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Studying the noncovalent interactions between proteins and polysaccharides is quite important mainly due to the wide number of applications such as developing pH-responsive complexes. Scallop Patinopecten yessoensis male gonad hydrolysates‑sodium alginate (SMGHs-SA) was investigated as noncovalent complexes at pH from 1 to 10. The critical pH values pH C (around 6) and pHφ (around 4) were independent of the SMGHs-SA ratio, indicating the formation of soluble and insoluble complexes. The pH response of SMGHs-SA complexes was evaluated by investigating the rheological behavior, moisture distribution, functional group change and microstructure. Compared to the co-soluble and soluble complexes phases, the SMGHs-SA complexes had a higher storage modulus and viscosity as well as a lower relaxation time (T 23) in the insoluble complexes phase (pHφ>3). Additionally, the amide I band and COO− stretching vibration peaks were redshifted and the amide A band vibration peaks were blueshifted by acidification. Electrostatic interactions and intermolecular/intramolecular hydrogen bonding led to SMGHs-SA agglomeration at pH 3, forming a uniform and dense gel network structure with strong gel strength and water-retention capacity. This study provides a theoretical and methodological basis for the design of novel pH-responsive complexes by studying SMGHs-SA complex coacervation. • Scallop gonad hydrolysates (SMGHs) and sodium alginate (SA) could coacervate. • Acidification promoted the formation of SMGHs-SA coacervations. • Electrostatic interactions were the main force for the SMGHs-SA complex at pH 3. • Hydrogen bonding also drove the interaction of SMGHs and SA. [ABSTRACT FROM AUTHOR]

Studying the noncovalent interactions between proteins and polysaccharides is quite important mainly due to the wide number of applications such as developing pH-responsive complexes. Scallop Patinopecten yessoensis male gonad hydrolysates‑sodium alginate (SMGHs-SA) was investigated as noncovalent complexes at pH from 1 to 10. The critical pH values pH C (around 6) and pHφ (around 4) were independent of the SMGHs-SA ratio, indicating the formation of soluble and insoluble complexes. The pH response of SMGHs-SA complexes was evaluated by investigating the rheological behavior, moisture distribution, functional group change and microstructure. Compared to the co-soluble and soluble complexes phases, the SMGHs-SA complexes had a higher storage modulus and viscosity as well as a lower relaxation time (T 23) in the insoluble complexes phase (pHφ>3). Additionally, the amide I band and COO− stretching vibration peaks were redshifted and the amide A band vibration peaks were blueshifted by acidification. Electrostatic interactions and intermolecular/intramolecular hydrogen bonding led to SMGHs-SA agglomeration at pH 3, forming a uniform and dense gel network structure with strong gel strength and water-retention capacity. This study provides a theoretical and methodological basis for the design of novel pH-responsive complexes by studying SMGHs-SA complex coacervation. • Scallop gonad hydrolysates (SMGHs) and sodium alginate (SA) could coacervate. • Acidification promoted the formation of SMGHs-SA coacervations. • Electrostatic interactions were the main force for the SMGHs-SA complex at pH 3. • Hydrogen bonding also drove the interaction of SMGHs and SA. [ABSTRACT FROM AUTHOR]

The purpose of this study was to characterize the electrostatic complexation between scallop Patinopecten yessoensis male gonad hydrolysates (SMGHs) and κ -carrageenan/xanthan gum (KC/XG) within pH 12–1 at different hydrolysate/polysaccharide ratios (9:1–1:9) and to investigate the influence of pH and ratios on gelation and microstructural properties for widening the application of marine-derived source. According to the phase diagram of SMGHs/KC/XG, pH c hold a constant value around pH 8.5, pH φ1 gradually shifted from 4.2 to 2.8, and pH max fluctuated within 2.4-1.4 as ratios decreasing from 9:1–2:8. Additionally, SMGHs/KC/XG showed higher gel strength in acid condition, as decreasing pH promoted the electrostatic attractive interactions within positively charged patches in SMGHs and negatively charged sulfate and carboxyl groups in KC/XG causing more tightly packed structures formation. Moreover, decreasing ratios from 9:1 to 3:7 could further enhance the gel strength of SMGHs/KC/XG, ascribing to the stronger gelation ability of polysaccharides and enough neutralization. Moreover, SMGHs/KC/XG exhibited well-organized microstructures with smaller pore sizes, denser and more homogeneous networks at more acid domains, supporting stronger gel strength. Therefore, this study provides theoretical and methodological basis for designing novel SMGHs/KC/XG hydrogels with considerable gel strength and microstructures through understanding the complex coacervation at different pH and ratios. • pH and ratio largely regulate turbidity changes of SMGHs/KC/XG complexes. • pH c exhibits ratio-independent, and pH φ1 , pH max exhibit ratio-dependent behaviors. • Higher KC/XG proportion supports stronger gel strength in soluble phases. • More SMGHs/KC/XG neutralization promotes gel formation in insoluble coacervate phase. • SMGHs/KC/XG exhibits well-organized and compact networks at acid condition. [ABSTRACT FROM AUTHOR]

