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Luminescence and magnetic properties of bifunctional nanoparticles composited by nitrogen-doped graphene quantum dots and gadolinium

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Journal of Rare Earths 2024年第4期42卷 716-723页

作者： Wanli Zhang Hao Zhou Meigui Ou Donghao Sun Chunlin Yang College of Materials and Metallurgy University of GuizhouGuiyang550025China National Local Co-construction engineering laboratory for High Performance Metal structure Material and Manufacture Technology Guiyang550025 China College of Chemistry and Materials engineering Guiyang UniversityGuiyang550003China

In this paper,nitrogen-doped graphene quantum dots(N-GQDs)were combined with gadolinium ions(Gd^(3+))by a surface modification to obtain magneto-optical dual-functional N-GQDs/Gd^(3+)*** morphology of obtained composite was characterized by field emission scanning electron microscopy and transmission electron *** and magnetic properties were measured by a fluorescence spectrophotometer and a vibrating sample magnetometer,*** indicate that well-dispersed spherical N-GQDs/Gd^(3+)nanoparticles have an average diameter of 7 nm.N-doping significantly increases the luminesce nce of particles with an optimal luminescence intensity at 20℃and pH=9.X-ray photoelectron spectroscopy results indicate that the N-doping introduces pyrrolic N as an electron donor,enhancing fluorescence by increasing the surface electron cloud density of *** addition,density functional theory calculation results reveal that N-doping reduces the band gap of NGQDs/Gd^(3+),enabling electronic transitions to higher energy levels and generating more activation sites,thereby enhancing *** to N-GQDs/Gd^(3+)prepared at 20℃,the saturated magnetization of particles prepared at 40℃is 0.85 emu/g,indicating a better magnetic *** above results suggest that bifunctional nanomaterials N-GQDs/Gd^(3+)with excellent optical properties and magnetism can be better used for fluorescence and magnetic resonance imaging.

关键词： Nitrogen-doped graphenequantum dots Gadolinium Luminescence Magnetism Rare earths

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Size-controlled synthesis and near-infrared photothermal response of Cp^(*)Rh-based metalla[2]catenanes and rectangular metallamacrocycles

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Chinese Chemical Letters 2024年第6期35卷 337-343页

作者： Ying Zhao Yin-Hang Chai Tian Chen Jie Zheng Ting-Ting Li Francisco Aznarez Li-Long Dang Lu-Fang Ma College of Chemistry and Chemical engineering Henan Key Laboratory of Function-Oriented Porous MaterialsLuoyang Normal UniversityLuoyang 471934China College of Chemistry Zhengzhou UniversityZhengzhou 450001China Shanghai Key laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of PolymersDepartment of ChemistryFudan UniversityShanghai 200438China

A variety of research reports on novel supramolecular topologies have been published over the last ***,it is still a great challenge to tap into the inner functional properties of these ***,two tetranuclear metallamacrocycles 1 and 2 and four octonuclear[2]catenanes 3-6 were constructed successfully via a coordination-driven self-assembly strategy,by conscious design and use of the tetramethyl bidentate pyridine ligand L1,and the appropriate selection of six binuclear half-sandwich rhodium building units with different longitudinal *** complexes have been fully characterized by single crystal X-ray diffraction analysis and NMR ***,near-infrared photothermal studies of the obtained[2]catenanes reveal different photothermal response in solid and solution states,which may be attributed to a strong fluorescence quenching effect of the half-sandwich organometallic fragment and different conjugated effect of Cp^(*)Rh based building blocks in the interlocking *** photothermal conversion efficiencies of[2]catenanes 4-6 fall in the range 30.5%-16.5% *** contribution aims to play a key role in the experimental development of Cp^(*)-based photothermal materials.

关键词： Catenanes Photothermal materials Supramolecular topologies Half-sandwich fragment 3,3'-N-donor analogues

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Electrochemical reconstruction: a new perspective on Sn metal-organic complex microbelts as robust anode for lithium storage

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Rare Metals 2024年第1期43卷 76-86页

作者： Jin-Ke Shen Nai-Teng Wu Li-Yuan Wang Gang Jiang Dong-Lei Guo Jin Li Gui-Long Liu Hong-Yu Mi Huan Pang Xian-Ming Liu Key laboratory of function-oriented Porous Materials of Henan Province College of Chemistry and Chemical EngineeringLuoyang Normal UniversityLuoyang 471934China State Key laboratory of Chemistry and Utilization of Carbon Based Energy Resources School of Chemical Engineering and TechnologyXinjiang UniversityUrumqi 830046China School of Chemistry and Chemical engineering Institute for Innovative Materials and EnergyYangzhou UniversityYangzhou 225009JiangsuChina

