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Selective synthesis and physical properties of a bismacrocycle:Cycloparaphenylene-pillar[5]arene

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Chinese Chemical Letters 2024年第3期35卷 273-276页

作者： Yu Zhou Guilin Zhuang Pingwu Du key laboratory of Precision and Intelligent Chemistry Hefei National Laboratory for Physical Sciences at the MicroscaleCAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China College of Chemical Engineering Zhejiang University of TechnologyHangzhou 310032China

Macrocyclic materials have attracted much attention due to their particular chemical and physical *** we report the precise synthesis and characterization of a new bismacrocycle structure base on cycloparaphenylene(CPP)and pillar[5]arene,named cycloparaphenylene-pillar[5]arenes(CPPn[5]).The bismacrocycle was fully characterized by NMR and *** photophysical properties of CPPn[5]were investigated by UV–vis,and the maximum absorption peak was located at 331 nm,which was consistent with density functional theory(DFT)*** fluorescence spectrum was further studied and the emission peak was maximized at 458 *** computational results indicate the strain energy of CPPn[5]is 27.80 kcal/mol and the HOMO-LUMO gap is 3.39 eV Notably,CPPn[5]showed interesting supramolecular properties.

关键词： Pillararene Cycloparaphenylene Bismacrocycles Supramolecular chemistry

Surface evolution of thermoelectric material KCu_(4)Se_(3) explored by scanning tunneling microscopy

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Chinese Physics B 2024年第8期33卷 422-427页

作者：夏玉敏马妮蔡德胜刘宇舟谷易通于淦霍思宇庞文慧肖翀秦胜勇 International Center for Quantum Design of Functional materials(ICQD) Hefei National Laboratory for Physical Sciences at Microscale(HFNL)University of Science and Technology of ChinaHefei 230026China cas key laboratory of Strong Coupled Quantum Matter Physics Department of PhysicsUniversity of Science and Technology of ChinaHefei 230026China hefei national laboratory for physical sciences at the microscale University of Science and Technology of ChinaHefei 230026China Institute of energy Hefei Comprehensive National Science CenterHefei 230031China Dalian national laboratory for Clean energy Chinese Academy of Sciences(CAS)Dalian 116023China hefei national laboratory University of Science and Technology of ChinaHefei 230088China

Novel two-dimensional thermoelectric materials have attracted significant attention in the field of thermoelectric due to their low lattice thermal conductivity.A comprehensive understanding of their microscopic structures is crucial for driving further the optimization of materials properties and developing novel functional ***,by using in situ scanning tunneling microscopy,we report the atomic layer evolution and surface reconstruction on the cleaved thermoelectric material KCu_(4)Se_(3) for the first *** clearly revealed each atomic layer,including the naturally cleaved K atomic layer,the intermediate Se^(2-)atomic layer,and the Se^(-)atomic layer that emerges in the thermodynamic-stable *** from the maj ority of studies that predominantly concentrate on macroscopic measurements of the charge transport,our results reveal the coexistence of potassium disorder and complex reconstructed patterns of selenium,which potentially influences charge carrier and lattice *** results provide direct insight into the surface microstructures and evolution of KCu_(4)Se_(3),and shed useful light on designing functional materials with superior performance.

关键词： thermoelectric KCu_(4)Se_(3) scanning tunneling microscopy(STM) evolution

Photoinduced Dehalocyclization to Access Oxindoles Using Formate as a Reductant

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Chinese Journal of Chemistry 2024年第11期42卷 1203-1208页

作者： Wei Ge Jia-Xin Wang Ming-Chen Fu Yao Fu hefei national Research Center for physical sciences at the microscale iChEMCAS Key Laboratory of Urban Pollutant ConversionAnhui Province Key Laboratory of Biomass Clean EnergyUniversity of Science and Technology of ChinaHefeiAnhui230026 China Anhui Province key laboratory of Value-Added Catalytic conversion and Reaction Engineering Hefei University of TechnologyHefeiAnhui230009 China

Herein,we report an efficient and practical protocol for the photoinduced dehalocyclization of ortho-halophenylacrylamides with formate by the engagement of a CO_(2) radical anion to access substituted *** method proceeds smoothly under mild conditions and exhibits a wide range of substrate as well as remarkable functional group compatibility.

关键词： Formate CO_(2)Radical ions Oxindole Photocatalysts Cyclization Organohalides

Cobalt-catalyzed reductive alkynylation to construct C(sp)-C(sp^(3))and C(sp)-C(sp^(2))bonds

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Chinese Chemical Letters 2024年第7期35卷 253-258页

作者： Lei Wan Yizhou Tong Xi Lu Yao Fu hefei national Research Center for physical sciences at the microscale iChEMCAS Key Laboratory of Urban Pollutant ConversionAnhui Province Key Laboratory of Biomass Clean EnergyUniversity of Science and Technology of ChinaHefei 230026China key laboratory of Precision and Intelligent Chemistry School of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei 230026China

Transition-metal-catalyzed cross-electrophile coupling has emerged as a reliable method for constructing carbon–carbon ***,we report a general method,cobalt-catalyzed reductive alkynylation,to construct C(sp)-C(sp^(3))and C(sp)-C(sp^(2))*** presented reaction has a broad substrate scope,enabling the efficient cross-electrophile coupling between alkynyl bromides with alkyl halides and aryl or alkenyl(pseudo)*** presented reaction is conducted under mild conditions,tolerating many functional groups,thus suitable for the modification and synthesis of biologically active molecules.

