Under the condition of solvothermal synthesis,the viologen ligand 1,1′-bis(3-carboxyphenyl)-(4,4′-bipyri-dine)dichloride(H_(2)bcbpy·2Cl)and KI are coordinated with the metal cadmium ions.A case of thermochromic...Under the condition of solvothermal synthesis,the viologen ligand 1,1′-bis(3-carboxyphenyl)-(4,4′-bipyri-dine)dichloride(H_(2)bcbpy·2Cl)and KI are coordinated with the metal cadmium ions.A case of thermochromic coor-dination polymer[Cd(bcbpy)I_(2)]·2H_(2)O(1)was constructed.Complex 1 displays a 1D chain structure and exhibits thermochromic behavior.Under different temperature stimulation,the complex(ground)slowly changed from green to yellow-green,and with the increase of temperature,the color of complex 1 gradually deepened,and finally became orange-yellow.Therefore,complex 1 was prepared as a thermochromic film.In addition,we also performed electrochemical tests on complex 1,which showed that the complex is a semiconductor material.CCDC:2391802.展开更多
Mesoporous metals with large surface area,high pore volume,and uniform pore structure hold excellent advantages for various applications.However,the state-of-the-art synthesis methods are still limited to wet chemistr...Mesoporous metals with large surface area,high pore volume,and uniform pore structure hold excellent advantages for various applications.However,the state-of-the-art synthesis methods are still limited to wet chemistry,which requires excessive solvents and a time-consuming drying process.Here,we report a facile and general mechanochemical coordination self-assembly strategy to prepare mesoporous metals(e.g.,Rh,Ru,Ir,Pt,Pd,Ag,Co,and Ni)with remarkable porous properties by using metal chlorides and cationic polymer interplay.Compared with the wet chemistry process,this method proceeds without solvents and does not need complicated experimental conditions and long synthetic periods,which not only greatly reduces the consumption of cost and energy and environmental pollution,but also improves the synthesis efficiency and yield of target products.We believe the developed approach will provide a general pathway for the scalable preparation of advanced porous materials.展开更多
A tin-oxygen coordination driving self-assembly was developed in the block copolymers containing organotin, which were prepared by the radical addition-fraction transfer（RAFT） method and characterized by the gel-per...A tin-oxygen coordination driving self-assembly was developed in the block copolymers containing organotin, which were prepared by the radical addition-fraction transfer（RAFT） method and characterized by the gel-permeation chromatography（GPC） and 1H-NMR. And the self-assemblies of these block copolymers with various chain length ratios in the different concentrations in CHCl3 were stable according to the results of DLS and TEM. Additionally, it was also given an insight investigation on the regulation of self-assembly of the block copolymers by adding dibutyltin dichloride and a possible mechanism was proposed.展开更多
Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-...Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-C_(3)N_(4) suffers from limited visible-light absorption and low charge-carrier mobility.In this study,a phosphorus-doped tubular carbon nitride(5P-TCN)was synthesized via a precursor self-assembly method using phosphoric acid and melamine as raw materials,eliminating the need for organic solvents or templates.The 5P-TCN catalyst demonstrated enhanced visible-light absorption,improved charge transfer capability,and a 5.25-fold increase in specific surface area(31.092 m^(2)/g),which provided abundant active sites to efficiently drive the PMS-assisted photocatalytic reaction.The 5P-TCN/vis/PMS system exhibited exceptional degradation performance for organic pollutants across a broad pH range(3–9),achieving over 92%degradation of Rhodamine B(RhB)within 15 min.Notably,the system retained>98%RhB degradation efficiency after three consecutive operational cycles,demonstrating robust operational stability and reusability.Moreover,key parameters influencing,active radi-cals,degradation pathways,and potential mechanisms for RhB degradation were systematically investigated.This work proposes a green and cost-effective strategy for developing high-efficiency photocatalysts,while demon-strating the exceptional capability of a PMS-assisted photocatalytic system for rapid degradation of RhB.展开更多
Traffic at urban intersections frequently encounters unexpected obstructions,resulting in congestion due to uncooperative and priority-based driving behavior.This paper presents an optimal right-turn coordination syst...Traffic at urban intersections frequently encounters unexpected obstructions,resulting in congestion due to uncooperative and priority-based driving behavior.This paper presents an optimal right-turn coordination system for Connected and Automated Vehicles(CAVs)at single-lane intersections,particularly in the context of left-hand side driving on roads.The goal is to facilitate smooth right turns for certain vehicles without creating bottlenecks.We consider that all approaching vehicles share relevant information through vehicular communications.The Intersection Coordination Unit(ICU)processes this information and communicates the optimal crossing or turning times to the vehicles.The primary objective of this coordination is to minimize overall traffic delays,which also helps improve the fuel consumption of vehicles.By considering information from upcoming vehicles at the intersection,the coordination system solves an optimization problem to determine the best timing for executing right turns,ultimately minimizing the total delay for all vehicles.The proposed coordination system is evaluated at a typical urban intersection,and its performance is compared to traditional traffic systems.Numerical simulation results indicate that the proposed coordination system significantly enhances the average traffic speed and fuel consumption compared to the traditional traffic system in various scenarios.展开更多
