Environment-sensitive fluorescent probes are commonly utilized in various fields,including fluorescence sensing and imaging.This paper describes the synthesis and photophysical properties of a novel class of solvatoch...Environment-sensitive fluorescent probes are commonly utilized in various fields,including fluorescence sensing and imaging.This paper describes the synthesis and photophysical properties of a novel class of solvatochromic fluorophores that incorporate biisoindolylidene as the core backbone.This study investigates the structure-property relationships of these newly developed fluorophores.The central biisoindolylidene acts as an efficient electron acceptor,and by modifying the aryl ring substituent at the 3,3 position,the photophysical properties of the fluorophores can be significantly enhanced,particularly in terms of photoluminescence quantum efficiency.Furthermore,when an electron-donor group replaces the aryl ring at the 3,3 position,intriguing solvatochromic behavior is observed.This leads to a red-shift in the maximum emission wavelength and an increase in the Stokes shift with increasing solvent polarity.In solvent dimethyl sulfoxide(DMSO),the maximum emission wavelength can reach up to 750 nm,with a Stokes shift of approximately 150 nm.Finally,the potential application of the fluorophore in the detection of volatile acids is explored in a preliminary manner.展开更多
Binary mixtures of 1,3-dialkylimidazolium based ionic liquids (ILs) and water were selected as solvent systems to investigate the solute-solvent and solvent-solvent interactions on the preferential solvation of solv...Binary mixtures of 1,3-dialkylimidazolium based ionic liquids (ILs) and water were selected as solvent systems to investigate the solute-solvent and solvent-solvent interactions on the preferential solvation of solvatochromic indicators at 25 ℃. Empirical solvatochromic pa- rameters, dipolarity/polarizability (π^*), hydrogen-bond donor acidity (α), hydrogen-bond acceptor basicity (β), and Reichardt's polarity parameters (ET^N) were measured from the ultraviolet-visible spectral shifts of 4-nitroaniline, 4-nitroanisole, and Reichardt's dye. The solvent properties of the IL-water mixtures were found to be influenced by IL type and IL mole fraction (XIL). All these studied systems showed the non-ideal behavior. The max- imum deviation to ideality for the solvatochromic parameters can be obtained in the XIL range from 0.i to 0.3. For most of the binary mixtures, the π^* values showed the synergistic effects instead of the ETN, α and β values. The observed synergy extent was dependent on the studied systems, such as the dye indicator and IL type. A preferential solvation model was utilized to gather information on the molecular interactions in the mixtures. The dye indicator was preferentially solvated on the following trend: IL〉IL-water complex〉water.展开更多
Solvatochromic materials have recently attracted increasing attention owing to their great significance in the security and sensor fields.In this study,ultrafast explicit and implicit information was collected regardi...Solvatochromic materials have recently attracted increasing attention owing to their great significance in the security and sensor fields.In this study,ultrafast explicit and implicit information was collected regarding a fluorescent nanocellulose membrane produced from nanocellulose membranes coated with a Zn-terpyridine complex(Zn-tpy)in a layer-by-layer manner.The fluorescent emissions of the nanocellulose membrane changed from yellow(CIE:x=0.37,y=0.45)to green(CIE:x=0.32,y=0.47)under a dichloromethane environment and 365-nm irradiation.Due to the ease of dichloromethane volatilization,fluorescent emissions quickly returned to the original state.These solvatochromic nanocellulose membranes,with ultrafast explicit and implicit information,exhibited valuable application prospects in anti-counterfeiting techniques.展开更多
Hexakis(4-methoxyphenyl)benzene (HPB-OMe(1)) and hexakis(2,6-dimethyl-4-methoxyphenyl)benzene (HPB-OMe(2)) were synthesized via organometallic complex catalysis. The treatment of HPB-OMe(1) with FeCl3 caused cyclodehy...Hexakis(4-methoxyphenyl)benzene (HPB-OMe(1)) and hexakis(2,6-dimethyl-4-methoxyphenyl)benzene (HPB-OMe(2)) were synthesized via organometallic complex catalysis. The treatment of HPB-OMe(1) with FeCl3 caused cyclodehydrogenation at two positions to yield an oligophenylene with an indeno[1,2-b]fluorene structure (IF-OMe). Deprotection of the methoxy groups of these compounds was conducted by treatment with BBr3. Deprotonation of the OH groups of HPB-OH(1), HPB-OH(2), and IF-OH through treatment with NaH caused a bathochromic shift in the absorption and photoluminescence (PL) peaks. The bathochromic shift of the deprotonated species increased with the donor number (DN) of the solvents. These observations can be explained as the consequence of intramolecular charge transfer (ICT) from the ONa groups to the inner benzene rings.展开更多
