Scaling properties of the shear modulus of polyelectrolyte complex coacervates: a time-pH superposition principle

Tekaat, M.; Bütergerds, Dörte; Schönhoff, Monika; Fery, Andreas; Cramer, Cornelia

doi:10.1039/c5cp02940f

Cited by 53 publications

(90 citation statements)

References 16 publications

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“…Data supportive of this hypothesis has been reported by various groups [61,79,103]. However, the opposite trend has also been reported.…”

Section: Frequency Sweepssupporting

confidence: 74%

“…In numerous examples, the elastic behavior dominates (i.e., the storage modulus (G') dominates) [8,61,137,138,171,175,[177][178][179][180], while in other coacervates the viscous or liquid-like behavior (i.e., the loss modulus (G") dominates) [95,103,171]. Meanwhile, there are other systems where a crossover is observed between the two regimes, with G" dominating at low frequencies, and G' dominating at higher frequencies [61,71,72,79,111,130,162,171].…”

Section: Frequency Sweepsmentioning

confidence: 99%

“…For instance, several reports have described a reduction in the rate of chain as a result of pH changes designed to decrease the charge density of one or more of the polyelectrolytes (Figure 7b) [75,103]. Tekaat et al, have speculated that this decrease in chain dynamics is due to an increase in hydrophobic interactions from the uncharged segments of the chain [103]. Additional studies are needed to further elucidate this subtle interplay of interactions.…”

Section: Frequency Sweepsmentioning

confidence: 99%

“…This difference in the dynamics of the various coacervate systems is intriguing and suggests that additional factors may be critical for understanding the dynamics of these systems. For instance, several reports have described a reduction in the rate of chain as a result of pH changes designed to decrease the charge density of one or more of the polyelectrolytes (Figure 7b) [75,103]. Tekaat et al, have speculated that this decrease in chain dynamics is due to an increase in hydrophobic interactions from the uncharged segments of the chain [103].…”

Section: Frequency Sweepsmentioning

confidence: 99%

“…This principle implied that the changes in polyelectrolyte charge density resulting from changing pH only influence the timescale of the relaxation dynamics, rather than altering the mechanism of their interaction. This work utilized complex coacervates composed of PAA, a weak polyanion, and PDADMAC, a strong polycation, in the presence of KCl [103]. Thus, at high pH both of the polymers will be fully charged, while the charge density of the polyanion will decrease at more acidic pH values.…”

Section: Time-ph Superpositionmentioning

confidence: 99%

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Linear viscoelasticity of complex coacervates

Liu

Winter

Perry

2017

Advances in Colloid and Interface Science

125

163

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Rheology is a powerful method for materials characterization that can provide detailed information about the self-assembly, structure, and intermolecular interactions present in a material. Here, we review the use of linear viscoelastic measurements for the rheological characterization of complex coacervate-based materials. Complex coacervation is an electrostatically and entropically-driven associative liquid-liquid phase separation phenomenon that can result in the formation of bulk liquid phases, or the self-assembly of hierarchical, microphase separated materials. We discuss the need to link thermodynamic studies of coacervation phase behavior with characterization of material dynamics, and provide parallel examples of how parameters such as charge stoichiometry, ionic strength, and polymer chain length impact self-assembly and material dynamics. We conclude by highlighting key areas of need in the field, and specifically call for the development of a mechanistic understanding of how molecular-level interactions in complex coacervate-based materials affect both selfassembly and material dynamics.

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“…Data supportive of this hypothesis has been reported by various groups [61,79,103]. However, the opposite trend has also been reported.…”

Section: Frequency Sweepssupporting

confidence: 74%

Section: Frequency Sweepsmentioning

confidence: 99%

Section: Frequency Sweepsmentioning

confidence: 99%

Section: Frequency Sweepsmentioning

confidence: 99%

Section: Time-ph Superpositionmentioning

confidence: 99%

See 3 more Smart Citations

Linear viscoelasticity of complex coacervates

Liu

Winter

Perry

2017

Advances in Colloid and Interface Science

125

163

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Bioinspired Processing: Complex Coacervates as Versatile Inks for 3D Bioprinting

et al. 2023

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3D bioprinting is a powerful fabrication technique in biomedical engineering, which is currently limited by the number of available materials that meet all physicochemical and cytocompatibility requirements for biomaterial inks. Inspired by the key role of coacervation in the extrusion and spinning of many natural materials, hyaluronic acid–chitosan complex coacervates are proposed here as tunable biomaterial inks. Complex coacervates are obtained through an associative liquid–liquid phase separation driven by electrostatic attraction between oppositely charged macromolecules. They offer bioactive properties and facile modulation of their mechanical properties through mild physicochemical changes in the environment, making them attractive for 3D bioprinting. Fine‐tuning the salt concentration, pH, and molecular weight of the constituent polymers results in biomaterial inks that are printable in air and water. The biomaterial ink, initially a viscoelastic fluid, transitions into a viscoelastic solid upon printing due to dehydration (for printing in air) or due to a change in pH and ionic composition (for printing in solution). Consequently, scaffolds printed using the complex coacervate inks are stable without the need for post‐printing processing. Fabricated cell culture scaffolds are cytocompatible and show long‐term topological stability. These results pave the way to a new class of easy‐to‐handle tunable biomaterials for biofabrication.

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New insights into protein–polysaccharide complex coacervation: Dynamics, molecular parameters, and applications

Zheng,

Van der Meeren,

Sun

2023

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For more than a decade, the discovery of liquid–liquid phase separation within living organisms has prompted colloid scientists to understand the connection between coacervate functionality, phase behavior, and dynamics at a multidisciplinary level. Although the protein–polysaccharide was the first system in which the coacervation phenomenon was discovered and is widely used in food systems, the phase state and relaxation dynamics of protein–polysaccharide complex coacervates (PPCC) have rarely been discussed previously. Consequently, this review aims to unravel the relationship between PPCC dynamics, thermodynamics, molecular architecture, applications, and phase states in past studies. Looking ahead, solving the way molecular architecture spreads to macro‐functionality, that is, establishing the relationship between molecular architecture–dynamics–application, will catalyze novel advancements in PPCC research within the field of foods and biomaterials.

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Scaling properties of the shear modulus of polyelectrolyte complex coacervates: a time-pH superposition principle

Cited by 53 publications

References 16 publications

Linear viscoelasticity of complex coacervates

Linear viscoelasticity of complex coacervates

Bioinspired Processing: Complex Coacervates as Versatile Inks for 3D Bioprinting

New insights into protein–polysaccharide complex coacervation: Dynamics, molecular parameters, and applications

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