On Complex Coacervate Core Micelles: Structure-Function Perspectives

Magana, José Rodrigo; Sproncken, Christian C. M.; Voets, Ilja K.

doi:10.3390/polym12091953

Cited by 50 publications

(83 citation statements)

References 214 publications

(260 reference statements)

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“…Advantageously, chemical modifications in the protective shell afford additional functionalities to the enzyme, such as targeted delivery and responsiveness to external stimuli. 7 The preparation of conventional protein capsules is commonly performed by statistically trapping enzymes into polymeric nanoparticles, vesicles, or inorganic surfaces. 8 Despite the advantages provided by these (in)organic armors, they only allow for the diffusion of relatively small substrates, which may drastically reduce enzymatic performance toward large substrates.…”

Section: Introductionmentioning

confidence: 99%

Single Enzyme Nanoparticles with Improved Biocatalytic Activity through Protein Entrapment in a Surfactant Shell

et al. 2021

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A polymeric corona consisting of an alkyl-glycolic acid ethoxylate (C X EO Y ) surfactant offers a promising approach toward endowing proteins with thermotropic phase behavior and hyperthermal activity. Typically, preparation of protein–surfactant biohybrids is performed via chemical modification of acidic residues followed by electrostatic conjugation of an anionic surfactant to encapsulate single proteins. While this procedure has been applied to a broad range of proteins, modification of acidic residues may be detrimental to function for specific enzymes. Herein, we report on the one-pot preparation of biohybrids via covalent conjugation of surfactants to accessible lysine residues. We entrap the model enzyme hen egg-white lysozyme (HEWL) in a shell of carboxyl-functionalized C 12 EO 10 or C 12 EO 22 surfactants. With fewer surfactants, our covalent biohybrids display similar thermotropic phase behavior to their electrostatically conjugated analogues. Through a combination of small-angle X-ray scattering and circular dichroism spectroscopy, we find that both classes of biohybrids consist of a folded single-protein core decorated by surfactants. Whilst traditional biohybrids retain densely packed surfactant coronas, our biohybrids display a less dense and heterogeneously distributed surfactant coverage located opposite to the catalytic cleft of HEWL. In solution, this surfactant coating permits 7- or 3.5-fold improvements in activity retention for biohybrids containing C 12 EO 10 or C 12 EO 22 , respectively. The reported alternative pathway for biohybrid preparation offers a new horizon to expand upon the library of proteins for which functional biohybrid materials can be prepared. We also expect that an improved understanding of the distribution of tethered surfactants in the corona will be crucial for future structure–function investigations.

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Section: Introductionmentioning

confidence: 99%

Single Enzyme Nanoparticles with Improved Biocatalytic Activity through Protein Entrapment in a Surfactant Shell

et al. 2021

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“…Power laws for each polymer length were averaged to determine the scaling laws of R h ∝ N A 0.26±0. 16 , N B 0.49±0. 18 , N C 0.03±0.08 .…”

Section: Resultsmentioning

confidence: 98%

“…7 They are used at multiple scales for purposes including underwater adhesives, [8][9][10] early Earth protocell models, [11][12][13] structured gels and networks, 14,15 and nanomedicine. 16 Block copolyelectrolytes (neutral-charged block copolymers) can phase separate at the nanoscale to form polyelectrolyte complex micelles (PCMs). Due to their hydrophilic and charged nature, PCMs offer delivery capabilities that differ from hydrophobically driven assemblies, as they can sequester different molecules and travel more freely throughout the body.…”

Section: Introductionmentioning

confidence: 99%

Physical Property Scaling Relationships for Polyelectrolyte Complex Micelles

Marras

Campagna

Vieregg

et al. 2021

Preprint

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<p>Polyelectrolyte complex micelles (PCMs) are widely used in the delivery of hydrophilic payloads. Their attractive features include an ability to tune physical attributes, which are strongly dependent on the size and chemical structure of each polymer block. Neutral blocks drive nanoscale phase separation while charged blocks control micelle core size and stability. An understanding of physical property behavior controlled by block size is crucial when designing for use in dynamic or biological environments and provides a greater understanding of the physics of polyelectrolyte assembly. In this work, we use small angle x-ray scattering, and light scattering to determine precise scaling behaviors of physical micelle parameters for commonly used polyelectrolytes. We then compare our results to accumulated published data and theory to show strong agreement, suggesting these laws are universal for PCMs.</p>

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“…With the progress of polymer technology, self-assembled supramolecular structures of precisely designed polymers have been receiving much attention for fundamental studies [1,2] and the development of functional biomaterials [3,4]. Among supramolecular assemblies, polyion complexes (PICs), which are formed by electrostatic interaction between oppositely charged polymers in aqueous conditions without using organic solvents, have shown exceptional features for constructing biomaterials with controlled behavior at the biointerface and wide-range applicability, such as drug delivery systems (DDS) [5,6], bioimaging [7] and artificial organelles [8].…”

Section: Introductionmentioning

confidence: 99%

Effect of Mixing Ratio of Oppositely Charged Block Copolymers on Polyion Complex Micelles for In Vivo Application

et al. 2020

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Self-assembled supramolecular structures based on polyion complex (PIC) formation between oppositely charged polymers are attracting much attention for developing drug delivery systems able to endure harsh in vivo environments. As controlling polymer complexation provides an opportunity for engineering the assemblies, an improved understanding of the PIC formation will allow constructing assemblies with enhanced structural and functional capabilities. Here, we focused on the influence of the mixing charge ratio between block aniomers and catiomers on the physicochemical characteristics and in vivo biological performance of the resulting PIC micelles (PIC/m). Our results showed that by changing the mixing charge ratio, the structural state of the core was altered despite the sizes of PIC/m remaining almost the same. These structural variations greatly affected the stability of the PIC/m in the bloodstream after intravenous injection and determined their biodistribution.

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On Complex Coacervate Core Micelles: Structure-Function Perspectives

Cited by 50 publications

References 214 publications

Single Enzyme Nanoparticles with Improved Biocatalytic Activity through Protein Entrapment in a Surfactant Shell

Single Enzyme Nanoparticles with Improved Biocatalytic Activity through Protein Entrapment in a Surfactant Shell

Physical Property Scaling Relationships for Polyelectrolyte Complex Micelles

Effect of Mixing Ratio of Oppositely Charged Block Copolymers on Polyion Complex Micelles for In Vivo Application

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