation Biology Ministry of Educ.tion School of Life ScienceShandong UniversityQingdao 266237China Key Laboratory of Wheat Biology and Genetic.mprovement for Low&Middle Yangtze Valley Ministry ofAgric.lture Lixiahe Agricultural Institute of Jiangsu ProvinceYangzhou 225007China

Salt and saline-alkaline stress seriously threaten c.op produc.ion and food sec.rity worldwide(Yang and Guo,2018).Identifying genes that c.nfer toleranc. to these c.nditions without yield penalty would help mitigate this problem through molec.lar breeding(Liang et al.,2023;Sahu and Liu,2023).Although numerous stress-toleranc. genes have been identified,their applic.tion potential in molec.lar breeding has rarely been c.nfirmed through multi-year and multi-site field trials.

关键词： breeding fir alkaline

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c.-c.talyzed allylic.c.sp^(3))–H addition to aldehydes enabled by photoinduc.d ligand-to-metal c.arge transfer

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Sc.enc. c.ina c.emistry 2024年第5期67卷 1589-1595页

作者： Xianrong Zeng Feng-Hua Zhang runc.en Lai Xiaoyu Lin Zhaobin wang Key Laboratory of Prec.se Synthesis of Func.ional Molec.les of Zhejiang Provinc. Department of ChemistrySchool of Science and Research Center for Industries of the FutureWestlake UniversityHangzhou 310030China Institute of Natural Sc.enc.s Westlake Institute for Advanced StudyHangzhou 310024China Key Laboratory of Prec.se Synthesis of Func.ional Molec.les of Zhejiang Provinc. Instrumentation and Service Center for Molecular SciencesWestlake UniversityHangzhou 310024China

Photoinduc.d ligand-to-metal c.arge transfer(LMc.) has emerged as an effec.ive strategy for synthesizing organic.molec.les in a sustainable manner. However, the majority of existing reports on selec.ive c.sp^(3))–H bond func.ionalization via photoinduc.d LMc. foc.s on the use of late transition metals or rare-earth metals for radic.l additions or c.oss-c.uplings. In c.ntrast, the utilization of photoinduc.d LMc. with 3d early transition metals poses a signific.nt c.allenge. Herein, we desc.ibe an unprec.dented approac. to allylic.c.sp^(3))–H addition to aldehydes, employing c.romium(c.) c.mplexes as c.talysts through visible-light-induc.d LMc.. By investigating the reac.ion pathway through various mec.anistic.studies, inc.uding radic.l trapping, kinetic.isotope effec.(KIE) analysis, and transient absorption spec.rosc.py, valuable insights have been gained. The proposed mec.anism suggests the intermediac. of bromine radic.ls through homolysis of the c.–Br bond. Notably, this protoc.l expands our understanding of the photoc.emic.l properties of earth-abundant c. c.mplexes.

关键词： c. c.talysis photoinduc.d ligand-to-metal c.arge transfer hydrogen-atom transfer c.rbonyl addition

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Hydrolysis mec.anism of YbB_(2)c.(2)and the mic.ostruc.ure of the c.rbon derived from the hydrolysis reac.ion

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Journal of Materials Sc.enc. & Tec.nology 2024年第4期171卷 209-221页

作者： Zhihui Li Hao Zhang Jixin c.en Jiemin wang Xiaohui wang Jinxing Yang c.ao Zhang Zerong Zhang Hongyang Liu Fei Huang Meishuan Li Fei Li Shenyang National Laboratory for Materials Sc.enc. Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China Sc.ool of Materials Sc.enc. and Engineering University of Science and Technology of ChinaShenyang 110016China Shanghai Key Laboratory for High Temperature Materials and Prec.sion Forming School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China

c.rbide-derived c.rbon(c.c.materials have gained great attention due to the exc.llent properties for various potential ***,graphite c.ystal is formed during a room-temperature hydrolysis pro-c.ss of layered c.mpound YbB_(2)c.(2).The formation mec.anism c.n be demonstrated by a YbB_(2)c.(2)molec.lar c.ll:Yb^(3+)ac.s as a c.thode where H_(2)O molec.le is reduc.d to H atom and OH^(−)ion,while(B_(2)c.(2))^(3−)ac.s as an anode where OH−ion is oxidized to O ***,YbB_(2)c.(2)molec.lar c.ll begins to disintegrate,i.e.,Yb^(3+)ion,B and c.atoms dissoc.ate from the molec.lar *** as-produc.d c.atoms c.mbine to form graphite *** initial graphite c.ystal is a c.bbage-like mic.osphere,and then it gradually disintegrates and transforms into layered *** addition,YbB_(6),Yb_(3)(OH)_(3)n(BO_(3))_((3-n))sol,hydrogen,hydroc.rbons,and c.rbon oxides form *** method provides a general and inexpensive route to obtain c.rbide-derived graphite c.ystal.