The precise tuning of magnetic nanoparticle size and magnetic domains,thereby shaping magnetic properties.However,the dynamic evolution mechanisms of magnetic domain configurations in relation to electromagnetic(EM)at...The precise tuning of magnetic nanoparticle size and magnetic domains,thereby shaping magnetic properties.However,the dynamic evolution mechanisms of magnetic domain configurations in relation to electromagnetic(EM)attenuation behavior remain poorly understood.To address this gap,a thermodynamically controlled periodic coordination strategy is proposed to achieve precise modulation of magnetic nanoparticle spacing.This approach unveils the evolution of magnetic domain configurations,progressing from individual to coupled and ultimately to crosslinked domain configurations.A unique magnetic coupling phenomenon surpasses the Snoek limit in low-frequency range,which is observed through micromagnetic simulation.The crosslinked magnetic configuration achieves effective low-frequency EM wave absorption at 3.68 GHz,encompassing nearly the entire C-band.This exceptional magnetic interaction significantly enhances radar camouflage and thermal insulation properties.Additionally,a robust gradient metamaterial design extends coverage across the full band(2–40 GHz),effectively mitigating the impact of EM pollution on human health and environment.This comprehensive study elucidates the evolution mechanisms of magnetic domain configurations,addresses gaps in dynamic magnetic modulation,and provides novel insights for the development of high-performance,low-frequency EM wave absorption materials.展开更多
Coordination-driven self-assembly was used to construct two metallacycles of a dicarboxylatefunctionalized dibenzo-18-crown-6 in combination with either a 0° anthracene-based clip-type acceptor or a 60° phen...Coordination-driven self-assembly was used to construct two metallacycles of a dicarboxylatefunctionalized dibenzo-18-crown-6 in combination with either a 0° anthracene-based clip-type acceptor or a 60° phenanthrene-based acceptor. The angularities of these moieties make them suitable for the formation of a [2 + 2] rectangle and a [3 + 3] triangle, respectively. The synthesis, characterization and host-vip chemistry of two metallacycles were described and supported by31P{1H},1H NMR spectra and electrospray mass spectrometry.展开更多
We herein report the synthesis and metal-directed coordination self-assembly behaviors of three new macrocyc- lic azacalix[4]aromatics that comprise various numbers of pyridine and pyrazine rings bridged by N-CH3 grou...We herein report the synthesis and metal-directed coordination self-assembly behaviors of three new macrocyc- lic azacalix[4]aromatics that comprise various numbers of pyridine and pyrazine rings bridged by N-CH3 groups. Structural characterization of 1--3 explored that their conformations are fluxional in solution and each adopts a 1,3-alternate configuration in crystalline solids. The macrocyclic skeletons in azacalixaromatic 1--3 afford a good platform to designedly arrange coordination sites in a unique way relative to conventional multidentate ligands. Solid-state structures of three coordination self-assembled silver complexes （13--15） of 1 --3 determined by X-ray crystallography suggest that the nitrogen atoms on procumbent aromatics have better coordination ability than those on perpendicular aromatics and dictate the whole coordination self-assemblies. Unique discrete and 1D chain-like structures were thus obtained. This system may afford a deeper insight into the coordination self-assembly studies of heteroatom-bridged calixaromatics, possibly extending potential application of this novel macrocyclic polyden- tate organic compounds in the synthesis of functional metal organic framework formation.展开更多
The novel one-dimensional coordination polymer {[Cu(L)2(H2O)]?2BF4?6H2O}∞ [1, L=1,2-bis(4-pyridinecarboxamido)ethane] was synthesized as single crystals and characterized by means of X-ray diffraction analysis, eleme...The novel one-dimensional coordination polymer {[Cu(L)2(H2O)]?2BF4?6H2O}∞ [1, L=1,2-bis(4-pyridinecarboxamido)ethane] was synthesized as single crystals and characterized by means of X-ray diffraction analysis, elemental analysis, IR spectroscopy and TG measurement. Structure 1 consists of looped chains. In addition, linked by hydrogen bonds, the one-dimensional chains were transformed into three-dimensional framework, which shows channels filled with anions and uncoordinated water molecules.展开更多
A novel coordination polymer {(C12H14N2)[Ag2I4]}n ([C12H14N2]2+ = N,N-1,2- ethyl-dipyridinium (EDP)) was synthesized by the reaction of AgI with EDP (pH = 6.5) at room temperature and structurally characterized by X-r...A novel coordination polymer {(C12H14N2)[Ag2I4]}n ([C12H14N2]2+ = N,N-1,2- ethyl-dipyridinium (EDP)) was synthesized by the reaction of AgI with EDP (pH = 6.5) at room temperature and structurally characterized by X-ray single-crystal diffraction analysis. The title compound crystallizes in monoclinic, space group P21/n with a = 7.278(2), b = 23.658(2), c = 12.038(2) , b = 98.25, V = 2051.3(7) 3, Z = 4, Dc = 2.945 g/cm3, F(000) = 1624, C12H14Ag2I4N2, Mr = 909.59, m(MoKa) = 7.922 mm-1, the final R = 0.0321 and wR = 0.0615 for 3079 observed reflections with I > 2s(I). The title compound consists of cations ([C12H14N2]2+) and anion chain (Ag2I42-) which are combined by static attracting forces in the crystal.展开更多
Two types of palladiu m(Ⅱ)-based metallacalixarenes[ML]^(2+)and[ML_(2)]^(2+)have been synthesized through coordination-driven self-assembly from a series of flexible pyridine-bridged diimidazole ligands[2,6-bis((1 H-...Two types of palladiu m(Ⅱ)-based metallacalixarenes[ML]^(2+)and[ML_(2)]^(2+)have been synthesized through coordination-driven self-assembly from a series of flexible pyridine-bridged diimidazole ligands[2,6-bis((1 H-imidazol-1-yl)methyl)pyridine(L^(1)),2,6-bis((1 H-benzo[d]imidazol-1-yl)methyl)pyridine(L^(2)),2,6-bis((1 H-naphtho[2,3-d]imidazol-1-yl)methyl)pyridine(L^(3))],with palladium(II)-based building blocks[Pd(BF_(4))_(2)(M^(1)-BF_4)and(tmeda)Pd(NO_(3))_(2)(M^(2)-NO_(3))(tmeda=N,N,N',N'-tetramethyl-ethylenediamine)].All complexes were characterized by NMR spectroscopy(^(1)H NMR and^(13)C NMR),mass spectrometry(CSIMS,ESI-HRMS)and elemental analysis.The single crystal X-ray diffraction analysis of[M^(1)L^(2)_2](NO_(3))_(2),[M^(1)L^(3)_2](NO_(3))_(2),[M^(1)L^(3)_2](PF_6)_2 and[M~2 L^(3)](NO_(3))_(2)further confirmed the uniquely single bowl-shape and double bowl-shape structures.The anion binding properties within the metallacalixarenes as receptors were also investigated by NMR titration experiments in DMSO.展开更多
