Magnetic electrochemiluminescent Fe3O4/CdSe-CdS nanoparticle/polyelectrolyte nanocomposite for highly efficient immunosensing of a cancer biomarker

Magnetic electrochemiluminescent Fe₃O₄/CdSe–CdS nanoparticle/polyelectrolyte nanostructures have been synthesized and used to fabricate an electrochemiluminescence (ECL) immunosensor for the detection of carcinoembryonic antigen (CEA). CEA is a protein used as a biomarker for several cancers; particularly, to monitor response to treatment in colon and rectal cancer patients. The nanocomposites can be easily separated and firmly attached to an electrode owing to their excellent magnetic properties. This represents a promising advantage for bioassay applications. More importantly, the nanostructures exhibit intense and stable ECL emissions in neutral solution, which makes them ideal for ECL immunosensing. The 3‐aminopropyltriethoxysilane (APS) polyelectrolyte shell on the nanostructure surface not only enhances the intensity and stability of the ECL signal, but also acts as a crosslinker for immunosensor fabrication. A CEA antibody immobilized onto a nanocomposite/APS/electrode with gold nanoparticles comprises the ECL immunosensor. The principle of ECL detection for CEA is based on a change in steric hindrance after immunoreaction, which leads to a decrease in ECL intensity. A wide detection range (0.064 pg ml^?1–10 ng ml^?1) and low detection limit (0.032 pg ml^?1) are achieved. The immunosensor is highly sensitive and selective, and exhibits excellent stability and good reproducibility. It thus has great potential for clinical protein detection. In particular, this approach uses a novel class of bifunctional nanocomposites that display both intense ECL and excellent magnetism, which renders them suitable for a large range of bioassay applications.     

空间分辨测量解析三(2,2'-联吡啶)钌(Ⅱ)电化学发光机理的研究进展

电化学发光(ECL)是由电化学反应引发,通过一系列化学反应产生激发态发光体进而辐射发光的过程,其产生的方式主要有湮灭型电化学发光和共反应剂型电化学发光.ECL是一种表面限域的发光过程,其发光层的厚度主要由反应中间体在电极表面的分布决定.空间分辨测量能够直接测得激发态发光体、共反应剂自由基等中间体在电极表面附近的分布,进...     

Recent Advances in Analytical Applications of Nanomaterials in Liquid-Phase Chemiluminescence

Abstract

In recent years, many nanomaterials-assisted chemiluminescence (CL) systems have been developed to improve the sensitivity and to expand the scope of their analytical applications. In these new systems, nanomaterials participate in CL reactions as catalysts, labels, reductants, luminophors, or energy acceptors. This review mainly focuses on the recent analytical applications of metal nanoparticles, magnetic nanoparticles, quantum dots (QDs), and carbon-based nanomaterials (carbon nanotubes and graphene) in liquid-phase CL systems. Recent advances in electrochemiluminescence based on nanotechnology and its analytical applications, especially in immunoassay, DNA analysis, and other biological analyses, are also summarized. Finally, we discuss some critical challenges in this field and speculate about their solutions. A total of 177 references mainly in the last 5 years are included in this review.     

Ultrafast Condensation of Carbon Nitride on Electrodes with Exceptional Boosted Photocurrent and Electrochemiluminescence

Semiconducting polymeric carbon nitride (CN) has drawn wide attention ranging from photocatalysis to more recent biosensing owing to unique defect‐tolerated optoelectronic properties and being metal‐free, cheap, and highly stable. However, at the core of electrical–optical interconversion, the preparation of the CN photoelectrode is still challenging. Now, the growth of CN on electrodes is achieved simply by microwave‐assisted condensation in seconds. The ultrafast heating not only addressed the thermodynamic contradiction of precursor volatilization during polymerization but also led to strongly adhesive CN layer on electrodes with gradient carbon‐rich texture, greatly accelerating the electron–hole separation and mobility. Consequently, the CN photoelectrode exhibited a remarkable photocurrent and a record cathodic efficiency of electrochemiluminescence up to 7 times that of benchmark Ru(bpy)₃Cl₂ in aqueous solution.     