Tin-based materials with high theoretical capacity and suitable working voltage are ideal anode materials for lithium-ion batteries(LIBs). However, to overcome their shortcomings(volume expansion and inferior stability), the preparation processes are usually complicated and expensive. Herein, a tin-based metal-organic complex(tin 1,2-benzenedicarboxylic acid, Sn-BDC)with one-dimensional microbelt morphology is synthesized by a facile, rapid and low-cost co-precipitation method, and served as anode material for LIBs without any post-treatment. Sn-BDC exhibits a high reversible capacity with609/440 m Ah·g^(-1) at 50/2000 m A·g^(-1), and robust cycling stability of 856 m Ah·g^(-1) after 200 cycles at 200 m A·g^(-1),which are obviously superior to that of the Sn Ox/C counterparts. Moreover, an electrochemical reconstruction perspective on the lithium storage mechanism of Sn-BDC is proposed by systematic ex-situ characterizations. The reconstructed SnO_(2) replaces Sn-BDC and becomes the active material in the subsequent cycles. As the by-product of the lithiation reaction, the formed Li-based metal-organic complex(Li-BDC, wrapped around the reconstructed SnO_(2)) plays an important role in alleviating volume expansion and accelerating the charge transfer *** work is beneficial to design and construct the new electrode materials based on the electrochemical reconstruction for advanced LIBs.

关键词： Electrochemical reconstruction Metal-organic complex Anode Lithium storage mechanism Lithium-ion batteries

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Variational quantum algorithms for scanning the complex spectrum of non-Hermitian systems

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Frontiers of physics 2024年第4期19卷 275-285页

作者： Xu-Dan Xie Zheng-Yuan Xue Dan-Bo Zhang Key laboratory of Atomic and Subatomic structure and Quantum Control(Ministry of Education) Guangdong Basic Research Center of Excellence for Structure and Fundamental Interactions of Matterand School of PhysicsSouth China Normal UniversityGuangzhou 510006China Guangdong Provincial Key laboratory of Quantum engineering and Quantum Materials Guangdong–Hong Kong Joint Laboratory of Quantum Matterand Frontier Research Institute for PhysicsSouth China Normal UniversityGuangzhou 510006China

Solving non-Hermitian quantum many-body systems on a quantum computer by minimizing the variational energy is challenging as the energy can be ***,we propose a variational quantum algorithm for solving the non-Hermitian Hamiltonian by minimizing a type of energy variance,where zero variance can naturally determine the eigenvalues and the associated left and right ***,the energy is set as a parameter in the cost function and can be tuned to scan the whole spectrum efficiently by using a two-step optimization *** numerical simulations,we demonstrate the algorithm for preparing the left and right eigenstates,verifying the biorthogonal relations,as well as evaluating the *** also investigate the impact of quantum noise on our algorithm and show that its performance can be largely improved using error mitigation ***,our work suggests an avenue for solving non-Hermitian quantum many-body systems with variational quantum algorithms on near-term noisy quantum computers.

关键词： quantum algorithm non-Hermitian physics quantum manybody systems

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A novel triple periodic minimal surface-like plate lattice and its data-driven optimization method for superior mechanical properties

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Applied Mathematics and Mechanics(English Edition) 2024年第2期45卷 217-238页

作者： Yanda WANG Yanping LIAN Zhidong WANG Chunpeng WANG Daining FANG State Key laboratory for Turbulence and Complex Systems&Center for Applied Physics and Technology College of EngineeringPeking UniversityBeijing 100871China Institute of Advanced structure Technology Beijing Institute of TechnologyBeijing 100081China

Lattice structures can be designed to achieve unique mechanical properties and have attracted increasing attention for applications in high-end industrial equipment,along with the advances in additive manufacturing(AM)*** this work,a novel design of plate lattice structures described by a parametric model is proposed to enrich the design space of plate lattice structures with high connectivity suitable for AM *** parametric model takes the basic unit of the triple periodic minimal surface(TPMS)lattice as a skeleton and adopts a set of generation parameters to determine the plate lattice structure with different topologies,which takes the advantages of both plate lattices for superior specific mechanical properties and TPMS lattices for high connectivity,and therefore is referred to as a TPMS-like plate lattice(TLPL).Furthermore,a data-driven shape optimization method is proposed to optimize the TLPL structure for maximum mechanical properties with or without the isotropic *** this method,the genetic algorithm for the optimization is utilized for global search capability,and an artificial neural network(ANN)model for individual fitness estimation is integrated for high efficiency.A set of optimized TLPLs at different relative densities are experimentally validated by the selective laser melting(SLM)fabricated *** is confirmed that the optimized TLPLs could achieve elastic isotropy and have superior stiffness over other isotropic lattice structures.