Polymerase chain reactions(PCR)are a very important tool for use in cloning,nucleic acid sequencing and diagnostic testing.The storage conditions of PCR reagents are limited to freezing and a lot of mixing steps are n...Polymerase chain reactions(PCR)are a very important tool for use in cloning,nucleic acid sequencing and diagnostic testing.The storage conditions of PCR reagents are limited to freezing and a lot of mixing steps are needed.In this paper,we report using metal ions to form coordination nanomaterials with the intrinsic components of the PCR reagents including dNTP,DNA primers and DNA polymerase as an integrated PCR reaction system.To complete PCR reactions,users need only to dissolve the coordination nanomaterials with a buffer and add template DNA.A few transition metal ions were screened and Cu^(2+)was found to be the most effective metal ion for this purpose.Then the encapsulation efficiency of PCR reagents was measured,which can reach close to 100%for the primers and DNA polymerase,but only 10%for dNTP because dNTP was excess.Further study also exhibited this integrated PCR reaction system can be used for DNA detection with a similar detection limit to the normal PCR,and showed good stability of encapsulated PCR nanomaterial after storage for a week.展开更多
A novel coordination polymer(CP){[Cd_(2)(L)(1,4-bimb)_(1.5)(DMF)_(2)]·DMF}n(1)(H_(4)L=5,5'-[1,1'-biphenyl-4,4'-diylbis(oxy)]diisophthalic acid,1,4-bimb=1,4-bis(imidazole-1-ylmethyl)-benzene)has been d...A novel coordination polymer(CP){[Cd_(2)(L)(1,4-bimb)_(1.5)(DMF)_(2)]·DMF}n(1)(H_(4)L=5,5'-[1,1'-biphenyl-4,4'-diylbis(oxy)]diisophthalic acid,1,4-bimb=1,4-bis(imidazole-1-ylmethyl)-benzene)has been designed and synthesized through solvothermal reaction.Structural analysis shows that Cd(Ⅱ)is connected by H4L and 1,4-bimb to form a 2D network,and 1,4-bimb further expands the 2D network into a 3D framework.CP 1 can be used as an excellent fluorescence sensor for Fe^(3+)and 4-nitrophenol(4-NP),with low detection limits and good anti-interference.The detection limits of Fe^(3+)and 4-NP were 0.034 and 0.031μmol·L^(-1),respectively.In addition,the fluorescence quenching mechanism was studied.1 was successfully applied to determine Fe^(3+)and 4-NP content in the Yanhe River water sample.CCDC:2351092.展开更多
Studying the coupling coordination development of new energy vehicles(NEVs)and the ecological environment in China is helpful in promoting the development of NEVs in the country and is of great significance in promoti...Studying the coupling coordination development of new energy vehicles(NEVs)and the ecological environment in China is helpful in promoting the development of NEVs in the country and is of great significance in promoting high-quality development of new energy in China.This paper constructs an evaluation index system for the development of NEVs and the ecological environment.It uses game theory combining weighting model,particle swarm optimized projection tracking evaluation model,coupling coordination degree model,and machine learning algorithms to calculate and analyze the level of coupling coordination development of NEVs and the ecological environment in China from 2010 to 2021,and identifies the driving factors.The research results show that:(i)From 2010 to 2021,the development index of NEVs in China has steadily increased from 0.085 to 0.634,while the ecological environment level index significantly rose from 0.170 to 0.884,reflecting the continuous development of China in both NEVs and the ecological environment.(ii)From 2010 to 2012,the two systems—new energy vehicle(NEV)development and the ecological environment—were in a period of imbalance and decline.From 2013 to 2016,they underwent a transition period,and from 2017 to 2021,they entered a period of coordinated development showing a trend of benign and continuous improvement.By 2021,they reached a good level of coordination.(iii)Indicators such as the number of patents granted for NEVs,water consumption per unit of GDP,and energy consumption per unit of GDP are the main driving factors affecting the coupling coordination development of NEVs and the ecological environment in China.展开更多
Recently,hollow carbon nanospheres(HCSs)have garnered significant attention as potential Li metal hosts owing to their unique large voids and ease of fabrication.However,similar to other nanoscale hosts,their practica...Recently,hollow carbon nanospheres(HCSs)have garnered significant attention as potential Li metal hosts owing to their unique large voids and ease of fabrication.However,similar to other nanoscale hosts,their practical performance is limited by inhomogeneous agglomeration,increased binder requirements,and high tortuosity within the electrode.To overcome these problems and high tortuosity within the electrode,this study introduces a pomegranate-like carbon microcluster composed of primary HCSs(P-CMs)as a novel Li metal host.This unique nanostructure can be easily prepared using the spray-drying technique,enabling its mass production.Comprehensive analyses with various tools demonstrate that compared with HCS hosts,the P-CM host requires a smaller amount of binder to fabricate a sufficiently robust and even surface electrode.Furthermore,owing to reduced tortuosity,the well-designed P-CM electrode can provide continuous and shortened pathways for electron/ion transport,accelerating the Li-ion transfer kinetics and prohibiting preferential Li plating at the upper region of the electrode.Due to these characteristics,Li metal can be effectively encapsulated in the large inner voids of the primary HCSs constituting the P-CM,thereby enhancing the electrochemical performance of P-CM hosts in Li metal batteries.Specifically,the Coulombic efficiency of the P-CM host can be maintained at 97%over 100 cycles,with a high Li deposition areal capacity of 3 mAh·cm^(-2)and long cycle life(1000 h,1 mA·cm^(-2),and 1.0 mAh·cm^(-2)).Furthermore,a full cell incorporating a LiFePO4 cathode exhibits excellent cycle life.展开更多
With the boom in maritime activities,the need for highly reliable maritime communication is becoming urgent,which is an important component of 5G/6G communication networks.However,the bandwidth reuse characteristic of...With the boom in maritime activities,the need for highly reliable maritime communication is becoming urgent,which is an important component of 5G/6G communication networks.However,the bandwidth reuse characteristic of 5G/6G networks will inevitably lead to severe interference,resulting in degradation in the communication performance of maritime users.In this paper,we propose a safe deep reinforcement learning based interference coordination scheme to jointly optimize the power control and bandwidth allocation in maritime communication systems,and exploit the quality-of-service requirements of users as the risk value references to evaluate the communication policies.In particular,this scheme designs a deep neural network to select the communication policies through the evaluation network and update the parameters using the target network,which improves the communication performance and speeds up the convergence rate.Moreover,the Nash equilibrium of the interference coordination game and the computational complexity of the proposed scheme are analyzed.Simulation and experimental results verify the performance gain of the proposed scheme compared with benchmarks.展开更多
