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Manipulating guest-responsive spin transition to achieve switchable fluorescence in a Hofmann-type framework

Science China Chemistry 2024年第10期67卷 3339-3346页

作者： Xue-Ru wu shu-qi wu Zhi-Kun Liu Ming-Xing Chen Jun Tao Osamu Sato Hui-Zhong Kou Engineering Research Center of Advanced Rare Earth Materials (Ministry of Education) Department of ChemistryTsinghua University Institute for Materials Chemistry and Engineering & IRCCS Kyushu University Key Laboratory of Cluster Science of Ministry of Education School of Chemistry and Chemical EngineeringLiangxiang CampusBeijing Institute of Technology Analytical Instrumentation Center College of Chemistry and Molecular EngineeringPeking University

The change of fluorescence emission manipulated by spin state transition attracts considerable attention owing to its potential applications in magneto-optical switching ***,we report two two-dimensional（2D） Hofmann-type spin crossover（SCO） metal-organic frameworks（MOFs）[FeⅡ（PNI）2{AgⅠ（CN）2}2]·CHCl3（3Ag·CHCl3） and[FeⅡ（PNI）2{AuⅠ（CN）2}2]·CHCl3（3Au·CHCl3） based on the fluorescent ligand N-（4-pyridylmethyl）-1,8-naphthalimide（PNI）.Both complexes exhibit interesting SCO behaviors switched by guest solvent molecules,namely three-step transitions for the solvated complexes and complete onestep hysteretic SCO for the desolvated ones,verified by temperature-dependent magnetic susceptibility measurements,Mossbauer spectra,structural analyses,and differential scanning calorimetry ***,temperature-dependent fluorescence spectra exhibit double peaks（monomer and excimer emission） with both emission peaks change consistent with the change in SCO properties during the solvent molecule *** this study,we integrated guest-responsive SCO behavior into MOFs to manipulate the multistability of spin state and fluorescence switching,providing a rational strategy for the development of stimuli-responsive multifunctional materials.

关键词： spin crossover fluorescence multifunctional materials metal-organic frameworks Hofmann-type

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Fluorescence emission modulation in cyanido-bridged Fe(Ⅱ)spin crossover coordination polymers

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Science China Chemistry 2022年第8期65卷 1569-1576页

作者： Xue-Ru wu Zhi-Kun Liu Min Zeng Ming-Xing Chen Jun Tao shu-qi wu Hui-Zhong Kou Department of Chemistry Tsinghua UniversityBeijing 100084China Key Laboratory of Cluster Science of Ministry of Education School of Chemistry and Chemical EngineeringLiangxiang CampusBeijing Institute of TechnologyBeijing 102488China Analytical Instrumentation Center College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Institute for Materials Chemistry and Engineering&IRCCS Kyushu University744 MotookaNishi-kuFukuoka 819-0395Japan

Synergistic fluorescent spin crossover(SCO)bifunctional molecular materials have novel applications in the molecule-based magneto-optical ***,we report two novel three-dimensional(3D)Hofmann-type fluorescent SCO complexes[Fe^(II)-(tppe)MI(CN)_(2)]ClO_(4)·nSolv(tppe=tetra-(4-pyridylphenyl)ethene,M=Ag(tppe-Ag),Au(tppe-Au)).Both complexes show one-step abrupt SCO with the transition temperature of 230 K for tppe-Ag,and 245 K for tppe-Au accompanied by a color change from red to light *** SCO process is confirmed by the variable-temperature single-crystal X-ray diffraction analysis on *** the first time,the abnormal increase in emission intensity and concomitant large bathochromic shifts in the fluorescence spectra during the SCO process are realized in the 3D Hofmann-type coordination polymers expanded by the tetradentate tppe ***,tppe-Ag exhibits the unprecedented fluorescence emission from green to the edge of yellow.

关键词： fluorescence spin crossover multifunctional materials coordination polymers synergetic effect

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Aggregation-induced emission meets magnetic bistability: Synergy between spin crossover and fluorescence in iron(Ⅱ) complexes

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Chinese Chemical Letters 2023年第4期34卷 608-613页

作者： Yao Li Mohammad Khurram Javed shu-qi wu Arshia Sulaiman Ying-Ying wu Zhao-Yang Li Osamu Sato Xian-He Bu School of Materials Science and Engineering Nankai UniversityTianjin 300350China Institute for Materials Chemistry and Engineering Kyushu UniversityFukuoka 819-0395Japan

Luminescent spin crossover(SCO) materials have attracted significant interest owing to their potential applications in magneto-optical switches. However, the majority of previously reported FeII-based SCO complexes are adversely affected by fluorescence quenching in the solid-state. Here, we have constructed the first mononuclear FeIIcomplex decorated with an aggregation-induced emission(AIE) luminophore(i.e., tetraphenylethylene) that exhibits synergistic SCO and fluorescence behavior. Intriguingly, we obtained two types of crystals in different solvent systems, both displaying distinct magnetic bistability and fluorescence properties. The fluorescence intensity was observed to track the magnetic susceptibility, which confirmed that SCO and solid-state fluorescence operate synergistically. We introduce a novel approach for the construction of luminescent SCO compounds using an AIEgen as a luminophore, which leads to fluorescence emission in the solid-state, thus allowing us to study the synergy between SCO and fluorescence.