关键词： lattice structure triple periodic minimal surface(TPMS) plate lattice structural optimization machine learning

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NHC-derived carbon-centered luminescent radicals with shortwavelength emission via suppression of Kasha's rule

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Science China Chemistry 2024年第8期67卷 2679-2685页

作者： Can Chen Xin Li Xinhua Ouyang Ying-Feng Han Key laboratory of Synthetic and Natural functional Molecule Chemistry of the Ministry of Education Xi’an Key Laboratory of Functional Supramolecular Structure and MaterialsCollege of Chemistry and Materials ScienceNorthwest UniversityXi’an 710127China College of Material engineering Fujian Agriculture and Forestry University Fuzhou 350108China

Luminescent organic radicals have garnered increasing attention owing to their versatile applications in sensing, imaging, and organic light-emitting diodes(OLEDs), attributed to their unique emission properties originating from the doublet spin ***, the natural narrow bandgap of organic free radicals typically limits their emission to the long-wavelength *** luminescent organic radicals with short-wavelength emission remains a significant challenge. Herein, a series of carbon-centered radicals with short-wavelength emission(383–476 nm) by combining N-heterocyclic carbenes with various polycyclic aromatic hydrocarbons(PAHs)(2-naphthyl, 2a~Ⅰ and 2b~Ⅰ;2-phenanthryl, 2a~Ⅱand 2b~Ⅱ;2-anthryl, 2a~Ⅲand 2b~Ⅲ;3-phenanthryl, 2a~Ⅳand 2b~Ⅳ). Theoretical calculations reveal that the introduction of PAHs significantly increases the ΔE_(D2-D1) in 2a^(Ⅰ–Ⅲ)and 2b^(Ⅰ–Ⅲ)compared to that in phenyl-derived radical congeners. Consequently, the internal transition from D2 to D1 is impeded, leading to a high yield of D2 emission and a suppressed Kasha's rule, thereby overcoming the limitations imposed by their narrow bandgap. For 2a~Ⅳ and 2b~Ⅳ, despite a moderately large ΔED2-D1value, the ΔED3-D1value exceeds 1 e V, indicating that their emission likely originates from the D3 state. Furthermore, we utilized 2a~Ⅲand 2b~Ⅲ as emissive materials in OLEDs,resulting in blue emissions with external quantum efficiencies of 7.5% and 6.5%, respectively.

关键词： N-heterocyclic carbenes luminescent organic molecules carbon-centered radicals short-wavelength emission

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Design and mechanical properties analysis of a cellular Waterbomb origami structure

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Theoretical & Applied Mechanics Letters 2024年第3期14卷 193-202页

作者： Yongtao Bai Zhaoyu Wang Yu Shi School of Civil engineering Chongqing UniversityChongqing 400045China Research Center of Steel structure engineering Chongqing UniversityChongqing 400045China

Cellular structures are commonly used to design energy-absorbing structures,and origami structures are becominga prevalent method of cellular structure *** paper proposes a foldable cellular structure based on theWaterbomb origami *** geometrical configuration of this structure is ***-static compressiontests of the origami tube cell of this cellular structure are conducted,and load-displacement relationship curvesare *** simulations are carried out to analyze the effects of aspect ratio,folding angle,thicknessand number of layers of origami tubes on initial peak force and specific energy absorption(SEA).Calculationformulas for initial peak force and SEA are obtained by the multiple linear regression *** degree ofinfluence of each parameter on the mechanical properties of the single-layer tube cell is *** resultsshow that the cellular structure exhibits negative stiffness and periodic load-bearing capacity,as well as foldingangle has the most significant effect on the load-bearing and energy-absorbing *** adjusting the designparameters,the stiffness,load-bearing capacity and energy absorption capacity of this cellular structure can beadjusted,which shows the programmable mechanical properties of this cellular *** foldability andthe smooth periodic load-bearing capacity give the structure potential for application as an energy-absorbing structure.

