Metal nanoclusters possess excellent electrochemical,optical,and catalytic properties,but correlating these properties remains challenging,which is the foundation to generate electrochemiluminescence(ECL).Herein,we re...Metal nanoclusters possess excellent electrochemical,optical,and catalytic properties,but correlating these properties remains challenging,which is the foundation to generate electrochemiluminescence(ECL).Herein,we report for the first time that a structurally determined Pt1Ag18 nanocluster generates intense ECL and simultaneously enhances the ECL of carbon dots(CDs)via an electrocatalytic effect.Pt^(1)Ag_(18)nanocluster show aggregation-induced emission enhancement and aggregation-induced ECL enhancement under light and electrochemical stimulation,respectively.In the presence of tripropylamine(TPrA)as a coreactant,solid Pt1Ag18 shows unprecedented ECL efficiency,which is more than nine times higher than that of 1 mM Ru(bpy)32+with the same TPrA concentration.Potential-resolved ECL spectra reveal two ECL emission bands in the presence of TPrA.The ECL emission centered at 650 nm is assigned to the solid Pt_(1)Ag_(18)nanocluster,consistent with the peak wavelength in self-annihilation ECL and photoluminescence of the solid state.The ECL emission centered at 820 nm is assigned to the CDs on the glassy carbon electrode.The electrocatalytic effect of the nanoclusters enhanced the ECL of the CDs by a factor of more than 180 in comparison to that without nanoclusters.Based on the combined optical and electrochemical results,the ECL generation pathways and mechanisms of Pt1Ag18 and CDs are proposed.These findings are extremely promising for designing multifunctional nanocluster luminophores with strong emissions and developing ratiometric sensing devices.展开更多
Carbon dots (CDs) are prepared through a simple one-step hydrothermal treatment of o-phenylendiamine (OPD) and show yellow photoluminescent (PL) emission under the ultraviolet excitation, which can be further enhanced...Carbon dots (CDs) are prepared through a simple one-step hydrothermal treatment of o-phenylendiamine (OPD) and show yellow photoluminescent (PL) emission under the ultraviolet excitation, which can be further enhanced by Cu2+ ions owing to Cu2+ ions induced aggregation of OPD-CDs through the coordination of Cu2+ with amino groups on the surface of OPD-CDs. The aggregation induced emission enhancement (AIEE) property enables it feasible to develop a simple, sensitive and selective method to detect environmental and intracellular copper (Ⅱ) ions. The limit of detection as lowas 0.28 μmol/L (3σ/k) and a dynamic range from 0.5 μmol/L to 40 μmol/L make it veryeasy to detect the copper content inwater samples, such as river closure reservoir. Furthermore, fluorescence imaging of intracellular Cu2+ suggests that the AIEE features of OPD-CDs specific to Cu2+ ions can be also applied in biological systems.展开更多
Polyelectrolyte PTPEPyH, containing tetraphenylethene (TPE) and pyridinium, was synthesized. Its optical properties were investigated with spectroscopies and the results showed that there were two emission-enhanced st...Polyelectrolyte PTPEPyH, containing tetraphenylethene (TPE) and pyridinium, was synthesized. Its optical properties were investigated with spectroscopies and the results showed that there were two emission-enhanced stages in the interaction between positive-charged PTPEPyH and negative-charged biomacromolecule heparin. The mechanism was very different due to the reduced non-radiative energy loss and the change of surroundings. The polyelectrolyte PTPEPyH, compared with ChS and HA, also showed high selectivity for heparin in the buffer solution and could be used as a potential bio-probe for heparin quantification in the clinical full range.展开更多
