Electroanalytical Evaluation of Antioxidant Activity of Cerium Oxide Nanoparticles by Nanoparticle Collisions at Microelectrodes

Sardesai, Naimish P.; Andreescu, Daniel; Andreescu, Silvana

doi:10.1021/ja408087s

Cited by 94 publications

(91 citation statements)

References 30 publications

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“…In contrast, the higher ratio CNP1 solution shows a more diffuse, wide peak at a similar potential; this behavior is consistent with complex catalysis mechanisms presented in literature 49 . Specifically, the peak character suggests that reduction initially occurs, however, the catalysis is kinetically restricted for high Ce 3+ :Ce 4+ formulations.…”

Section: Resultssupporting

confidence: 91%

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Picomolar Detection of Hydrogen Peroxide using Enzyme-free Inorganic Nanoparticle-based Sensor

Neal

Gupta

Barkam

et al. 2017

Sci Rep

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A philosophical shift has occurred in the field of biomedical sciences from treatment of late-stage disease symptoms to early detection and prevention. Ceria nanoparticles (CNPs) have been demonstrated to neutralize free radical chemical species associated with many life-threatening disease states such as cancers and neurodegenerative diseases by undergoing redox changes (Ce3+ ↔ Ce4+). Herein, we investigate the electrochemical response of multi-valent CNPs in presence of hydrogen peroxide and demonstrate an enzyme-free CNP-based biosensor capable of ultra-low (limit of quantitation: 0.1 pM) detection. Several preparations of CNPs with varying Ce3+:Ce4+ are produced and are analyzed by electrochemical methods. We find that an increasing magnitude of response in cyclic voltammetry and chronoamperometry correlates with increasing Ce4+ relative to Ce3+ and utilize this finding in the design of the sensor platform. The sensor retains sensitivity across a range of pH’s and temperatures, wherein enzyme-based sensors will not function, and in blood serum: reflecting selectivity and robustness as a potential implantable biomedical device.

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Section: Resultssupporting

confidence: 91%

“…The peaks common to all formulations occur at ~0 V (hereafter, peak 1 ), −0.23 V ( peak 2 ) and 0.4–0.7 V ( peak 3 ). These are attributed to the CNP-mediated reduction of H 2 O 2 ( peaks 1 and 2 ) and the oxidation of the Au electrode ( peak 3 ) 48, 49 , respectively.…”

Section: Resultsmentioning

confidence: 99%

Picomolar Detection of Hydrogen Peroxide using Enzyme-free Inorganic Nanoparticle-based Sensor

Neal

Gupta

Barkam

et al. 2017

Sci Rep

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“…11 As discussed next, the experiment reported here is most similar to the latter approach. Finally, we note that the research groups of Unwin, 12,13 Zhang, 14,15 Koper, 12,16 Andreescu, 17 Alpuche-Aviles, 18 Crooks, 2,19–21 Stevenson, 22–24 and MacPherson 25 have all made important contributions to the general field of single-particle collision electrochemistry that have influenced the findings reported here.…”

Section: Introductionmentioning

confidence: 72%

Electrocatalytic amplification of DNA-modified nanoparticle collisions via enzymatic digestion

et al. 2016

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“…Nanoceria is a versatile nanozyme, displaying oxidase, 16,20 catalase, 24,25 superoxide dismutase, 26,27 and phosphatase 28 activities under different conditions. In 2009, Asati and co-workers first reported the oxidase-like activity of nanoceria.…”

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confidence: 99%

Boosting the oxidase mimicking activity of nanoceria by fluoride capping: rivaling protein enzymes and ultrasensitive F⁻detection