关键词： Cellular structure Waterbomb origami Mechanical metamaterial Numerical simulation Energy absorption

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Synthesis of highly stable Ni nanoparticles via electrostatic self-assembly for enhanced hydrogen storage of MgH2

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Rare Metals 2024年第9期43卷 4356-4366页

作者： Qin-Ke Tang Jiang-Chuan Liu Rui Shi Yun-Feng Zhu Ji-Guang Zhang Ya-Na Liu Jun Wang Yao Zhang Xiao-Hui Hu Zhi-Bin Liu Li-Quan Li College of Materials Science and engineering Jiangsu Collaborative Innovation Centre for Advanced Inorganic Function CompositesNanjing Tech University School of Materials Science and engineering Southeast University

Magnesium-based hydrides have been widely recognized as an appropriate choice for solid-state hydrogen ***,its undesirable thermodynamics and sluggish hydrogenation/dehydrogenation kinetics are major bottlenecks for its ***,a highly stable and highly dispersed Ni-based catalyst （Ni/Al2O3/GN） was fabricated to promote the hydrogen storage performance of MgH2via the electrostatic effect of NiAl-LDH/GN precursor with a co-calcination reduction ***2-5wt % Ni/Al2O3/GN exhibits excellent hydrogen storage performance,releasing about 5.7 wt % hydrogen in 3500 s at 250℃,and can reach a saturation hydrogen absorption of about 6.15 wt% in 3000 s at 100℃.Furthermore,it also shows low dehydrogenation apparent activation energy of 89.1 and 118.2 kJ·***,the catalyst ensures the stability of both the physical phase and structure during ball milling and cycling *** role of each phase in Ni/Al2O3/GN on the hydrogen storage performance of MgH2was also discussed through experiments and theoretical calculation,and the synergistic catalytic mechanism of Ni/Al2O3/GN was clearly *** work provides a unique perspective for the preparation of highly stable and highly dispersible catalysts.

关键词： Catalytic mechanism Hydrogen storage performance Magnesium hydride Ni/Al2O3/GN

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Organic Brønsted Acid-Catalyzed Stereoselective Cationic RAFT Polymerization:The Effect of RAFT Agents

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Chinese Journal of Polymer Science 2024年第6期42卷 711-717页

作者： Zheng-Yi Zhang Zan Yang Yun Liao Sai-Hu Liao Key laboratory of Molecule Synthesis and function Discovery(Fujian Province University) College of ChemistryFuzhou UniversityFuzhou350108China State Key laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China Beijing National laboratory for Molecular Sciences Beijing100190China

The tacticity of vinyl polymers is a key factor affecting the properties of ***,organic Brønsted acids have been demonstrated as effective catalysts for the development of highly stereoselective cationic reversible addition-fragmentation chain transfer(RAFT)polymerizations of vinyl ethers,in which the use of RAFT agents could allow the control the molecular weight and tacticity of polymer products ***,the effect of RAFT agents on the tacticity-regulation remains elusive and lacks of *** this study,we synthesized four types of RAFT agents and evaluated their influence in the stereoselective cationic polymerization of isobutyl vinyl ether in the presence of PADI as a Brønsted acid catalyst,which unveils that the Z group of RAFT agents could not only affect the polydispersity of the products,but also exert a profound effect on the *** extensive screening of the RAFT agents,high stereoregularity(isotacticity,90%m)was obtained when using dithiocarbonate ester-type RAFT agents with a benzyloxy Z group.

关键词： Bronsted acid catalysis Stereoselective cationic polymerization RAFT polymerization Chain transfer agents Tacticity

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Water-Driven Malleable,Weldable and Eco-Friendly Recyclable Carbon Fiber Reinforced Dynamic Composites

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Chinese Journal of Chemistry 2024年第5期42卷 516-522页

作者： Ping Yu Qirui Huang Yi Wang Wan Peng Zichen Jia Haiyue Wang Juanjuan Ma Chunyu Wang Xuzhou Yan School of Environmental and Chemical engineering Jiangsu Key Laboratory of Function Control Technology for Advanced MaterialsJiangsu Ocean UniversityLianyungangJiangsu222005 China School of Chemistry and Chemical engineering Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai200240 China

Traditional carbon fiber-reinforced polymers based on thermoset matrix have been extensively used in the fields of wind turbine blades,automotive sector,and aerospace,among many ***,there is still a major challenge of recycling those polymers due to the high cost and adverse impacts on the *** this work,we apply a polyimine network as matrix,which possess considerable tensile and thermal properties,to prepare the carbon fiber reinforced polyimine materials with trifluoromethyl diphenoxybenzene units(CFRFP)using a prepreg-based compression molding *** CFRFP can be reshaped or reprocessed by heat or with water rapidly,and exhibited multifunction,including welding,chemical recycling,*** unique findings gained from our study will facilitate the manufacturing capability and enrich the types of fiber-reinforced composites.

关键词： Dynamic chemistry Green chemistry Fiber-reinforced composites Fluoropolyimine Welding Reshaping Recycling Renewable resources

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