The evolution of bicontinuous polymeric nanospheres in aqueous solution

McKenzie, Beulah E.; Visser, Joël F. de; Portale, Giuseppe; Hermida‐Merino, Daniel; Friedrich, Heiner; Bomans, Paul H. H.; Bras, Wim; Monaghan, Olivia R.; Holder, Simon J.; Sommerdijk, Nico A. J. M.

doi:10.1039/c6sm00053c

Cited by 21 publications

(27 citation statements)

References 52 publications

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“…The vesicle wall thickness is about 23 nm according to the Bragg equation of d = 2π q −1 determined by the small-angle X-ray scattering (SAXS) experiment ( Fig. 2h) 33,34 , which agrees well with the SEM results. The self-assembly of THPG 11 also generated spherical vesicles according to the TEM image ( Supplementary Fig.…”

Section: Preparation and Characterization Of Thpg Polymer Vesiclessupporting

confidence: 81%

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In situ supramolecular polymerization-enhanced self-assembly of polymer vesicles for highly efficient photothermal therapy

et al. 2020

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Vesicular photothermal therapy agents (PTAs) are highly desirable in photothermal therapy (PTT) for their excellent light-harvesting ability and versatile hollow compartments. However, up to now, the reported vesicular PTAs are generally self-assembled from small molecules like liposomes, and polymer vesicles have seldom been used as PTAs due to the unsatisfactory photothermal conversion efficiency resulting from the irregular packing of chromophores in the vesicle membranes. Here we report a nano-sized polymer vesicle from hyperbranched polyporphyrins with favorable photothermal stability and extraordinarily high photothermal efficiency (44.1%), showing great potential in imaging-guided PTT for tumors through in vitro and in vivo experiments. These excellent properties are attributed to the in situ supramolecular polymerization of porphyrin units inside the vesicle membrane into well-organized 1D monofilaments driven by π-π stacking. We believe the supramolecular polymerization-enhanced self-assembly process reported here will shed a new light on the design of supramolecular materials with new structures and functions.

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Section: Preparation and Characterization Of Thpg Polymer Vesiclessupporting

confidence: 81%

“…The photothermal conversion efficiency (η), was calculated using the following Eq. (1) 16,[33][34][35] .…”

Section: Methodsmentioning

confidence: 99%

In situ supramolecular polymerization-enhanced self-assembly of polymer vesicles for highly efficient photothermal therapy

et al. 2020

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“…Copyright Wiley-VCH. Panels (b–d) and (e–j) reproduced, respectively, from the Supporting Information and main text of ref (23) with permission from the Royal Society of Chemistry.…”

Section: Complex Macromolecular Assemblies In Solutionmentioning

confidence: 99%

CryoTEM as an Advanced Analytical Tool for Materials Chemists

Patterson

Moradi

et al. 2017

Acc. Chem. Res.

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ConspectusMorphology plays an essential role in chemistry through the segregation of atoms and/or molecules into different phases, delineated by interfaces. This is a general process in materials synthesis and exploited in many fields including colloid chemistry, heterogeneous catalysis, and functional molecular systems. To rationally design complex materials, we must understand and control morphology evolution. Toward this goal, we utilize cryogenic transmission electron microscopy (cryoTEM), which can track the structural evolution of materials in solution with nanometer spatial resolution and a temporal resolution of <1 s.In this Account, we review examples of our own research where direct observations by cryoTEM have been essential to understanding morphology evolution in macromolecular self-assembly, inorganic nucleation and growth, and the cooperative evolution of hybrid materials. These three different research areas are at the heart of our approach to materials chemistry where we take inspiration from the myriad examples of complex materials in Nature. Biological materials are formed using a limited number of chemical components and under ambient conditions, and their formation pathways were refined during biological evolution by enormous trial and error approaches to self-organization and biomineralization. By combining the information on what is possible in nature and by focusing on a limited number of chemical components, we aim to provide an essential insight into the role of structure evolution in materials synthesis. Bone, for example, is a hierarchical and hybrid material which is lightweight, yet strong and hard. It is formed by the hierarchical self-assembly of collagen into a macromolecular template with nano- and microscale structure. This template then directs the nucleation and growth of oriented, nanoscale calcium phosphate crystals to form the composite material. Fundamental insight into controlling these structuring processes will eventually allow us to design such complex materials with predetermined and potentially unique properties.

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“…Bicontinuous nanospheres (BCNs) are one example of such a lyotropic soft nanoarchitecture and have attracted much attention for their large surface area, ability to solubilize payloads of diverse polarity and potential to function as slow release nanomatrices. 3,4 Cryogenic transmission electron microscopy (cryoTEM) and small-angle X-ray scattering (SAXS) have revealed diverse internal geometries for BCNs, 5,6 which present as continuous self-assembled bilayers perforated with separate non-intersecting water channels of varying degrees of organization 7 (Fig. 1).…”

Section: Introductionmentioning

confidence: 99%

Flash nanoprecipitation permits versatile assembly and loading of polymeric bicontinuous cubic nanospheres

2018

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Polymeric bicontinuous nanospheres (BCNs) that are analogous to lipid cubosomes possess high internal surface area and porosity that can accommodate the loading of a wide range of hydrophobic and hydrophilic molecules for diverse applications. Self-assembly of BCNs has been reported using complex amphiphilic polymeric structures, with co-solvent dispersion being the only documented method of formation. Here, we report a simple amphiphilic diblock copolymer, poly(ethylene glycol)-block-poly(propylene sulfide) (PEG-bl-PPS), to form BCNs using the rapid and scalable technique of flash nanoprecipitation (FNP). Dynamic light scattering (DLS) and cryogenic transmission electron microscopy (cryoTEM) verified low polydispersity and the formation of bicontinuous structures with internal aqueous channels, respectively. Small-angle X-ray scattering (SAXS) confirmed a primitive cubic (Im3m) internal organization for BCNs assembled by FNP. Both hydrophobic and hydrophilic molecules were effectively loaded into BCNs via FNP, and encapsulated payloads were found to release in controlled manner in aqueous solutions. Due to the oxidation-sensitivity of PPS, biologically relevant concentrations of reactive oxygen species could trigger payload release on demand. BCNs were found to be non-toxic and endocytosed by phagocytic cells. Furthermore, an in vitro functional assay showed BCNs co-loaded with antigen ovalbumin and adjuvant monophosphoryl lipid A (MPL) to promote peptide/MHCI surface presentation by dendritic cells, a critical step for vaccine formulations during immunization. In conclusion, FNP supports the facile and scalable assembly and loading of PEG-bl-PPS BCNs, making them an attractive nanoscale delivery vehicle for both hydrophilic and hydrophobic molecules.

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The evolution of bicontinuous polymeric nanospheres in aqueous solution

Cited by 21 publications

References 52 publications

In situ supramolecular polymerization-enhanced self-assembly of polymer vesicles for highly efficient photothermal therapy

In situ supramolecular polymerization-enhanced self-assembly of polymer vesicles for highly efficient photothermal therapy

CryoTEM as an Advanced Analytical Tool for Materials Chemists

Flash nanoprecipitation permits versatile assembly and loading of polymeric bicontinuous cubic nanospheres

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