Transition metal ions(Pb^(2+),Zn^(2+),Cd^(2+),Co^(2+),Mn^(2+),Cu^(2+),Ni^(2+),Hg^(2+),Ag^(+),Fe^(3+))in water are used to quench emission of 2-(6-oxido-6H-dibenz<c,e><1,2>oxaphosphorin-6-yl)-1,4-phenylene-...Transition metal ions(Pb^(2+),Zn^(2+),Cd^(2+),Co^(2+),Mn^(2+),Cu^(2+),Ni^(2+),Hg^(2+),Ag^(+),Fe^(3+))in water are used to quench emission of 2-(6-oxido-6H-dibenz<c,e><1,2>oxaphosphorin-6-yl)-1,4-phenylene-bis(p-pentyloxylbenzoate)s(MD5)with aggregation-induced emission enhancement(AIEE)in water-acetonitrile(AN)mixture(80:20 by volume).Among all metal ions,Fe^(3+)exhibits the highest quenching efficiency on AIEE of MD5 even when the concentration of Fe^(3+)is lower than 1×10^(-6) mol/L.The quenching efficiency of Hg^(2+)is lower than that of Fe^(3+)at the same concentration,though MD5 is used to detect Hg^(2+)efficiently,too.To other metal ions,low quenching efficiency has few relations with a wider concentration range.The UV absorbance spectra show only red shift of absorbance wavelength in the presence of Hg^(2+)and Fe^(3+),which indicates a salt-induced Jaggregation.SEM photos reveal larger aggregation and morphological change of nanoparticles of MD5 in water containing Hg^(2+)and Fe^(3+),which reduce the surface area of MD5 emission for further aggregation.The selective quenching effect of transition metal ions to emission of MD5 has a potential application in chemical sensors of some metal ions.展开更多
以邻苯二胺、丙二酸及对苯二甲醛为原料,通过Knoevenagel反应合成了一种多苯并咪唑有机光电材料2,2,2′,2′-四(1H-苯并咪唑-2-基)-1,4-二乙烯基苯。采用包括元素分析、FTIR和1 H NMR分析在内的方法对其结构进行了表征,并测试研究了产...以邻苯二胺、丙二酸及对苯二甲醛为原料,通过Knoevenagel反应合成了一种多苯并咪唑有机光电材料2,2,2′,2′-四(1H-苯并咪唑-2-基)-1,4-二乙烯基苯。采用包括元素分析、FTIR和1 H NMR分析在内的方法对其结构进行了表征,并测试研究了产物的光物理性能、电化学特性和热稳定性。结果表明:该化合物的最大紫外吸收谱在398nm附近的近紫外光区。其溶液荧光为λem≈500nm的蓝绿色光,固体薄膜荧光为λem=554nm的绿色光,且具有明显的聚集诱导发光增强(AIEE)效应。通过CV测得其Eg=3.10eV,IP=5.57eV,EA=2.47eV,表明该化合物是一种潜在空穴传输材料。测得其热分解温度接近500℃,具有良好的热稳定性。采用密度泛函(DFT)理论计算其主要光电性能参数,与实验结果相符,量化计算证明该分子具有显著的非共平面性的π共轭体系以及分子内电荷转移特性。展开更多
Polyelectrolyte PTPEPyH,containing tetraphenylethene(TPE)and pyridinium,was synthesized.Its optical properties were investigated with spectroscopies and the results showed that there were two emission-enhanced stages ...Polyelectrolyte PTPEPyH,containing tetraphenylethene(TPE)and pyridinium,was synthesized.Its optical properties were investigated with spectroscopies and the results showed that there were two emission-enhanced stages in the interaction between positive-charged PTPEPyH and negative-charged biomacromolecule heparin.The mechanism was very different due to the reduced non-radiative energy loss and the change of surroundings.The polyelectrolyte PTPEPyH,compared with ChS and HA,also showed high selectivity for heparin in the buffer solution and could be used as a potential bio-probe for heparin quantification in the clinical full range.展开更多
基金National Natural Science Foundation of China,Grant/Award Numbers:22004001,21631001,21871001Anhui Provincial Natural Science Foundation,Grant/Award Number:2008085QB84the Ministry of Education,the University Synergy Innovation Program of Anhui Province,Grant/Award Number:GXXT-2020-053。
文摘Metal nanoclusters possess excellent electrochemical,optical,and catalytic properties,but correlating these properties remains challenging,which is the foundation to generate electrochemiluminescence(ECL).Herein,we report for the first time that a structurally determined Pt1Ag18 nanocluster generates intense ECL and simultaneously enhances the ECL of carbon dots(CDs)via an electrocatalytic effect.Pt^(1)Ag_(18)nanocluster show aggregation-induced emission enhancement and aggregation-induced ECL enhancement under light and electrochemical stimulation,respectively.In the presence of tripropylamine(TPrA)as a coreactant,solid Pt1Ag18 shows unprecedented ECL efficiency,which is more than nine times higher than that of 1 mM Ru(bpy)32+with the same TPrA concentration.Potential-resolved ECL spectra reveal two ECL emission bands in the presence of TPrA.The ECL emission centered at 650 nm is assigned to the solid Pt_(1)Ag_(18)nanocluster,consistent with the peak wavelength in self-annihilation ECL and photoluminescence of the solid state.The ECL emission centered at 820 nm is assigned to the CDs on the glassy carbon electrode.The electrocatalytic effect of the nanoclusters enhanced the ECL of the CDs by a factor of more than 180 in comparison to that without nanoclusters.Based on the combined optical and electrochemical results,the ECL generation pathways and mechanisms of Pt1Ag18 and CDs are proposed.These findings are extremely promising for designing multifunctional nanocluster luminophores with strong emissions and developing ratiometric sensing devices.
