Frictional behaviour of molten chocolate as a function of fat content.

Soft tribology is used to probe the lubrication behaviour of molten chocolate between soft contacts, analogous to in-mouth interactions between the tongue and palate. Molten chocolate is a concentrated suspension of solid particles (sugar, cocoa and milk solids) in cocoa butter. We hypothesise that the complex frictional behaviour of molten chocolate depends on its particulate nature and thus solid volume fraction (sugar & cocoa solids/fat content). In this work, we assess the properties of molten chocolate as a function of fat content by diluting milk chocolate containing 26, 27 and 29% fat with cocoa butter. The tribological behaviour of molten chocolate deviates notably from the typical Stribeck curve of Newtonian fluids. Additional transitions are observed in mixed and elastohydrodynamic lubrication which are respectively attributed to the effect of shear-thinning rheology (i.e. breakdown of aggregates) and the selective entrainment or exclusion of particles depending on interfacial gap height. These transitions are more pronounced in chocolate of high solid fraction, and correlate with the influence of particle aggregation on rheology. In addition, we assess oral lubrication by preparing model chocolate boluses with aqueous buffer, which produces a ternary system of oil droplets and insoluble cocoa solids dispersed within a continuous aqueous phase. The frictional behaviour of chocolate boluses is determined by the viscosity ratio between cocoa butter and aqueous phase, in agreement with previous findings for oil-in-water emulsions. We provide a conceptual model to interpret how fat content influences the oral lubrication and mouthfeel of chocolate during consumption.

Enabling the Rational Design of Low-Fat Snack Foods: Insights from In Vitro Oral Processing.

Texture perception is conceptualized as an emergent cognitive response to food characteristics that comprise several physical and chemical properties. Contemporary oral processing research focuses on revealing the relationship between the sensory perceptions and food properties, with the goal of enabling rational product design. One major challenge is associated with revealing the complex molecular and biocolloidal interactions underpinning even simple texture percepts. Here, we introduce in vitro oral processing, which considers oral processing in terms of discrete units of operation (first bite, comminution, granulation, bolus formation, and tribology). Within this framework, we systematically investigate the material properties that govern each specific oral processing unit operation without being impacted by the biological complexity of the oral environment. We describe how this framework was used to rationally design a low-fat potato chip with improved sensory properties by investigating the impact from adding back, to a low-fat potato chip, a small amount of oil mixed with the surface-active agent polyglycerol polyricinoleate (PGPR). The relevance of instrumental measures is validated by sensory assessment, whereby panelists ranked the perceived oiliness of three different types of potato chips. The sensory results indicate that perceived oiliness was higher when a low-fat potato chip was supplemented with an additional 0.5% (w/w) topical coating (the coating comprised 15%, w/w, PGPR in oil) compared to the unaltered low-fat potato chip. The perceived difference in oiliness is hypothesized to correspond to the dynamic friction measured in vitro with a saliva-coated substrate in the presence and absence of PGPR. The study illustrates how dividing oral processing into distinct units provides a rational approach to food product design focused on controlling key sensory attributes.

Ring Shear Tester as an in-vitro testing tool to study oral processing of comminuted potato chips.

Oral processing of solid foods is an extremely dynamic and complicated activity that involves multiple processes in tandem such as comminution, mixing, dilution, hydration and enzymatic breakdown that gradually transform the food from a morsel or a bite to a bolus that is ready for swallowing. It is hypothesised that just after "first bite" and initial particle reduction and hydration of solid brittle foods, the response to deformation of food particles is analogous to studies on the flowability and cohesion of wetted powders, which are effectively characterised using a Ring Shear Tester (RST). We examine this hypothesis and determine whether the RST measures properties of solid snack foods (potato chips or crisps, PCs) that are relevant to their dynamic sensory response, which includes capturing the effect of hydration on comminuted PCs. The RST is found to differentiate PCs obtained from different manufacturing sources (e.g. baked versus fried), and its measurements of cohesion and friction can be considered in context of the structure and composition of the PCs as well as oral processing. Remarkably, RST measurements for this small set of PC samples correlate with several sensory attributes that arise during mastication, which includes Sharpness and Ease of Clearance. This study highlights the potential of the RST as a new tool for oral processing research.

