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过一硫酸盐在协同增强的单原子 Co/Co@C 上的活化用于增强三(联吡啶)钌(II)衍生物的化学发光。

Peroxymonosulfate Activation on Synergistically Enhanced Single-Atom Co/Co@C for Boosted Chemiluminescence of Tris(bipyridine) Ruthenium(II) Derivative.

机构信息

Key Laboratory of Pesticides and Chemical Biology of Ministry of Education, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China.

Institute of Modern Physics, Chinese Academy of Science, Lanzhou 730000, P. R. China.

出版信息

Anal Chem. 2022 May 10;94(18):6866-6873. doi: 10.1021/acs.analchem.2c00881. Epub 2022 Apr 29.

Abstract

Tris(bipyridine) ruthenium(II)-based luminophores have been well developed in the area of electrochemiluminescence, while their applications in chemiluminescence (CL) are rarely studied due to the poor luminous efficiency and complicated CL reaction. Herein, a novel tris(bipyridine) ruthenium(II)-based ternary CL system is proposed by introducing cobalt single atoms integrated with graphene-encapsulated cobalt nanoparticles (Co SAs/Co@C) and peroxymonosulfate (PMS) as advanced coreaction accelerator and promising coreactant, respectively. On the basis of the experimental results and density functional theory calculations, it is concluded that Co@C can synergistically modulate the adsorption behavior of PMS on Co SAs and then efficiently activate PMS to produce massive singlet oxygen for remarkable CL emission. Under the optimum conditions, the as-prepared CL biosensor exhibits a good linear range, excellent sensitivity, and selectivity, holding great potential for the practical detection of prostate-specific antigen in human serum.

摘要

基于三(2,2′-联吡啶)钌(II)的发光体在电化学发光领域得到了很好的发展,但其在化学发光(CL)中的应用由于发光效率低和 CL 反应复杂而很少被研究。本文通过引入钴单原子与石墨烯包裹的钴纳米粒子(Co SAs/Co@C)结合,并将过一硫酸盐(PMS)分别作为先进的共反应加速剂和有前途的共反应物,提出了一种新型的基于三(2,2′-联吡啶)钌(II)的三元 CL 体系。基于实验结果和密度泛函理论计算,得出 Co@C 可以协同调节 PMS 在 Co SAs 上的吸附行为,从而有效地激活 PMS 产生大量单线态氧,实现显著的 CL 发射。在最佳条件下,所制备的 CL 生物传感器具有良好的线性范围、优异的灵敏度和选择性,在人血清中前列腺特异性抗原的实际检测中具有很大的应用潜力。

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