The high incidence and mortality of lung cancer have present threaten in front of people all over the world.Researches in clinical trials find that mutations of some genes influence progress of lung cancer directly or...The high incidence and mortality of lung cancer have present threaten in front of people all over the world.Researches in clinical trials find that mutations of some genes influence progress of lung cancer directly or indirectly,therefore,some kinds of molecular inhibitors benefit patients in clinical therapy,which helpfully prolong survival time of patients and show great potential in lung cancer therapy.siRNA is a kind of nucleic acid molecules which can silence targeted gene translation through binding to mRNA completely to cure diseases.The delivery of siRNA for cancer therapy mostly can be classified into loading through electrostatic interaction,physical surrounding,and chemically modification.Yet delivering siRNA by coordination has not been reported.This study unprecedently utilizes the coordination between siRNA and Fe^(2+)to form a self-assembly structure in which doxorobicin(DOX) and human serum albumin(HSA) were used to stabilize the whole nanoplatform followed polyethylenimine(PEI) coating.Through the heat incubation strategy,highly loading efficiency for siRNA and DOX was achieved.This nanoplatform with stability and sustain release of drugs exhibited good lysosome escape,gene silencing effect and cytotoxicity which provided new horizon for co-deli very of siRNA and other molecular or protein drugs.展开更多
Four glycoluril-based amphiphilic molecular clips(AMCs)M1~M4 have been prepared for intracellular delivery of short DNA.M1~M4 have two methyl groups on its convex surface and four cations on its aromatic side arm,whic...Four glycoluril-based amphiphilic molecular clips(AMCs)M1~M4 have been prepared for intracellular delivery of short DNA.M1~M4 have two methyl groups on its convex surface and four cations on its aromatic side arm,which can be used to construct self-assembled nanoparticles in aqueous solution driven by hydrophobic interaction.Dynamic light scattering experiments show that M1 and M2 can be driven hydrophobically to aggregate into extremely stable nanoparticles in water at the micromolar concentrations.Fluorescence titration and zeta potential experiments support that the nanoparticles formed by M1 and M2 are able to efficiently encapsulate short DNA(sDNA).Fluorescence imaging and flow cytometry studies reveal that their nano sizes enable intracellular delivery of the encapsulated sDNA into both normal and cancer cells,with delivery percentage reaching up to 94%,while in vitro experiments indicate that the two compounds have excellent biocompatibility and low cytotoxicity.展开更多
One Yb(Ⅲ)-based coordination polymer,{[Yb(H_(2)dhtp)1.5(H_(2)O)_(4)]·3H_(2)O}n(1)(H_(4)dhtp=2,5-dihydroxytere-phthalic acid),was fabricated and structurally characterized by single-crystal X-ray diffraction,IR,p...One Yb(Ⅲ)-based coordination polymer,{[Yb(H_(2)dhtp)1.5(H_(2)O)_(4)]·3H_(2)O}n(1)(H_(4)dhtp=2,5-dihydroxytere-phthalic acid),was fabricated and structurally characterized by single-crystal X-ray diffraction,IR,powder X-ray diffraction,X-ray diffraction,and elemental analysis.Complex 1 displays a 1D chain structure,and belongs to P1 group.The solid-state luminescent spectrum of 1 showed an emission band with the maximum at 508 nm(λex=408 nm).It exhibited the emission characteristic of the H_(4)dhtp ligand.The fluorescence of 1 in water displayed the stron-gest intensity.In detecting various metal ions,adding Zr^(4+)led to a blue shift in fluorescence,accompanied by an increase in intensity,whereas the presence of Fe^(3+)resulted in a decrease in luminescence.The changes observed in the IR spectrum indicate an interaction between Fe^(3+)/Zr^(4+)and complex 1,resulting in the variation of luminescence properties.展开更多
Three monomers,namely A2,B2,and GH,were designed and synthesized.By utilizing double host-vip interactions,the monomers A2+B2+GH underwent self-assembly to form a supramolecular linear polymer(SLP)at high concentrat...Three monomers,namely A2,B2,and GH,were designed and synthesized.By utilizing double host-vip interactions,the monomers A2+B2+GH underwent self-assembly to form a supramolecular linear polymer(SLP)at high concentrations.Long fibers could be pulled from the concentrated SLP solution.Upon the addition of PdCl_(2)(PhCN)_(2)into the SLP solution,a structural transformation occurred from SLP to a supramolecular crosslinked polymer(SCP)through metal coordination interaction.This transformation induced fluorescence quenching,test paper strips for ion detection experiment confirmed that the SLP had good detection ability for Pd^(2+).Furthermore,the SCP underwent a transformation into a gel when the concentration exceeded 145 mmol/L.The SCP gel demonstrated sensitivity to different stimuli,such as K^(+)ions and changes in temperature,accompanied by a reversible transition between sol and gel states.Additionally,rheological analyses indicated that the gel possessed favorable self-healing properties.展开更多
文摘Under the condition of solvothermal synthesis,the viologen ligand 1,1′-bis(3-carboxyphenyl)-(4,4′-bipyri-dine)dichloride(H_(2)bcbpy·2Cl)and KI are coordinated with the metal cadmium ions.A case of thermochromic coor-dination polymer[Cd(bcbpy)I_(2)]·2H_(2)O(1)was constructed.Complex 1 displays a 1D chain structure and exhibits thermochromic behavior.Under different temperature stimulation,the complex(ground)slowly changed from green to yellow-green,and with the increase of temperature,the color of complex 1 gradually deepened,and finally became orange-yellow.Therefore,complex 1 was prepared as a thermochromic film.In addition,we also performed electrochemical tests on complex 1,which showed that the complex is a semiconductor material.CCDC:2391802.
