Turbulent-shear-induced coagulation of monodisperse particles was examined experimentally in the nearly isotropic, spatially decaying turbulence generated by an oscillating grid. The 3.9 μm polystyrene microspheres used in the experiments were made neutrally buoyant and unstable by suspending them in a density-matched saline solution. In this way, particle settling, double-layer repulsion and particle inertia were negligible and the effect of turbulent shear was isolated. The coagulation rate was measured by monitoring the loss of singlet particles as a function of time and reactor turbulence intensity. By restricting consideration to experimental conditions where the singlet concentration was in excess, the effect of higher-order aggregate (i.e. triplet) formation was negligible and nonlinear regression using an integral rate expression that included terms for doublet formation and breakup was used to obtain the turbulent coagulation rate constant. The strength of the van der Waals attractions was characterized with the Hamaker constant obtained from Brownian coagulation experiments. Since particle bulk mixing was fast compared to the coagulation rate, the observed coagulation rate constants were averages over the local coagulation rates within the grid-stirred reactor. Knowledge of the spatial variation of turbulence within the reactor was necessary for quantitative prediction of the experiments because model predictions for the coagulation rate are nonlinear functions of shear rate. The investigation was conducted with particles smaller than the length scales of turbulence and since the smallest turbulent length scales, the Kolmogorov scales, have the highest shear rate they controlled the rate of particle aggregation. The distribution of the Kolmogorov shear rate at various grid oscillation frequencies was obtained by measuring the turbulent kinetic energy (E) using acoustic Doppler velocimetry and relating E to the Kolmogorov shear rate using scaling arguments. The experimentally measured turbulent coagulation rate constants were significantly lower than theoretical predictions that neglect interparticle interactions; however, simulations that included particle interactions showed excellent agreement with the experimental results. The favourable comparison provides evidence that the computer simulations capture the important physics of turbulent coagulation. That is, particle transport on length scales comparable to the particle radius controls the rate of turbulent shear coagulation and particle interactions are significant.

Theoretical predictions for the coagulation rate induced by turbulent shear have often been based on the hypothesis that the turbulent velocity gradient is persistent (Saffman & Turner 1956) and that hydrodynamic and interparticle interactions (van der Waals attraction and electrostatic double-layer repulsion) between colloidal particles can be neglected. In the present work we consider the effects of interparticle forces on the turbulent coagulation rate, and we explore the response of the coagulation rate to changes in the Lagrangian velocity gradient correlation time (i.e. the characteristic evolution time for the velocity gradient in a reference frame following the fluid motion). Stokes equations of motion apply to the relative motion of the particles whose radii are much smaller than the lengthscales of turbulence (i.e. small particle Reynolds numbers). We express the fluid motion in the vicinity of a pair of particles as a locally linear flow with a temporally varying velocity gradient. The fluctuating velocity gradient is assumed to be isotropic and Gaussian with statistics taken from published direct numerical simulations of turbulence (DNS). Numerical calculations of particle trajectories are used to determine the rate of turbulent coagulation in the presence and absence of particle interactions. Results from the numerical simulations correctly reproduce calculated coagulation rates for the asymptotic limits of small and large total strain where total strain is a term used to describe the product of the characteristic strain rate and its correlation time. Recent DNS indicate that the correlation times for the fluctuating strain and rotation rate are of the same order as the Kolmogorov time (Pope 1990), suggesting theories that assume either small or large total strain may poorly approximate the turbulent coagulation rate. Indeed, simulations for isotropic random flows with intermediate total strain indicate that the coagulation rate in turbulence is significantly different from the analytical limits for large and small total strain. The turbulent coagulation rate constant for non-interacting monodisperse particles scaled with the Kolmogorov time and the particle radius is 8.62±0.02, whereas the commonly used model of Saffman & Turner (1956) predicts a value of 10.35 for non-rotational flows in the limit of persistent turbulent velocity gradients. Additional simulations incorporating hydrodynamic interactions and van der Waals attraction were used to estimate the actual rate of particle coagulation. For typical values of these parameters, particle interactions reduced the coagulation rate constant by at least 50%. In general, the collision efficiency (the ratio of coagulation with particle interactions to that without) decreased with increasing particle size and Kolmogorov shear rate.