Drecun, Olivera; (2023) Towards a mesoscale rheology model for aqueous particulate suspensions. Doctoral thesis (Ph.D), UCL (University College London).

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Abstract

Particulate suspensions are ubiquitous and diverse; pharmaceutical formulations, biological fluids, magma and foodstuffs are just few of numerous examples. In many cases, the flow behaviour (rheology) of the suspension is critical to its function. A key rheological property is viscosity; a measure of a substance’s resistance to flow. This work aims to understand molecular-level mechanisms responsible for determining flow behaviour in moderately dense suspensions; 35% particles by volume (i.e., volume fraction 0.35). The industrial application of interest to this thesis is catalysis; namely, the ‘washcoat’, a key component in the performance of catalytic converters. A typical washcoat formulation is an aqueous suspension, comprising a high surface-area support powder, an active catalyst material, together with organic additives and certain salts used to optimise properties of the washcoat; including its flow behaviour. Of these components, this work investigates ‘salt-specific effects’; i.e. the influence of differing salt-types. Investigation is conducted at molecular and macroscopic resolution via simulations and experiments, respectively. The research approach probes the constituents of a suspension: the aqueous phase, the particle-aqueous phase interface, and particle interactions. Molecular dynamics simulations are employed as the foundation of this analysis, with experiments - rheology, nuclear magnetic resonance and dynamic light scattering - utilised alongside. A final set of rheology experiments is conducted on particulate suspensions of 35% volume fraction, in pure water and the aqueous salt solutions of interest. At all stages of analysis, results suggest that macroscopic behaviours are a cumulative manifestation of phenomena at molecular resolution. However, such phenomena are varied; the challenge lies in identifying which mechanisms are relevant to the behaviour of interest, how they work together, and how they manifest cumulatively. Towards a mesoscale rheology model for aqueous particulate suspensions, results are discussed in terms of input for such a model, which would predict rheology as a function of particle loading, ionic strength and possibly other factors, in future work.

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