In this study,we present a novel multicomponent self-assembly approach that offers good potential for crafting heterometallic complexes with exceptional constitutional control.This method generates metal ions from a s...In this study,we present a novel multicomponent self-assembly approach that offers good potential for crafting heterometallic complexes with exceptional constitutional control.This method generates metal ions from a sacrificial anode by using an electric field,which then coordinates with a metal complex precursor.As a proof-of-concept demonstration,we successfully synthesized single crystals of a heterometallic platinum(Ⅱ)-copper(Ⅰ)(Pt[Ⅱ]-Cu[Ⅰ])complex at an exceptionally rapid rate within 30 s by applying a voltage to an acetonitrile solution of[Pt(ppy)(CN)_(2)]^(−)Bu_(4)N^(+),using copper foil as the anode.Intriguingly,by finely adjusting the intensity and duration of the electric field,we achieved a variety of supramolecular structures,spanning from spherical to rod-like and even flower-like morphologies.Additionally,we found that the photoluminescence property of the resultant crystal can be reversibly shifted among green,orange,and cyan by merely altering the solvent environment.Finally,the crafted heterometallic Pt(Ⅱ)-Cu(Ⅰ)complex has shown great promise in advanced anti-counterfeiting applications.展开更多
The robustness of blood filtration in the kidney is supported by two major functions:the molecular sieve of the glomerulus and reabsorption of the proximal tubules.Detecting glomerular dysfunction is challenging becau...The robustness of blood filtration in the kidney is supported by two major functions:the molecular sieve of the glomerulus and reabsorption of the proximal tubules.Detecting glomerular dysfunction is challenging because of the compensatory nature of proximal tubule reabsorption.To facilitate pathophysiological studies of the vertebrate kidney,zebrafish pronephroi are used,owing to their simple glomerular and proximal tubular configuration.In this study,a solvatochromic dye with an affinity for plasma proteins was used to detect urinary proteins leaking into the ureter of zebrafish.Aristolochic acid exposure to fertilized eggs of transgenic zebrafish expressing green fluorescent protein from the proximal tubules to the excretory pore induced concentrationdependent renal dysfunction.The solvatochromic dye ZMB741 was applied via static immersion to analyze leaked dye−plasma−protein complexes in the ureter;their axial distribution was imaged by using confocal microscopy.The effect of resveratrol,an attenuator of aristolochic acid nephropathy,was further analyzed.This method enables individual-level analysis of podocytopathy,a mild glomerular disease that does not necessarily lead to the excretion of proteinuria.Moreover,it will be useful for pathophysiological studies of renal function and the identification of potential therapeutic drugs.展开更多
Stimuli-responsive two-dimensional (2D) covalent organic frameworks (COFs) with precise structures and permanent porosity have been employed as platforms for sensors. The slight change of backbones inside frameworks l...Stimuli-responsive two-dimensional (2D) covalent organic frameworks (COFs) with precise structures and permanent porosity have been employed as platforms for sensors. The slight change of backbones inside frameworks leads to different electronic states by external stimuli, such as solvent, pH, and water. Herein, we introduced an alkynyl-based building block (ETBA) with high planarity to synthesize two imine-based alkynyl-COFs (ETBA-TAPE-COF and ETBA-PYTA-COF) with high yield, good crystallinity, and chemical stability. Due to the presence of acetylene bonds, ETBA-TAPE-COF does not adopt the completely overlapping AA stacking mode. Slight interlayer displacement occurs along the parallel direction relative to the acetylene linkages, which facilitates lower configurational energy. Additionally, the introduction of pyrene group contributes to high π-electron mobility of ETBA-PYTA-COF. The interactions between electron-withdrawing group (ETBA) and electron-donating group (PYTA) during the processes of protonation and intramolecular charge transfer (ICT) endow ETBA-PYTA-COF with excellent acidochromic and solvatochromic properties, respectively. Based on this, a fluorescence sensor is successfully established, which can be used for rapid response to trace amounts of water in organic solvents. In contrast, ETBA-TAPE-COF does not exhibit these photophysical properties due to its higher HOMO–LUMO gap compared to ETBA-PYTA-COF. This work proposes a new strategy for designing and preparing COFs with unique photophysical properties without introducing additional functional groups.展开更多
Carbon dots(CDs)with solvatochromic emission colors in different solvents have attracted much attention as a new class of luminescent nanomaterial owing to their facile synthesis and low production cost.In this work,w...Carbon dots(CDs)with solvatochromic emission colors in different solvents have attracted much attention as a new class of luminescent nanomaterial owing to their facile synthesis and low production cost.In this work,we prepared two kinds of CDs with solvatochromic emissions:green emission CDs(G-CDs)and multicolor emission CDs(M-CDs).G-CDs synthesized from o-phenylenediamine exhibited weak photoluminescence emission(quantum yield 2.8%-6.1%)and 39 nm solvatochromic shifts(492-531 nm).In contrast,M-CDs prepared from o-phenylenediamine and 4-aminophenol showed 87 nm solvatochromic shift range(505-592 nm)and much higher photoluminescence quantum yield(18.4%-32.5%).The two CDs exhibited different emission,absorption,and photoluminescence lifetime.The origin of solvatochromic shifts and the formation mechanism of CDs were demonstrated by analyzing the structures and compositions of two CDs.High percentages of pyrrolic nitrogen and amino nitrogen make wider solvatochromic shifts and higher quantum yields.The results were well supported by density functional theory calculations.This effective strategy to expand solvatochromic shift range and improve quantum yields could open a new window to prepare satisfied solvatochromic carbon dots.展开更多