基金supported by the National Natural Science Foundation of China(22105033,22105192)the National Key Research and Development Program of China(2023YFA1506300)+1 种基金the Programme of Introducing Talents of Discipline to Universities(B17020)the Jilin Province Science and Technology Development Plan(YDZJ202101ZYTS137,20210101123JC).
文摘Mesoporous metals with large surface area,high pore volume,and uniform pore structure hold excellent advantages for various applications.However,the state-of-the-art synthesis methods are still limited to wet chemistry,which requires excessive solvents and a time-consuming drying process.Here,we report a facile and general mechanochemical coordination self-assembly strategy to prepare mesoporous metals(e.g.,Rh,Ru,Ir,Pt,Pd,Ag,Co,and Ni)with remarkable porous properties by using metal chlorides and cationic polymer interplay.Compared with the wet chemistry process,this method proceeds without solvents and does not need complicated experimental conditions and long synthetic periods,which not only greatly reduces the consumption of cost and energy and environmental pollution,but also improves the synthesis efficiency and yield of target products.We believe the developed approach will provide a general pathway for the scalable preparation of advanced porous materials.
基金financially supported by the National Natural Science Foundation of China(Nos.21072099,21202084 and 21372120)
文摘A tin-oxygen coordination driving self-assembly was developed in the block copolymers containing organotin, which were prepared by the radical addition-fraction transfer（RAFT） method and characterized by the gel-permeation chromatography（GPC） and 1H-NMR. And the self-assemblies of these block copolymers with various chain length ratios in the different concentrations in CHCl3 were stable according to the results of DLS and TEM. Additionally, it was also given an insight investigation on the regulation of self-assembly of the block copolymers by adding dibutyltin dichloride and a possible mechanism was proposed.
文摘Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-C_(3)N_(4) suffers from limited visible-light absorption and low charge-carrier mobility.In this study,a phosphorus-doped tubular carbon nitride(5P-TCN)was synthesized via a precursor self-assembly method using phosphoric acid and melamine as raw materials,eliminating the need for organic solvents or templates.The 5P-TCN catalyst demonstrated enhanced visible-light absorption,improved charge transfer capability,and a 5.25-fold increase in specific surface area(31.092 m^(2)/g),which provided abundant active sites to efficiently drive the PMS-assisted photocatalytic reaction.The 5P-TCN/vis/PMS system exhibited exceptional degradation performance for organic pollutants across a broad pH range(3–9),achieving over 92%degradation of Rhodamine B(RhB)within 15 min.Notably,the system retained>98%RhB degradation efficiency after three consecutive operational cycles,demonstrating robust operational stability and reusability.Moreover,key parameters influencing,active radi-cals,degradation pathways,and potential mechanisms for RhB degradation were systematically investigated.This work proposes a green and cost-effective strategy for developing high-efficiency photocatalysts,while demon-strating the exceptional capability of a PMS-assisted photocatalytic system for rapid degradation of RhB.
基金supported by the Japan Society for the Promotion of Science(JSPS)Grants-in-Aid for Scientific Research(C)23K03898.
文摘Traffic at urban intersections frequently encounters unexpected obstructions,resulting in congestion due to uncooperative and priority-based driving behavior.This paper presents an optimal right-turn coordination system for Connected and Automated Vehicles(CAVs)at single-lane intersections,particularly in the context of left-hand side driving on roads.The goal is to facilitate smooth right turns for certain vehicles without creating bottlenecks.We consider that all approaching vehicles share relevant information through vehicular communications.The Intersection Coordination Unit(ICU)processes this information and communicates the optimal crossing or turning times to the vehicles.The primary objective of this coordination is to minimize overall traffic delays,which also helps improve the fuel consumption of vehicles.By considering information from upcoming vehicles at the intersection,the coordination system solves an optimization problem to determine the best timing for executing right turns,ultimately minimizing the total delay for all vehicles.The proposed coordination system is evaluated at a typical urban intersection,and its performance is compared to traditional traffic systems.Numerical simulation results indicate that the proposed coordination system significantly enhances the average traffic speed and fuel consumption compared to the traditional traffic system in various scenarios.
基金supported by the National Natural Science Foundation of China(22265021,52231007,and 12327804)the Aeronautical Science Foundation of China(2020Z056056003)Jiangxi Provincial Natural Science Foundation(20232BAB212004).