关键词： Cobalt-catalysis Cross-electrophile coupling Carbon-carbon bond formation Reductive alkynylation Alkyne synthesis

High-rate CH_(4)-to-C_(2)H_(6) photoconversion enabled by Au/ZnO porous nanosheets under oxygen-free system

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Science China Chemistry 2024年第3期67卷 869-875页

作者： Kai Zheng Xiaojing Zhang Jun Hu Chengbin Xu Juncheng Zhu Jing Li Mingyu Wu Shan Zhu Li Li Shumin Wang Yumei Lv Xin He Ming Zuo Chengyuan Liu Yang Pan Junfa Zhu Yongfu Sun Yi Xie hefei national laboratory for physical sciences at microscale National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China key laboratory of Photochemical conversion and Optoelectronic materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China State Grid Anhui Electric Power Research Institute Hefei 230601China

Photocatalytic CH_(4) coupling into high-valued C_(2)H_(6) is highly attractive,whereas the photosynthetic rate,especially under oxygen-free system,is still ***,we designed the negatively charged metal supported on metal oxide nanosheets to activate the inert C-H bond in CH_(4)and hence accelerate CH_(4) coupling *** an example,the synthetic Au/ZnO porous nanosheets exhibit the C_(2)H_(6) photosynthetic rate of 1,121.6μmol g^(-1)_(cat)h^(-1)and the CH_(4) conversion rate of 2,374.6μmol g^(-1)_(cat)h^(-1) under oxygen-free system,2 orders of magnitude higher than those of previously reported *** virtue of several in situ spectroscopic techniques,it is established that the generated Au^(δ-)and O^-species together polarized the C-H bond,while the Au^(δ-)and O^-species jointly stabilized the CH_(3) intermediates,which favored the coupling of CH_(3) intermediate to photosynthesize C_(2)H_(6) instead of overoxidation into CO_(x).Thus,the design of dual active species is beneficial for achieving high-efficient CH_(4)-to-C_(2)H_(6) photoconversion.

关键词： dual surface-active sites selective methane coupling ethane room temperature

Recent Advances in Cobalt-Catalyzed Regio-or Stereoselective Hydrofunctionalization of Alkenes and Alkynes

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CCS Chemistry 2024年第5期6卷 1130-1156页

作者： Yan Li Xi Lu Yao Fu hefei national Research Center for physical sciences at the microscale CAS Key Laboratory of Urban Pollutant ConversionAnhui Province Key Laboratory of Biomass Clean EnergyUniversity of Science and Technology of ChinaHefei 230026 key laboratory of Precision and Intelligent Chemistry Department of Applied ChemistrySchool of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei 230026

Hydrofunctionalization of alkenes and alkynes is increasingly important in preparing and modifying carbon-centered organic molecules such as pharmaceuticals,agrochemicals,andmaterial *** development of transition-metal-catalysts has revolutionized the hydrofunctionalization of unsaturated hydrocarbons,greatly improving the synthetic efficiency and selectivity of these *** recent years,notable progress has been achieved in low-cost metal-catalyzed alkene and alkyne hydrofunctionalization reactions following the utilization of traditional precious metal catalysts,including palladium,platinum,and ***-abundant cobalt catalysts,which are low in toxicity and exhibit unique reactivity and selectivity,are widely implemented in academic and industrial *** this review,we highlight recent examples of cobalt-catalyzed hydrofunctionalization of alkenes and alkynes to provide an overview of hydrofunctionalization methods,particularly hydroalkylation *** reactions greatly expand the scope and utility of cobalt-catalyzed couplings of carbon—carbon *** also highlight the mechanistic considerations and selective determinants *** hope our discussion will be informative for future developments in cobalt catalysis and hydrofunctionalization reactions.

关键词： hydrofunctionalization cobalt-catalysis alkene alkyne regioselectivity stereoselectivity

Larger in-plane upper critical field and superconducting diode effect observed in topological superconductor candidate InNbS_(2)nanoribbons

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Nano Research 2024年第7期17卷 6686-6694页

作者： Bo Zheng Changlong Wang Xukun Feng Xiaozhen Sun Shasha Wang Dawei Qiu Xiang Ma Ruimin Li Guanglei Cheng Lan Wang Yalin Lu Peng Li Shengyuan A.Yang Bin Xiang Department of materials Science and Engineering CAS Key Lab of Materials for Energy ConversionAnhui Laboratory of Advanced Photon Science and TechnologyUniversity of Science and Technology of ChinaHefei 230026China Research laboratory for Quantum materials Singapore University of Technology and DesignSingapore 487372Singapore School of Microelectronics University of Science and Technology of ChinaHefei 230052China cas key laboratory of microscale Magnetic Resonance and School of physical sciences University of Science and Technology of ChinaHefei 230026China Lab of Low Dimensional Magnetism and Spintronic Devices School of PhysicsHefei University of TechnologyHefei 230009China Research laboratory for Quantum materials IAPMEUniversity of MacaoMacaoChina

