Food Polymers, Gels and Colloids
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All rights reserved. View In: Mobile Desktop. Strand like elongated networks of P-gel formed fewer intersections in between two or more networks compared to N- and AB-gels; whereas AB-gels displayed maximum intersections due to its random structure. Finally, due this morphological organization the void areas in P-gels were highest compared to other ones.
Morphology of gelatin based colloidal gels. Lower panel images are enlarged version for better visualization. While SEM images provided information at scale length relevant to individual cell, we performed confocal imaging of the gels to capture the morphological features at a larger length scale hundreds of microns relevant to multicellular dimension. Confocal images with a zoomed view in lower panel images and their corresponding 3D surface interactive plot generated from z-stacks using ImageJ in Fig. N-gels were dense with less and constricted voids whereas P-gels were evolved with interconnected strands with more extended and connected voids, and AB-gels showed characteristics heterogeneous features where some regions are dense and some are dispersed.
This variation of morphology in these gels essentially creates a significantly different spatial microenvironment at multicellular dimension for cells to organize owing to the organization of the particles.
Food polymers, gels and colloids
These features are self-similar with increasing particle content because the network expands in 3D in a hierarchical manner, due to which the similar morphological features were observed at the same length scale, when the gels were formed at 0. To analyze the mechanical properties, we studied the rheological responses and correlated to the colloidal gel structure. Typical strain amplitude response of N-, P- and AB-gels formed with different particle fractions are shown in Fig.
Elastic moduli of the N- and P-gels at 0. Scaling of elastic moduli with particle fraction was most pronounced for N-gel because the networks evolved from the compact dense organization of particles, whereas for P-gel the networks grew as strands of interconnected particles.
This can also be explained in terms of longer characteristic length and fewer interconnections of networks in P-gels compared to that of N-gel. In contrast, AB-gel showed least dependence on particle fraction indicating heterogeneous anisotropic growth of networks. N- and P-gels evolved in homogeneous manner to maintain similar microstructure across several length scales, which can create a spatially uniform microenvironment for cells. In contrast, the heterogeneous microstructure of AB-gel, which is inherently devoid of self-similarity, showed less scaling of moduli with particle fraction.
All gels at all particle fractions showed a value lower than one indicating elastic moduli higher than viscous moduli. Compared to the reported gelatin based colloidal gel 22 , 60 , elastic moduli of the gels in this studies were lower because the particle fractions used here were based on swelled particle rather than the absolute dry weight basis.
Additionally, the viscoelastic moduli i. Results show Fig. S5 that the elasticity and viscoelastic responses of the colloidal gels were not altered under this condition.
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Mechanical characterizations of colloidal gel from rheology. Further insight into the mechanomorphology was assessed by analyzing the viscosity of the gels with respect to the shear rate Fig.
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All the gels showed a shear thinning response with increased shear rate, however the responses were dependent on the gel type. P-gels showed enhanced flow behavior because the strand-like networks can easily deform and the interstitial fluid can flow through the interconnected voids with increasing shear rate, compared to compact dense N- and AB-gel. Furthermore, as the particle fraction was increased for a given gel, flow behavior decreased because the extended networks can resist deformation.
Particularly, at low particle fractions, P-gels reached a Newtonian plateau as the shear rate increased, indicating that the smaller strands of P-gel were deformed to respond as fluid, whereas N- and AB-gels showed continued shear thinning. Thus, the shear rheological measurements of the three gels provided supportive evidence for the mechanomorphology of the gels. Finally, we measured the creep response at constant stress below the yield by measuring the deformation of the gels to analyze the time-dependent changes. Creep response of colloidal gels depends on the mechanics and the morphology 55 , 62 , 63 , 64 , because the network structures of colloidal gels develop from the aggregation of particles.
P-gels due to their strand-like elongated networks experienced significant deformation Fig.
7.10: Colloids and their Uses
As particle fraction increases, the creep responses are decreased because the larger networks prevented the deformation Moreover, creep of N-gels almost plateaued after the instantaneous strain whereas P-gel continued to deform with time. In comparison, AB-gel showed least deformation due to its heterogeneous microstructure which is relatively random and anisotropic in 3D.
Creep ringing phenomena arises due to inertial effect but is also reflective of gel mechanomorphology 65 , Ringing response is more pronounced in dense gels with closed structure and is also dependent on interfacial effect from the movement of interstitial fluid 67 , P-gel due to its open structure showed lesser oscillation compared to N- and AB-gel which are denser.
As, the particle fraction increased P-gels showed increased ringing as networks are evolved and due to the greater ability of interstitial fluid to flow through interconnected voids. Whereas, for N- and AB- gels, at 0. Time-dependent viscoelastic response from creep measurement. Overall, this data collectively shows that gelatin based colloidal gels can be engineered through electrostatic interaction mediated aggregation of particles.
Depending on the mode of aggregation and the particle fraction, these gel show a tunable combination of microstructural morphology and mechanical properties. Morphologically, N-gels are compact and dense while P-gels are branched strands network, and AB-gels show heterogeneous anisotropic character.
As these gels evolve with particle aggregation, these microstructures are self-similar and is independent of the particle fraction from which the gels are formed. But as the particle fraction increased, stiffness of the gels increases due to the growth of the network structure. Elastic moduli of N-gels showed increased scaling with particles due to its compact microstructure compared but P-gels showed relatively lesser enhancement of moduli; and AB-gel due to its heterogeneity showed least dependence of moduli on particle fraction.
Thus, gelatin based colloidal gels provide a uniquely complete system to tune the mechanomorphological properties in a controlled and independent manner. In all conditions, cells exhibited similar viability measured by quantifying DNA content, Fig.