Switching the Photoluminescence and Electrochemiluminescence of Liposoluble Porphyrin in Aqueous Phase by Molecular Regulation

By a facile peripheral decoration of 5-(4-aminophenyl)-10,15,20-triphenylporphyrin (ATPP) with inherent aggregation-induced emission (AIE) active tetraphenylethene (TPE), a versatile AIEgenic porphyrin derivative (ATPP-TPE) was obtained, which greatly abolishes the detrimental π–π stacking and thus surmounts the notorious aggregation-caused quenching (ACQ) effect of ATPP in aqueous phase. The photoluminescence of ATPP-TPE is 4.5-fold stronger than ATPP at aggregation state. Moreover, an unequivocal aggregation induced electrochemiluminescence (AIECL) of ATPP-TPE was found to be seriously dependent on its aggregation property in aqueous solution with efficiency of 34 %, which is 6 times higher than pure ATPP. The versatility of this molecular structure modulation strategy along with the ACQ-to-AIE transformation in this work provides direction to guide for applying liposoluble porphyrins in aqueous phase by designs of synthetic porphyrin AIEgens.     

碳点对鲁米诺电化学发光体系抑制作用的研究及其在DNA分析中的应用

发现碳点对鲁米诺电化学发光体系有明显的抑制作用, 并且由于碳点对单双链DNA的吸附性差异, 与单双链结合的碳点对鲁米诺电化学发光体系的抑制程度不同, 基于此实现了对DNA的快速、简便、灵敏的检测. 考察了碳点粒径、浓度对鲁米诺电化学发光体系的抑制行为的影响. 优化了溶液pH值, 鲁米诺浓度等电化学发光条件. 在优化的最佳实验条件下, 该方法检测DNA的线性范围为1.0×10^-10～7.5×10^-9 mol/L, 检出限为5.2×10^-11 mol/L.     

二茂铁催化鲁米诺电致化学发光反应的研究

在碱性Tris缓冲体系中 ,鲁米诺与过氧化氢的电致化学发光反应要在 4 5 0mV以上的电位下才可以发生 ,加入羧基二茂铁 (FCA)可以使这一发光反应的起始电位负移 ,而且发光信号随电极电位的增大而急剧增强。详细考察了这一催化发光体系 ,研究了影响发光强度的各种因素 ,建立了Luminol H2 O2 FCA发光体系测定FCA的电致化学发光新方法。方法测定二茂铁的检出限可达 1.5nmol/L ,二茂铁浓度在 5 .0× 10 -9～ 2 .0×10 -4mol/L范围内与电致化学发光强度呈良好的线性响应关系     

Differential Photoluminescent and Electrochemiluminescent Detection of Anions with a Modified Ruthenium(II)–Bipyridyl Complex

Different lights, different selectivies : Luminescence of a new guanidinium 3,3′‐functionalized bipyridyl–Ru^II complex has been studied for sensing of several anions. L ‐Glutamate and dihydrogenphosphate are both detected by photoluminescence and electrochemiluminescence. However, the complex displays differential selectivities for these anions depending on the sensing channels (see scheme).

     

基于多壁碳纳米管修饰电极的保泰松的电致化学发光检测

基于保泰松对联吡啶钌的电致化学发光信号有较强的增敏作用, 使用多壁碳纳米管修饰玻碳电极作为工作电极, 建立了一种保泰松的电致化学发光检测方法. 对测定条件进行了一系列优化, 结果表明, 当发光试剂联吡啶钌的浓度为1.0×10－5 mol/L时, 在0.05 mol/L pH 10.20 的Na2HPO4-NaOH介质中保泰松对联吡啶钌电化学发光信号的增敏效果最强. 在此条件下, 保泰松的线性范围为0.5～200 μmol/L, 检测限(S/N＝3)为0.2 μmol/L, 与使用未经修饰的裸玻碳电极相比, 检测限下降了约一个数量级. 该检测方法还被用于加标人血清样品中保泰松的测定, 回收率在85.3%～95.0%之间, 结果令人满意, 可望用于保泰松的药物临床分析与质量监控.     

磺酸基卟啉的电化学发光研究及应用

以四(4-磺酸基苯基)卟啉（TSPP）为发光体,过硫酸钾（K₂S₂O₈）为共反应剂,构建了一个新的电化学发光（ECL）体系. 在扫描范围为0~-1.5V时,该体系出现两个阴极ECL峰,分别为TSPP的还原峰（-0.8V）和K₂S₂O₈ 的还原峰 (-1.2V). 亚甲基蓝能有效猝灭四(4-磺酸基苯基)卟啉的电化学发光,根据猝灭效率与亚甲基蓝浓度的线性关系,建立了一种测定亚甲基蓝含量的新方法.