Particle Size-Controlled Oxygen Reduction and Evolution Reaction Nanocatalysts Regulate Ru(bpy)_(3)^(2+)’s Dual-potential Electrochemiluminescence for Sandwich Immunoassay  

作　　者：Shijun Wang Shu Zhu Ziqi Kang Xiangxiu Wang Zixin Deng Kun Hu Jianjun Hu Xiancheng Liu Guixue Wang Guangchao Zang Yuchan Zhang 

机构地区：[1]Institute of Life Science and Laboratory of Tissue and Cell Biology,Lab Teaching&Management Center,Chongqing Medical University,Chongqing 400016,China [2]Key Laboratory for Biorheological Science and Technology of Ministry of Education,State and Local Joint Engineering Laboratory for Vascular Implants,Bioengineering College of Chongqing University,Chongqing 400030,China [3]Jinfeng Laboratory,Chongqing 401329,China [4]Department of Pathophysiology,Chongqing Medical University,Chongqing 400016,China [5]Department of Pathology,Guizhou Provincial People’s Hospital,Guiyang,Guizhou 550002,China

出　　处：《Research》2023年第4期701-715,共15页研究（英文）

基　　金：This work was supported by grants from the Natural Science Foundation of Chongqing(cstc2020jcyj-msxmX0330,cstc2021jsyj-yzysbA0057,and cstc2019jcyj-zdxmX0028);the National Natural Science Foundation of China(31971242 and 12032007);the Project of Tutorial System of Medical Undergraduate in Lab Teaching&Management Center in Chongqing Medical University(LTMCMTS202005 and LTMCMTS202110);the JinFeng Laboratory Foundation of Chongqing(jfkyjf202203001);the Scientific and Technological Research Program of Chongqing Municipal Education Commission(KJQN202200426);the Scientific Research,the CQMU Program for Youth Innovation in Future Medicine(W0015);the Innovation Experimental Project of Chongqing Medical University(SRIEP202105).

摘　　要：Multiple signal strategies remarkably improve the accuracy and efficiency of electrochemiluminescence(ECL)immunoassays,but the lack of potential-resolved luminophore pairs and chemical cross talk hinders their development.In this study,we synthesized a series of gold nanoparticles(AuNPs)/reduced graphene oxide(Au/rGO)composites as adjustable oxygen reduction reaction and oxygen evolution reaction catalysts to promote and modulate tris(2,2′-bipyridine)ruthenium(II)(Ru(bpy)_(3)^(2+))’s multisignal luminescence.With the increase in the diameter of AuNPs(3 to 30 nm),their ability to promote Ru(bpy)_(3)^(2+)’s anodic ECL was first impaired and then strengthened,and cathodic ECL was first enhanced and then weakened.Au/rGOs with medium-small and medium-large AuNP diameters remarkably increased Ru(bpy)_(3)^(2+)’s cathodic and anodic luminescence,respectively.Notably,the stimulation effects of Au/rGOs were superior to those of most existing Ru(bpy)_(3)^(2+)co-reactants.Moreover,we proposed a novel ratiometric immunosensor construction strategy using Ru(bpy)_(3)^(2+)’s luminescence promoter rather than luminophores as tags of antibodies to achieve signal resolution.This method avoids signal cross talk between luminophores and their respective co-reactants,which achieved a good linear range of 10−7 to 10−1 ng/ml and a limit of detection of 0.33 fg/ml for detecting carcinoembryonic antigen.This study addresses the previous scarcity of the macromolecular co-reactants of Ru(bpy)_(3)^(2+),broadening its application in biomaterial detection.Furthermore,the systematic clarification of the detailed mechanisms for converting the potential-resolved luminescence of Ru(bpy)_(3)^(2+)could facilitate an in-depth understanding of the ECL process and should inspire new designs of Ru(bpy)_(3)^(2+)luminescence enhancers or applications of Au/rGOs to other luminophores.This work removes some impediments to the development of multisignal ECL biodetection systems and provides vitality into their widespread applications.

关 键 词：LUMINESCENCE POTENTIAL reactant 

分 类 号：O64[理学—物理化学]