We analyzed statistically the linear correlation of the solvatochromic shifts of the stilbazolium-like dyes in the nonselected solvents with the reaction field function, L(?T) — bL(n2), and the solvent polarity param...We analyzed statistically the linear correlation of the solvatochromic shifts of the stilbazolium-like dyes in the nonselected solvents with the reaction field function, L(?T) — bL(n2), and the solvent polarity parameter, ENT respectively, and observed that there were not perfectly linearity relationships between them, so we introduced ENT into L(?T) — bL( n2) to form a new reaction field function, L(?T) — bL(n2) + g ENT called as me modified reaction field function, which can be perfectly linearly correlated with the solvatochromic shifts of the stilbazolium-like dyes in the nonselected solvents.展开更多
Long-term fluorescence monitoring of subcellular organelles is crucial for cellular physiology and pathology studies.Lipid droplets(LDs)are increasingly recognized for their involvement in various biological processes...Long-term fluorescence monitoring of subcellular organelles is crucial for cellular physiology and pathology studies.Lipid droplets(LDs)are increasingly recognized for their involvement in various biological processes,to influence disease development through diverse behaviors However,existing LD probes face challenges in achieving high targeting and long-term monitoring due to poor photostability and long-term phototoxicity.Carbon quantum dots(CQDs)have gained prominence due to their exceptional fluorescence properties,but their prevalent blue excitation wavelength presents difficulties for long-term imaging.Herein,we synthesized red-emissive carbon quantum dot(R-CQDs)with superior photobleaching resistance and red-emission,thus enabling harmlessly fluorescence monitoring of cells longer than3 h.In addition,R-CQD exhibits suitable amphiphilicity and remarkable solvatochromic effect,allowing rapid targeting to LDs for immediate imaging without cumbersome washing steps.Hence,R-CQD shows high performance for extended observation of dynamic LD behavior in various biological processes,which is confirmed by documenting the course of LDs during starvation as well as lipotoxicity.Compared to commercial probes,R-CQD extends live cell imaging time by at least 9-fold,facilitating the study of LD behavioral characteristics under diverse physiological or pathological conditions.This work provides a reliable fluorescence tool for tracking intercellular microenvironment dynamically thus to understand the divers biological or disease mechanism.展开更多
Three discrete tetrahedral metallo-supramolecular cages were designed and constructed using truxenepended base ligands.Owing to the synergistic rigidifying effect of unsymmetric cyano-substituted oligo(pphenylene-viny...Three discrete tetrahedral metallo-supramolecular cages were designed and constructed using truxenepended base ligands.Owing to the synergistic rigidifying effect of unsymmetric cyano-substituted oligo(pphenylene-vinylene)(u-COPV)suspended by the truxene skeleton,the resulting supramolecular cages were confirmed to exhibit significant aggregation-induced emission(AIE)accompanied by an interesting solvatochromic fluorescent behavior as well as a porous honeycomb-like state during aggregation.In particular,the anti-counterfeiting performance and emission behaviors of the cages in the solid state under external hydrostatic pressure were investigated.展开更多
It was found that Dynol-604, a non-fluorous and no silicon-containing nonionic surfactant, was soluble in supercritical (SC) CO2. The phase behavior of SC CO2/Dynol-604/water system was studied. The results showed t...It was found that Dynol-604, a non-fluorous and no silicon-containing nonionic surfactant, was soluble in supercritical (SC) CO2. The phase behavior of SC CO2/Dynol-604/water system was studied. The results showed that one-phase water-in-CO2 microemulsions could be formed. The solubilization of methyl orange in the microemulsions proved further the existence of water domain in the microemulsions.展开更多
The reaction of a new salicylideneaniline ligand, (Z)-4-(2-hydroxybenzylideneamino)-2-hydroxybenzoic acid (HL) with COCl2-6H2O yields one Co(Ⅱ) complex, [CoL2(CH3OH)2 (H2O)2]. This complex crystallizes in...The reaction of a new salicylideneaniline ligand, (Z)-4-(2-hydroxybenzylideneamino)-2-hydroxybenzoic acid (HL) with COCl2-6H2O yields one Co(Ⅱ) complex, [CoL2(CH3OH)2 (H2O)2]. This complex crystallizes in monoclinic P21/n space group, with a = 5.4992(5), b = 18.2200(15), c = 14.8678(14) ,A, β= 98.64(1)°, V = 1472.8(2)A3, C30H32CoN2O12, Mr = 671.51, Z = 2, Dc = 1.51416 g/cm^3, F(000) = 698, μ = 0.652 mm^-1, T = 298(2) K, R = 0.0514 and wR = 0.1735 for all 2675 observed reflections (I 〉 2σ(I)). In this complex, the imine N does not link to Co(H) and a remarkable torsion around C=N bond is observed. Through hydrogen bonds, the monomers aggregate into an interesting "Z-shape" framework.展开更多
