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Subsurface deposition determines whether soils, aquifers, or ocean sediment represent a sink or temporary reservoir for microplastics. Deposition is generally studied by applying the Smoluchowski–Levich equation to determine a particle’s sticking efficiency, which relates the number of particles filtered by sediment to the probability of attachment occurring from an interaction between particles and sediment. Sticking efficiency is typically measured using column experiments or estimated from theory using the Interaction Force Boundary Layer (IFBL) model. However, there is generally a large discrepancy (orders of magnitude) between the values predicted from IFBL theory and the experimental column measurements. One way to bridge this gap is to directly measure a microparticle’s interaction forces using Atomic Force Microscopy (AFM). Herein, an AFM method is presented to measure sticking efficiency for a model polystyrene microparticle (2 μm) on a model geomaterial surface (glass or quartz) in environmentally relevant, synthetic freshwaters of varying ionic strength (de-ionized water, soft water, hard water). These data, collected over nanometer length scales, are compared to sticking efficiencies determined through traditional approaches. Force measurement results show that AFM can detect extremely low sticking efficiencies, surpassing the sensitivity of column studies. These data also demonstrate that the 75th to 95th percentile, rather than the mean or median force values, provides a better approximation to values measured in model column experiments or field settings. This variability of the methods provides insight into the fundamental mechanics of microplastic deposition and suggests AFM is isolating the physicochemical interactions, while column experiments also include physical interactions like straining. Advantages of AFM over traditional column/field experiments include high throughput, small volumes, and speed of data collection. For example, at a ramp rate of 1 Hz, 60 sticking efficiency measurements could be made in only a minute. Compared to column or field experiments, the AFM requires much less liquid (μL volume) making it effortless to examine the impact of solution chemistry (temperature, pH, ionic strength, valency of dissolved ions, presence of organics, etc.). Potential limitations of this AFM approach are presented alongside possible solutions (e.g., baseline correction, numerical integration). If these challenges are successfully addressed, then AFM would provide a completely new approach to help elucidate which subsurface minerals represent a sink or temporary storage site for microparticles on their journey from terrestrial to oceanic environments.