Fluoride-capped nanoceria as a highly efficient oxidase-mimicking nanozyme: inhibiting product adsorption and increasing oxygen vacancies

Zhao, Yilin; Wang, Yawen; Mathur, Avi; Wang, Yaoqiang; Maheshwari, Vivek; Su, Haijia; Liu, Juewen

doi:10.1039/c9nr05346h

Cited by 84 publications

(95 citation statements)

References 58 publications

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“…When the surface active sites are consumed, the nanozyme became inactivated. A similar kinetic behavior was also observed for reacting CeO 2 with ABTS (CeO 2 being an oxidase‐mimic), and it was attributed to the adsorption of the oxidation product of ABTS inhibiting the adsorption of new substrates . A similar mechanism could also take place here such as by the products as an inhibitor.…”

Section: Resultssupporting

confidence: 60%

“…Our nanoceria had an average size of around 5 nm (Figure B). Other characterizations of it including XPS, XRD, DLS and high‐resolution TEM were published previously, and not repeated here. Nanoceria has been shown to have phosphatase‐like activity with a few substrates, including p‐NPP .…”

Section: Resultsmentioning

confidence: 99%

“…In addition, some Ce(III) complexes were also reported to have similar activities . For very small CeO 2 nanoparticles, a large fraction of the surface cerium species are Ce(III) . Therefore, it is interesting to compare the activity of Ce(IV), Ce(III) and CeO 2 alongside with alkaline phosphatase (ALP), a protein‐based enzyme, for dephosphorylation.…”

Section: Introductionmentioning

confidence: 99%

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Self‐limited Phosphatase‐mimicking CeO₂ Nanozymes

Liu

2020

ChemNanoMat

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CeO2 nanoparticles or nanoceria is a very interesting enzyme mimic (nanozyme) with a diverse range of catalytic activities. Most of the previous studies focused on its redox chemistry for mimicking oxidase, peroxidase, and catalase‐like activities, and as a scavenger of reactive oxygen species. Considering CeO2 has both Ce(III) and Ce(IV) species and both interact strongly with inorganic phosphate, nanoceria has also been studied for its phosphatase‐like activity. We herein compared these species along with alkaline phosphatase (ALP). First, CeO2 and Ce(IV) have good activity using p‐nitrophenylphosphate (p‐NPP) as a substrate, while other metal ions failed to show this activity. Since a reaction product is inorganic phosphate and we observed an interesting enzyme kinetic profile, the effect of phosphate was studied, which inhibited both CeO2 and ALP. The inhibition constant was about 5‐fold smaller for CeO2. The inhibition effect of polyphosphates was even stronger. Due to the product inhibition effect, CeO2 is unlikely to be a typical multiple turnover nanozyme, and the system is self‐limited. For the other anions, only F− showed a moderate inhibition effect on the cerium species, while adsorption of DNA did not inhibit the activity. Finally, heat treated ALP lost the activity, but CeO2 and Ce(IV) remained active. This study has deepened our understanding of CeO2 as a phosphatase mimicking nanozyme, which could be useful for biosensing and chemical biology applications.

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Section: Resultssupporting

confidence: 60%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Self‐limited Phosphatase‐mimicking CeO₂ Nanozymes

Liu

2020

ChemNanoMat

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“…•− could also be efficiently produced by welldesigned nanocatalysts with oxidative activity. [36][37][38][39][40][41][42][43][44] Ideally, a nanomaterial could catalytically generate O 2…”

Section: Introductionmentioning

confidence: 99%

A pH‐Responsive Polymer‐CeO₂ Hybrid to Catalytically Generate Oxidative Stress for Tumor Therapy