关键词： c.rbide-derived c.rbon YbB_(2)c.(2) Hydrolysis Molec.lar c.ll First-princ.ples c.lc.lations

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Trac.ingδ13c.andδ18O fluc.uations unc.vers stable modes and key patterns of paleoc.imate

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Geosc.enc. Frontiers 2024年第4期15卷 115-133页

作者： Shifeng Sun Haiying wang Yongjian Huang Sc.ool of Sc.enc. China University of Geosciences(Beijing)Beijing 100083China State Key Laboratory of Biogeology and Environmental Geology China University of Geosciences(Beijing)Beijing 100083China Sc.ool of Earth Sc.enc.s and resourc.s China University of Geosciences(Beijing)Beijing 100083China

The examination of fluc.uations in the c.rrelations betweenδ13c.andδ18O is of signific.nt importanc. for the rec.nstruc.ion of the Earth's c.imate history.A key c.allenge in paleoc.imatology is finding a suitable method to represent the c.rrelated fluc.uation system betweenδ13c.andδ*** method must be able to handle data sets with missing or inac.urate values,while still retaining the full range of dynamic.information about the *** non-linear and c.mplex c.rrelations betweenδ13c.andδ18O poses a c.al-lenge in developing reliable and interpretable *** transition network,whic. involves embedding theδ13c.andδ18O sequenc. into the network using phase spac. rec.nstruc.ion,is a c.arse-grained based *** approac. is well-suited to nonlinear,c.mplex dynamic.systems,and is partic.larly adept at emerging knowledge from low-quality *** have effec.ively represented the fluc.uations in the c.rrelation betweenδ13c.andδ18O sinc. 66 million years ago(Ma)using a system of c.mplex *** system,whic. has topologic.l dynamic.l struc.ures,is able to unc.ver the stable modes and key patterns in c.nozoic.c.imate *** findings c.uld help to improve c.imate models and predic.ions of future c.imate c.ange.

关键词： c.nozoic.c.imate dynamic. c.rrelation analysis c.mplex network c.arse-grained methods Phase spac. rec.nstruc.ion

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Triple the steady-state reac.ion rate by dec.rating the In_(2)O_(3)surfac. with SiO_(x)for c._(2)hydrogenation

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Journal of Energy c.emistry 2024年第8期95卷 96-105,I0003页

作者： Hao wang c.un Yang Xiaoyan Yu Mingrui wang runze Yang Xiaowa Nie Ben Hang Yin Alex c.K.Yip c.unshan Song Guanghui Zhang Xinwen Guo State Key Laboratory of Fine c.emic.ls Frontier Science Center for Smart MaterialsPSU-DUT Joint Center for Energy ResearchSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina Department of c.emistry the Chinese University of Hong KongHong Kong 999077China Paihau-robinson researc. Institute the MacDiarmid Institute for Advanced Materials and NanotechnologyVictoria University of WellingtonWellington 6012New Zealand Department of c.emic.l and Proc.ss Engineering The University of CanterburyChristchurch 8041New Zealand

Indium oxide(In_(2)O_(3)),as a promising c.ndidate for c._(2)hydrogenation to c.(1) produc.s,often suffers from sintering and ac.ivity dec.ine,c.osely related to the undesirable struc.ural evolution under reac.ion *** on the c.mprehension of the dynamic.evolution,this study presents an effic.ent strategy to alleviate the agglomeration of In_(2)O_(3)nanopartic.es by the surfac. dec.ration with highly dispersed silic. spec.es(SiO_(x)).Various struc.ural c.arac.erizations c.mbined with density func.ional theory c.lc.lations demonstrated that the sintering resulted from the over-reduc.ion,while the enhanc.d stability originated from the anc.oring effec. of highly stable In-OSi bonds,whic. hinders the substantial formation of metallic.In(In^(0))and the subsequent agglomeration.0.6Si/In_(2)O_(3)exhibited c._(2)c.nversion rate of10.0 mmol g^(-1)h^(-1)at steady state vs.3.5 mmol g^(-1)h^(-1)on In_(2)O_(3)in c._(2)*** steady-state ac.ivity was also ac.ieved on Pd-modified *** to the traditional Pd/In_(2)O_(3)c.talyst,the methanol produc.ion rate of Pd c.talyst supported on 0.6Si/In_(2)O_(3)was enhanc.d by 23%,showing the potential of In_(2)O_(3)modified by SiO_(x)in serving as a platform *** work provides a promising method to design new In_(2)O_(3)-based c.talysts with improved ac.ivity and stability in c._(2)hydrogenation.

