Hydrodynamic crossover in dynamic microparticle adhesion on surfaces of controlled nanoscale heterogeneity

This note documents the crossover from a regime where shear flow hinders microparticle adhesion on collecting surfaces to that where increased flow aids particle capture. Flow generally works against adhesion and successfully hinders particle capture when the net physicochemical attractions between the particles and collector are weak compared with hydrodynamic forces on the particle. Conversely, with strong attractions between particles and collector, flow aids particle capture by increasing the mass transport of particles to the interfacial region. Here, local hydrodynamics still generally oppose adhesion but are insufficient to pull particles off of the surface. Thus, flow actually increases the particle capture rate through the increased transport to the surface. These behaviors are demonstrated using 1 mum silica spheres flowing over electrostatically heterogeneous (length scales near 10 nm) collecting surfaces at shear rates from 22 to 795 s(-1). The net surface charge on the collector is varied systematically from strongly negative (pure silica) to strongly positive (a saturated polycationic overlayer), demonstrating the interplay between physicochemical and hydrodynamic contributions. These results clearly apply to situations where heterogeneous particle-surface interactions are electrostatic in nature; however, qualitatively similar behavior was previously reported for the effect receptor density on bacterial adhesion.     

Non-specific adhesion on biomaterial surfaces driven by small amounts of protein adsorption

This work explores how long-range non-specific interactions, resulting from small amounts of adsorbed fibrinogen, potentially influence bioadhesion. Such non-specific interactions between protein adsorbed on a biomaterial and approaching cells or bacteria may complement or even dominate ligand–receptor mating. This work considers situations where the biomaterial surface and the approaching model cells (micron-scale silica particles) exhibit strong electrostatic repulsion, as may be the case in diagnostics and lab-on-chip applications. We report that adsorbed fibrinogen levels near 0.5 mg/m² produce non-specific fouling. For underlying surfaces that are less fundamentally repulsive, smaller amounts of adsorbed fibrinogen would have a similar effect. Additionally, it was observed that particle adhesion engages sharply and only above a threshold loading of fibrinogen on the collector. Also, in the range of ionic strength, I, below about 0.05 M, increases in I reduce the fibrinogen needed for microparticle capture, due to screening of electrostatic repulsions. Surprisingly, however, ionic strengths of 0.15 M reduce fibrinogen adsorption altogether. This observation opposes expectations based on DLVO arguments, pointing to localized electrostatic attractions and hydration effects to drive silica–fibrinogen adhesion. These behaviors are benchmarked against microparticle binding on silica surfaces carrying small amounts of a polycation, to provide insight into the role of electrostatics in fibrinogen-driven non-specific adhesion.     

Particle capture via discrete binding elements: systematic variations in binding energy for randomly distributed nanoscale surface features

This work examines how the binding strength of surface-immobilized "stickers" (representative of receptors or, in nonbiological systems, chemical heterogeneities) influences the adhesion between surfaces that are otherwise repulsive. The study focuses on a series of surfaces designed with fixed average adhesive energy per unit area and demonstrates quantitatively how a redistribution of the adhesive functionality into progressively larger clusters (stronger stickers) increases the probability of adhesive events. The work employs an electrostatic model system: relatively uniform, negative 1 μm silica spheres flow gently over negative silica flats. The flats contain small amounts of randomly positioned nanoscale cationic patches. The silica-silica interaction is repulsive; however, the cationic patches (present at sufficiently low levels that the overall surface charge remains substantially negative) produce local attractions. In this study, the attractions are relatively weak so that multiple patches engage to capture flowing particles. Experiments reveal an adhesion signature characteristic of a renormalized random distribution when the sticker strength is increased at an overall fixed binding strength per unit area of surface. The form of the particle capture curves are in good quantitative agreement with a simple model that assumes only a fixed adhesion energy needed for particle capture. Aside from the quantitative details that provide a simple formalism for anticipating particle adhesion, this work demonstrates how increasing the heterogeneities in the surface functionality can cause a system to go from being nonadhesive to becoming strongly adhesive. Indeed, systems containing small amounts of discretized adhesive functionality are always more adhesive than systems in which the same functionality is distributed uniformly over the surface (the mean field scenario).