Electrogenerated chemiluminescence(electrochemiluminescence, ECL) generates species at electrode surfaces, which undergoes electron-transfer reactions and forms excited states to emit light. It has become a very power...Electrogenerated chemiluminescence(electrochemiluminescence, ECL) generates species at electrode surfaces, which undergoes electron-transfer reactions and forms excited states to emit light. It has become a very powerful analytical technique and has been widely used in such as clinical testing, biowarfare agent detection, and pharmaceutical analysis. This review focuses on the current trends of molecular recognition-based biosensing methods for pharmaceutical analysis since 2010. It introduces a background of ECL and presents the recent ECL developments in ECL immunoassay(ECLIA), immunosensors, enzyme-based biosensors, aptamer-based biosensors, and molecularly imprinted polymers(MIP)-based sensors. At last, the future perspective for these analytical methods is briefly discussed.展开更多
Intracellular p H undertakes critical functions in various biological and pathological processes. It is important to monitor intracellular p H fluctuations for understanding physiological and pathological processes.He...Intracellular p H undertakes critical functions in various biological and pathological processes. It is important to monitor intracellular p H fluctuations for understanding physiological and pathological processes.Here, one aldehyde-bearing cyclometalated iridium(Ⅲ) complex([(4-pba)_(2)Ir(dcphen)]PF_(6), 4-pba = 4-(2-pyridyl) benzaldehyde, dcphen = 4,7-dichloro-1,10-phenanthroline, probe 1) was synthesized and used to track intracellular p H fluctuations. Probe 1 displayed p H-dependent luminescence property in p H range of 1.81–6.81 with an evaluated p Kavalue of 4.30 in BR buffer-DMSO(v:v = 99:1). An intramolecular hydrogen bonds assisted p H-responsive mechanism was proposed for the p H-responsive behavior of probe1. Probe 1 was successfully applied for imaging and tracking p H fluctuations in He La cells under external stimulation with fast response time, good photostability as well as low cytotoxicity and high cell permeability. This work demonstrates that aldehyde-bearing cyclometalated iridium(Ⅲ) complex can be used as alternative p H-responsive probe for real-time tracking intracellular p H fluctuations, which provides a strategy for the design of p H-responsive probe in versatile applications.展开更多
Main observation and conclusion A single particle-based confocal laser scanning microscopy was developed for the visual detection of copper ions in confined space.A fluorescence microparticle,named AuNCs/ZIF-8,was syn...Main observation and conclusion A single particle-based confocal laser scanning microscopy was developed for the visual detection of copper ions in confined space.A fluorescence microparticle,named AuNCs/ZIF-8,was synthesized by coating gold nanoclusters(AuNCs)onto the outer surface of zeolitic imidazolate framework-8(ZIF-8).展开更多
A highly sensitive electrochemiluminescence(ECL) biosensing method was developed for monitoring casein kinase Ⅱ(CK2) at subcellular level via bio-bar-code assay.A bio-bar-code probe(h-DNA/AuNPs/pDNA) prepared by conj...A highly sensitive electrochemiluminescence(ECL) biosensing method was developed for monitoring casein kinase Ⅱ(CK2) at subcellular level via bio-bar-code assay.A bio-bar-code probe(h-DNA/AuNPs/pDNA) prepared by conjugating phosphorylated DNA(p-DNA) and hairpin DNA(h-DNA) onto gold nanoparticles(AuNPs) was used as a carrier for ECL signal reagent(Ru(phen)32+) while a specific peptide was used as a recognition substance.A gold ultramicroelectrode with a diameter of 400 nm was fabricated and then modified with the specific peptide via self-assembly technique to obtain peptide modified gold ultramicroelectrode.The peptide on gold ultramicroelectrode was phosphorylated in the presence of CK2 and adenosine 5’-triphosphate,and then the phosphorylated peptide was integrated with the h-DNA/AuNPs/p-DNA through a process mediated by zirconium cations(Zr4+),and finally Ru(phen)32+ was intercalated into h-DNA.A "signal on" ECL method was developed for the detection of CK2 in the range of 0.005-0.2 U/mL with a detection limit of 0.001 U/mL.Additionally,combined efficient subcellular phosphorylation in vivo with bio-bar-code-based ECL biosensing method,the ECL method was further applied to monitor CK2 at subcellular level without tedious subcellular fractionation.It was found that the concentration of CK2 by inserting the peptide modified gold ultramicroelectrode into the nucleus was higher than that into cytoplasm of HeLa cells.A distinct heterogeneity among CK2 concentrations in single cells was observed for cellular heterogeneity assessment.展开更多
