Capillary Flow-MRI: Quantifying Micron-Scale Cooperativity in Complex Dispersions

• Published in: Analytical chemistry (Washington) Vol. 95; no. 41; pp. 15162 - 15170
• Main Authors: Milc, Klaudia W., Oerther, Thomas, Dijksman, Joshua A., van Duynhoven, John P. M., Terenzi, Camilla
• Format: Journal Article
• Language: English
• Published: Washington American Chemical Society 17-10-2023
• Subjects: Capillary flow; Capillary pressure; Confined flow; Confinement; Cooperativity; Cosmetics; Diameters; Dispersions; Fluid flow; High resolution; Hydrophobicity; Image resolution; Magnetic resonance imaging; Particle interactions; Spatial discrimination; Spatial resolution; Thin films; Three dimensional printing; Velocimetry
• ISSN: 0003-2700; 1520-6882
• DOI: 10.1021/acs.analchem.3c01108

Strongly confined flow of particulate fluids is encountered in applications ranging from three-dimensional (3D) printing to the spreading of foods and cosmetics into thin layers. When flowing in constrictions with gap sizes, w, within 102 times the mean size of particles or aggregates, d, structured fluids experience enhanced bulk velocities and inhomogeneous viscosities, as a result of so-called cooperative, or nonlocal, particle interactions. Correctly predicting cooperative flow for a wide range of complex fluids requires high-resolution flow imaging modalities applicable in situ to even optically opaque fluids. To this goal, we here developed a pressure-driven high-field magnetic resonance imaging (MRI) velocimetry platform, comprising a pressure controller connected to a capillary. Wall properties and diameter could be modified respectively as hydrophobic/hydrophilic, or within w ∼ 100–540 μm. By achieving a high spatial resolution of 9 μm, flow cooperativity length scales, ξ, down to 15 μm in Carbopol with d ∼ 2 μm could be quantified by means of established physical models with an accuracy of 13%. The same approach was adopted for a heterogeneous fat crystal dispersion (FCD) with d and ξ values up to an order of magnitude higher than those for Carbopol. We found that for strongly confined flow of Carbopol in the 100 μm capillary, ξ is independent of flow conditions. For the FCD, ξ increases with gap size and applied pressures over 0.25–1 bar. In both samples, nonlocal interactions span domains up to about 5–8 particles but, at the highest confinement degree explored, ∼8% for FCD, domains of only ∼2 particles contribute to cooperative flow. The developed flow-MRI platform is easily scalable to ultrahigh field MRI conditions for chemically resolved velocimetric measurements of, e.g., complex fluids with anisotropic particles undergoing alignment. Future potential applications of the platform encompass imaging extrusion under confinement during the 3D printing of complex dispersions or in in vitro vascular and perfusion studies.