Endowing Single-Chain Polymer Nanoparticles with Enzyme-Mimetic Activity.

ACS Macro Lett

Centro de Física de Materiales (CSIC, UPV/EHU)-Materials Physics Center, Paseo Manuel de Lardizabal 5, 20018 San Sebastián, Spain.

Published: September 2013

The development of simple, efficient, and robust strategies affording the facile construction of biomimetic organocatalytic nano-objects is currently a subject of great interest. Herein, a new pathway to artificial organocatalysts based on partially collapsed individual soft nano-objects displaying useful and diverse biomimetic catalytic functions is reported. Single-chain polymer nanoparticles endowed with enzyme-mimetic activity synthesized following this new route display (i) a relatively extended morphology under good solvent conditions, as revealed by small angle neutron scattering and coarse-grained molecular dynamics simulation results, (ii) multiple, compartmentalized, and accessible catalytic sites in which borane catalytic units are retained via B···O interactions, and (iii) unprecedented reductase and polymerase enzyme-mimetic properties.

Download full-text PDF

Source
http://dx.doi.org/10.1021/mz4003744DOI Listing

Publication Analysis

Top Keywords

single-chain polymer
8
polymer nanoparticles
8
enzyme-mimetic activity
8
endowing single-chain
4
nanoparticles enzyme-mimetic
4
activity development
4
development simple
4
simple efficient
4
efficient robust
4
robust strategies
4

Similar Publications

Analysis of the internal motions of thermoresponsive polymers and single chain nanoparticles.

Soft Matter

January 2025

Department of Macromolecular Science and Engineering, Case Western Reserve University, 10900 Euclid Ave., Cleveland, OH 44122, USA.

Data-driven techniques, such as proper orthogonal decomposition (POD) and uniform manifold approximation & projection (UMAP), are powerful methods for understanding polymer behavior in complex systems that extend beyond ideal conditions. They are based on the principle that low-dimensional behaviors are often embedded within the structure and dynamics of complex systems. Here, the internal motions of a thermoresponsive, LCST polymer are investigated for two cases: (1) the coil-to-globule transition that occurs as the system is heated above its critical temperature and (2) intramolecularly crosslinked, single chain nanoparticles (SCNPs) both above and below the critical temperature ().

View Article and Find Full Text PDF

Efficient Cytosolic Delivery of Single-Chain Polymeric Artificial Enzymes for Intracellular Catalysis and Chemo-Dynamic Therapy.

J Am Chem Soc

January 2025

The State Key Laboratory of Molecular Engineering of Polymers and Department of Macromolecular Science, Fudan University, Shanghai 200438, P. R China.

Designing artificial enzymes for in vivo catalysis presents a great challenge due to biomacromolecule contamination, poor biodistribution, and insufficient substrate interaction. Herein, we developed single-chain polymeric nanoparticles with Cu/N-heterocyclic carbene active sites (SCNP-Cu) to function as peroxidase mimics for in vivo catalysis and chemo-dynamic therapy (CDT). Compared with the enzyme mimics based on unfolded linear polymer scaffold and multichain cross-linked scaffold, SCNP-Cu exhibits improved tumor accumulation and CDT efficiency both in vitro and in vivo.

View Article and Find Full Text PDF

We have previously found that the presence of an H-type excitonic dimer formed by two fluorophores covalently bound to an oligonucleotide allows the delivery of such a polymer into live cells without inducing toxicity. We are now using time-resolved fluorescence measurements in solution to understand the molecular dynamics of an antisense probe and how pairing with complementary sense strands of various lengths and degrees of complementarity affects the antisense strand's properties. We report that a DNA strand composed of 30 residues and labeled with an H-type excitonic Cyanine-5/Cyanine-5 dimer shows a predominant 1.

View Article and Find Full Text PDF

Compositions of ethylene glycol dicyclopentenyl ether methacrylate (EGDEMA), a vegetable oil based alkyl methacrylate (C13MA), and furfuryl methacrylate (FMA) were terpolymerized for dual-crosslinked networks with tailored mechanical and thermal properties. Specifically, initiators for continuous activator regeneration (ICAR) atom transfer radical polymerization (ATRP) afforded materials with tailored glass transition temperature ( ) and incorporation of furan and norbornene functionalities within a single chain. The terpolymer with high furan and norbornene functionality (Ter2: = 0.

View Article and Find Full Text PDF

Photoinduced Energy/Electron Transfer within Single-Chain Nanoparticles.

Angew Chem Int Ed Engl

January 2025

Queensland University of Technology, School of Chemistry and Physics, 2 George Street, 4000, Brisbane, AUSTRALIA.

We demonstrate that single-chain nanoparticles (SCNPs) - compact covalently folded single polymer chains - can increase photocatalytic performance of an embedded catalytic center, compared to the comparable catalytic system in free solution. In particular, we demonstrate that the degree of compaction allows to finely tailor the catalytic activity, thus evidencing that molecular confinement is a key factor in controlling photocatalysis. Specifically, we decorate a linear parent polymer with both photoreactive chalcone moieties as well as Ru(bpy)3 catalytic centers.

View Article and Find Full Text PDF

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!