A highly selective and sensitive electrochemical method was developed for the detection of serotonin (5-hydroxytryptamine, 5-HT) at gold nanoflowers (Au NFs) and overoxidized polypyrrole (OPPy) modified carbon fiber m...A highly selective and sensitive electrochemical method was developed for the detection of serotonin (5-hydroxytryptamine, 5-HT) at gold nanoflowers (Au NFs) and overoxidized polypyrrole (OPPy) modified carbon fiber microelectrode (CFME). Carbon fiber was firstly modified with gold nanoflowers using electroless deposition method, and then modified with overoxidized polypyrrole using electrochemical polymerization and overoxidization to obtain OPPy/Au NFs/CFME. The obtained OPPy/Au NFs/CFME was characterized by field emission scanning electron microscopy and electrochemical techniques. It was found that the OPPy/Au NFs/CFME showed good sensitivity for the detection of 5-HT in the range of 10 nmol/L-7.0μmol/L with detection limit of 2.3 nmol/L, and negligible interferences from ascorbic acid, 5-hydroxyindole acetic acid and uric acid. The OPPy/Au NFs/CFME was successfully applied to the detection of 5-HT in human serum samples with good recovery. The work demonstrates that the electrochemical method, incorporating signal amplification of Au NFs with higher cation selection of OPPy, provides a promising tool for the detection of 5-HT in biological systems.展开更多
文摘Electrogenerated chemiluminescence(electrochemiluminescence, ECL) generates species at electrode surfaces, which undergoes electron-transfer reactions and forms excited states to emit light. It has become a very powerful analytical technique and has been widely used in such as clinical testing, biowarfare agent detection, and pharmaceutical analysis. This review focuses on the current trends of molecular recognition-based biosensing methods for pharmaceutical analysis since 2010. It introduces a background of ECL and presents the recent ECL developments in ECL immunoassay(ECLIA), immunosensors, enzyme-based biosensors, aptamer-based biosensors, and molecularly imprinted polymers(MIP)-based sensors. At last, the future perspective for these analytical methods is briefly discussed.
基金supported by the National Natural Science Foundation of China (Nos. 22074087, 21804106 and 11727813)the Fundamental Research Funds for the Central Universities (No. 2021TS032)。
文摘Intracellular p H undertakes critical functions in various biological and pathological processes. It is important to monitor intracellular p H fluctuations for understanding physiological and pathological processes.Here, one aldehyde-bearing cyclometalated iridium(Ⅲ) complex([(4-pba)_(2)Ir(dcphen)]PF_(6), 4-pba = 4-(2-pyridyl) benzaldehyde, dcphen = 4,7-dichloro-1,10-phenanthroline, probe 1) was synthesized and used to track intracellular p H fluctuations. Probe 1 displayed p H-dependent luminescence property in p H range of 1.81–6.81 with an evaluated p Kavalue of 4.30 in BR buffer-DMSO(v:v = 99:1). An intramolecular hydrogen bonds assisted p H-responsive mechanism was proposed for the p H-responsive behavior of probe1. Probe 1 was successfully applied for imaging and tracking p H fluctuations in He La cells under external stimulation with fast response time, good photostability as well as low cytotoxicity and high cell permeability. This work demonstrates that aldehyde-bearing cyclometalated iridium(Ⅲ) complex can be used as alternative p H-responsive probe for real-time tracking intracellular p H fluctuations, which provides a strategy for the design of p H-responsive probe in versatile applications.
