Endowing Single-Chain Polymer Nanoparticles with Enzyme-Mimetic Activity

Perez-Baena, Irma; Barroso‐Bujans, Fabienne; Gasser, Urs; Arbe, Arantxa; Moreno, Angel J.; Colmenero, Juan; Pomposo, José A.

doi:10.1021/mz4003744

Cited by 138 publications

(197 citation statements)

References 39 publications

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“…Among the various techniques employed to these ends, the collapse of single polymer chains (precursors) via purely intramolecular cross-linking, into single-chain nanoparticles (SCNPs), has gained increasing interest over recent years [2][3][4][5] . Significant effort is being devoted to endow SCNPs with useful functions for multiple applications in, e.g., nanomedicine, biosensing, bioimaging or catalysis [6][7][8][9][10] .…”

Section: Introductionmentioning

confidence: 99%

“…Recent investigations by experiments and simulations have highlighted that, in general, the usual synthesis protocols in good solvent conditions produce SCNPs with open, sparse conformations 8,9,11,12 . As revealed by extensive simulations 11 , this feature originates from a fundamental property: the self-avoiding conformations of the linear precursors in good solvent.…”

Section: Introductionmentioning

confidence: 99%

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Tunable slow dynamics in a new class of soft colloids

et al. 2016

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By means of extensive simulations, we investigate concentrated solutions of globular single-chain nanoparticles (SCNPs), an emergent class of synthetic soft nano-objects. By increasing the concentration, the SCNPs show a reentrant behaviour in their structural and dynamical correlations, as well as a soft caging regime and weak dynamic heterogeneity. The latter is confirmed by validation of the Stokes-Einstein relation up to concentrations far beyond the overlap density. Therefore SCNPs arise as a new class of soft colloids, exhibiting slow dynamics and actualizing in a real system structural and dynamical anomalies proposed by models of ultrasoft particles. Quantitative differences in the dynamical behaviour depend on the SCNP deformability, which can be tuned through the degree of internal cross-linking.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Tunable slow dynamics in a new class of soft colloids

et al. 2016

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“…We 7 and others 8,9 have demonstrated that catalytic properties can be imparted to singlechain nanoparticles through polymer folding/collapse accompanied by efficient catalyst immobilization. The potential use of single-chain nanoparticles as drug / siRNA nanocarriers and photostable bioimaging agents relies on the improved construction of functional folded/collapsed single polymer chains.…”

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confidence: 99%

“Michael” Nanocarriers Mimicking Transient-Binding Disordered Proteins

Akbari²,

et al. 2013

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ABSTRACT:We report herein a very efficient synthesis strategy for the construction of artificial transient-binding protein-mimic nano-objects. Michael addition-mediated multidirectional self-assembly of individual polymeric chains at r.t. leads to "Michael" nanocarriers that in solution resemble disordered multidomain proteins, as revealed by a combination of small angle neutron scattering (SANS) measurements and coarse-grained molecular dynamics (MD) results, whereas in the dry state adopt a collapsed, globular morphology, as observed by transmission electron microscopy (TEM). This extended-to-compact morphology transition taking place upon solvent removal is of paramount importance, among other applications, for the construction of efficient biosensors based on immobilized protein-mimic nano-objects and for the development of transient vitamin-binding systems. As a proof of concept, we show the controlled delivery of vitamin B 9 from these novel transient-binding nanocarriers.Nature is a continuous source of inspiration for scientists across different disciplines.1 In particular, the specific -native-conformation of proteins allowing these large biomolecules to carry out sophisticated tasks such as catalysis inspired the construction of a first generation of artificial enzymes based on a variety of molecular and macromolecular structures such as macrocyclic compounds, 2 star and helical polymers, 3 dendrimers 4 and micelles.

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“…SCNPs are obtained, generally at highly diluted conditions, through purely intramolecular cross-linking of single polymer precursors. A series of investigations by small-angle neutron (SANS) and X-ray scattering (SAXS) [8,13,19,20] have revealed that SCNPs synthesized through coventional routes are usually sparse objects with open topologies. A compilation of literature results for SCNPs in solution with very different chemical structures [21] reveals scaling behavior, R ∼ N ν , of the macromolecular radius R with the polymerization degree N, with an average exponent ν ≈ 0.5.…”

Section: Introductionmentioning

confidence: 99%

Effect of chain stiffness on the structure of single-chain polymer nanoparticles

Moreno

Bačová

Verso

et al. 2017

J. Phys.: Condens. Matter

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Abstract.Polymeric single-chain nanoparticles (SCNPs) are soft nano-objects synthesized by purely intramolecular cross-linking of single polymer chains. By means of computer simulations, we investigate the conformational properties of SCNPs as a function of the bending stiffness of their linear polymer precursors. We investigate a broad range of characteristic ratios from the fully flexible case to those typical of bulky synthetic polymers. Increasing stiffness hinders bonding of groups separated by short contour distances and increases looping over longer distances, leading to more compact nanoparticles with a structure of highly interconnected loops. This feature is reflected in a crossover in the scaling behaviour of several structural observables. The scaling exponents change from those characteristic for Gaussian chains or rings in θ-solvents in the fully flexible limit, to values resembling fractal or 'crumpled' globular behaviour for very stiff SCNPs. We characterize domains in the SCNPs. These are weakly deformable regions that can be seen as disordered analogues of domains in disordered proteins. Increasing stiffness leads to bigger and less deformable domains. Surprisingly, the scaling behaviour of the domains is in all cases similar to that of Gaussian chains or rings, irrespective of the stiffness and degree of cross-linking. It is the spatial arrangement of the domains which determines the global structure of the SCNP (sparse Gaussian-like object or crumpled globule). Since intramolecular stiffness can be varied through the specific chemistry of the precursor or by introducing bulky side groups in its backbone, our results propose a new strategy to tune the global structure of SCNPs.

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Endowing Single-Chain Polymer Nanoparticles with Enzyme-Mimetic Activity

Cited by 138 publications

References 39 publications

Tunable slow dynamics in a new class of soft colloids

Tunable slow dynamics in a new class of soft colloids

“Michael” Nanocarriers Mimicking Transient-Binding Disordered Proteins

Effect of chain stiffness on the structure of single-chain polymer nanoparticles

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