Interfacial Tension of Complex Coacervated Mussel Adhesive Protein According to the Hofmeister Series

Abstract

Complex coacervation is a liquid-liquid phase separation in a colloidal system of two oppositely charged polyelectrolytes or colloids. The interfacial tension of the coacervate phase is the key parameter for micelle formation and interactions with the encapsulating material. However, the relationship between interfacial tensions and various salt solutions is poorly understood in complex coacervation. In the present work, the complex coacervate dynamics of recombinant mussel adhesive protein (MAP) with hyaluronic acid (HA) were determined in the presence of Hofmeister series salt ions. Using measurements of absorbance, hydrodynamic diameter, capillary force, and receding contact angle in the bulk phase, the interfacial tensions of complex coacervated MAP/HA were determined to be 0.236, 0.256, and 0.287 mN/m in 250 mM NaHCOO, NaCl, and NaNO3 solutions, respectively. The sequences of interfacial tensions and contact angles of the complex coacervates in the presence of three sodium salts with different anions were found to follow the Hofmeister ordering. The tendency of interfacial tension between the coacervate and dilute phases in the presence of different types of Hofmeister salt ions could provide a better understanding of Hofmeister effects on complex coacervated materials based on the protein-polysaccharide system. This information can also be utilized for microencapsulation and adsorption by controlling intramolecular interactions. In addition, the injection molding dynamics of mussel byssus formation was potentially explained based on the measured interfacial tension of coacervated MAP.

Mussel adhesion-employed water-immiscible fluid bioadhesive for urinary fistula sealing

“…Along with the superior underwater adhesion ability, the high stability and durability of WIMBA satisfied the requirements for fistula repair. Moreover, WIMBA possesses additional useful properties, such as extremely low interfacial tension [32] and microencapsulation/complexation capability [25,44]. Therefore, non-invasive laparoscopic and robotic surgical techniques or drug delivery might also be possible.…”

“…The immiscibility in water can prevent the coacervated WIMBA from being washed out by body fluids and can provide strong bulk adhesion in underwater environments. Additionally, the extremely low interfacial tension and the shear-thinning flow characteristics of coacervates [31,32] can make them suitable for injection during laparoscopic or endoscopic surgery. These intriguing properties of WIMBA have important implications for its potential use in internal body applications.…”

The Effect of Salt on the Complex Coacervation of Vinyl Polyelectrolytes

“…Consideration of these variables is critical in the design of self-assembled materials. For instance, electrostatic complexation between oppositely-charged polyelectrolytes has been used in drug and gene delivery [7,[14][15][16][17][18], thin film coatings [19][20][21], processed food [22], and underwater adhesives [23][24][25][26]. Clearly, the functionality of the material must be considered in the context of the operational environment.…”

Linear viscoelasticity of complex coacervates

“…The self-assembly of these materials is driven by entropy, where the initial electrostatic attraction between oppositely-charged macro-ions results in the release of small, bound counter-ions and the restructuring of water molecules [1][2][3][4]. Complex coacervates have a long history of use in the food [5][6][7][8][9][10][11][12][13] and personal care [14,15] industries, and have found increasing utility as a platform for drug and gene delivery [1][2][3][4], as well as underwater adhesives [5][6][7][8][9][10][11][12][13][48][49][50][51][52][53][54][55][56][57][58][59][60][61][62]. Coacervation has also recently been implicated in the formation of various biological assemblies [1,[14][15][16]55,…”