基金This work is supported by the National Natural Science Foundation of China(Nos.21775097 and 21775098)the Fundamental Research Funds for the Central Universities(No.2017TS021).
文摘Main observation and conclusion A single particle-based confocal laser scanning microscopy was developed for the visual detection of copper ions in confined space.A fluorescence microparticle,named AuNCs/ZIF-8,was synthesized by coating gold nanoclusters(AuNCs)onto the outer surface of zeolitic imidazolate framework-8(ZIF-8).
基金supported by the National Natural Science Foundation of China(Nos.21775097 and 21775098)the Fundamental Research Funds for the Central Universities(No.GK201801006)。
文摘A highly sensitive electrochemiluminescence(ECL) biosensing method was developed for monitoring casein kinase Ⅱ(CK2) at subcellular level via bio-bar-code assay.A bio-bar-code probe(h-DNA/AuNPs/pDNA) prepared by conjugating phosphorylated DNA(p-DNA) and hairpin DNA(h-DNA) onto gold nanoparticles(AuNPs) was used as a carrier for ECL signal reagent(Ru(phen)32+) while a specific peptide was used as a recognition substance.A gold ultramicroelectrode with a diameter of 400 nm was fabricated and then modified with the specific peptide via self-assembly technique to obtain peptide modified gold ultramicroelectrode.The peptide on gold ultramicroelectrode was phosphorylated in the presence of CK2 and adenosine 5’-triphosphate,and then the phosphorylated peptide was integrated with the h-DNA/AuNPs/p-DNA through a process mediated by zirconium cations(Zr4+),and finally Ru(phen)32+ was intercalated into h-DNA.A "signal on" ECL method was developed for the detection of CK2 in the range of 0.005-0.2 U/mL with a detection limit of 0.001 U/mL.Additionally,combined efficient subcellular phosphorylation in vivo with bio-bar-code-based ECL biosensing method,the ECL method was further applied to monitor CK2 at subcellular level without tedious subcellular fractionation.It was found that the concentration of CK2 by inserting the peptide modified gold ultramicroelectrode into the nucleus was higher than that into cytoplasm of HeLa cells.A distinct heterogeneity among CK2 concentrations in single cells was observed for cellular heterogeneity assessment.
基金the National Natural Science Foundation of China (Nos. 21775097 and 21804106)the China Postdoctoral Science Foundation (No. 2017M620444)the Fundamental Research Funds for the Central Universities (Nos. XJJ2018247 and GK201801006)
文摘A highly selective and sensitive electrochemical method was developed for the detection of serotonin (5-hydroxytryptamine, 5-HT) at gold nanoflowers (Au NFs) and overoxidized polypyrrole (OPPy) modified carbon fiber microelectrode (CFME). Carbon fiber was firstly modified with gold nanoflowers using electroless deposition method, and then modified with overoxidized polypyrrole using electrochemical polymerization and overoxidization to obtain OPPy/Au NFs/CFME. The obtained OPPy/Au NFs/CFME was characterized by field emission scanning electron microscopy and electrochemical techniques. It was found that the OPPy/Au NFs/CFME showed good sensitivity for the detection of 5-HT in the range of 10 nmol/L-7.0μmol/L with detection limit of 2.3 nmol/L, and negligible interferences from ascorbic acid, 5-hydroxyindole acetic acid and uric acid. The OPPy/Au NFs/CFME was successfully applied to the detection of 5-HT in human serum samples with good recovery. The work demonstrates that the electrochemical method, incorporating signal amplification of Au NFs with higher cation selection of OPPy, provides a promising tool for the detection of 5-HT in biological systems.