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Ni-catalyzed highly regio- and stereo-selective diborylative cyclization of 1,6-enynes with diboron reagent

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Science China chemistry 2024年第3期67卷 981-989页

作者： Qitao Guan Zhen Shen Yiqiang Tian Genping Huang Chun Zhang Institute of Molecular Plus Tianjin Key Laboratory of Molecular Optoelectronic ScienceDepartment of ChemistrySchool of SciencesTianjin UniversityTianjin 300072China State Key Laboratory of Elemento-Organic chemistry Nankai UniversityTianjin 300071China

The Ni-catalyzed highly selective diborylative cyclization of 1,6-enynes with diboron reagent has been developed. When pinB-Bdan was used, multiple types of boron-containing functional groups could be installed into organic molecule with great chemoselectivity and regioselectivity though this reaction. Meanwhile, if B_2pai_2 was employed, the asymmetric diborylative cyclization could be well induced by using strategy of dynamic kinetic resolution. Importantly, the above reactions could afford desired product with 100% atomic economy, and could be compatible with different series of substituents. The studies of further transformation well illustrated that different type products could serve diverse synthetic strategy. Notably, the reaction mechanism was intensively studied by density functional theory(DFT) calculations, which could reveal the mechanism of regio- and enantio-selective control.

关键词： nickel-catalyzed organoboron cyclization regioselectivity enantioselectivity

Emerging perovskite materials for supercapacitors:Structure,synthesis,modification,advanced characterization,theoretical calculation and electrochemical performance

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Journal of Energy chemistry 2024年第2期89卷 41-70,I0003页

作者： Yuehua Qian Qingqing Ruan Mengda Xue Lingyun Chen department of Applied chemistry School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China

As a new generation electrode materials for energy storage,perovskites have attracted wide attention because of their unique crystal structure,reversible active sites,rich oxygen vacancies,and good *** this review,the design and engineering progress of perovskite materials for supercapacitors(SCs)in recent years is ***,the review will focus on four types of perovskites,perovskite oxides,halide perovskites,fluoride perovskites,and multi-perovskites,within the context of their intrinsic structure and corresponding electrochemical performance.A series of experimental variables,such as synthesis,crystal structure,and electrochemical reaction mechanism,will be carefully analyzed by combining various advanced characterization techniques and theoretical *** applications of these materials as electrodes are then featured for various ***,we look forward to the prospects and challenges of perovskite-type SCs electrodes,as well as the future research direction.

关键词： Perovskite Modification engineering Oxygen vacancy Theoretical calculation methodology Supercapacitor

Recent Advances in Mn,Fe,Co,and Ni-Catalyzed Organic Reactions

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CCS chemistry 2024年第3期6卷 537-584页

作者： Lu-Jie Li Yuli He Yunhui Yang Jun Guo Zhan Lu Congyang Wang Shaolin Zhu Shou-Fei Zhu College of chemistry Nankai UniversityTianjin 300071 School of chemistry and Chemical Engineering Nanjing UniversityNanjingJiangsu Province 210093 Institute of chemistry Chinese Academy of Sciences and University of Chinese Academy of SciencesBeijing 100190 department of chemistry Zhejiang UniversityHangzhouZhejiang Province 310058

This paper reviewed the recent research progress of organic reactions catalyzed by four typical earthabundant and 3d metal catalysts:Mn,Fe,Co,and Ni complexes and mainly focused on the reactions in which these 3d metal catalysts exhibited obvious advantages over other *** mechanism that makes these 3d metal catalysts show unusual properties is another focus of this *** outlook on 3d metal complexes-catalyzed organic reactions was also considered.

关键词： Earth-abundant metal catalysts sustainable organic synthesis structure-function relationships organometallic intermediates hydrocarbon transformations

Micro/nanoelectrode-based electrochemical methodology for single cell and organelle analysis

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Nano Research 2024年第1期17卷 196-206页

作者： Chuchu Xu De Yang Yuchan Wang Ruolin Liu Fan Wang Zhongqun Tian Keke Hu department of chemistry College of Chemistry&Chemical EngineeringXiamen UniversityXiamen 361005China

Cells are the basic unit of *** analysis of single cells/organelles is essential for uncovering the molecular mechanisms of physiological and pathological processes that are difficult to elucidate on a larger *** paper provides an overview of the commonly used fabrication methods for micro/nanoelectrodes applied in the investigations of single cells/organelles as well as the corresponding electrochemical measurements over the last four years including extracellular measurement,combination of extra and intracellular measurement,intracellular reactive oxygen species and reactive nitrogen species(ROS/RNS)measurement,and isolated organelles measurement.