Cellulose-pectin composite hydrogels: Intermolecular interactions and material properties depend on order of assembly.

Plant cell walls have a unique combination of strength and flexibility however, further investigations are required to understand how those properties arise from the assembly of the relevant biopolymers. Recent studies indicate that Ca2+-pectates can act as load-bearing components in cell walls. To investigate this proposed role of pectins, bioinspired wall models were synthesised based on bacterial cellulose containing pectin-calcium gels by varying the order of assembly of cellulose/pectin networks, pectin degree of methylesterification and calcium concentration. Hydrogels in which pectin-calcium assembly occurred prior to cellulose synthesis showed evidence for direct cellulose/pectin interactions from small-angle scattering (SAXS and SANS), had the densest networks and the lowest normal stress. The strength of the pectin-calcium gel affected cellulose structure, crystallinity and material properties. The results highlight the importance of the order of assembly on the properties of cellulose composite networks and support the role of pectin in the mechanics of cell walls.

Pectin impacts cellulose fibre architecture and hydrogel mechanics in the absence of calcium.

Pectin is a major polysaccharide in many plant cell walls and recent advances indicate that its role in wall mechanics is more important than previously thought. In this work cellulose hydrogels were synthesised in pectin solutions, as a biomimetic tool to investigate the influence of pectin on cellulose assembly and hydrogel mechanical properties. Most of the pectin (60-80%) did not interact at the molecular level with cellulose, as judged by small angle scattering techniques (SAXS and SANS). Despite the lack of strong interactions with cellulose, this pectin fraction impacted the mechanical properties of the hydrogels through poroelastic effects. The other 20-40% of pectin (containing neutral sugar sidechains) was able to interact intimately with cellulose microfibrils at the point of assembly. These results support the need to revise the role of pectin in cell wall architecture and mechanics, and; furthermore they assist the design of cellulose-based products through controlling the viscoelasticity of the fluid phase.

Influence of hydration and starch digestion on the transient rheology of an aqueous suspension of comminuted potato snack food.

Oral processing of most foods is inherently destructive: solids are broken into particles before reassembly into a hydrated bolus while salivary enzymes degrade food components. In order to investigate the underlying physics driving changes during oral processing, we capture the transient rheological behaviour of a simulated potato chip bolus during hydration by a buffer with or without α-amylase. In the absence of amylase and for all oil contents and solids weight fractions tested, we find a collapse of the transient data when graphed according to simple Fickian diffusion. In the presence of amylase, we find effects on the transient and pseudo steady state bolus rheology. Within the first minute of mixing, the amylase degrades only ≈6% of the starch but that leads to an order of magnitude reduction in the bolus elasticity, as compared to the case without amylase. Thus, for an in vitro bolus, only a small amount of starch needs to be digested to have a large impact on the bolus rheology very soon after mixing.

Particle interactions in kaolinite suspensions and corresponding aggregate structures.

The surface charge densities of the silica face surface and the alumina face surface of kaolinite particles, recently determined from surface force measurements using atomic force microscopy, show a distinct dependence on the pH of the system. The silica face was found to be negatively charged at pH>4, whereas the alumina face surface was found to be positively charged at pH<6, and negatively charged at pH>8. The surface charge densities of the silica face and the alumina face were utilized in this study to determine the interaction energies between different surfaces of kaolinite particles. Results indicate that the silica face-alumina face interaction is dominant for kaolinite particle aggregation at low pH. This face-face association increases the stacking of kaolinite layers, and thereby promotes the edge-face (edge-silica face and edge-alumina face) and face-face (silica face-alumina face) associations with increasing pH, and hence the maximum shear-yield stress at pH 5-5.5. With further increase in pH, the face-face and edge-face association decreases due to increasing surface charge density on the silica face and the edge surfaces, and decreasing surface charge density on the alumina face. At high pH, all kaolinite surfaces become negatively charged, kaolinite particles are dispersed, and the suspension is stabilized. The face-face association at low pH has been confirmed from cryo-SEM images of kaolinite aggregates taken from suspension which show that the particles are mostly organized in a face-face and edge-face manner. At higher pH conditions, the cryo-SEM images of the kaolinite aggregates reveal a lower degree of consolidation and the edge-edge association is evident.