Tian

Liu

Guo

et al. 2020

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effect), a lower pH value, as well as a high level of oxidative stress. [4-9] Especially, the overproduction of reactive oxygen species (ROS) induces a serious oxidative stress, which is strongly implicated to various tumors. [8,9] In addition, a high ROS level is also considered to be an endpoint of the alteration of several important metabolic pathways in tumors. [8-11] Thus, modulation of the intratumor ROS level, either by scavenging ROS or increasing ROS, is a promising approach to anticancer therapy and ROS-related biomedical fields. [10-19] Recently, nanomaterial-enabled biocatalytic chemodynamic therapy has been demonstrated as a promising method for therapeutic intervention in a variety of tumors. [11-16,20] Through this biocatalytic tumor therapy, intratumor H 2 O 2 can be converted into toxic hydroxyl radicals (• OH) with the help of catalysts that can then induce tumor cell apoptosis and death through oxidative damage to various biomacromolecules, including DNA, lipids, and proteins. Nevertheless, the relatively deficient intratumoral H 2 O 2 level significantly lowers the biocatalytic therapeutic efficiency. [21-27] Thus, the focus has been on increasing the intratumoral H 2 O 2 level through oxidization of intratumoral molecules Catalytic generation of reactive oxygen species has been developed as a promising methodology for tumor therapy. Direct O 2 •− production from intratumor oxygen exhibits exceptional tumor therapeutic efficacy. Herein, this therapy strategy is demonstrated by a pH-responsive hybrid of porous CeO 2 nanorods and sodium polystyrene sulfonate that delivers high oxidative activity for O 2 •− generation within acidic tumor microenvironments for chemodynamic therapy and only limited oxidative activity in neutral media to limit damage to healthy organs. The hydrated polymer-nanorod hybrids with large hydrodynamic diameters form nanoreactors that locally trap oxygen and biological substrates inside and improve the charge transfer between the catalysts and substrates in the tumor microenvironment, leading to enhanced catalytic O 2 •− production and consequent oxidation. Together with successful in vitro and in vivo experiments, these data show that the use of hybrids provides a compelling opportunity for the delivery selective chemodynamic tumor therapy.

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“…For example, the coating of DNA or other biomolecules have been found for inhibiting the activities of nanozymes [17,18]. However, in some cases, a modification would form a favorable environment to enhance or recover the activities of nanozymes [19][20][21]. For instance, phosphite was reported to recover the oxidase-like activity of nickel oxide nanoparticles [21].…”

Section: Introductionmentioning

confidence: 99%

Enhancement of the Peroxidase-Like Activity of Iodine-Capped Gold Nanoparticles for the Colorimetric Detection of Biothiols

et al. 2020

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A colorimetric assay was developed for the detection of biothiols, based on the peroxidase-like activity of iodine-capped gold nanoparticles (AuNPs). These AuNPs show a synergetic effect in the form of peroxidase-mimicking activity at the interface of AuNPs, while free AuNPs and iodine alone have weak catalytic properties. Thus, iodine-capped AuNPs possess good intrinsic enzymatic activity and trigger the oxidation of 3,3’,5,5’-tetramethylbenzidine (TMB), leading to a change in color from colorless to yellow. When added to solution, biothiols, such as cysteine, strongly bind to the interface of AuNPs via gold-thiol bonds, inhibiting the catalytic activity of AuNPs, resulting in a decrease in oxidized TMB. Using this strategy, cysteine could be linearly determined, at a wide range of concentrations (0.5 to 20 μM), with a detection limit of 0.5 μM using UV-Vis spectroscopy. This method was applied for the detection of cysteine in diluted human urine.

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Fluoride-capped nanoceria as a highly efficient oxidase-mimicking nanozyme: inhibiting product adsorption and increasing oxygen vacancies

Abstract: Fluoride capping prevents the oxidation product from inhibiting the CeO2 nanozyme, and increases the oxygen vacancy concentration for more efficient catalysis.

Cited by 84 publications

References 58 publications

Self‐limited Phosphatase‐mimicking CeO₂ Nanozymes

Self‐limited Phosphatase‐mimicking CeO₂ Nanozymes

A pH‐Responsive Polymer‐CeO₂ Hybrid to Catalytically Generate Oxidative Stress for Tumor Therapy

Enhancement of the Peroxidase-Like Activity of Iodine-Capped Gold Nanoparticles for the Colorimetric Detection of Biothiols

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Fluoride-capped nanoceria as a highly efficient oxidase-mimicking nanozyme: inhibiting product adsorption and increasing oxygen vacancies

Abstract: Fluoride capping prevents the oxidation product from inhibiting the CeO2 nanozyme, and increases the oxygen vacancy concentration for more efficient catalysis.

Cited by 84 publications

References 58 publications

Self‐limited Phosphatase‐mimicking CeO2 Nanozymes

Self‐limited Phosphatase‐mimicking CeO2 Nanozymes

A pH‐Responsive Polymer‐CeO2 Hybrid to Catalytically Generate Oxidative Stress for Tumor Therapy

Enhancement of the Peroxidase-Like Activity of Iodine-Capped Gold Nanoparticles for the Colorimetric Detection of Biothiols

Contact Info

Product

Resources

About

Self‐limited Phosphatase‐mimicking CeO₂ Nanozymes

Self‐limited Phosphatase‐mimicking CeO₂ Nanozymes

A pH‐Responsive Polymer‐CeO₂ Hybrid to Catalytically Generate Oxidative Stress for Tumor Therapy