Much interest has been devoted to organometallic NLO materials. We have become interested in exploring the utility of ferrocenyl group as the conjugating bridge. Thus, we synthesized 1-{{[1,3-(5-methylbenzo)dithiol]-2...Much interest has been devoted to organometallic NLO materials. We have become interested in exploring the utility of ferrocenyl group as the conjugating bridge. Thus, we synthesized 1-{{[1,3-(5-methylbenzo)dithiol]-2-yli- dene}methyl}-1’-[2-(p-nitrophenyl)-(E)-ethenyl]ferrocene (1). This new ferrocenyl compound has a donor and an acceptor group in 1,1’-positions. Investigations of the solvatochromic property of the compound revealed that it has polarized structure in a polar solvent, such as DMF. SHG efficiency of the compound was estimated by an SHEW (second-harmonic generation with the evanescent wave) method.展开更多
Cyanine dyes of zero/bis-zero methine incorporating imid-azo(1,2-a)Pyridine (quinoline) or pyrazino(1,2-a)pyridine (quinoline) with stable C-N bond were synthesized using keto-oxime methylene C-link heterocyclic quate...Cyanine dyes of zero/bis-zero methine incorporating imid-azo(1,2-a)Pyridine (quinoline) or pyrazino(1,2-a)pyridine (quinoline) with stable C-N bond were synthesized using keto-oxime methylene C-link heterocyclic quaternary salts [1-phenyl-3-methyl-pyrazolino-4-keto-oxime-α-methylene-bis-pyridin-(quinoin)-1(4)-di-ium-iodide(ethiodide) salts and 1-phenyl-3-methyl-pyrazolino- 4-ketooxime-α-methylene-N-2-methyl-bis pyridin (quinoin)-1(4)-di-ium-iodide(ethiodide) salts]. Such heterocyclic precursors and related dyes were identified by elemental and spectral analyses. The absorption spectra properties of such dyes were investigated in 95% Ethanol to attempt and throw some light on the influence of such new heterocyclic nuclei and to compare or evaluate spectral behaviors. The absorption spectra of dyes in different pure solvents were examined in the visible region showing solvatochromism and the colour changes of dyes with solvents having different polarities. This permits a selection of the optimal solvent (fractional solvent) when such dyes are applied as photosensitizers. The spectral behavior of some selected newly synthesized cyanine dyes is observed in mixed solvents of different polarities and progressively increasing quantities of one solvent over the other were studied and showed an increase in the absorbance of CT band with increasing proportion of that solvent. Evidence for hydrogen bond formation between the solute molecules and solvent molecules allows measurement of certain energies such as hydrogen bonding, orientation, and free energies.展开更多
The solvatochromic behavior of acetone in supercritical CO? was investigated from 75 bar to 239 bar and at 318.15K. A clustering model is proposed to investigate the formation of solute-solvent and solute-solute clust...The solvatochromic behavior of acetone in supercritical CO? was investigated from 75 bar to 239 bar and at 318.15K. A clustering model is proposed to investigate the formation of solute-solvent and solute-solute clusters, based on the solvatochromic study and some reasonable assumptions. At lower pressures, there were more than one solute molecules in one cluster. At higher pressures, however, each cluster only contained one solute and the clustering of solute-solvent was dominant.展开更多
1 Introduction Nonlinear optical materials(NLO) have drawn a great intrest of some scholars and scientists in the last dacades because of their tremendous potential application in optoelectronic. The fabrication of...1 Introduction Nonlinear optical materials(NLO) have drawn a great intrest of some scholars and scientists in the last dacades because of their tremendous potential application in optoelectronic. The fabrication of efficient optoelectron devices is a challenging task because such systems need to meet the stringentable requirements for high optical quality and large and sustainable electro-optical(EO) response. In pursuit of NLO materials with excellent optoelectronic property,展开更多
In this study,6-chloro-4-hydroxy-2-quinolone and 6-flouro-4-hydroxy-2-quinolone were synthesized from corresponding dianilides.These compounds were coupled with some diazotized aromatic amines to give the correspondin...In this study,6-chloro-4-hydroxy-2-quinolone and 6-flouro-4-hydroxy-2-quinolone were synthesized from corresponding dianilides.These compounds were coupled with some diazotized aromatic amines to give the corresponding azo disperse dyes.The structures of the quinolone derivatives and new azo dyes were confirmed by UV-vis,FT-IR,;H NMR and elemental analysis.展开更多
A new series of (E)-5-[2-(N-hexylcarbazolyl)vinyl]furan chromophores with various accepters have been synthesized by the Knoevenagel condensation of (E)-5-[2-(N- hexylcarbazolyl) vinyl]-2-furaldehydes with malononitri...A new series of (E)-5-[2-(N-hexylcarbazolyl)vinyl]furan chromophores with various accepters have been synthesized by the Knoevenagel condensation of (E)-5-[2-(N- hexylcarbazolyl) vinyl]-2-furaldehydes with malononitrile, 1,3-diethyl-2-thiobarbituric acid, or 3-phenyl-5-isoxazol one, respectively. They are characterized by H-1-NMR, FT- IR, UV-VIS, MS and elemental analysis, and have shown strong solvatochromism and high thermal stability.展开更多
