Mobility of water-soluble aerosol organic matters (WSAOMs) and their effects on soil colloid-mediated transport of heavy metal ions in saturated porous media.

Sediment organic carbon dominates the heteroaggregation of suspended sediment and nanoplastics in natural and surfactant-polluted aquatic environments.

We discuss colloidal-suspension-nano transport in porous media with particle detachment and further capture by the matrix. Previous works formulate particle-scale detachment conditions and porous-media-scale transport equations with empirical coefficients, which are determined from flow tests and cannot be predicted from the particle scale. The present work derives the upscaling technique by stochastic distribution of torque and force balances on the attached particle, yielding a macro-scale equation for detachment. The upscaled detachment equation has the form of the maximum retained concentration of attached particles as a function of velocity, pH, salinity, and temperature of the carrier fluid. The upscaling procedure allows for direct calculations of the maximum retention function (MRF) from micro-scale parameters. The sensitivity analysis shows that MRF is most sensitive to the particle aspect ratio and pore size, while it is less sensitive to the standard deviations of the lever-arm ratio and particle size distributions. The exact solution for 1D flow problem is used to determine the MRF from laboratory tests and matches it with the stochastic microscale model for detachment. The high match obtained for four colloidal coreflood experiments validates the stochastic model and upscaling procedure. 

Colloidal detachment in porous media: Stochastic model and upscaling

Particulate contaminants, such as microplastics (1 μm to 5 mm) and nanoplastics (<1 μm), are disseminated in many terrestrial environments. However, it is still unclear how particles' properties drive their mobility through soils and aquifers due to (i) poor environmental relevance of the model particles that are studied (e.g., spherical and monodisperse) and (ii) the use of packed bed experiments which do not allow a direct observation of deposition dynamics. Using transparent 2D porous media, this study analyzes deposition dynamics of rough polystyrene fragments with irregular shapes and with a size continuum (≈10 nm to 5 μm). Using in situ and ex situ measurements, particle deposition as a function of size was monitored over time under repulsive conditions. In the absence of natural organic matter (NOM), micrometric particles rapidly deposit and promote the physical interception of smaller nanoparticles by creating local porous roughness or obstacles. In the presence of NOM, differences according to particle size were no longer observed, and all fragments were more prone to being re-entrained, thereby limiting the growth of deposits. This work demonstrates the importance of pore surface roughness and porosity of the pore surface for the deposition of colloidal particles, such as microplastics and nanoplastics, under repulsive conditions.

Role of Ripening in the Deposition of Fragments: The Case of Micro- and Nanoplastics.

This work investigates the influence of cation type (Ca2+ as compared to K+) on the co-transport and deposition of functionalized multi-walled carbon nanotubes (MWCNTs) with negatively (bentonite nanoparticles, BNPs) or positively (goethite nanoparticles, GNPs) charged natural nanoparticles under the same ionic strength (IS=1 mM) conditions. In packed column tests with quartz sand (QS), the co-transport of MWCNTs was slightly increased by BNPs and inhibited by GNPs in both CaCl2 and KCl solutions, whereas the co-transport of BNPs or GNPs was facilitated by MWCNTs in both solutions. However, the co-transport of MWCNTs in the presence of BNPs or GNPs exhibited a different dependency on the cation type in quartz crystal microbalance with dissipation (QCM-D) tests. No deposition of MWCNTs and BNPs was observed in QCM-D studies in the presence of KCl, while enhanced deposition of MWCNTs and GNPs occurred in this same solution. In contrast, the deposition of both MWCNTs and BNPs or MWCNTs and GNPs increased in QCM-D in the presence of CaCl2. In both column and QCM-D studies, Ca2+ exhibited a more significant impact on co-transport than K+, especially for MWCNTs with GNPs than BNPs. Results from molecular dynamic simulations, aggregation studies, and interaction energy calculations indicate that non-DLVO interactions (e.g., H-bonding and cation-π interaction) between two nanoparticles (MWCNTs with BNPs or GNPs) played a non-negligible role in interpreting the deposition and co-transport in the presence of the divalent cation Ca2+. Mathematical modeling of breakthrough curves and retention profiles and aggregation results suggest that both straining and competitive blocking were enhanced and played dominant roles in the co-transport of MWCNTs in the presence of BNPs or GNPs in QS, especially in the presence of Ca2+. This work sheds novel insights on the contribution of divalent cations to interactions between two colloids and their co-transport in porous media. This information is needed to assess the environmental fate and risks of engineered nanoparticles (ENPs) and natural nanoparticles in aquatic and soil environments with abundant divalent cations. 