关键词： single cell/organelle micro/nanoelectrode electrochemical measurement chemical transmitters

Nonalternant isomer of pentacene fusing two azulene units

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Chinese Chemical Letters 2024年第5期35卷 244-248页

作者： Bo Yu Pengchen Du Jianwen Guo Hanshen Xin Jianhua Zhang department of chemistry College of SciencesShanghai UniversityShanghai 200444China School of Microelectronics Shanghai UniversityShanghai 201800China

Azulene is a promising building block for creating innovative polycyclic aromatic hydrocarbons. This study involved the construction of three nonalternant isomers of pentacene by fusing two azulene units, named Az-PH1/2/3. Az-PH1 was initially developed through the rhodium(Ⅱ)-catalyzed cyclization of bis(N-tosylhydrazone)s. Intriguingly, Az-PH1 was also unexpectedly obtained during a nickel(0)-catalyzed one-step tandem reaction. We investigated the optical and electrochemical properties, aromaticity, and photo-oxidative stability of Az-PH1, comparing it with the well-known pentacene using density functional theory, electrochemical, and photophysical tests. Our results showed that the azulene-fusing strategy resulted in a molecule with narrow optical bandgaps(2.046 eV) and a long half-life time under ambient air conditions.

关键词： Azulene Isomer Polycyclic aromatic hydrocarbon Nickel(0)-catalyzed Photo-oxidative stability

A Golden Touch in the Design of Multifunctional Porphyrin Metallacages:Host-Guest chemistry for Drug-Target Interactions

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CCS chemistry 2024年第7期6卷 1662-1671页

作者： Tamara Rodríguez-Prieto Darren Wragg Nicole Heiduk Mihyun Park Nicole Strittmatter Roland A.Fischer Angela Casini Guillermo Moreno-Alcántar Chair of Medicinal and Bioinorganic chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Professorship for Analytical chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Chair of Inorganic and MetalOrganic chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Munich Data Science Institute(MDSI) Technical University of Munich85748 Garching b.München

The use of three-dimensional self-assembled metallacages(MCgs)as multimodal drug platforms holds great ***,the synthesis of MCgs with increased complexity and functionality is a great challenge since understanding of the interaction of MCgs with biological targets is still *** this context,this work reports on the integration of a gold(III)porphyrin scaffold into a prismatic MCg structure and explores its application for multimodal therapy of cancer in vitro,namely enabling both photodynamic therapy and *** experimental approaches with a state-of-the-art metadynamics theoretical study,we discovered that the gold cage shows unprecedented host-guest interaction-driven selective stabilization of guanine-quadruplex(G4)structures-validated anticancer drug targets-disclosing a new mechanism to pursue in the design of supramolecular drugs.

关键词： gold metallacages porphyrins G4stabili-zation host-guestchemistry anticanceragents

Interfacial oxidized Pd species dominate catalytic hydrogenation of polar unsaturated bonds

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Nano Research 2024年第1期17卷 228-234页

作者： Pengyao You Shaoqi Zhan Pengpeng Ruan Ruixuan Qin Shiguang Mo Yazhou Zhang Kunlong Liu Lansun Zheng Nanfeng Zheng State Key Laboratory for Physical chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China department of chemistry BMCUppsala UniversityBMC Box 576Uppsala S-75123Sweden department of chemistry University of OxfordOxford OX13QZUK

The determination of catalytically active sites is crucial for the design of efficient and stable catalysts toward desired ***,the complexity of supported noble metal catalysts has led to controversy over the locations of catalytically active sites(e.g.,metal,support,and metal/support interface).Here we develop a structurally controllable catalyst system(Pd/SBA-15)to reveal the catalytic active sites for the selective hydrogenation of ketones to alcohol using acetophenone hydrogenation as model *** investigations demonstrated that unsupported Pd nanocrystals have no catalytic activity for acetophenone ***,oxidized Pd species were catalytically highly active for acetophenone *** catalytic activity decreased with the decreased oxidation state of *** work provides insights into the hydrogenation mechanism of ketones but also other unsaturated compounds containing polar bonds,e.g.,nitrobenzene,N-benzylidene-benzylamine,and carbon dioxide.

