Nanozymes: Gold‐Nanoparticle‐Based Transphosphorylation Catalysts

Manea, Flavio; Houillon, Florence Bodar; Pasquato, Lucia; Scrimin, Paolo

doi:10.1002/ange.200460649

Cited by 164 publications

(135 citation statements)

References 48 publications

(22 reference statements)

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“…These particles can resemble biomolecules and biomolecular assemblies in terms of size and chemical composition and sometimes function (for example, enzymatic activity) 27,28 , but their tightly packed ligand shell 24 lacks the structural flexibility of proteins or peptide assemblies and instead is composed of an ordered layer of surface functional groups. Simple reactions enable the synthesis of these particles coated with single-as well as multicomponent ligand shells, the composition and morphology of which can be easily and precisely controlled 29 .…”

mentioning

confidence: 99%

Surface-structure-regulated cell-membrane penetration by monolayer-protected nanoparticles

Verma¹,

Uzun²,

et al. 2008

Nature Mater

1,182

1,203

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Nanoscale objects are typically internalized by cells into membrane-bounded endosomes and fail to access the cytosolic cell machinery. Whereas some biomacromolecules may penetrate or fuse with cell membranes without overt membrane disruption, no synthetic material of comparable size has shown this property yet. Cationic nano-objects pass through cell membranes by generating transient holes, a process associated with cytotoxicity. Studies aimed at generating cell-penetrating nanomaterials have focused on the effect of size, shape and composition. Here, we compare membrane penetration by two nanoparticle 'isomers' with similar composition (same hydrophobic content), one coated with subnanometre striations of alternating anionic and hydrophobic groups, and the other coated with the same moieties but in a random distribution. We show that the former particles penetrate the plasma membrane without bilayer disruption, whereas the latter are mostly trapped in endosomes. Our results offer a paradigm for analysing the fundamental problem of cell-membrane-penetrating bio-and macro-molecules. Nanomaterials are of great interest for use in biomedicine as imaging tools 1-3 , phototherapy agents 4,5 and gene delivery carriers 6,7 . Their interactions with cell membranes are of central importance for all such applications. For example, many drugdelivery systems are based on the transport of therapeutic agents to the cytosol or nucleus of cells by nanoparticles; efficient delivery must be achieved while avoiding cytotoxicity during passage through cell membranes to reach intracellular target compartments 8,9 . Indeed, membrane penetration by synthetic 10 as well as by biologically derived 11 molecules/particles is currently under intense investigation. Some biomacromolecules, such as cell-penetrating peptides (CPPs), may be capable of penetrating membranes without overt lipid bilayer disruption/poration 12-15 . Likewise, synthetic nanomaterials with very small dimensions (molecules, metal nanoclusters 16 , small dendrimers 10 and carbon nanotubes 17 ) can also pass through cell membranes. However, to the best of our knowledge, no synthetic material larger than a few nanometres in size can pass through membranes without disrupting the integrity of these biological barriers. For example, charged particles (such as cationic quantum dots or dendrimers, mostly assisted by some degree of hydrophobicity) induce transient poration of cell membranes to enter cells, a process associated with cytotoxicity 18 . Alternatively, nanoparticles have been designed to explicitly disrupt endolysosomal membranes to enter the cell by force 19 or enter the cell aided by exogenous agents such as CPP chaperones 20 . In contrast, most nanoparticles are trapped in endosomes 21 and hence do not reach the cytosol.The surface properties of nanomaterials play a critical role in determining the outcome of their interactions with cells 22 . Recently, we found that when gold nanoparticles are coated with binary mixtures of hydrophobic and hydrophilic organic mo...

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mentioning

confidence: 99%

Surface-structure-regulated cell-membrane penetration by monolayer-protected nanoparticles

Verma¹,

Uzun²,

et al. 2008

Nature Mater

1,182

1,203

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“…Recently, ceria NPs with different Ce 4+ /Ce 3+ ratios showed the ability to act as mimics of superoxide dismutase, catalase and oxidase, thus proving to be efficient artificial enzymes (often referenced as nanozymes) 31 able to protect cells from the oxidative stress due to an excess of reactive oxygen species. 9,10,11,12,13,32,33 In a recent work, Peng et al 33 asserted that CeO 2 NPs, instead of working as a catalyst, behave as an oxidizing agent, due to the progressive dissolution of Ce 3+ in the reactive mixture.…”

Section: Reactivity Of Core-shell Nps As Artificial Enzymesmentioning

confidence: 99%

TiO₂@CeO_x Core–Shell Nanoparticles as Artificial Enzymes with Peroxidase-Like Activity

Artiglia

Agnoli

Paganini

et al. 2014

ACS Appl. Mater. Interfaces

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The Ce 4+ ↔ Ce 3+ redox switch is at the basis of an all-inorganic catalytic cycle that is capable to mimic the activity of several natural redox enzymes. The efficiency of these artificial enzymes (nanozymes) strongly depends on the Ce 4+ /Ce 3+ ratio. By capitalizing on the results obtained on oxide/oxide model systems, we implemented a simple and effective procedure to obtain conformal TiO 2 @CeO x core-shell nanoparticles whose thickness is controlled with single layer precision. Since the Ce 3+ species are stabilized only at the interface by the electronic hybridization with the TiO 2 states, the modulation of the shell thickness offers a simple method to tailor the Ce 4+ /Ce 3+ ratio and therefore the catalytic properties. The activity of these nanoparticles as artificial peroxidase-like enzymes was tested, showing exceptional 2 performances, even better than natural horseradish peroxidase enzyme. The main advantage with respect to other oxide/oxide nanozymes is that our nanoparticles, having a tunable Ce 4+ /Ce 3+ ratio, are efficient already at low H 2 O 2 concentrations.