Divalent cation contributions to the co-transport and deposition of functionalized multi-walled carbon nanotubes in porous media in the presence of bentonite or goethite nanoparticles: Experiment and simulation

This study conducted saturated column experiments to systematically investigate deposition of 1 μm positively charged polystyrene latex micro-colloids (representing microplastic particles) on negatively charged rough sand, glass beads, and soil with pore water velocities (PWV) from 4.9 × 10-5 to 8.8 × 10-4 m/s. A critical value of PWV was found below which colloidal attachment efficiency (AE) increased with increasing PWV. The increase in AE with PWV was attributed to enhanced delivery of the colloids and subsequent attachment at concave locations of rough collector surfaces. The AE decreased with further increasing PWV beyond the threshold because the convex sites became unavailable for colloid attachment. By simulating the rough surfaces using the Weierstrass-Mandelbrot equation, the extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) interaction energy calculations and torque analysis revealed that the adhesive torques could be reduced to be comparable or smaller than hydrodynamic torques even under the favorable conditions. Interestingly, scanning electron microscopic experiments showed that blocking occurred at convex sites at all ionic strengths (ISs) (e.g., even when the colloid-colloid interaction was attractive), whereas at concave sites, blocking and ripening (i.e., attached colloids favor subsequent attachment) occurred at low and high ISs, respectively. To our knowledge, our work was the first to show coexistence of blocking and ripening at high ISs due to variation of the collector surface morphology.

Important Role of Concave Surfaces in Deposition of Colloids under Favorable Conditions as Revealed by Microscale Visualization.

While the facilitated transport of heavy metals by colloids such as clay particles has been widely recognized, the influence of heavy metals on transport of the colloids has received much less attention. This study conducted saturated column experiments to systematically examine influence of multivalent heavy metal cations on transport of natural clay colloids and fullerene nC60 nanoparticles in glass bead porous media. Results showed that the presence of Cd2+ in the solution can cause more deposition of clay colloids in glass beads compared to Ca2+ at a given ionic strength (IS), and the subsequent release by IS reduction was less, demonstrating that the presence of Cd2+ increased the irreversibility of attachment. When the glass beads were initially adsorbed with Ca2+ and Cd2+, the release of clay colloids was significantly reduced due to strong cation bridge between the clay colloids and collector surfaces via the heavy metal cations. The release of clay colloids was significantly increased upon reduction of solution IS if the Na+ was used to exchange for the Ca2+ or Cd2+ before the IS reduction. Additional experiments showed that the nC60 nanoparticles that were deposited in the presence of Fe3+ and Cu2+ cannot be released by reduction of solution IS. However, the nanoparticle release occurred when the Ca2+ was used to exchange for the Fe3+ and Cu2+. Our work was the first to reveal the influence of heavy metal cations on the irreversibility of colloid attachment, and the findings have important implication to fabrication of functional nanomaterials for stabilization of heavy metals in soil and development of mathematic models for accurate prediction of cotransport of heavy metals and colloids in subsurface environments.

Impact of heavy metal cations on deposition and release of clay colloids in saturated porous media

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Important Role of Concave Surfaces in Deposition of Colloids under Favorable Conditions as Revealed by Microscale Visualization.

Impact of heavy metal cations on deposition and release of clay colloids in saturated porous media