Enzyme-Mimetic Antioxidant Luminescent Nanoparticles for Highly Sensitive Hydrogen Peroxide Biosensing

生物传感器 过氧化氢 过氧化氢酶 纳米颗粒 化学 纳米材料 抗氧化剂 纳米技术 组合化学 材料科学 生物化学
作者
Anna Pratsinis,Georgios A. Kelesidis,Stefanie Zuercher,Frank Krumeich,Sreenath Bolisetty,Raffaele Mezzenga,Jean‐Christophe Leroux,Georgios A. Sotiriou
出处
期刊:ACS Nano [American Chemical Society]
卷期号:11 (12): 12210-12218 被引量:125
标识
DOI:10.1021/acsnano.7b05518
摘要

Hydrogen peroxide (H 2 O 2 ) is an abundant molecule associated with biological functions and reacts with natural enzymes, such as catalase. Even though direct H 2 O 2 measurement can be used to diagnose pathological conditions, such as infection and inflammation, H 2 O 2 quantification further enables the detection of disease biomarkers in enzyme-linked assays ( e.g., ELISA) in which enzymatic reactions may generate or consume H 2 O 2 . Such a quantification is often measured optically with organic dyes in biological media that suffer, however, from poor stability. Currently, the optical H 2 O 2 biosensing without organic-dyes in biological media and at low, submicromolar, concentrations has yet to be achieved. Herein, we rationally design biomimetic artificial enzymes based on antioxidant CeO 2 nanoparticles that become luminescent upon their Eu 3+ doping. We vary systematically their diameter from 4 to 16 nm and study their catalase-mimetic antioxidant activity, manifested as catalytic H 2 O 2 decomposition in aqueous solutions, revealing a strong nanoparticle surface area dependency. The interaction with H 2 O 2 influences distinctly the particle luminescence rendering them highly sensitive H 2 O 2 biosensors down to 0.15 μM (5.2 ppb) in solutions for biological assays. Our results link two, so far, unrelated research domains, the CeO 2 nanoparticle antioxidant activity and luminescence by rare-earth doping. When these enzyme-mimetic nanoparticles are coupled with alcohol oxidase, biosensing can be extended to ethanol exemplifying how their detection potential can be broadened to additional biologically relevant metabolites. The enzyme-mimetic nanomaterial developed here could serve as a starting point of sophisticated in vitro assays toward the highly sensitive detection of disease biomarkers.
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