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Double stimulus-responsive palladium catalysts for ethylene polymerization and copolymerization

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Chinese Chemical Letters 2024年第7期35卷 407-411页

作者： Hailong He Wenbing Wang Wenmin Pang Chen Zou Dan Peng CAS Key laboratory of Soft Matter Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei National Laboratory for Physical Sciences at the MicroscaleHefei 230026China

The external stimulus response strategy has been evolved rapidly in the field of olefin *** this work,we modularly synthesized three types of double stimulus responsiveα-diimine palladium catalysts,combining redox regulation and other regulation together,such as light,Lewis acid and alkali *** catalytic activities and the molecular weight of polyethylene products can be regulated for 4 times in ethylene *** palladium complexes were also used for the copolymerization reaction of ethylene and polar monomers,such as methyl 10-undecylenate and methyl acrylate,effectively regulating the catalytic activities,the molecular weight and polar monomer incorporation of the prepared *** research on these dual-regulated palladium complexes makes full use of prepared catalysts and provides new inspirations for regulating olefin polymerization.

关键词： Dual-regulated Stimulus-responsive Palladium Ethylene polymerization Polar monomer

Topological and superconducting properties of monolayered CoN and CoP:A first-principles comparative study

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Science China(physics,Mechanics & Astronomy) 2024年第5期67卷 98-108页

作者： Jiaqing Gao Zhenyu Zhang Ping Cui International Center for Quantum Design of Functional Materials(ICQD) Hefei National Research Center for Physical Sciences at Microscale(HFNL)University of Science and Technology of ChinaHefei 230026China hefei national laboratory University of Science and Technology of ChinaHefei 230088China

Two-dimensional systems that simultaneously harbor superconductivity and nontrivial band topology may serve as appealing platforms for realizing topological superconductivity with promising applications in fault-tolerant quantum ***,based on first-principles calculations,we show that monolayered Co N and Co P with the isovalent Fe Se-like structure are stable in freestanding form,even though their known bulk phases have no resemblance to *** two systems are further revealed to display intrinsic band inversions due to crystal field splitting,and such orderings are preserved with the inclusion of spin-orbit coupling(SOC),which otherwise is able to open a curved band gap,yielding a non-zero Z2 topological invariant in each *** a mechanism of topologicalization is distinctly contrasted with that identified recently for the closely related monolayers of CoX(X=As,Sb,Bi),where the SOC plays an indispensable role in causing a nontrivial band ***,we demonstrate that,by applying equi-biaxial tensile strain,the electron-phonon coupling strength in monolayered CoN can be significantly enhanced,yielding a superconducting transition temperature(Tc)up to 7-12 K for the Coulomb pseudopotential ofμ*=0.2-0.1,while the CoP monolayer shows very low Tc even under pronounced *** different superconducting behaviors can be attributed to different variations in lattice softening and electronic density of states around the Fermi level upon *** central findings enrich the understanding of different mechanisms of band inversions and topologicalization and offer platforms for achieving the coexistence of superconductivity and nontrivial band topology based on two-dimensional systems.

关键词： topological yielding otherwise

Electrochemical construction of 2,5-diaryloxazoles via N–H and C(sp_(3))-H functionalization

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Chinese Chemical Letters 2024年第4期35卷 340-345页

作者： Tong Li Leping Pan Yan Zhang Jihu Su Kai Li Kuiliang Li Hu Chen Qi Sun Zhiyong Wang hefei national Center for physical sciences at microscale Key Laboratory of Precision and Intelligent ChemistrySchool of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei 230026China Anhui University of Science and Technology Huainan 232001China CAS Key laboratory of microscale Magnetic Resonance Department of Modern PhysicsUniversity of Science and Technology of ChinaHefei 230026China

An efficient N–H and C(sp~3)-H functionalization of aryl ketones with benzylamines/amino acids was developed under mild conditions by virtue of anodic oxidation. A variety of functionalized 2,5-diaryloxazoles were obtained with good to excellent yields. Moreover, some important natural products can be prepared by this method. The reaction features a broad substrate scope, scalability, metal-free and chemical oxidant-free.