Seven electron-deficient A_2 B type H_3-triarylcorroles have been synthesized and characterized. The solvent dependence of the electronic absorption and magnetic circular dichroism(MCD) spectra and a series of TD-DF...Seven electron-deficient A_2 B type H_3-triarylcorroles have been synthesized and characterized. The solvent dependence of the electronic absorption and magnetic circular dichroism(MCD) spectra and a series of TD-DFT calculations have been used to analyze trends in the electronic structures. Significant differences are observed in the optical spectra when solvents of differing polarity are used,which can be assigned to the effect of NH-tautomerism.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22225107,22301302)。
文摘Environment-sensitive fluorescent probes are commonly utilized in various fields,including fluorescence sensing and imaging.This paper describes the synthesis and photophysical properties of a novel class of solvatochromic fluorophores that incorporate biisoindolylidene as the core backbone.This study investigates the structure-property relationships of these newly developed fluorophores.The central biisoindolylidene acts as an efficient electron acceptor,and by modifying the aryl ring substituent at the 3,3 position,the photophysical properties of the fluorophores can be significantly enhanced,particularly in terms of photoluminescence quantum efficiency.Furthermore,when an electron-donor group replaces the aryl ring at the 3,3 position,intriguing solvatochromic behavior is observed.This leads to a red-shift in the maximum emission wavelength and an increase in the Stokes shift with increasing solvent polarity.In solvent dimethyl sulfoxide(DMSO),the maximum emission wavelength can reach up to 750 nm,with a Stokes shift of approximately 150 nm.Finally,the potential application of the fluorophore in the detection of volatile acids is explored in a preliminary manner.
文摘Binary mixtures of 1,3-dialkylimidazolium based ionic liquids (ILs) and water were selected as solvent systems to investigate the solute-solvent and solvent-solvent interactions on the preferential solvation of solvatochromic indicators at 25 ℃. Empirical solvatochromic pa- rameters, dipolarity/polarizability (π^*), hydrogen-bond donor acidity (α), hydrogen-bond acceptor basicity (β), and Reichardt's polarity parameters (ET^N) were measured from the ultraviolet-visible spectral shifts of 4-nitroaniline, 4-nitroanisole, and Reichardt's dye. The solvent properties of the IL-water mixtures were found to be influenced by IL type and IL mole fraction (XIL). All these studied systems showed the non-ideal behavior. The max- imum deviation to ideality for the solvatochromic parameters can be obtained in the XIL range from 0.i to 0.3. For most of the binary mixtures, the π^* values showed the synergistic effects instead of the ETN, α and β values. The observed synergy extent was dependent on the studied systems, such as the dye indicator and IL type. A preferential solvation model was utilized to gather information on the molecular interactions in the mixtures. The dye indicator was preferentially solvated on the following trend: IL〉IL-water complex〉water.
基金supported by National Natural Science Foundation of China(21703131,31370578)Doctoral Scientific Research Foundation of Shaanxi University of Science and Technology(2016BJ-40)+2 种基金State Key Laboratory of Pulp and Paper Engineering(201821)China Postdoctoral Science Foundation(2018M643707)Natural Science Foundation of Shaanxi Provincial Department of Education(18JK0122)
文摘Solvatochromic materials have recently attracted increasing attention owing to their great significance in the security and sensor fields.In this study,ultrafast explicit and implicit information was collected regarding a fluorescent nanocellulose membrane produced from nanocellulose membranes coated with a Zn-terpyridine complex(Zn-tpy)in a layer-by-layer manner.The fluorescent emissions of the nanocellulose membrane changed from yellow(CIE:x=0.37,y=0.45)to green(CIE:x=0.32,y=0.47)under a dichloromethane environment and 365-nm irradiation.Due to the ease of dichloromethane volatilization,fluorescent emissions quickly returned to the original state.These solvatochromic nanocellulose membranes,with ultrafast explicit and implicit information,exhibited valuable application prospects in anti-counterfeiting techniques.
文摘Hexakis(4-methoxyphenyl)benzene (HPB-OMe(1)) and hexakis(2,6-dimethyl-4-methoxyphenyl)benzene (HPB-OMe(2)) were synthesized via organometallic complex catalysis. The treatment of HPB-OMe(1) with FeCl3 caused cyclodehydrogenation at two positions to yield an oligophenylene with an indeno[1,2-b]fluorene structure (IF-OMe). Deprotection of the methoxy groups of these compounds was conducted by treatment with BBr3. Deprotonation of the OH groups of HPB-OH(1), HPB-OH(2), and IF-OH through treatment with NaH caused a bathochromic shift in the absorption and photoluminescence (PL) peaks. The bathochromic shift of the deprotonated species increased with the donor number (DN) of the solvents. These observations can be explained as the consequence of intramolecular charge transfer (ICT) from the ONa groups to the inner benzene rings.