• pH and ratio largely governed turbidity changes of SMGHs/ κ -C complexes. • pH c exhibited ratio-independent, and pH φ1 , pH max exhibited ratio-dependent behaviors. • SMGHs aggregates and agglomerated SMGHs/ κ -C support the gel strength at acid pH. • SMGHs/ κ -C at acid pH had greater interaction with water to support the gel formation. • SMGHs/ κ -C formed a denser network at acid pH with stronger gel strength. The electrostatic complex coacervation between scallop Patinopecten. yessoensis male gonad hydrolysates (SMGHs) and κ -carrageenan (κ -C) were monitored by using turbidimetry at various pH (1–12) and biopolymer mixing ratio (9:1–1:9). The pH c exhibited ratio-independent behavior, and pH φ1 , pH max exhibited ratio-dependent behavior, respectively. The decreasing ratio enhanced the gel strength of SMGHs/ κ -C at higher pH while inversely at lower pH, ascribing to more SMGHs aggregates and stronger neutralization between positively charged patches in SMGHs and κ -C at lower pH and higher ratio. Moreover, SMGHs/ κ -C gel at acid condition exhibited lower relaxation times (T 21 and T 23). Furthermore, the rheological and relaxation time T 2 data were well associated with microscopy images which indicated that SMGHs/ κ -C gel showed a well-distributed network structure at more acidic domains, supporting stronger gel rigidity and water-holding capacity. [ABSTRACT FROM AUTHOR]

• Complex coacervation of SMGHs/ κ -C is largely governed by NaCl/KCl. • pH c and pH φ1 exhibited salt-dependent behaviors. • Optical density of SMGHs/ κ -C was regulated by salt-enhanced and -reduced effect. • Salt addition enhanced SMGHs/ κ -C gels mainly driven by electrostatic forces. • SMGHs/ κ -C showed more flocculation, larger pore and thicker network wall with salt. The complex coacervation between scallop Patinopecten yessoensis male gonad hydrolysates (SMGHs) and κ -carrageenan (κ -C) as influenced by ionic strength (NaCl and KCl) were monitored by using turbidimetric analysis at pH 1–12. The optical density of SMGHs/ κ -C complexes initially increased at lower ionic strength (0–0.5 M) whereas decreased at higher ionic strength (0.5–1.5 M) as a result of the salt-enhanced and salt-reduced effect, respectively. Both of pH c and pH φ1 exhibited ionic strength-dependent behavior that firstly shifted to acidic pH followed by an increase as salt increasing. Moreover, salt addition strongly promoted the gelation of SMGHs/ κ -C which was mainly driven by electrostatic forces, as reflected by increasing storage modulus G' from 3621 to 6559 Pa, 2681–25631 Pa at 0.1 Hz and decreasing T 23 relaxation time from 349.10 to 296.89 ms, 241.07–186.89 ms by 0–0.5 M NaCl/KCl, respectively. Furthermore, the rheological and relaxation time T 2 data were well associated with microscopy images that SMGHs/ κ -C gels with NaCl/KCl showed a denser network with more flocculation formation and larger pore sizes with thicker network wall, especially in KCl group, which indeed supported the gel elasticity. Taken together, this study could provide theoretical and methodological basis for new functional hydrogel products with modified gel strength and microstructure by understanding the complex coacervation in gel system. [ABSTRACT FROM AUTHOR]

Electrostatic complex coacervation between chia seed gum (CSG) and whey protein isolate (WPI) under different pH values (8-1), WPI/CSG mass ratios (16:1-1:1, w/w), and NaCl concentrations (0–400 mM) was investigated. Stronger complexation occurred at relatively high mass ratios (16:1, 8:1, and 4:1) and pH below the isoelectric point of WPI. Moreover, the complexation of WPI and CSG was weakened after adding NaCl and completely suppressed at 400 mM NaCl. Complexation with CSG decreased the α-helix and β-turn contents, increased the β-sheet content, and reduced the fluorescence intensity and surface hydrophobicity of WPI. The results of phase behavior and structural alteration suggested that the strongest electrostatic interaction occurred at pH 4, mass ratio 4:1, and 0 mM NaCl. The thermal stability of WPI/CSG complex coacervates was improved in comparison with that of WPI. Furthermore, rheological data and microscopy images indicated that stronger interactions between WPI and CSG resulted in greater viscosity and viscoelastic modulus, as well as denser structures. This study offers a theoretical reference for developing innovative and functional food products via understanding the interactions between WPI and CSG under different conditions. [Display omitted] • The complex coacervation between WPI and CSG occurred by electrostatic interaction. • The complexation was controlled by pH, WPI/CSG mass ratio, and NaCl concentration. • The addition of NaCl weakened the intensity of electrostatic complexation. • Hydrogen bonds and hydrophobic interactions also participated in the complexation. • A stronger complexation led to higher viscoelastic properties and denser network. [ABSTRACT FROM AUTHOR]