关键词： oxidized Pd metal/oxide interface constant particle size Pd/SBA-15 acetophenone hydrogenation

High Temperature Iron Ethylene Polymerization Catalysts Bearing N,N,N'-2-(1-(2,4-Dibenzhydryl-6-fluorophenylimino)ethyl)-6-(1-(arylphenylimino)ethyl)pyridines

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Chinese Journal of Polymer Science 2024年第2期42卷 188-201,I0007页

作者： Chantsalnyam Bariashir Qiu-Yue Zhang Bayasgalan Ulambayar Gregory A.Solan Tong-Ling Liang Wen-Hua Sun Institute of chemistry and Chemical Technology Mongolian Academy of SciencesUlaanbaatar13330Mongolia Key Laboratory of Engineering Plastics and Beijing National Laboratory for Molecular Science Institute of ChemistryChinese Academy of SciencesBeijing100190China department of chemistry University of LeicesterUniversity RoadLeicesterLE17RHUK State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou730000China

The N,N,N'-ferrous chloride complexes,[2-{CMeN(2,4-(CHPh)_(2)-6-FC_(6)H_(2))}-6-(CMeNAr)C_(5)H_(3)N]FeCl_(2)(Ar=2,6-Me_(2)C_(6)H_(3) Fe1,2,6-Et_(2)C_(6)H_(3)Fe2,2,6-^(i)Pr_(2)C_(6)H_(3) Fe3,2,4,6-Me_(3)C_(6)H_(2) Fe4 and 2,6-Et_(2)-4-MeC_(6)H_(2) Fe5),each possessing one N-2,4-dibenzhydryl-6-fluorophenyl group,were readily synthesized from their respective unsymmetrical bis(imino)pyridines,*** identification of Fe2 highlighted the variation in the steric properties provided by the dissimilar N-aryl *** pre-treatment with either MAO or MMAO,complexes Fe1-Fe5 all displayed,at an operating temperature of 80℃,high activities for ethylene polymerization with levels falling in the order:Fe4> Fe1> Fe5> Fe2> ***,Fe4/MAO displayed the highest activity of 1.94×10^(7) g_(PE)·mol_(Fe)^(-1)·h^(-1) of the study with only a modest loss in performance at 90℃.Generally,the resulting polyethylenes were highly linear(T_(m) range:122-132℃),narrowly disperse and of low molecular weight(M_(w) range:6.73-46.04kg·mol^(-1)),with the most sterically hindered Fe3 forming the highest molecular weight polymer of the ***-group analysis by ^(1)H-and ^(13)CNMR spectroscopy revealed saturated alkyl(n-propyl and i-propyl) and unsaturated vinyl chain ends indicative of the role of both β-H elimination and chain transfer to aluminum as termination *** comparison with previou sly reported iron precatalysts with similar tridentate ligand skeletons,it is evident that the introduction of a large benzhydryl group in combination with a fluorine as the ortho-substituents of one N-aryl group has the effect of enhancing thermal stability of the iron polymerization catalyst whilst maintaining appreciable polymer molecular weight.

关键词： Iron catalyst Ethylene polymerization Linear polyethylene Fluoride effect Thermal stability

Luminescent metal-halide perovskites:fundamentals,synthesis,and light-emitting devices

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Science China chemistry 2024年第6期67卷 1776-1838页

作者： Kang Wang Jeong Hui Kim Jie Yang Xiaoke Liu Yixuan Dou Yuxuan Li Weijian Tao Haiyun Dong Haiming Zhu Kaifeng Wu Li Na Quan Feng Gao Jianpu Wang Letian Dou Yong Sheng Zhao Beijing National Laboratory for Molecular sciences(BNLMS) Key Laboratory of PhotochemistryInstitute of ChemistryChinese Academy of SciencesBeijing100190China Davidson School of Chemical Engineering Purdue UniversityWest LafayetteIN47907USA School of Chemical sciences University of Chinese Academy of SciencesBeijing100049China Key Laboratory of Flexible Electronics(KLOFE) Institute of Advanced Materials(IAM)&School of Flexible Electronics(Future Technologies)Nanjing Tech University(NanjingTech)Nanjing211816China department of Physics Linköping UniversityLinköping58183Sweden department of chemistry Virginia TechBlacksburgVA24060USA State Key Laboratory of Molecular Reaction Dynamics Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China department of chemistry Zhejiang UniversityHangzhou310058China Changzhou University Changzhou213164China department of chemistry Purdue UniversityWest LafayetteIN47907USA

Metal-halide perovskites have garnered considerable research attention as highly efficient light emitters in recent years due to their outstanding optoelectronic properties with remarkable tunability and excellent solution *** advancements have been achieved in the development of novel halide perovskites,and the exploitations of these materials in lightemitting *** review comprehensively outlines recent breakthroughs in metal-halide perovskites,encompassing the rational design of perovskite materials with tunable light emission properties,the controllable growth of single crystal for a deeper understanding of their structure-property relationships,as well as the fundamental insights into the photophysics and carrier dynamics in perovskite ***,it provides an overview of recent applications of perovskite materials in high-performance light-emitting diodes(LEDs)and lasers.

关键词： metal-halide perovskites perovskite luminescent materials perovskite synthesis excited-state processes perovskite light-emitting diodes perovskite lasers

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