基金Wai-Yeung Wong acknowledges the financial support from the National Key R&D Program of China(2022YFE0104100)the National Natural Science Foundation of China(52073242)+4 种基金the RGC Senior Research Fellowship Scheme(SRFS2021-5S01)General Research Fund(PolyU 15301922)the Research Institute for Smart Energy(CDAQ)the Research Centre for Nanoscience and Nanotechnology(CE2H),the Research Centre for Carbon-Strategic Catalysis(CE01 and CE2L)Miss Clarea Au for the Endowed Professorship in Energy(847S).
文摘In this study,we present a novel multicomponent self-assembly approach that offers good potential for crafting heterometallic complexes with exceptional constitutional control.This method generates metal ions from a sacrificial anode by using an electric field,which then coordinates with a metal complex precursor.As a proof-of-concept demonstration,we successfully synthesized single crystals of a heterometallic platinum(Ⅱ)-copper(Ⅰ)(Pt[Ⅱ]-Cu[Ⅰ])complex at an exceptionally rapid rate within 30 s by applying a voltage to an acetonitrile solution of[Pt(ppy)(CN)_(2)]^(−)Bu_(4)N^(+),using copper foil as the anode.Intriguingly,by finely adjusting the intensity and duration of the electric field,we achieved a variety of supramolecular structures,spanning from spherical to rod-like and even flower-like morphologies.Additionally,we found that the photoluminescence property of the resultant crystal can be reversibly shifted among green,orange,and cyan by merely altering the solvent environment.Finally,the crafted heterometallic Pt(Ⅱ)-Cu(Ⅰ)complex has shown great promise in advanced anti-counterfeiting applications.
基金supported in part by JSPS KAKENHI(Grant JP21H02670)。
文摘The robustness of blood filtration in the kidney is supported by two major functions:the molecular sieve of the glomerulus and reabsorption of the proximal tubules.Detecting glomerular dysfunction is challenging because of the compensatory nature of proximal tubule reabsorption.To facilitate pathophysiological studies of the vertebrate kidney,zebrafish pronephroi are used,owing to their simple glomerular and proximal tubular configuration.In this study,a solvatochromic dye with an affinity for plasma proteins was used to detect urinary proteins leaking into the ureter of zebrafish.Aristolochic acid exposure to fertilized eggs of transgenic zebrafish expressing green fluorescent protein from the proximal tubules to the excretory pore induced concentrationdependent renal dysfunction.The solvatochromic dye ZMB741 was applied via static immersion to analyze leaked dye−plasma−protein complexes in the ureter;their axial distribution was imaged by using confocal microscopy.The effect of resveratrol,an attenuator of aristolochic acid nephropathy,was further analyzed.This method enables individual-level analysis of podocytopathy,a mild glomerular disease that does not necessarily lead to the excretion of proteinuria.Moreover,it will be useful for pathophysiological studies of renal function and the identification of potential therapeutic drugs.
基金supported by the National Natural Science Foundation of China(22172055)the Science Fund for Distinguished Young Scholars of Guangdong Province(2023B1515040026)+1 种基金the Key Area Research and Development Program of Guangdong Province(2023B0101200008)the Natural Science Foundation of Guangdong Province(2022A1515011892).
文摘Stimuli-responsive two-dimensional (2D) covalent organic frameworks (COFs) with precise structures and permanent porosity have been employed as platforms for sensors. The slight change of backbones inside frameworks leads to different electronic states by external stimuli, such as solvent, pH, and water. Herein, we introduced an alkynyl-based building block (ETBA) with high planarity to synthesize two imine-based alkynyl-COFs (ETBA-TAPE-COF and ETBA-PYTA-COF) with high yield, good crystallinity, and chemical stability. Due to the presence of acetylene bonds, ETBA-TAPE-COF does not adopt the completely overlapping AA stacking mode. Slight interlayer displacement occurs along the parallel direction relative to the acetylene linkages, which facilitates lower configurational energy. Additionally, the introduction of pyrene group contributes to high π-electron mobility of ETBA-PYTA-COF. The interactions between electron-withdrawing group (ETBA) and electron-donating group (PYTA) during the processes of protonation and intramolecular charge transfer (ICT) endow ETBA-PYTA-COF with excellent acidochromic and solvatochromic properties, respectively. Based on this, a fluorescence sensor is successfully established, which can be used for rapid response to trace amounts of water in organic solvents. In contrast, ETBA-TAPE-COF does not exhibit these photophysical properties due to its higher HOMO–LUMO gap compared to ETBA-PYTA-COF. This work proposes a new strategy for designing and preparing COFs with unique photophysical properties without introducing additional functional groups.
基金We appreciate the financial supports from the Board or Regent Supporting Fund(BORSF)Endowed Professorshipthe Lousiana State University Shreveport(LSUS)R&D Funds+1 种基金the Qingdao Municipal Science and Technology Commission(No.16-5-1-86-jch)the Scientific Research Foundation of Qingdao University of Science and Technology(QUST)(No.210/010022914).
