Division of Biological and Life Sciences, School of Arts and Sciences, Ahmedabad University, Central Campus, Navrangpura, Ahmedabad 380009, Gujarat, India.
Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA 99354, United States.
J Colloid Interface Sci. 2018 Mar 1;513:831-842. doi: 10.1016/j.jcis.2017.11.064. Epub 2017 Dec 22.
Catalytically active individual gold (Au) and cerium oxide (CeO) nanoparticles (NPs) are well known to exhibit specific enzyme-like activities, such as natural catalase, oxidase, superoxide dismutase, and peroxidase enzymes. These activities have been maneuvered to design several biological applications such as immunoassays, glucose detection, radiation and free radical protection and tissue engineering. In biological systems, multienzyme complexes are involved in catalyzing important reactions of essential metabolic processes such as respiration, biomolecule synthesis, and photosynthesis. It is well known that metabolic processes linked with multienzyme complexes offer several advantages over reactions catalyzed by individual enzymes. A functional nanozyme depicting multienzyme like properties has eluded the researchers in the nanoscience community for the past few decades. In the current report, we have designed a functional multienzyme in the form of Gold (core)-CeO (shell) nanoparticles (Au/CeO CSNPs) exhibiting excellent peroxidase, catalase, and superoxide dismutase enzyme-like activities that are controlled simply by tuning the pH. The reaction kinetic parameters reveal that the peroxidase-like activity of this core-shell nanozyme is comparable to natural horseradish peroxidase (HRP) enzyme. Unlike peroxidase-like activity exhibited by other nanomaterials, Au/CeO CSNPs showed a decrease in hydroxyl radical formation, suggesting that the biocatalytic reactions are performed by efficient electron transfers. A significant enzyme-like activity of this core-shell nanoparticle was conserved at extreme pH (2-11) and temperatures (up to 90 °C), clearly suggesting the superiority over natural enzymes. Further, the utility of peroxidase-like activity of this core-shell nanoparticles was extended for the detection of glucose, which showed a linear range of detection between (100 µM to 1 mM). It is hypothesized that the proximity of the redox potentials of Au/Au and Ce (III)/Ce (IV) may result in a redox couple promoting the multienzyme activity of core-shell nanoparticles. Au/CeO CSNPs may open new directions for development of single platform sensors in multiple biosensing applications.
催化活性的单个金(Au)和氧化铈(CeO)纳米粒子(NPs)众所周知,具有特定的酶样活性,如天然过氧化氢酶、氧化酶、超氧化物歧化酶和过氧化物酶。这些活性已被用于设计几种生物应用,如免疫测定、葡萄糖检测、辐射和自由基保护以及组织工程。在生物系统中,多酶复合物参与催化重要的代谢过程反应,如呼吸、生物分子合成和光合作用。众所周知,与多酶复合物相关的代谢过程提供了几个优于单个酶催化的反应的优点。在过去几十年中,纳米科学领域的研究人员一直难以设计出具有多酶样特性的功能性纳米酶。在本报告中,我们设计了一种功能性的多酶,形式为金(核)-氧化铈(壳)纳米粒子(Au/CeO CSNPs),具有出色的过氧化物酶、过氧化氢酶和超氧化物歧化酶样活性,这些活性可通过简单地调节 pH 值来控制。反应动力学参数表明,这种核壳纳米酶的过氧化物酶样活性可与天然辣根过氧化物酶(HRP)酶相媲美。与其他纳米材料表现出的过氧化物酶样活性不同,Au/CeO CSNPs 显示羟基自由基形成减少,表明生物催化反应是通过有效的电子转移进行的。这种核壳纳米粒子的显著酶样活性在极端 pH(2-11)和温度(高达 90°C)下得以保留,明显优于天然酶。此外,这种核壳纳米粒子的过氧化物酶样活性的用途扩展到了葡萄糖的检测,其检测范围在(100µM 至 1mM)之间呈线性。据推测,Au/Au 和 Ce(III)/Ce(IV)的氧化还原电位的接近可能导致一个氧化还原对促进核壳纳米粒子的多酶活性。Au/CeO CSNPs 可能为在多个生物传感应用中开发单一平台传感器开辟新的方向。
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