基金financially supported by the National Natural Science Foundation of China (NSFC, No. 21535006)
文摘Carbon dots (CDs) are prepared through a simple one-step hydrothermal treatment of o-phenylendiamine (OPD) and show yellow photoluminescent (PL) emission under the ultraviolet excitation, which can be further enhanced by Cu2+ ions owing to Cu2+ ions induced aggregation of OPD-CDs through the coordination of Cu2+ with amino groups on the surface of OPD-CDs. The aggregation induced emission enhancement (AIEE) property enables it feasible to develop a simple, sensitive and selective method to detect environmental and intracellular copper (Ⅱ) ions. The limit of detection as lowas 0.28 μmol/L (3σ/k) and a dynamic range from 0.5 μmol/L to 40 μmol/L make it veryeasy to detect the copper content inwater samples, such as river closure reservoir. Furthermore, fluorescence imaging of intracellular Cu2+ suggests that the AIEE features of OPD-CDs specific to Cu2+ ions can be also applied in biological systems.
基金the National Basic Research Pro- gram of China (973 Program 2013CB834704)+2 种基金the National Natural Scientific Foundation of China (21004004 and 51061160500)the Specialized Research Fund for the Doctoral Program of Higher Education of China (20101101120029 and 20091101110031)the Scientific Research Foundation for the Returned Overseas Chinese Scholars, State Education Ministry (20120932001)
文摘Polyelectrolyte PTPEPyH, containing tetraphenylethene (TPE) and pyridinium, was synthesized. Its optical properties were investigated with spectroscopies and the results showed that there were two emission-enhanced stages in the interaction between positive-charged PTPEPyH and negative-charged biomacromolecule heparin. The mechanism was very different due to the reduced non-radiative energy loss and the change of surroundings. The polyelectrolyte PTPEPyH, compared with ChS and HA, also showed high selectivity for heparin in the buffer solution and could be used as a potential bio-probe for heparin quantification in the clinical full range.
基金This project was supported by the National Natural Science Foundation of China(No.20634020)the Basic Research Foundation of Beijing Institute of Technology(BIT-UBF-200504B4213,BIT-UBF-200504B4215).
文摘Transition metal ions(Pb^(2+),Zn^(2+),Cd^(2+),Co^(2+),Mn^(2+),Cu^(2+),Ni^(2+),Hg^(2+),Ag^(+),Fe^(3+))in water are used to quench emission of 2-(6-oxido-6H-dibenz<c,e><1,2>oxaphosphorin-6-yl)-1,4-phenylene-bis(p-pentyloxylbenzoate)s(MD5)with aggregation-induced emission enhancement(AIEE)in water-acetonitrile(AN)mixture(80:20 by volume).Among all metal ions,Fe^(3+)exhibits the highest quenching efficiency on AIEE of MD5 even when the concentration of Fe^(3+)is lower than 1×10^(-6) mol/L.The quenching efficiency of Hg^(2+)is lower than that of Fe^(3+)at the same concentration,though MD5 is used to detect Hg^(2+)efficiently,too.To other metal ions,low quenching efficiency has few relations with a wider concentration range.The UV absorbance spectra show only red shift of absorbance wavelength in the presence of Hg^(2+)and Fe^(3+),which indicates a salt-induced Jaggregation.SEM photos reveal larger aggregation and morphological change of nanoparticles of MD5 in water containing Hg^(2+)and Fe^(3+),which reduce the surface area of MD5 emission for further aggregation.The selective quenching effect of transition metal ions to emission of MD5 has a potential application in chemical sensors of some metal ions.
文摘以邻苯二胺、丙二酸及对苯二甲醛为原料,通过Knoevenagel反应合成了一种多苯并咪唑有机光电材料2,2,2′,2′-四(1H-苯并咪唑-2-基)-1,4-二乙烯基苯。采用包括元素分析、FTIR和1 H NMR分析在内的方法对其结构进行了表征,并测试研究了产物的光物理性能、电化学特性和热稳定性。结果表明:该化合物的最大紫外吸收谱在398nm附近的近紫外光区。其溶液荧光为λem≈500nm的蓝绿色光,固体薄膜荧光为λem=554nm的绿色光,且具有明显的聚集诱导发光增强(AIEE)效应。通过CV测得其Eg=3.10eV,IP=5.57eV,EA=2.47eV,表明该化合物是一种潜在空穴传输材料。测得其热分解温度接近500℃,具有良好的热稳定性。采用密度泛函(DFT)理论计算其主要光电性能参数,与实验结果相符,量化计算证明该分子具有显著的非共平面性的π共轭体系以及分子内电荷转移特性。
文摘Polyelectrolyte PTPEPyH,containing tetraphenylethene(TPE)and pyridinium,was synthesized.Its optical properties were investigated with spectroscopies and the results showed that there were two emission-enhanced stages in the interaction between positive-charged PTPEPyH and negative-charged biomacromolecule heparin.The mechanism was very different due to the reduced non-radiative energy loss and the change of surroundings.The polyelectrolyte PTPEPyH,compared with ChS and HA,also showed high selectivity for heparin in the buffer solution and could be used as a potential bio-probe for heparin quantification in the clinical full range.