文摘Carbon dots(CDs)with solvatochromic emission colors in different solvents have attracted much attention as a new class of luminescent nanomaterial owing to their facile synthesis and low production cost.In this work,we prepared two kinds of CDs with solvatochromic emissions:green emission CDs(G-CDs)and multicolor emission CDs(M-CDs).G-CDs synthesized from o-phenylenediamine exhibited weak photoluminescence emission(quantum yield 2.8%-6.1%)and 39 nm solvatochromic shifts(492-531 nm).In contrast,M-CDs prepared from o-phenylenediamine and 4-aminophenol showed 87 nm solvatochromic shift range(505-592 nm)and much higher photoluminescence quantum yield(18.4%-32.5%).The two CDs exhibited different emission,absorption,and photoluminescence lifetime.The origin of solvatochromic shifts and the formation mechanism of CDs were demonstrated by analyzing the structures and compositions of two CDs.High percentages of pyrrolic nitrogen and amino nitrogen make wider solvatochromic shifts and higher quantum yields.The results were well supported by density functional theory calculations.This effective strategy to expand solvatochromic shift range and improve quantum yields could open a new window to prepare satisfied solvatochromic carbon dots.
基金Project supported by the National Natural Science Foundation of China (No. 29682001 and 29832030).
文摘We analyzed statistically the linear correlation of the solvatochromic shifts of the stilbazolium-like dyes in the nonselected solvents with the reaction field function, L(?T) — bL(n2), and the solvent polarity parameter, ENT respectively, and observed that there were not perfectly linearity relationships between them, so we introduced ENT into L(?T) — bL( n2) to form a new reaction field function, L(?T) — bL(n2) + g ENT called as me modified reaction field function, which can be perfectly linearly correlated with the solvatochromic shifts of the stilbazolium-like dyes in the nonselected solvents.
基金supported by the National Natural Science Foundation of China(Nos.52003178,52273141 and 51973132)Natural Science Foundation of Sichuan Province(No.2023NSFSC0338)。
文摘Long-term fluorescence monitoring of subcellular organelles is crucial for cellular physiology and pathology studies.Lipid droplets(LDs)are increasingly recognized for their involvement in various biological processes,to influence disease development through diverse behaviors However,existing LD probes face challenges in achieving high targeting and long-term monitoring due to poor photostability and long-term phototoxicity.Carbon quantum dots(CQDs)have gained prominence due to their exceptional fluorescence properties,but their prevalent blue excitation wavelength presents difficulties for long-term imaging.Herein,we synthesized red-emissive carbon quantum dot(R-CQDs)with superior photobleaching resistance and red-emission,thus enabling harmlessly fluorescence monitoring of cells longer than3 h.In addition,R-CQD exhibits suitable amphiphilicity and remarkable solvatochromic effect,allowing rapid targeting to LDs for immediate imaging without cumbersome washing steps.Hence,R-CQD shows high performance for extended observation of dynamic LD behavior in various biological processes,which is confirmed by documenting the course of LDs during starvation as well as lipotoxicity.Compared to commercial probes,R-CQD extends live cell imaging time by at least 9-fold,facilitating the study of LD behavioral characteristics under diverse physiological or pathological conditions.This work provides a reliable fluorescence tool for tracking intercellular microenvironment dynamically thus to understand the divers biological or disease mechanism.
基金the National Natural Science Foundation of China(Nos.22101267,21672192,21803059,U2004191,U1904212,21801063)for financial support。
文摘Three discrete tetrahedral metallo-supramolecular cages were designed and constructed using truxenepended base ligands.Owing to the synergistic rigidifying effect of unsymmetric cyano-substituted oligo(pphenylene-vinylene)(u-COPV)suspended by the truxene skeleton,the resulting supramolecular cages were confirmed to exhibit significant aggregation-induced emission(AIE)accompanied by an interesting solvatochromic fluorescent behavior as well as a porous honeycomb-like state during aggregation.In particular,the anti-counterfeiting performance and emission behaviors of the cages in the solid state under external hydrostatic pressure were investigated.
基金The authors are grateful to the National Natural Science Foundation of China and Ministry of Science and Technology for the financial support(29725308,G20000781).
文摘It was found that Dynol-604, a non-fluorous and no silicon-containing nonionic surfactant, was soluble in supercritical (SC) CO2. The phase behavior of SC CO2/Dynol-604/water system was studied. The results showed that one-phase water-in-CO2 microemulsions could be formed. The solubilization of methyl orange in the microemulsions proved further the existence of water domain in the microemulsions.
基金Supported by grant from the 973 Program (2009CB220000)the National Natural Science Foundation of China (No. 20633020)+1 种基金the Natural Science Foundation of Fujian Province (No.2008J0175)the Youth Foundation of Fujian Province (No. 2007F3112)
文摘The reaction of a new salicylideneaniline ligand, (Z)-4-(2-hydroxybenzylideneamino)-2-hydroxybenzoic acid (HL) with COCl2-6H2O yields one Co(Ⅱ) complex, [CoL2(CH3OH)2 (H2O)2]. This complex crystallizes in monoclinic P21/n space group, with a = 5.4992(5), b = 18.2200(15), c = 14.8678(14) ,A, β= 98.64(1)°, V = 1472.8(2)A3, C30H32CoN2O12, Mr = 671.51, Z = 2, Dc = 1.51416 g/cm^3, F(000) = 698, μ = 0.652 mm^-1, T = 298(2) K, R = 0.0514 and wR = 0.1735 for all 2675 observed reflections (I 〉 2σ(I)). In this complex, the imine N does not link to Co(H) and a remarkable torsion around C=N bond is observed. Through hydrogen bonds, the monomers aggregate into an interesting "Z-shape" framework.