关键词： Electrochemical Metal-free Oxazole Oxidant-free

Room-temperature ferrimagnetism and size-modulated electronic structures in two-dimensional cluster-based metal-organic frameworks

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Science China Chemistry 2024年第4期67卷 1334-1340页

作者： Jing Cheng Xingxing Li Jinlong Yang Key laboratory of Precision and Intelligent Chemistry University of Science and Technology of ChinaHefei 230026China department of Chemical physics University of Science and Technology of ChinaHefei 230026China hefei national Research Center for physical sciences at the microscale University of Science and Technology of ChinaHefei 230026China hefei national laboratory University of Science and Technology of ChinaHefei 230088China

Cluster-assembled materials have attracted particular attention for their complex hierarchical structures and unique ***,the majority of cluster-based assemblies developed so far are either non-magnetic or only exhibit magnetic ordering with a relatively low Curie temperature,limiting their applications in ***,two-dimensional(2D)cluster-assembled materials with room-temperature magnetism remain highly *** this purpose,based on first principles calculations,we design a series of thermodynamically stable 2D cluster-based metal-organic frameworks(MOFs)Fe_(n)-(pyz)(n=1-6)by utilizing Fenmetal clusters as nodes and nitrogen-containing pyrazine ligands as organic *** 2D cluster-based MOFs exhibit robust ferrimagnetic ordering due to the strong d-p direct exchange interaction between d-electron spin of Fe_(n)(n=1-6)clusters and charge transfer-induced p-electron spin of pyrazine *** particular,the ferrimagnetic Curie temperatures are well above room temperature(up to 836 K).Additionally,altering the size of Fe_(n)clusters in Fe_(n)-(pyz)(n=1-6)MOFs results in diverse functional spintronic properties,including bipolar magnetic semiconductors,half semiconductors and Dirac half ***,these 2D assembled MOFs possess sizable magnetic anisotropy energies,up to 9.16 me V per formula.

关键词： metal-organic framework two-dimensional material half metal bipolar magnetic semiconductor magnet

Alloy strategy to synthesize Pt-early transition metal oxide interfacial catalysts

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Nano Research 2024年第4期17卷 3390-3397页

作者： Shi-Long Xu Hang Nan Wanqun Zhang Yue Lin Sheng-Qi Chu Hai-Wei Liang hefei national Research Center for physical sciences at the microscale Department of ChemistryUniversity of Science and Technology of ChinaHefei 230026China School of Materials and Chemical Engineering Anhui Jianzhu UniversityHefei 230601China Institute of High Energy physics Chinese Academy of SciencesBeijing 100049China

Metal oxide supported metal catalysts show promising catalytic performance in many industry-relevant ***,the enhancement of performance is often limited by the insufficient metal/metal oxide *** this work,we demonstrate a general synthesis of Pt-early transition metal oxide(Pt-MO_(x),M=Ti,Zr,V,and Y)catalysts with rich interfacial sites,which is based on the air-induced surface segregation and oxidation of M in the supported Pt-M alloy *** characterizations verify the dynamic structural response of Pt-M alloy catalysts to air and the formation of Pt-MO_(x) catalysts with abundant interfacial *** prepared Pt-TiO_(x) interfacial catalysts exhibit improved performance in hydrogenation reactions of benzaldehyde,nitrobenzene,styrene,and furfural,as a result of the heterolytic dissociation of H_(2) at Pt-metal oxide interfacial sites.

关键词： Pt-early transition metal oxide interfacial catalyst alloy oxidation strategy interfacial sites hydrogenation reactions heterolytic dissociation

Normal and Superconducting Properties of La3Ni2O7

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Chinese physics Letters 2024年第7期41卷 145-156页

作者：王猛闻海虎吴涛姚道新向涛 Guangdong Provincial Key laboratory of Magnetoelectric physics and Devices School of PhysicsSun Yat-Sen University national laboratory of Solid State Microstructures and department of physics Collaborative Innovation Center of Advanced Microstructures Nanjing University hefei national Research Center for physical sciences at the microscale University of Science and Technology of China Institute of physics Chinese Academy of Sciences School of physics University of Chinese Academy of Sciences

This review provides a comprehensive overview of current research on the structural,electronic,and magnetic characteristics of the recently discovered high-temperature superconductor La3Ni2O7under high *** present the experimental results for synthesizing and characterizing this material,derived from measurements of transport,thermodynamics,and various spectroscopic techniques,and discuss their physical implications.