文摘The precise tuning of magnetic nanoparticle size and magnetic domains,thereby shaping magnetic properties.However,the dynamic evolution mechanisms of magnetic domain configurations in relation to electromagnetic(EM)attenuation behavior remain poorly understood.To address this gap,a thermodynamically controlled periodic coordination strategy is proposed to achieve precise modulation of magnetic nanoparticle spacing.This approach unveils the evolution of magnetic domain configurations,progressing from individual to coupled and ultimately to crosslinked domain configurations.A unique magnetic coupling phenomenon surpasses the Snoek limit in low-frequency range,which is observed through micromagnetic simulation.The crosslinked magnetic configuration achieves effective low-frequency EM wave absorption at 3.68 GHz,encompassing nearly the entire C-band.This exceptional magnetic interaction significantly enhances radar camouflage and thermal insulation properties.Additionally,a robust gradient metamaterial design extends coverage across the full band(2–40 GHz),effectively mitigating the impact of EM pollution on human health and environment.This comprehensive study elucidates the evolution mechanisms of magnetic domain configurations,addresses gaps in dynamic magnetic modulation,and provides novel insights for the development of high-performance,low-frequency EM wave absorption materials.
基金the National Natural Science Foundation of China (Nos. 22071040 and 21773052)the Natural Science Foundation of Zhejiang Province (No. LY22B040001)+1 种基金the Science & Technology Innovation Program of Zhejiang Province (No. 2018R52051)the National Natural Science Foundation of China (Nos. 22035006 and 21620102006) for financial support。
文摘Coordination-driven self-assembly was used to construct two metallacycles of a dicarboxylatefunctionalized dibenzo-18-crown-6 in combination with either a 0° anthracene-based clip-type acceptor or a 60° phenanthrene-based acceptor. The angularities of these moieties make them suitable for the formation of a [2 + 2] rectangle and a [3 + 3] triangle, respectively. The synthesis, characterization and host-vip chemistry of two metallacycles were described and supported by31P{1H},1H NMR spectra and electrospray mass spectrometry.
基金Financial support by the National Natural Science Foundation of China，the National Basic Research Program of China (973 program,2011CB932501 and 2013CB834501) is gratefully acknowledged.This work is also supported by Tsinghua University Initiative Scientific Research Program
文摘We herein report the synthesis and metal-directed coordination self-assembly behaviors of three new macrocyc- lic azacalix[4]aromatics that comprise various numbers of pyridine and pyrazine rings bridged by N-CH3 groups. Structural characterization of 1--3 explored that their conformations are fluxional in solution and each adopts a 1,3-alternate configuration in crystalline solids. The macrocyclic skeletons in azacalixaromatic 1--3 afford a good platform to designedly arrange coordination sites in a unique way relative to conventional multidentate ligands. Solid-state structures of three coordination self-assembled silver complexes （13--15） of 1 --3 determined by X-ray crystallography suggest that the nitrogen atoms on procumbent aromatics have better coordination ability than those on perpendicular aromatics and dictate the whole coordination self-assemblies. Unique discrete and 1D chain-like structures were thus obtained. This system may afford a deeper insight into the coordination self-assembly studies of heteroatom-bridged calixaromatics, possibly extending potential application of this novel macrocyclic polyden- tate organic compounds in the synthesis of functional metal organic framework formation.
文摘The novel one-dimensional coordination polymer {[Cu(L)2(H2O)]?2BF4?6H2O}∞ [1, L=1,2-bis(4-pyridinecarboxamido)ethane] was synthesized as single crystals and characterized by means of X-ray diffraction analysis, elemental analysis, IR spectroscopy and TG measurement. Structure 1 consists of looped chains. In addition, linked by hydrogen bonds, the one-dimensional chains were transformed into three-dimensional framework, which shows channels filled with anions and uncoordinated water molecules.
基金This work was supported by the Foundation of Education Committee of Fujian province (JB01020)
文摘A novel coordination polymer {(C12H14N2)[Ag2I4]}n ([C12H14N2]2+ = N,N-1,2- ethyl-dipyridinium (EDP)) was synthesized by the reaction of AgI with EDP (pH = 6.5) at room temperature and structurally characterized by X-ray single-crystal diffraction analysis. The title compound crystallizes in monoclinic, space group P21/n with a = 7.278(2), b = 23.658(2), c = 12.038(2) , b = 98.25, V = 2051.3(7) 3, Z = 4, Dc = 2.945 g/cm3, F(000) = 1624, C12H14Ag2I4N2, Mr = 909.59, m(MoKa) = 7.922 mm-1, the final R = 0.0321 and wR = 0.0615 for 3079 observed reflections with I > 2s(I). The title compound consists of cations ([C12H14N2]2+) and anion chain (Ag2I42-) which are combined by static attracting forces in the crystal.
基金supported by the National Natural Science Foundation of China(No.21906002)Beijing Municipal Science and Technology Project(No.KM202010005010)+2 种基金Beijing Municipal Natural Science Fund Project of Beijing Education Committee science and technology project key project(No.KZ201710005001)Beijing municipal high level innovative team building program(No.IDHT20180504)Beijing Outstanding Young Scientist Program(No.BJJWZYJH01201910005017)。
文摘Two types of palladiu m(Ⅱ)-based metallacalixarenes[ML]^(2+)and[ML_(2)]^(2+)have been synthesized through coordination-driven self-assembly from a series of flexible pyridine-bridged diimidazole ligands[2,6-bis((1 H-imidazol-1-yl)methyl)pyridine(L^(1)),2,6-bis((1 H-benzo[d]imidazol-1-yl)methyl)pyridine(L^(2)),2,6-bis((1 H-naphtho[2,3-d]imidazol-1-yl)methyl)pyridine(L^(3))],with palladium(II)-based building blocks[Pd(BF_(4))_(2)(M^(1)-BF_4)and(tmeda)Pd(NO_(3))_(2)(M^(2)-NO_(3))(tmeda=N,N,N',N'-tetramethyl-ethylenediamine)].All complexes were characterized by NMR spectroscopy(^(1)H NMR and^(13)C NMR),mass spectrometry(CSIMS,ESI-HRMS)and elemental analysis.The single crystal X-ray diffraction analysis of[M^(1)L^(2)_2](NO_(3))_(2),[M^(1)L^(3)_2](NO_(3))_(2),[M^(1)L^(3)_2](PF_6)_2 and[M~2 L^(3)](NO_(3))_(2)further confirmed the uniquely single bowl-shape and double bowl-shape structures.The anion binding properties within the metallacalixarenes as receptors were also investigated by NMR titration experiments in DMSO.
