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Title: Gold core/ceria shell-based redox active nanozyme mimicking the biological multienzyme complex phenomenon

Abstract

Catalytically active individual gold (Au) and cerium oxide (CeO2) nanoparticles 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. A functional nanozyme depicting multienzyme like properties that functions as a synthetic super enzyme has eluded the researchers in the nanoscience community for past decade. In current report, we have designed a functional multienzyme in the form of Gold (core)-CeO2 (shell) nanoparticles (Au@CeO2 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 HRP enzyme. Unlike peroxidase-like activity exhibited by other nanomaterials, Au@CeO2 CSNPs showed decrease in hydroxyl radical formation, suggesting that the bio catalytic 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 nanoparticlesmore » was extended for the detection of glucose, which showed a linear range of detection between (100 µM – 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@CeO2 CSNPs may open new directions for development of single platform sensors in multiple biosensing applications.« less

Authors:
; ; ; ; ; ORCiD logo
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1439652
Report Number(s):
PNNL-SA-128017
Journal ID: ISSN 0021-9797; 39891; KP1704020
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Colloid and Interface Science; Journal Volume: 513; Journal Issue: C
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Bhagat, Stuti, Srikanth Vallabani, N. V., Shutthanandan, Vaithiyalingam, Bowden, Mark, Karakoti, Ajay S., and Singh, Sanjay. Gold core/ceria shell-based redox active nanozyme mimicking the biological multienzyme complex phenomenon. United States: N. p., 2018. Web. doi:10.1016/j.jcis.2017.11.064.
Bhagat, Stuti, Srikanth Vallabani, N. V., Shutthanandan, Vaithiyalingam, Bowden, Mark, Karakoti, Ajay S., & Singh, Sanjay. Gold core/ceria shell-based redox active nanozyme mimicking the biological multienzyme complex phenomenon. United States. doi:10.1016/j.jcis.2017.11.064.
Bhagat, Stuti, Srikanth Vallabani, N. V., Shutthanandan, Vaithiyalingam, Bowden, Mark, Karakoti, Ajay S., and Singh, Sanjay. Thu . "Gold core/ceria shell-based redox active nanozyme mimicking the biological multienzyme complex phenomenon". United States. doi:10.1016/j.jcis.2017.11.064.
@article{osti_1439652,
title = {Gold core/ceria shell-based redox active nanozyme mimicking the biological multienzyme complex phenomenon},
author = {Bhagat, Stuti and Srikanth Vallabani, N. V. and Shutthanandan, Vaithiyalingam and Bowden, Mark and Karakoti, Ajay S. and Singh, Sanjay},
abstractNote = {Catalytically active individual gold (Au) and cerium oxide (CeO2) nanoparticles 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. A functional nanozyme depicting multienzyme like properties that functions as a synthetic super enzyme has eluded the researchers in the nanoscience community for past decade. In current report, we have designed a functional multienzyme in the form of Gold (core)-CeO2 (shell) nanoparticles (Au@CeO2 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 HRP enzyme. Unlike peroxidase-like activity exhibited by other nanomaterials, Au@CeO2 CSNPs showed decrease in hydroxyl radical formation, suggesting that the bio catalytic 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 – 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@CeO2 CSNPs may open new directions for development of single platform sensors in multiple biosensing applications.},
doi = {10.1016/j.jcis.2017.11.064},
journal = {Journal of Colloid and Interface Science},
number = C,
volume = 513,
place = {United States},
year = {Thu Mar 01 00:00:00 EST 2018},
month = {Thu Mar 01 00:00:00 EST 2018}
}