Sand filtration systems (SF) are a well-established approach in ensuring the availability of clean water. Understanding the transport properties of colloidal particles within SF systems is of paramount importance for optimizing their performance. This study investigated the potential utilization of silica-encapsulated DNA particles, equipped with a magnetic core to enhance particle separation and quantification efficiency (SiDNAMag). These particles were evaluated as tracers for delineating complex pathways and conducting source tracking within sand filtration (SF) systems for particulate substances. The study focused on exploring the sensitivity of SiDNAMag to solution chemistry, while elucidating the underlying mechanisms governing their transport and retention in sand filtration systems. Laboratory columns and HYDRUS-1D modeling were employed to analyze a range of water chemistry solutions, encompassing NaCl, NaHCO₃, CaCl₂, and MgCl₂, with ionic strengths ranging from 0.1 mM to 20 mM. The results revealed that the transport of DNA-tagged silica particles could be described by a first-order kinetic attachment and detachment rate coefficient. Elevated ionic strengths consistently led to increased particle adhesion and decreased rates of detachment. The sticking efficiencies of SiDNAMag particles exhibited a range of 0.7 to 1. The remarkable adhesive effectiveness can be ascribed to the comparatively low negative charge exhibited by SiDNAMag particles. This leads to the creation of unstable colloids and encourages the aggregation of these colloidal particles, thereby limiting the potential application of these particles as a tracer. In conclusion, this work underlines the potential of SiDNAMag particles as a potential subsurface tracer. However, further research is warranted to investigate strategies for reducing the interaction between these particles and sand, particularly in response to the chemistry of the infiltrated water.

Recently, superparamagnetic silica encapsulated DNA microparticles (SiDNAFe) were designed and in various experiments used as a hydrological tracer. We investigated the effect of bed characteristics on the transport behaviour and especially the mass loss of SiDNAFe in open channel injection experiments. Hereto, a series of laboratory injection experiments were conducted with four channel bed conditions (no sediment, fine river sediment, coarse sand, and goethite-coated coarse sand) and two water qualities (tap water and Meuse water). Breakthrough curves (BTCs) were analysed and modelled. Mass loss of SiDNAFe was accounted for as a first-order decay process included in a 1-D advection and dispersion model with transient storage (OTIS). SiDNAFe BTCs could be adequately described by advection and dispersion with or without a first-order decay process. SiDNAFe mass recoveries exhibited a wide range, varying from 50% to 120% from sediment-free conditions to coarse (coated) sediment. In 6 out of 8 cases, SiDNAFe mass recovery was complete. Retention of SiDNAFe was 1–2 orders of magnitude greater than gravitational settling rates, as determined in Tang et al. (Hydrological Processes, e14801, 2023). We reason this was due to grain-scale hyporheic flows and coupled water-sediment-particle interactions. The dispersive behaviour of SiDNAFe generally mimicked that of NaCl tracer. We concluded that SiDNAFe can be used in tracing experiments. However, water quality and sediment characteristics may affect the fate of SiDNAFe in river environments. SiDNAFe is a promising tool for particulate multi-tracing in large rivers.

Particle tracers are sometimes used to track sources and sinks of riverine particulate and contaminant transport. A potentially new particle tracer is ~200 nm sized superparamagnetic silica encapsulated DNA (SiDNAFe). The main objective of this research was to understand and quantify the settling and aggregation behaviour of SiDNAFe in river waters based on laboratory settling experiments. Our results indicated, that in quiescent conditions, more than 60% of SiDNAFe settled within 30 h, starting with a rapid settling phase followed by an exponential-like slow settling phase in the three river waters we used (Meuse, Merkske, and Strijbeek) plus MilliQ water. In suspensions of 1000× higher particle concentrations, the hydrodynamic diameter (D_h-DLS) of SiDNAFe increased over time, with its polydispersity index (PDI) positively correlated with particle size. From these observations, we inferred that the rapid SiDNAFe settling was mainly due to homo-aggregation and not due to hetero-aggregation (e.g., with particulate matter present in river water). Incorporating a first-order mass loss term which mimics the exponential phase of the settling in quiescent conditions seems to be an adequate step forward when modelling the transport of SiDNAFe in river injection experiments. Furthermore, we validated the applicability of magnetic separation and up-concentration of SiDNAFe in real river waters, which is an important advantage for carrying out field-scale SiDNAFe tracing experiments.

Surface water tracing is a widely used technique to investigate in-stream mass transport including contaminant migration. Recently, a microparticle tracer was developed with unique synthetic DNA encapsulated in an environmentally-friendly silica coating (Si-DNA microparticle). Previous tracing applications of such tracers reported detection and quantification, but a massive loss of tracer mass. However, the transport behavior of these DNA-tagged microparticle tracers has not been rigorously quantified and compared with that of solute tracers. Therefore, we compared the transport behavior of Si-DNA microparticles to the behavior of solute NaCl in 6 different, environmentally representative water types using breakthrough curves (BTCs), obtained from laboratory open channel injection experiments, whereby no Si-DNA microparticle tracer mass was lost. Hereafter, we modelled the BTCs using a 1-D advection-dispersion model with one transient storage zone (OTIS) by calibrating the hydrodynamic dispersion coefficient D and a storage zone exchange rate coefficient. We concluded that the transport behavior of Si-DNA microparticles resembled that of NaCl in surface-water relevant conditions, evidenced by BTCs with a similar range of D; however, the Si-DNA microparticle had a more erratic BTC than its solute counterpart, whereby the scatter increased as a function of water quality complexity. The overall larger confidence interval of D_Si-DNA was attributed to the discrete nature of colloidal particles with a certain particle size distribution and possibly minor shear-induced aggregations. This research established a solid methodological foundation for field application of Si-DNA microparticles in surface water tracing, providing insight in transport behavior of equivalent sized and mass particles in rivers.