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“…Among the countless examples of artificial enzymes, the emergence of and recent advances in nanotechnology and biology provide new opportunities for designing functional nanomaterials with enzyme-like characteristics. 4,[6][7][8] These materials might serve as novel and promising artificial enzymes with the advantages of facile preparation, tunability of catalytic activity and high stability under stringent conditions. Owing to the excellent catalytic properties of these nanomaterials, Scrimin and co-workers 7 called them 'nanozymes' in analogy to the nomenclature of catalytically active polymers (synzymes).…”

Section: Introductionmentioning

confidence: 99%

Incorporating ATP into biomimetic catalysts for realizing exceptional enzymatic performance over a broad temperature range

Lin

Ren

2014

NPG Asia Mater

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There has been great interest in the development of artificial inorganic nanomaterials that mimic natural peroxidases. Unfortunately, these nanomaterials usually possess relatively low catalytic activity and are generally considered to work effectively only within a narrow temperature range (for example, they are inactive at high temperatures). Intriguingly, adenosine triphosphate (ATP) is not only the ubiquitous energy currency of life, it is also known to form charge transfer complexes with aromatic molecules and to participate in free radical redox chemistry. Inspired by its unique properties, for the first time, we reveal a novel catalytic role for ATP and show that ATP is an ideal boosting agent for markedly improving the catalytic activity of a peroxidase mimic over a broad temperature range and, more significantly, making it possible to achieve exceptionally efficient high-temperature catalytic reactions. These observations pave the way for identifying highly effective modulators that promote the overall performance of artificial enzymes. NPG Asia Materials (2014) 6, e114; doi:10.1038/am.2014.42; published online 18 July 2014 INTRODUCTION Natural enzymes, which are biological molecules of immense catalytic force and high substrate specificity, have attracted considerable attention for use in pharmaceutical processes, agrochemical production, biosensing and food industry applications. 1-3 However, their applications are largely limited by their intrinsic properties, such as the sensitivity of catalytic activity to environmental conditions and low operational stability (owing to denaturation and digestion), as well as by the high costs of preparation and purification. 4,5 To circumvent the aforementioned limitations, tremendous efforts have been made to develop biomimetic catalysts. Among the countless examples of artificial enzymes, the emergence of and recent advances in nanotechnology and biology provide new opportunities for designing functional nanomaterials with enzyme-like characteristics. 4,[6][7][8] These materials might serve as novel and promising artificial enzymes with the advantages of facile preparation, tunability of catalytic activity and high stability under stringent conditions. Owing to the excellent catalytic properties of these nanomaterials, Scrimin and co-workers 7 called them 'nanozymes' in analogy to the nomenclature of catalytically active polymers (synzymes). Magnetic nanoparticles, 4,9 CeO 2 , 6,10-12 V 2 O 5 , 13,14 gold nanoparticles, 7,8,[15][16][17][18] PtPd ÀFe 3 O 4 , 19,20 carbon nanotubes, 21,22 graphene oxide and graphene nanocomposites 23,24 and other types of nanoparticle have been found to exhibit unique enzyme-like catalytic activities and have

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Nanozymes: Gold‐Nanoparticle‐Based Transphosphorylation Catalysts

Cited by 164 publications

References 48 publications

Surface-structure-regulated cell-membrane penetration by monolayer-protected nanoparticles

Surface-structure-regulated cell-membrane penetration by monolayer-protected nanoparticles

TiO₂@CeO_x Core–Shell Nanoparticles as Artificial Enzymes with Peroxidase-Like Activity

Incorporating ATP into biomimetic catalysts for realizing exceptional enzymatic performance over a broad temperature range

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Nanozymes: Gold‐Nanoparticle‐Based Transphosphorylation Catalysts

Cited by 164 publications

References 48 publications

Surface-structure-regulated cell-membrane penetration by monolayer-protected nanoparticles

Surface-structure-regulated cell-membrane penetration by monolayer-protected nanoparticles

TiO2@CeOx Core–Shell Nanoparticles as Artificial Enzymes with Peroxidase-Like Activity

Incorporating ATP into biomimetic catalysts for realizing exceptional enzymatic performance over a broad temperature range

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TiO₂@CeO_x Core–Shell Nanoparticles as Artificial Enzymes with Peroxidase-Like Activity