2016

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Nanomaterial-based enzyme mimics (nanozymes) are currently a new forefront of chemical research. However, the application of nanozymes is limited by its low catalytic activity and low turnover numbers. Cerium dioxide nanoparticles (nanoceria) is among the few with oxidase activity. Herein, we report an interesting finding addressing its limitations. The oxidase activity of nanoceria is improved by over 100-fold by fluoride capping, rendering it more close to real oxidases (e.g., cytochrome P450). The turnover number reached 700 in 15 min, drastically improved from ~15 turnovers for the naked particles. The mechanism is attributed to surface charge modulation and facilitated electron transfer by Fcapping based on ζ-potential and free radical measurement. Ultrasensitive sensing of fluoride was achieved with a detection limit of 0.64 µM F -in water and in toothpastes, while no other tested anions can achieve the activity enhancement.Developing nanomaterial-based enzyme mimics, known as nanozymes, is a new frontier in inorganic, materials and analytical chemistry. [1][2][3][4][5][6][7] Nanozymes are a subset of nanoparticle-based catalysts that catalyze enzyme-like reactions at ambient conditions. Nanozymes are attractive not only for their high stability and lowcost, but also for studying fundamental processes at nanoscale surfaces. 2 Many nanoparticles such as gold, 4,8,9 graphene oxide, 10,11 and various metal oxides 1,3,5,12-19 possess oxidase, peroxidase, and/or catalase like activities. It is interesting to note that while many peroxidase nanozymes were reported (i.e., using H2O2 as a cosubstrate), very few have oxidase activity. 9,[19][20][21][22][23] The best known examples are gold nanoparticles for glucose oxidation, 9 and CeO2 nanoparticles (nanoceria) that oxidize a diverse range of substrates. 20 Oxidase nanozymes are important since they do not require unstable H2O2 as a co-substrate.Nanoceria is a versatile nanozyme, displaying oxidase, 16,20 catalase, 24,25 superoxide dismutase, 26,27 and phosphatase 28 activities under different conditions. In 2009, Asati and co-workers first reported the oxidase-like activity of nanoceria. 20 Since then, nanoceria has become an attractive system receiving extensive studies. The catalytic activities of nanoceria were attributed to the mixed oxidation states of Ce 3+ and Ce 4+ , and related oxygen vacancies. 29,30 The role of redox states, 24 surface coating, 20 pH, 31 buffer composition, 32 and nucleotide triphosphate 16 were investigated. We hypothesize that surface chemistry plays a critical role in modulating substrate/product adsorption and electron transfer, thus influencing catalytic efficiency. A challenge in the nanozyme field is poor catalytic activity and low turnover, which is in sharp contrast to their highly efficient protein counterparts.

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Electroanalytical Evaluation of Antioxidant Activity of Cerium Oxide Nanoparticles by Nanoparticle Collisions at Microelectrodes

Cited by 94 publications

References 30 publications

Picomolar Detection of Hydrogen Peroxide using Enzyme-free Inorganic Nanoparticle-based Sensor

Picomolar Detection of Hydrogen Peroxide using Enzyme-free Inorganic Nanoparticle-based Sensor

Electrocatalytic amplification of DNA-modified nanoparticle collisions via enzymatic digestion

Boosting the oxidase mimicking activity of nanoceria by fluoride capping: rivaling protein enzymes and ultrasensitive F⁻detection

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Electroanalytical Evaluation of Antioxidant Activity of Cerium Oxide Nanoparticles by Nanoparticle Collisions at Microelectrodes

Cited by 94 publications

References 30 publications

Picomolar Detection of Hydrogen Peroxide using Enzyme-free Inorganic Nanoparticle-based Sensor

Picomolar Detection of Hydrogen Peroxide using Enzyme-free Inorganic Nanoparticle-based Sensor

Electrocatalytic amplification of DNA-modified nanoparticle collisions via enzymatic digestion

Boosting the oxidase mimicking activity of nanoceria by fluoride capping: rivaling protein enzymes and ultrasensitive F−detection

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Boosting the oxidase mimicking activity of nanoceria by fluoride capping: rivaling protein enzymes and ultrasensitive F⁻detection