A brief user's guide to single-chain nanoparticles

Lyon, Christopher K.; Prasher, Alka; Hanlon, Ashley M.; Tuten, Bryan T.; Tooley, Christian; Frank, Peter; Berda, Erik B.

doi:10.1039/c4py01217h

Cited by 272 publications

(270 citation statements)

References 90 publications

(246 reference statements)

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“…15,16 Most of the covalent strategies are performed in organic solvents and require highly diluted polymer solutions (usually <1 mg/mL), high temperatures and/or the presence of metal catalysts. The preparation of SCPNs through "continuous addition" avoids ultra-dilution conditions, which is beneficial for multigram scale preparations.…”

Section: Synthesis and Functionalization Of Dextran-based Single-chaimentioning

confidence: 99%

Synthesis and functionalization of dextran-based single-chain nanoparticles in aqueous media

et al. 2017

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Synthesis and Functionalization of Dextran-Based Single-Chain Nanoparticles in Aqueous Media IK4-CIDETEC, Pº Miramón 196, 20014, Donostia-San Sebastián, Spain. b. Radiochemistry and Nuclear Imaging Group, CIC biomaGUNE, Pº Miramón 182, 20014, Donostia-San Sebastián, Spain. Water-dispersible dextran-based single-chain polymer nanoparticles (SCPNs) were prepared in aqueous media and mild conditions. Radiolabeling of the resulting biocompatible materials allowed the study of lung deposition of aqueous aerosols after intratracheal nebulization by means of single-photon emission computed tomography (SPECT), demostrating their potential use as imaging contrast agents.Advances in engineering polymer chains at the molecular level 1 have pushed the development of synthetic strategies for the controlled compaction of single polymer coils into unimolecular soft nano-objects, named single-chain polymer nanoparticles (SCPNs).2-4 SCPNs based on synthetic polymers benefit from the possibility of a controlled construction of the precursors in order to prepare tuned SCPNs with desired size and functionality.3 Additionally, a wide variety of biocompatible, non-toxic and ready-to-use natural polymers are available. Consequently, SCPNs have gained interest as potential mimetics of biomacromolecules such as proteins 5,6 and for application in different fields including nanomedicine.7-9 Among natural polymers, polysaccharides can be envisaged as natural analogues of polyethylene glycol (PEG). For example, dextrans have been used in several biomedical applications due to aqueous solubility, biocompatibility, biodegradability, wide availability, ease of modification and non-fouling properties.10,11 However, in vivo application of SCPNs can be limited due to their small size. Rapid blood clearance is expected after intravenous administration of particles below 5 nm size. 12 In the last years, non-invasive lung administration route has been broadly studied, 13 and SCPNs could be beneficial due to their small size.14 Synthetic routes to SCPNs are mainly based on intrachain homo-and hetero-coupling or cross-linking-induced collapseof pre-functionalized polymers through covalent, dynamic covalent, and non-covalent bonding. 15,16 Most of the covalent strategies are performed in organic solvents and require highly diluted polymer solutions (usually <1 mg/mL), high temperatures and/or the presence of metal catalysts. The preparation of SCPNs through "continuous addition" avoids ultra-dilution conditions, which is beneficial for multigram scale preparations. 17 Recently, it has been described that the presence of oligo(ethylene glycol) brushes as side-chains allows to achieve SCPNs at high polymer concentrations (100 mg/mL). 18 However, the development of general procedures to obtain functionalizable SCPNs in aqueous media, mild conditions and scalable conditions is still a challenging issue.Our group reported a strategy to generate structurally defined and water-dispersible poly(methacrylic acid)-based SCPNs.19 In pursuit of novel types of...

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Section: Synthesis and Functionalization Of Dextran-based Single-chaimentioning

confidence: 99%

Synthesis and functionalization of dextran-based single-chain nanoparticles in aqueous media

et al. 2017

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“…[8][9][10][11][12][13][14] Although the design and synthesis of single chain objects has recently received great attention, 15 the development in this field is still in its initial phase. So far, several types of strategies to mediate the single chain collapse to form SCNPs have been explored, [16][17][18][19][20][21][22] ranging from hydrogen bonding, 23-27, 10, 28-31 covalent bonding, [32][33][34][35][36] to dynamic covalent bonding. [37][38][39][40] All these recent advances have provided versatile approaches to induce the folding of a single polymer chain.…”

Section: Introductionmentioning

confidence: 99%

Synthesis of Sequence-Controlled Multiblock Single Chain Nanoparticles by a Stepwise Folding–Chain Extension–Folding Process

et al. 2016

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Copyright and reuse:The Warwick Research Archive Portal (WRAP) makes this work by researchers of the University of Warwick available open access under the following conditions. Copyright © and all moral rights to the version of the paper presented here belong to the individual author(s) and/or other copyright owners. To the extent reasonable and practicable the material made available in WRAP has been checked for eligibility before being made available.Copies of full items can be used for personal research or study, educational, or not-for profit purposes without prior permission or charge. Provided that the authors, title and full bibliographic details are credited, a hyperlink and/or URL is given for the original metadata page and the content is not changed in any way. Publisher's statement:"This document is the Accepted Manuscript version of a Published Work that appeared in final form in Macromolecules copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work http://pubs.acs.org/page/policy/articlesonrequest/index.html ." A note on versions:The version presented here may differ from the published version or, version of record, if you wish to cite this item you are advised to consult the publisher's version. Please see the 'permanent WRAP URL above for details on accessing the published version and note that access may require a subscription. ABSTRACTThe specific activity of proteins can be traced back to their highly defined tertiary structure, which is a result of a perfectly controlled intra-chain folding process. In the herein presented work the folding of different distinct domains within a single macromolecule is demonstrated. RAFT polymerization was used to produce multi-block copolymers, which are decorated with pendant hydroxyl groups in foldable sections, separated by non-functional spacer blocks in between. OH-bearing blocks were folded using an isocyanate cross linker prior to chain extension to form single chain nanoparticles (SCNP). After addition of a spacer block and a further OH decorated block, folding was repeated to generate individual SCNP within a polymer chain. Control experiments were performed indicating the absence of inter block cross linking. SCNP were found to be condensed by a combination of covalent and supra molecular (hydrogen bonds) linkage. The approach was used to create a highly complex penta-block copolymer having three individually folded subdomains with an overall dispersity of 1.21. The successful formation of SCNP was confirmed by size exclusion chromatography (SEC), nuclear magnetic resonance (NMR), differential scanning calorimetry (DSC) and atomic force microscopy (AFM).

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“…A growing interest is being devoted in recent years to the synthesis of polymeric singlechain nanoparticles (SCNPs) [1,2,3,4,5,6] with potential applications in, e.g., nanomedicine [7,8], bioimaging [9,10], biosensing [11], catalysis [12,13,14,15], or rheology [16,17,18]. SCNPs are obtained, generally at highly diluted conditions, through purely intramolecular cross-linking of single polymer precursors.…”

Section: Introductionmentioning

confidence: 99%

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

Moreno

Bačová

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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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A brief user's guide to single-chain nanoparticles

Cited by 272 publications

References 90 publications

Synthesis and functionalization of dextran-based single-chain nanoparticles in aqueous media

Synthesis and functionalization of dextran-based single-chain nanoparticles in aqueous media

Synthesis of Sequence-Controlled Multiblock Single Chain Nanoparticles by a Stepwise Folding–Chain Extension–Folding Process

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

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