基金the Natural Sciences and Engineering Research Council of Canada(NSERC)the National Natural Science Foundation of China(Nos.31901776 and 32072181)+1 种基金Agricultural Science and Technology Innovation Program(No.CAAS-ASTIP-2021-IFST-SN2021-05)received a China Scholarship Council(CSC)Scholarship to visit the University of Waterloo。
文摘Polymerase chain reactions(PCR)are a very important tool for use in cloning,nucleic acid sequencing and diagnostic testing.The storage conditions of PCR reagents are limited to freezing and a lot of mixing steps are needed.In this paper,we report using metal ions to form coordination nanomaterials with the intrinsic components of the PCR reagents including dNTP,DNA primers and DNA polymerase as an integrated PCR reaction system.To complete PCR reactions,users need only to dissolve the coordination nanomaterials with a buffer and add template DNA.A few transition metal ions were screened and Cu^(2+)was found to be the most effective metal ion for this purpose.Then the encapsulation efficiency of PCR reagents was measured,which can reach close to 100%for the primers and DNA polymerase,but only 10%for dNTP because dNTP was excess.Further study also exhibited this integrated PCR reaction system can be used for DNA detection with a similar detection limit to the normal PCR,and showed good stability of encapsulated PCR nanomaterial after storage for a week.
文摘A novel coordination polymer(CP){[Cd_(2)(L)(1,4-bimb)_(1.5)(DMF)_(2)]·DMF}n(1)(H_(4)L=5,5'-[1,1'-biphenyl-4,4'-diylbis(oxy)]diisophthalic acid,1,4-bimb=1,4-bis(imidazole-1-ylmethyl)-benzene)has been designed and synthesized through solvothermal reaction.Structural analysis shows that Cd(Ⅱ)is connected by H4L and 1,4-bimb to form a 2D network,and 1,4-bimb further expands the 2D network into a 3D framework.CP 1 can be used as an excellent fluorescence sensor for Fe^(3+)and 4-nitrophenol(4-NP),with low detection limits and good anti-interference.The detection limits of Fe^(3+)and 4-NP were 0.034 and 0.031μmol·L^(-1),respectively.In addition,the fluorescence quenching mechanism was studied.1 was successfully applied to determine Fe^(3+)and 4-NP content in the Yanhe River water sample.CCDC:2351092.
基金Supported by the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX24_0102)the China Scholarship Council Program(202406190114)。
文摘Studying the coupling coordination development of new energy vehicles(NEVs)and the ecological environment in China is helpful in promoting the development of NEVs in the country and is of great significance in promoting high-quality development of new energy in China.This paper constructs an evaluation index system for the development of NEVs and the ecological environment.It uses game theory combining weighting model,particle swarm optimized projection tracking evaluation model,coupling coordination degree model,and machine learning algorithms to calculate and analyze the level of coupling coordination development of NEVs and the ecological environment in China from 2010 to 2021,and identifies the driving factors.The research results show that:(i)From 2010 to 2021,the development index of NEVs in China has steadily increased from 0.085 to 0.634,while the ecological environment level index significantly rose from 0.170 to 0.884,reflecting the continuous development of China in both NEVs and the ecological environment.(ii)From 2010 to 2012,the two systems—new energy vehicle(NEV)development and the ecological environment—were in a period of imbalance and decline.From 2013 to 2016,they underwent a transition period,and from 2017 to 2021,they entered a period of coordinated development showing a trend of benign and continuous improvement.By 2021,they reached a good level of coordination.(iii)Indicators such as the number of patents granted for NEVs,water consumption per unit of GDP,and energy consumption per unit of GDP are the main driving factors affecting the coupling coordination development of NEVs and the ecological environment in China.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.2020R1C1C1003375)。
文摘Recently,hollow carbon nanospheres(HCSs)have garnered significant attention as potential Li metal hosts owing to their unique large voids and ease of fabrication.However,similar to other nanoscale hosts,their practical performance is limited by inhomogeneous agglomeration,increased binder requirements,and high tortuosity within the electrode.To overcome these problems and high tortuosity within the electrode,this study introduces a pomegranate-like carbon microcluster composed of primary HCSs(P-CMs)as a novel Li metal host.This unique nanostructure can be easily prepared using the spray-drying technique,enabling its mass production.Comprehensive analyses with various tools demonstrate that compared with HCS hosts,the P-CM host requires a smaller amount of binder to fabricate a sufficiently robust and even surface electrode.Furthermore,owing to reduced tortuosity,the well-designed P-CM electrode can provide continuous and shortened pathways for electron/ion transport,accelerating the Li-ion transfer kinetics and prohibiting preferential Li plating at the upper region of the electrode.Due to these characteristics,Li metal can be effectively encapsulated in the large inner voids of the primary HCSs constituting the P-CM,thereby enhancing the electrochemical performance of P-CM hosts in Li metal batteries.Specifically,the Coulombic efficiency of the P-CM host can be maintained at 97%over 100 cycles,with a high Li deposition areal capacity of 3 mAh·cm^(-2)and long cycle life(1000 h,1 mA·cm^(-2),and 1.0 mAh·cm^(-2)).Furthermore,a full cell incorporating a LiFePO4 cathode exhibits excellent cycle life.