文摘Much interest has been devoted to organometallic NLO materials. We have become interested in exploring the utility of ferrocenyl group as the conjugating bridge. Thus, we synthesized 1-{{[1,3-(5-methylbenzo)dithiol]-2-yli- dene}methyl}-1’-[2-(p-nitrophenyl)-(E)-ethenyl]ferrocene (1). This new ferrocenyl compound has a donor and an acceptor group in 1,1’-positions. Investigations of the solvatochromic property of the compound revealed that it has polarized structure in a polar solvent, such as DMF. SHG efficiency of the compound was estimated by an SHEW (second-harmonic generation with the evanescent wave) method.
文摘Cyanine dyes of zero/bis-zero methine incorporating imid-azo(1,2-a)Pyridine (quinoline) or pyrazino(1,2-a)pyridine (quinoline) with stable C-N bond were synthesized using keto-oxime methylene C-link heterocyclic quaternary salts [1-phenyl-3-methyl-pyrazolino-4-keto-oxime-α-methylene-bis-pyridin-(quinoin)-1(4)-di-ium-iodide(ethiodide) salts and 1-phenyl-3-methyl-pyrazolino- 4-ketooxime-α-methylene-N-2-methyl-bis pyridin (quinoin)-1(4)-di-ium-iodide(ethiodide) salts]. Such heterocyclic precursors and related dyes were identified by elemental and spectral analyses. The absorption spectra properties of such dyes were investigated in 95% Ethanol to attempt and throw some light on the influence of such new heterocyclic nuclei and to compare or evaluate spectral behaviors. The absorption spectra of dyes in different pure solvents were examined in the visible region showing solvatochromism and the colour changes of dyes with solvents having different polarities. This permits a selection of the optimal solvent (fractional solvent) when such dyes are applied as photosensitizers. The spectral behavior of some selected newly synthesized cyanine dyes is observed in mixed solvents of different polarities and progressively increasing quantities of one solvent over the other were studied and showed an increase in the absorbance of CT band with increasing proportion of that solvent. Evidence for hydrogen bond formation between the solute molecules and solvent molecules allows measurement of certain energies such as hydrogen bonding, orientation, and free energies.
文摘The solvatochromic behavior of acetone in supercritical CO? was investigated from 75 bar to 239 bar and at 318.15K. A clustering model is proposed to investigate the formation of solute-solvent and solute-solute clusters, based on the solvatochromic study and some reasonable assumptions. At lower pressures, there were more than one solute molecules in one cluster. At higher pressures, however, each cluster only contained one solute and the clustering of solute-solvent was dominant.
基金Supported by the National Natural Science Foundation of China(No.50573023)the Program for Changjiang Scholars and Innovative Research Team in University,China(No.IRTO422)
文摘1 Introduction Nonlinear optical materials(NLO) have drawn a great intrest of some scholars and scientists in the last dacades because of their tremendous potential application in optoelectronic. The fabrication of efficient optoelectron devices is a challenging task because such systems need to meet the stringentable requirements for high optical quality and large and sustainable electro-optical(EO) response. In pursuit of NLO materials with excellent optoelectronic property,
文摘In this study,6-chloro-4-hydroxy-2-quinolone and 6-flouro-4-hydroxy-2-quinolone were synthesized from corresponding dianilides.These compounds were coupled with some diazotized aromatic amines to give the corresponding azo disperse dyes.The structures of the quinolone derivatives and new azo dyes were confirmed by UV-vis,FT-IR,;H NMR and elemental analysis.
基金This work was supported by the NationalNatural Science Foundation of China(No.29774018).
文摘A new series of (E)-5-[2-(N-hexylcarbazolyl)vinyl]furan chromophores with various accepters have been synthesized by the Knoevenagel condensation of (E)-5-[2-(N- hexylcarbazolyl) vinyl]-2-furaldehydes with malononitrile, 1,3-diethyl-2-thiobarbituric acid, or 3-phenyl-5-isoxazol one, respectively. They are characterized by H-1-NMR, FT- IR, UV-VIS, MS and elemental analysis, and have shown strong solvatochromism and high thermal stability.
基金financially supported by the National Natural Science Foundation of China(No.21171076)Natural Science Foundation of Jiangsu Province(No.BK20160499)to XL and WZ and an NRF of South Africa CSUR grant(uid:93627)to JM
文摘Seven electron-deficient A_2 B type H_3-triarylcorroles have been synthesized and characterized. The solvent dependence of the electronic absorption and magnetic circular dichroism(MCD) spectra and a series of TD-DFT calculations have been used to analyze trends in the electronic structures. Significant differences are observed in the optical spectra when solvents of differing polarity are used,which can be assigned to the effect of NH-tautomerism.