Recently,the coexistence of topology and superconductivity has garnered considerable ***,the dimensionality of these materials is crucial for the realization of topological quantum ***,the naturally grown materials,especially with one-dimensional feature that exhibits the coexistence of topology and superconductivity,still face challenges in terms of experimental realization and scalability,which hinders the fundamental research development and the potential to revolutionize quantum ***,we report the first experimental synthesis of quasi-one-dimensional InNbS_(2)nanoribbons that exhibit the coexistence of topological order and superconductivity via a chemical vapor transport ***,the inplane upper critical field of InNbS_(2)nanoribbons exceeds the Pauli paramagnetic limit by more than 2.2 times,which can be attributed to the enhanced spin-orbit coupling and the weakened interlayer interaction between the NbS_(2)layers induced by the insertion of In atoms,making InNbS_(2)exhibit spin-momentum locking similar to that of monolayer NbS_(2).Moreover,for the first time,we report the superconducting diode effect in a quasi-one-dimensional superconductor system without any inherent geometric *** measured maximum efficiency is manifested as 14%,observed atμ0H≈±60 mT,and we propose that the superconducting diode effect can potentially be attributed to the presence of the nontrivial topological *** work provides a platform for studying exotic phenomena in condensed matter physics and potential applications in quantum computing and quantum information processing.

关键词： topological order superconductivity nanoribbon superconducting anisotropy superconducting diode

Volume-complementary bipolar layered oxide enables stable symmetric sodium-ion batteries

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Nano Research 2024年第5期17卷 4125-4133页

作者： Bo Peng Feng Wang Nazir Ahmad Lai Yu Shenghua Chen Genqiang Zhang School of materials Science and Engineering Key Laboratory of Efficient Conversion and Solid-state Storage of Hydrogen and Electricity of Anhui ProvinceAnhui University of TechnologyMa’anshan 243002China hefei national Research Center for physical sciences at the microscale Chinese Academy of Sciences(CAS)Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China national Innovation Platform(Center)for Industry-Education Integration of energy Storage Technology School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an 710049China

The commercialization of sodium-ion batteries is based on developing low-cost,highly stable,and safe cathode and anode ***,the promising hard carbon anode and layered oxide cathode suffer from low sodium-embedded potential near 0.1 V and severe phase transitions,which cause safe problem and short lifespan,***,we design a low-strain bipolar P2-Na_(0.7)Ni_(0.25)Fe_(0.2)Ti_(0.55)O_(2) to solve the mentioned obstacles,whereas(Ni,Fe)and Ti provide charge compensation when it is used as cathode and anode,*** is revealed that the bipolar layered oxide undergoes solid-solution reaction when used as cathode or anode,and exhibits volume-complementary feature in a sodium-ion full-cell,as identified by in-situ X-ray ***,the safe symmetric sodium-ion full-cell exhibits excellent cyclic stability with 91.7%capacity retention after 200 *** work will provide a new horizon for designing safe and stable sodium-ion batteries.

关键词： sodium-ion batteries bipolar layered oxides solid-solution reaction volume complementation symmetric battery

Advances in bio-inspired electrocatalysts for clean energy future

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Nano Research 2024年第2期17卷 515-533页

作者： Jing-Wen Duan Mu Min-Rui Gao Division of Nanomaterials&Chemistry Hefei National Laboratory for Physical Sciences at the MicroscaleDepartment of ChemistryUniversity of Science and Technology of ChinaHefei 230026China

Electrocatalysis can enable efficient energy storage and conversion and thus is an effective way to achieve carbon *** unique structure and function of organisms can offer many ideas for the design of electrocatalysts,which has become one of the most promising research ***,the understanding of the mechanism of bio-inspired electrocatalysis has become clearer,which has promoted the design of bio-inspired catalysts and catalytic *** bio-inspired catalysts(enzyme-like catalysts,layered porous catalysts,superhydrophobic/superhydrophilic surfaces,and so on)have been developed to enable efficient electrocatalytic ***,we discuss the key advances in the field of bio-inspired electrocatalysts progressed in recent ***,the role of bio-inspiration in increasing the intrinsic activity and number of active sites of catalysts is ***,the structure and mechanism of layered porous catalytic systems that mimic biological transport systems are comprehensively ***,the design of three-phase interfaces from micro-nanoscale to atomic scale is highlighted,including the wettability of the electrode surface and the transport system near the *** conclude the review by identifying challenges in bio-inspired electrocatalysts and providing insights into future prospects for the exciting research field.

关键词： bio-inspired electrocatalysts active sites layered porous structure three-phase interface