关键词： Magnetic bistability Spin crossover Luminescence Aggregation-induced emission Supramolecular structures

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A novel method for determining the resistivity of compressed superconducting materials

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Matter and Radiation at Extremes 2024年第4期9卷 1-3页

作者： Liling Sun qi wu shu Cai Yang Ding Ho-kwang Mao Center for High Pressure Science and Technology Advanced Research Beijing 100094China Institute of Physics Chinese Academy of SciencesBeijing 100190China

The measurement of resistivity in a compressed material within a diamond anvil cell presents significant *** high-pressure exper-imental setup makes it difficult to directly measure the size changes induced by pressure in the three crystallographic directions of the *** this study,we introduce a novel and effective method that addresses these technical *** method is anticipated to offer a valuable foundation for high-pressure investigations on quantum materials,particularly those with anisotropic layered structures.

关键词： resistivity method foundation

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Phase-dependent lithium-alloying reactions for lithium-metal batteries

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Chinese Chemical Letters 2024年第4期35卷 1-2页

作者： shu Lin Kezhen qi College of Pharmacy Dali UniversityDali 671000China

With the increasing demand for higher energy lithium-ion batteries (LIBs), it is imperative to develop high-capacity electrode materials [1–4]. Due to the unique electrochemical Li-alloying reactions, Li-alloys offer high theoretical capacity, especially lithiumrich phase alloys, which exceeds the theoretical capacity of graphite anodes [5–7]. Phase-transition, which significantly influences lithium alloy reactions, determines high voltage hysteresis,low Coulombic efficiency (CE), and short cycling life [8,9].

关键词： alloying alloys cycling

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Rapid Phase Ambiguity Elimination Methods for DOA Estimator via Hybrid Massive MIMO Receive Array

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Chinese Journal of Electronics 2024年第1期33卷 175-184页

作者： Xichao ZHAN Zhongwen SUN Feng shu Yiwen CHEN Xin CHENG Yuanyuan wu qi ZHANG Yifan LI Peng ZHANG School of Information and Communication Engineering Hainan University School of Electronic and Optical Engineering Nanjing University of Science and Technology

For a sub-connected hybrid multiple-input multiple-output(MIMO) receiver with K subarrays and N antennas, there exists a challenging problem of how to rapidly remove phase ambiguity in only single time-slot. A direction of arrival(DOA) estimator of maximizing received power(Max-RP) is proposed to find the maximum value of K-subarray output powers, where each subarray is in charge of one sector, and the center angle of the sector corresponding to the maximum output is the estimated true DOA. To make an enhancement on precision, Max-RP plus quadratic interpolation(Max-RP-qi) method is designed. In the proposed Max-RP-qi, a quadratic interpolation scheme is adopted to interpolate the three DOA values corresponding to the largest three receive powers of *** achieve the Cramer Rao lower bound, a Root-MUSIC plus Max-RP-qi scheme is developed. Simulation results show that the proposed three methods eliminate the phase ambiguity during one time-slot and also show low computational complexities. The proposed Root-MUSIC plus Max-RP-qi scheme can reach the Cramer Rao lower bound,and the proposed Max-RP and Max-RP-qi are still some performance losses 2–4 d B compared to the Cramer Rao lower bound.

关键词： Phased arrays Interpolation Wireless sensor networks Direction-of-arrival estimation Simulation Receiving antennas Massive MIMO

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CuInS_(2)quantum-dot-modified g-C_(3)N_(4)S-scheme heterojunction photocatalyst for hydrogen production and tetracycline degradation

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Journal of Materials Science & Technology 2024年第5期172卷 145-155页

作者： Jingjing Zhang Yue Zhao Kezhen qi shu-yuan Liu College of Pharmacy Dali UniversityDali 671000China Department of Pharmacology Shenyang Medical CollegeShenyang 110034China

