Highly Efficient Electrogenerated Chemiluminescence Quenching on Lipid-Coated Multifunctional Magnetic Nanoparticles for the Determination of Proteases

化学 猝灭(荧光) 化学发光 电子转移 联吡啶 光化学 纳米颗粒 荧光 结晶学 有机化学 催化作用 纳米技术 物理 晶体结构 材料科学 量子力学
作者
Xiaolin Yang,Yuxi Wei,Zimei Wang,Junxia Wang,Honglan Qi,Qiang Gao,Chengxiao Zhang
出处
期刊:Analytical Chemistry [American Chemical Society]
卷期号:94 (4): 2305-2312 被引量:18
标识
DOI:10.1021/acs.analchem.1c05033
摘要

This work reports a highly efficient electrogenerated chemiluminescence (ECL) quenching on lipid-coated multifunctional magnetic nanoparticles (MMNP) for the determination of proteases incorporating membrane-confined quenching with a specific cleavage reaction for the first time. A new ruthenium complex [Ru(bpy)2(ddcbpy)](PF6)2 (bpy = 2,2′-bipyridine, ddcbpy = 4,4′-didodecyl-carbonyl-2,2′-bipyridine with two hydrophobic long alkyl chains) was synthesized as a signal probe, while [cholesterol-(CH2)6-HSSKLQK(peptide)-ferrocene (quencher)] was designed as a specific peptide-quencher probe. The MMNP were prepared by inserting both the signal probe and the peptide-quencher probe into the cholesterol–phospholipid-coated Fe3O4 magnetic nanoparticles (Fe3O4 NP, ∼200 nm). When prostate specific antigen (PSA) taken as a model analyte was introduced into the suspension of MMNP, PSA cleaved the amide bond of SK in cholesterol-(CH2)6-HSSKLQK-Fc, and then the cleaved peptide-motif-Fc-quencher was deviated from the MMNP, resulting in the increase in the ECL intensity. It was found that the ECL quenching constant of [Ru(bpy)2(ddcbpy)]2+ on MMNP (KSV, NP/lipECL =2.68 × 107 M–1) is 137-folds higher than that on the lipid-coated electrode (KSV, lipECL=1.95 × 105 M–1) and 391-folds higher than that in the solution (KSV, aqECL =6.86 × 104 M–1). The ECL emission of Ru(bpy)32+ derivative-attached Fe3O4 NP was observed at ∼1.2 V, involving the tunnel-electron transfer pathway (TPA• + Ru(bpy)33+ = Ru(bpy)32+*). Based on the highly efficient ECL quenching of the ruthenium complex by ferrocene on the MMNP, a new ECL method was developed for PSA with a linear range from 0.01 to 1.0 ng/mL and a limit of detection of 3.0 pg/mL. This work demonstrates that the approach of ECL quenching by ferrocene on lipid-coated Fe3O4 NP is promising and could be easily extended to determine other proteases.
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