Controlled node growth on the surface of polymersomes

Thomas, Marjolaine; Varlas, Spyridon; Wilks, Thomas R.; Fielden, Stephen D. P.; O'Reilly, Rachel K.

doi:10.1039/d3sc05915d

Cited by 4 publications

(3 citation statements)

References 72 publications

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“…Nucleobase interactions have also been shown to affect nanoparticle morphology via postassembly modifications. ,,− We have previously reported a morphological transformation process where a spherical micelle containing thymine within the core was elongated into anisotropic worms of a controlled length via the addition of a specified amount of linear polymers containing the complementary nucleobase . This approach can also be used to control the growth of nodes from polymersomes . Yan et al have also demonstrated a similar transformation, a postself-assembly morphological transformation driven by nucleobase interactions …”

Section: Introductionmentioning

confidence: 93%

“…12 This approach can also be used to control the growth of nodes from polymersomes. 22 Yan et al have also demonstrated a similar transformation, a postself-assembly morphological transformation driven by nucleobase interactions. 19 While most of the research exploiting nucleobase interactions in polymers primarily focuses on the adeninethymine pair, there is limited research using cytosine or guanine, even though it exhibits stronger binding due to the increased number of hydrogen bonding sites.…”

Section: ■ Introductionmentioning

confidence: 99%

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Harnessing Cytosine for Tunable Nanoparticle Self-Assembly Behavior Using Orthogonal Stimuli

Parkinson,

Fielden,

Thomas

et al. 2024

Biomacromolecules

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Nucleobases control the assembly of DNA, RNA, etc. due to hydrogen bond complementarity. By combining these unique molecules with state-of-the-art synthetic polymers, it is possible to form nanoparticles whose self-assembly behavior could be altered under orthogonal stimuli (pH and temperature). Herein, we report the synthesis of cytosinecontaining nanoparticles via aqueous reversible addition-fragmentation chain transfer polymerization-induced self-assembly. A poly(N-acryloylmorpholine) macromolecular chain transfer agent (mCTA) was chain-extended with cytosine acrylamide, and a morphological phase diagram was constructed. By exploiting the ability of cytosine to form dimers via hydrogen bonding, the self-assembly behavior of cytosine-containing polymers was altered when performed under acidic conditions. Under these conditions, stable nanoparticles could be formed at longer polymer chain lengths. Furthermore, the resulting nanoparticles displayed different morphologies compared to those at pH 7. Additionally, particle stability post-assembly could be controlled by varying pH and temperature. Finally, small-angle X-ray scattering was performed to probe their dynamic behavior under thermal cycling.

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Section: Introductionmentioning

confidence: 93%

Section: ■ Introductionmentioning

confidence: 99%

Harnessing Cytosine for Tunable Nanoparticle Self-Assembly Behavior Using Orthogonal Stimuli

Parkinson,

Fielden,

Thomas

et al. 2024

Biomacromolecules

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“…Only spherical micelles formed if the polymer chains are instead premixed and assembly induced by a solvent switch. This approach has recently been extended to grow nodes of controlled length on the surface of polymersomes . Combining polymers with different chemical composition is likely to prove a powerful way to fine-tune assembly shape and properties …”

Section: Kinetically Controlled Assembly Of Preformed Block Copolymersmentioning

confidence: 99%

Kinetically Controlled and Nonequilibrium Assembly of Block Copolymers in Solution

Fielden

2024

J. Am. Chem. Soc.

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Covalent polymers are versatile macromolecules that have found widespread use in society. Contemporary methods of polymerization have made it possible to construct sequence polymers, including block copolymers, with high precision. Such copolymers assemble in solution when the blocks have differing solubilities. This produces nano-and microparticles of various shapes and sizes. While it is straightforward to draw an analogy between such amphiphilic block copolymers and phospholipids, these two classes of molecules show quite different assembly characteristics. In particular, block copolymers often assemble under kinetic control, thus producing nonequilibrium structures. This leads to a rich variety of behaviors being observed in block copolymer assembly, such as pathway dependence (e.g., thermal history), nonergodicity and responsiveness. The dynamics of polymer assemblies can be readily controlled using changes in environmental conditions and/or integrating functional groups situated on polymers with external chemical reactions. This perspective highlights that kinetic control is both pervasive and a useful attribute in the mechanics of block copolymer assembly. Recent examples are highlighted in order to show that toggling between static and dynamic behavior can be used to generate, manipulate and dismantle nonequilibrium states. New methods to control the kinetics of block copolymer assembly will provide endless unanticipated applications in materials science, biomimicry and medicine.

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Switchable pH-Responsive Morphologies of Coassembled Nucleobase Copolymers

Arsenie,

Semsarilar,

Benkhaled

et al. 2024

Biomacromolecules

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This work presents supramolecular coassembled nucleobase copolymers with transitional morphologies upon pH changes (from 7.4 to 10). Uracil-and adenine-containing copolymers were prepared by RAFT, which allowed us to finely tailor the polymerization degree and the composition. The coassembled formulations prepared in an aqueous buffer at two distinct pH (7.4 and 10) formed spherical morphologies at physiological pH. The increase of the pH induced the apparition of various large, irreversible anisotropic supramolecular architectures. Isothermal titration calorimetry revealed that the coassembly at pH 7.4 was mainly guided by H-bonds between complementary nucleobases, while the experiments conducted at pH 10 showed that the assemblies were mainly driven by hydrophobic interactions. These results highlight that the nature of supramolecular interactions (H-bonds or hydrophobic interactions) has a great influence on the morphology of nucleobase-containing coassemblies when changing the pH. These findings may provide further perspectives in the field of advanced nanomaterials.

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Controlled node growth on the surface of polymersomes

Abstract: Incorporating nucleobases into synthetic polymers has proven to be a versatile method for controlling self-assembly. The formation of strong directional hydrogen bonds between complementary nucleobases provides a driving force that...

Cited by 4 publications

References 72 publications

Harnessing Cytosine for Tunable Nanoparticle Self-Assembly Behavior Using Orthogonal Stimuli

Harnessing Cytosine for Tunable Nanoparticle Self-Assembly Behavior Using Orthogonal Stimuli

Kinetically Controlled and Nonequilibrium Assembly of Block Copolymers in Solution

Switchable pH-Responsive Morphologies of Coassembled Nucleobase Copolymers

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