CuInS_(2)quantum-dot(CIS QD)-modified g-C_(3)N_(4)(CN)catalysts(CIS/CN)were prepared with the aid of an in-situ growth *** as-obtained photocatalysts were explored by measuring their crystallinity,surface morphology,binding energy and light absorption *** photocatalytic efficiency of the pho-tocatalysts was evaluated through photocatalytic water splitting for hydrogen production and tetracycline(TC)antibiotic degradation under the simulated solar light and visible light *** optimized sample(10CIS/CN)showed the best photocatalytic activity:producing 102.4μmol g^(-1)h^(-1)of hydrogen in 1 h,or degrading 52.16%of TC in 120 min,which were respectively 48 or 3.4 times higher than the photocatalytic activity of CN *** enhancement in the efficiency of the composite system was prin-cipally accredited to the enlargement of light absorption,the more effective in charge transfer and the dropping of the charge carrier pair recombination through a formed S-scheme heterojunctional *** work is an effort to adjust CN-based polysulfide QD for speedy *** enriched photo-catalytic activity grants a new sense for adjusting the optical properties of CN.

关键词： CuInS_(2)QDs g-C_(3)N_(4) Photocatalysis Hydrogen production S-scheme heterojunction

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Euphorstranoids A and B,two highly rearranged ingenane diterpenoids from Euphorbia stracheyi:structural elucidation,chemical transformation,and lipid-lowering activity

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Organic Chemistry Frontiers 2022年第3期9卷 775-780页

作者： Fang-Yu Yuan Yue-Hua Pan Ai-Ping Yin Wei Li Dong Huang Xue-Long Yan shu-qi wu Gui-Hua Tang Rong Pu Sheng Yin School of Pharmaceutical Sciences Sun Yat-sen UniversityGuangzhouGuangdong 510006People’s Republic of China Department of Clinical Laboratory the Third People’s Hospital of DongguanDongguan 523326People’s Republic of China

Euphorstranoids A(1)and B(2),two highly rearranged ingenane diterpenoids with an unusual 5/6/7/3 carbon ring system,were isolated from Euphorbia *** structures were determined by a combination of spectral,chemical,and X-ray diffraction *** plausible biosynthetic pathway of 1 and 2 was proposed and chemically *** 1 and 2 significantly inhibited the triglyceride(TG)level in 3T3-L1 adipocytes via retarding cell adipogenesis at the early stage.

关键词： methods chemical elucidation

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Development of component stiffness equations for thread-fixed one-side bolt connections to an enclosed rectangular hollow section column under tension

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Frontiers of Structural and Civil Engineering 2024年第4期18卷 568-586页

作者： Fu-Wei wu Yuan-qi LI Department of Structural Engineering Tongji UniversityShanghai 200092China State Key Laboratory of Disaster Reduction in Civil Engineering Tongji UniversityShanghai 200092China

The derivation and validation of analytical equations for predicting the tensile initial stiffness of threadfixed one-side bolts(TOBs),connected to enclosed rectangular hollow section(RHS)columns,is presented in this *** unknown stiffness components are considered:the TOBs connection and the enclosed RHS ***,the trapezoidal thread of TOB,as an equivalent cantilevered beam subjected to uniformly distributed loads,is analyzed to determine the associated *** on the findings,the thread-shank serial-parallel stiffness model of TOB connection is *** analysis of the tensile stiffness of the enclosed RHS face due to two bolt forces,the four sidewalls are treated as rotation constraints,thus reducing the problem to a two-dimensional plate *** to the load superposition method,the deflection of the face plate is resolved into three components under various boundary and load *** to the plate deflection theory of Timoshenko,the analytical solutions for the three deflections are derived in terms of the variables of bolt spacing,RHS thickness,height to width ratio,***,the validity of the above stiffness equations is verified by a series of finite element(FE)models of T-stub *** proposed component stiffness equations are an effective supplement to the component-based method.

关键词： initial stiffness component based method thread-fixed one-side bolt rectangular hollow sections analytical equation

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A Molecular Crystal Shows Multiple Correlated Magnetic and Ferroelectric Switchings

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CCS Chemistry 2021年第9期3卷 2464-2472页

作者： Yun Li shu-qi wu Jin-Peng Xue Xiao-Lei Wang Osamu Sato Zi-shuo Yao Jun Tao Key Laboratory of Cluster Science of Ministry of Education School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081 Institute for Materials Chemistry and Engineering Kyushu UniversityFukuoka 819-0395

Simultaneous control of the magnetic and electric properties of materials is crucial for their application in next-generation memory and sensor ***,we report a single-crystal Co(II)complex that exhibits unprecedented two-step magnetic switching accompanied by paraelectric–ferroelectric–paraelectric phase *** ferroelectricity of the material is governed by changes in the directionality of the sulfate dianions therein that trigger nonpolar–polar–nonpolar variation of the crystal symmetry and induce slight structural changes in the Co(II)complex.

关键词： molecular ferroelectric magnetic switching phase transition symmetry breaking Co(II)

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