关键词： Nickel compounds

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

Iron oxide/CNT-based artificial nacre for electromagnetic interference shielding

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Nano Research 2024年第7期17卷 6560-6566页

作者： Cheng-Xin Yu Yu-Feng Meng Bo Yang Jun Pang Xiang-Sen Meng Zi-Ye Zhao Qing-Yue Wang Li-Bo Mao Zhi-Kun Wu Shu-Hong Yu Institute of physical Science and Information Technology Anhui UniversityHefei 230601China Key laboratory of Materials physics Anhui Key Laboratory of Nanomaterials and NanotechnologyCAS Center for Excellence in NanoscienceInstitute of Solid State PhysicsHFIPSChinese Academy of SciencesHefei 230031China department of Chemistry New Cornerstone Science LaboratoryInstitute of Biomimetic Materials&ChemistryAnhui Engineering Laboratory of Biomimetic MaterialsDivision of Nanomaterials&ChemistryHefei National Research Center for Physical Sciences at the MicroscaleUniversity of Science and Technology of ChinaHefei 230026China

Biological structural materials,despite consisting of limited kinds of compounds,display multifunctionalities due to their complex hierarchical *** some biomimetic strategies have been applied in artificial materials to enhance their mechanical stability,the simultaneous optimization of other functions along with the mechanical properties via biomimetic designs has not been thoroughly ***,iron oxide/carbon nanotube(CNT)-based artificial nacre with both improved mechanical and electromagnetic interference(EMI)shielding performance is fabricated via the mineralization of Fe_(3)O_(4)onto a CNTincorporated *** micro-and nano-structures of the artificial nacre are similar to those of natural nacre,which in turn improves its mechanical *** alternating electromagnetic wave-reflective CNT layers and the wave-absorptive iron oxide layers can improve the multiple reflections of the waves on the surfaces of the reflection layers,which then allows sufficient interactions between the waves and the absorption ***,compared with the reflection-dependent EMI-shielding of the non-structured material,the artificial nacre exhibits strong absorption-dependent shielding behavior even with a very low content of wave-absorptive *** to the high mechanical stability,the shielding effectiveness of the artificial nacre that deeply cut by a blade is still maintained at approximately 70%−96%depending on the incident wave *** present work provides a new way for designing structural materials with concurrently enhanced mechanical and functional properties,and a path to combine structural design and intrinsic properties of specific materials via a biomimetic strategy.

关键词： artificial nacre electromagnetic interference shielding biomineralization biomimetic material hierarchical structure

Interstitial carbon induces enriched Cu^(δ+)sites in Cu_(2)O nanoparticles to facilitate CO_(2)electroreduction to C_(2+)products

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Nano Research 2024年第8期17卷 7013-7019页

作者： Haoran Wang Rongbo Sun Peigen Liu Haohui Hu Chen Ling Xiao Han Yi Shi Xusheng Zheng Geng Wu Xun Hong Center of Advanced Nanocatalysis(CAN) Department of Applied ChemistryHefei National Laboratory for Physical Sciences at the MicroscaleUniversity of Science and Technology of ChinaHefei 230026China Sinochem Holdings Co Ltd Xiongan New AreaHebei 071700China national Synchrotron Radiation laboratory(NSRL) University of Science and Technology of ChinaHefei 230029China

The electrochemical CO_(2)reduction reaction(CO_(2)RR)holds significant promise in advancing carbon *** catalysts for the electrochemical CO_(2)RR to multi-carbon(C_(2+))products(e.g.,C_(2)H_(4))under industrial-level current density is urgently needed and ***,we report the Cu_(2)O nanoparticles doped with interstitial carbon atoms(denoted as C-Cu_(2)O NPs)for the conversion of CO_(2)to C_(2+)*** interstitial carbon promotes the C-Cu_(2)O NPs to possess abundant unsaturated Cu–O bonds,leading to a high-density Cu^(δ+)(0<δ<1)*** obtained C-Cu_(2)O NPs exhibited significant Faradic efficiency(FE)of C_(2+)products approaching 76.9%and a partial current density reaching 615.2 mA·cm^(–2)under an industrial-level current density of 800 mA·cm^(–2).Furthermore,the efficient electrosynthesis of C_(2)H_(4)achieved an FE of 57.4%with a partial current density of 459.2 mA·cm^(–2).In situ electrochemical attenuated total reflection Fourier transform infrared spectroscopy and in situ Raman spectroscopy analyses revealed that C-Cu_(2)O NPs stabilized the intermediate*CO and facilitated C–C coupling,leading to increased selectivity towards C_(2+)products.

关键词： CO_(2)electroreduction C-C coupling interstitial carbon *CO coverage industrial-level current density