文摘With the boom in maritime activities,the need for highly reliable maritime communication is becoming urgent,which is an important component of 5G/6G communication networks.However,the bandwidth reuse characteristic of 5G/6G networks will inevitably lead to severe interference,resulting in degradation in the communication performance of maritime users.In this paper,we propose a safe deep reinforcement learning based interference coordination scheme to jointly optimize the power control and bandwidth allocation in maritime communication systems,and exploit the quality-of-service requirements of users as the risk value references to evaluate the communication policies.In particular,this scheme designs a deep neural network to select the communication policies through the evaluation network and update the parameters using the target network,which improves the communication performance and speeds up the convergence rate.Moreover,the Nash equilibrium of the interference coordination game and the computational complexity of the proposed scheme are analyzed.Simulation and experimental results verify the performance gain of the proposed scheme compared with benchmarks.
基金financially supported by the Program for International S and T Cooperation Projects of the Ministry of Science and Technology of China (No.2018YFE0117200)the National Natural Science Foundation of China (No.31971318)+1 种基金the Special Project for Research and Development in Key Areas of Guangdong Province (No.2020B0101020001)the StrategicPriority Research Program of Chinese Academy of Sciences (No.XDB36000000)。
文摘The high incidence and mortality of lung cancer have present threaten in front of people all over the world.Researches in clinical trials find that mutations of some genes influence progress of lung cancer directly or indirectly,therefore,some kinds of molecular inhibitors benefit patients in clinical therapy,which helpfully prolong survival time of patients and show great potential in lung cancer therapy.siRNA is a kind of nucleic acid molecules which can silence targeted gene translation through binding to mRNA completely to cure diseases.The delivery of siRNA for cancer therapy mostly can be classified into loading through electrostatic interaction,physical surrounding,and chemically modification.Yet delivering siRNA by coordination has not been reported.This study unprecedently utilizes the coordination between siRNA and Fe^(2+)to form a self-assembly structure in which doxorobicin(DOX) and human serum albumin(HSA) were used to stabilize the whole nanoplatform followed polyethylenimine(PEI) coating.Through the heat incubation strategy,highly loading efficiency for siRNA and DOX was achieved.This nanoplatform with stability and sustain release of drugs exhibited good lysosome escape,gene silencing effect and cytotoxicity which provided new horizon for co-deli very of siRNA and other molecular or protein drugs.
文摘Four glycoluril-based amphiphilic molecular clips(AMCs)M1~M4 have been prepared for intracellular delivery of short DNA.M1~M4 have two methyl groups on its convex surface and four cations on its aromatic side arm,which can be used to construct self-assembled nanoparticles in aqueous solution driven by hydrophobic interaction.Dynamic light scattering experiments show that M1 and M2 can be driven hydrophobically to aggregate into extremely stable nanoparticles in water at the micromolar concentrations.Fluorescence titration and zeta potential experiments support that the nanoparticles formed by M1 and M2 are able to efficiently encapsulate short DNA(sDNA).Fluorescence imaging and flow cytometry studies reveal that their nano sizes enable intracellular delivery of the encapsulated sDNA into both normal and cancer cells,with delivery percentage reaching up to 94%,while in vitro experiments indicate that the two compounds have excellent biocompatibility and low cytotoxicity.
文摘One Yb(Ⅲ)-based coordination polymer,{[Yb(H_(2)dhtp)1.5(H_(2)O)_(4)]·3H_(2)O}n(1)(H_(4)dhtp=2,5-dihydroxytere-phthalic acid),was fabricated and structurally characterized by single-crystal X-ray diffraction,IR,powder X-ray diffraction,X-ray diffraction,and elemental analysis.Complex 1 displays a 1D chain structure,and belongs to P1 group.The solid-state luminescent spectrum of 1 showed an emission band with the maximum at 508 nm(λex=408 nm).It exhibited the emission characteristic of the H_(4)dhtp ligand.The fluorescence of 1 in water displayed the stron-gest intensity.In detecting various metal ions,adding Zr^(4+)led to a blue shift in fluorescence,accompanied by an increase in intensity,whereas the presence of Fe^(3+)resulted in a decrease in luminescence.The changes observed in the IR spectrum indicate an interaction between Fe^(3+)/Zr^(4+)and complex 1,resulting in the variation of luminescence properties.
基金supported by the National Natural Science Foundation of China(Nos.22161020,22022107,21801100)the Natural Science Foundation of Jiangxi Province(No.20212BAB203014)the Program of Qingjiang Excellent Young Talents,Jiangxi University of Science and Technology。
文摘Three monomers,namely A2,B2,and GH,were designed and synthesized.By utilizing double host-vip interactions,the monomers A2+B2+GH underwent self-assembly to form a supramolecular linear polymer(SLP)at high concentrations.Long fibers could be pulled from the concentrated SLP solution.Upon the addition of PdCl_(2)(PhCN)_(2)into the SLP solution,a structural transformation occurred from SLP to a supramolecular crosslinked polymer(SCP)through metal coordination interaction.This transformation induced fluorescence quenching,test paper strips for ion detection experiment confirmed that the SLP had good detection ability for Pd^(2+).Furthermore,the SCP underwent a transformation into a gel when the concentration exceeded 145 mmol/L.The SCP gel demonstrated sensitivity to different stimuli,such as K^(+)ions and changes in temperature,accompanied by a reversible transition between sol and gel states.Additionally,rheological analyses indicated that the gel possessed favorable self-healing properties.