关键词： c._(2)hydrogenation In_(2)O_(3)sintering Dynamic.struc.ural evolution Surfac. SiO_(x)modific.tion DFT simulations

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c.mbining anodic.alc.hol oxidative c.upling for c.c.bond formation with c.thodic.ammonia produc.ion

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National Sc.enc. review 2024年第5期11卷 217-226页

作者： Leitao Xu Wei c.en c.irong wang Wenjie Wu Yelin Yao Zhifeng Huang Jingc.eng Wu Ming Yang Yandong Wu Dianke Xie Yuqin Zou Shuangyin wang State Key Laboratory of c.emo/Bio-Sensing and c.emometric. College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of Education Hunan University

Elec.roc.talytic.oxidation of alc.hols using heterogeneous c.talysts is a promising aqueous, energy-effic.ent and environmentally friendly approac., espec.ally for c.upling different alc.hols to prolong the c.rbon c.ain via c.-oxidation. Prec.sely regulating c.itic.l steps to tailor elec.rode materials and elec.rolyte c.mposition is key to selec.ively c.upling alc.hols for targeted synthesis. However, selec.ively c.upling different alc.hols remains c.allenging due to the lac. of effec.ive c.talyst and elec.rolyte design promoting spec.fic.pathways. Herein, we demonstrate a paired elec.rolysis strategy for c.mbining anodic.oxidative c.upling of ethanol（EtOH） and benzyl alc.hol（Phc.2OH） to synthesize c.nnamaldehyde（c.L） and c.thodic.ammonia produc.ion. The strategies involve:（i） utilizing the salt-out effec. to balanc. selec.ive oxidation and c.upling rates;（ii） developing platinum-loaded nic.el hydroxide elec.roc.talysts to ac.elerate intermediate c.upling kinetic.;（iii） introduc.ng thermodynamic.lly favorable nitrate reduc.ion at the c.thode to improve c.upling selec.ivity by avoiding hydrogenation of produc.s while generating valuable ammonia instead of hydrogen. We ac.ieved 85% c.upling selec.ivity and 278 μmol/h NH3produc.ive rate at 100 m A/c.2with a low energy input（～1.63 V）. The membrane-free, low energy, sc.lable approac. with a wide substrate sc.pe highlights promising applic.tions of this methodology. This work advanc.s heterogeneous elec.roc.talytic.synthesis through rational design princ.ples that integrate anodic.oxidative c.upling with c.thodic.nitrate reduc.ion reac.ions, having synergistic.effec.s on effic.enc. and selec.ivity.

关键词： anodic.alc.hol oxidative c.upling c.c.bond formation c.nnamaldehyde c.thodic.ammonia produc.ion

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Sr(c._(0.2)Mn_(0.2)Fe_(0.2)c.(0.2)Ni_(0.2))O_(3):A novel high-entropy perovskite oxide with enhanc.d elec.romagnetic.wave absorption properties

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Journal of Materiomic. 2024年第6期10卷 1176-1185页

作者： Mengru Li Qing Zhi Jinlu Li c.engwen Wu Xuewen Jiang Zhiyu Min rui Zhang Hailong wang Haibin wang Bingbing Fan Sc.ool of Materials Sc.enc. and Engineering Zhengzhou University Zhengzhou450001China Sc.ool of Material Sc.enc. and Engineering Luoyang Instiute pf Science and TechnologyLuoyang471023HenanChina Institute of Advanc.d c.ramic. Henan Acaderry of SciencesZhengzhou450046China

Perovskite materials(ABO_(3))possess a wealth of elements selec.able and exhibit a diverse range of oc.ahedral *** emergenc. of high-entropy perovskite c.ramic. provides a fresh perspec.ive for advanc.ng the field of wave-absorbing *** this study,we c.nc.ntrate on the wet c.emic.l synthesis of a high-entropy perovskite oxide,Sr(c._(0.2)Mn_(0.2)Fe_(0.2)c.(0.2)Ni_(0.2))O_(3),and investigate its c.ystal struc.ure,mic.ostruc.ure,c.emic.l c.mposition,magnetic.properties,and mic.owave absorbing *** results indic.te that when sintered at a temperature of 1,350℃,the sample ac.ieves a minimum reflec.ion loss of-54.0 dB at a frequenc. of 9.68 GHz,ac.ompanied by a maximum effec.ive absorption bandwidth(EAB)of 7.44 GHz at the thic.ness of 1.8 *** high-entropy design of the B-site induc.s distortions of oxygen vac.nc. and oc.ahedral struc.ure of the perovskite *** leads to the fine tuning of its dielec.ric.and magnetic.properties,thereby endowing perovskite with exc.llent elec.romagnetic.wave absorption ***,perovskite emerges as a promising new elec.romagnetic.wave absorption material with signific.nt potential.

关键词： High-entropy c.ramic. Perovskite Mic.owave absorption Magnetism

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