Fig 1 Link Between Colloid Transport and Contaminant Adsorption in Soils
Rainwater runoff and pore water migrating through soils contain large amounts of fine colloids ranging from a few nanometers to several micrometers in size, including clay minerals as well as organic matter and microorganisms, and metal oxides (Fig. 1). It has been pointed out that the surfaces of these colloidal particles are electrically charged, enabling them to adsorb contaminants and nutrients and thereby act as carriers for their transport.
The mobility of colloids strongly depends on aggregation processes, in which colloids collide and attach to one another (coagulate) to form aggregates, as well as on deposition processes, in which colloids are captured by the soil matrix.
Through research on aggregation and deposition, we aim to contribute to a better understanding of fate and transport of substances/contaminants in water and soil environments.
In particular, by leveraging approaches from colloid and interfacial chemistry, we have been continuously conducting fundamental research that supports the prediction of the environmental fate and transport of nano- and microplastic particles, whose impacts have raised increasing concern in recent years.
Direct observation of deposition and related phenomena in microfluidic channels (collaborative project; details in preparation)
Aggregation experiments and simulations of model microplastic particles in well-characterized flow fields
Transport experiments and analysis of nanoparticles and nano-/microplastic particles in porous media
Aggregation of Microplastic Particles under Flow: Experiments and Theoretical Modeling
Fig 2 Aggregation in Flow Fields and the Role of Interparticle Interactions.
Flows are ubiquitous in natural environments, so verifying — both experimentally and theoretically — how interparticle forces influence aggregation rates under flow is essential for predicting the environmental fate of microplastics (Fig. 2).
We therefore measured aggregation rates under flow using model microplastic particles whose surface charges can be accurately characterised, and carried out theoretical analysis.
In particular, using the baffled flask developed by the U.S. Environmental Protection Agency, we showed that the measured aggregation rates agreed well with the Brunk-Koch model — which accounts for turbulent fluctuations — with no fitting parameters either for the turbulence intensity or the strength of the van der Waals attraction.
Concentrated Colloidal Suspension Rheology: Experiments and Simulations
Fig 3 Effects of electrical repulsion on non-Newtonian flow behavior of concentrated colloidal suspensions
Concentrated colloidal suspensions undergo shear thickening—a steep rise in viscosity—once the shear stress exceeds a critical value. How this thickening manifests depends on the forces acting between particles, yet the specific role of electric double layer (EDL) repulsions had not been quantified (Fig. 3).
We therefore measured the viscosity of colloidal silica suspensions as a function of shear stress across particle diameters of 100–2500 nm at different salt concentrations, using a refractive-index-matching solvent to suppress van der Waals attraction, and complemented the experiments with numerical simulations.
Raising the salt concentration weakens EDL repulsions, which reduces both the shear-thinning slope and the critical shear stress σc marking the onset of thickening. Above a certain salt concentration σc becomes essentially constant; we term this the critical concentration for critical stress (CCCS), a counterpart to the critical coagulation concentration (CCC) of DLVO theory.
Heteroaggregation Between Oppositely Charged Particles in the Presence of Specifically Adsorbing Ions
Fig 4 Heteroaggregation of Oppositely Charged Colloids with Counterion Adsorption.
Phosphate, an essential nutrient, and highly toxic arsenic are present in dissolved form as anions, and are known to adsorb onto positively charged clay minerals and metal oxides in soils.
When such specifically adsorbing ions accumulate excessively at particle surfaces, they can neutralize the original colloidal charge and induce charge reversal, in which the sign of the net surface charge becomes opposite. Once a positively charged colloid undergoes charge reversal, its newly acquired negative charge generates electrostatic repulsion against coexisting negatively charged clay colloids, leading to repulsion-dominated heteroaggregation.
To investigate this problem, we conducted measurements under conditions where collisions occur via Brownian motion, and performed theoretical analyses. As a result, we successfully explained—using a standard theoretical model—the experimental observation that heteroaggregation becomes repulsive within the salt-concentration range where charge reversal occurs.
Effects of Deposited Colloids in Porous Media on Nanobubble Transport
Fig 5 Deposited solid colloids (nanoplastic particles) capture nanobubbles and inhibit their transport.
In recent years, nano-bubbles—fine bubbles with diameters of a few micrometers or less—have attracted attention for their potential to remediate contaminated soils.
However, when injecting nanobubbles into soils, it has remained unclear how coexisting soil colloids affect nanobubble transport (Fig. 5).
To address this issue, we conducted column transport experiments using a model soil system in which colloids and nanobubbles coexist. We employed a resonant mass measurement technique that distinguishes and counts solid colloids (nanoplastic particles) and nanobubbles based on differences in particle–fluid density.
We found that when colloids were introduced first, the deposited colloids acted as new adsorption sites for nanobubbles via physicochemical interactions. As a result, nanobubble transport was more strongly hindered than in the absence of colloid deposition.