Mechanistic Modeling of Pollutant Mass Redistribution (Sorption/Desorption) in Heterogeneous Systems Explaining Unexpected Slow Kinetics.

Redistribution of pollutants between different solid phases occurs frequently in field and laboratory settings. Examples include the input of urban particles carrying pollutants into soils or rivers with suspended particles or passive sampling. Since multiple mass transfer mechanisms are involved and natural particles typically are very heterogeneous, modeling of sorption/desorption kinetics is challenging.

Passive sampling of polycyclic aromatic hydrocarbons with low-density polyethylene: Equilibration limitations in aqueous suspensions.

Polyethylene (PE) and other polymers are widely and successfully used as passive samplers for organic pollutants in the environment. This study provides high-resolution experimental data from batch shaking tests on the uptake, reversibility, and linear equilibrium partitioning of polycyclic aromatic hydrocarbons (PAHs) using two different PE sheets of 30 µm and 80 µm thickness. Kinetics for phenanthrene are well described by a mechanistic first-order model with mass transfer limited by an aqueous boundary layer (with a mean thickness of 170 µm).

Ensemble surrogate modeling of advective-dispersive transport with intraparticle diffusion model for column-leaching test.

Column-leaching tests are a common approach for assessing the leaching behavior and resulting environmental risks of contaminated soils and waste materials, which are frequently reused for various construction purposes. The observed breakthrough curves of the contaminants are influenced by the complex dynamics of solute transport and kinetic inter-phase mass transfer. Disentangling these interactions necessitates numerical models.

Adaptation of the TIMBRE methodology for brownfields gully erosion analysis in urban areas.

Soil erosion is a concern in many parts of the world, causing environmental and social impacts. Aiming at obtaining indicators of the recovery of brownfields created by gullies in urban areas, this study adapts the Tailored Improvement of Brownfield Regeneration in Europe (TIMBRE) for the analysis and classification of areas affected by gullies in the city of Bauru, Brazil. The TIMBRE methodology assists in the decision-making of priority areas for remediation and their reinsertion in urban spaces.

Assessing sorption of fluoroquinolone antibiotics in soils from a K compilation based on pure organic and mineral components.

The presence of fluoroquinolone (FQ) antibiotics in soils may cause a threat to human health due to overexposure and the generation of antibiotic resistance genes. Understanding their sorption behavior in soils is important to predict subsequent FQ (bio) availability. Here, FQ sorption in pure soil organic (i.

In situ incubation of iron(II)-bearing minerals and Fe(0) reveals insights into metabolic flexibility of chemolithotrophic bacteria in a nitrate polluted karst aquifer.

Groundwater nitrate pollution is a major reason for deteriorating water quality and threatens human and animal health. Yet, mitigating groundwater contamination naturally is often complicated since most aquifers are limited in bioavailable carbon. Since metabolically flexible microbes might have advantages for survival, this study presents a detailed description and first results on our modification of the BacTrap© method, aiming to determine the prevailing microbial community's potential to utilize chemolithotrophic pathways.

Applicability of machine learning models for the assessment of long-term pollutant leaching from solid waste materials.

Column leaching tests are a common approach for evaluating the leaching behavior of contaminated soil and waste materials, which are often reused for various construction purposes. Standardized up-flow column leaching tests typically require about 7 days of laboratory work to evaluate long-term leaching behavior accurately. To reduce testing time, we developed linear and ensemble models based on parametric and non-parametric Machine Learning (ML) techniques.

Production of perfluoroalkyl acids (PFAAs) from precursors in contaminated agricultural soils: Batch and leaching experiments.

Contamination of soils with per- and polyfluoroalkyl substances (PFAS) (e.g., aqueous film forming foams (AFFFs) or PFAS containing biosolids applied to agricultural soils) can lead to large scale groundwater pollution.

A Fractional-order dual-continuum model to capture non-Fickian solute transport in a regional-scale fractured aquifer.

Contaminant transport in fractured media exhibits complex dynamics, including multiple peaks in breakthrough curves (BTCs) and non-Fickian diffusion, thereby posing significant challenges to the application of traditional transport models. Here we undertook a detailed study of a natural-gradient tracer test conducted in a regional-scale fractured carbonate aquifer situated in southwestern Germany, where the observed BTCs contained both dual peaks and positive skewness. These BTCs were used to optimize parameters and interpret their physical meanings for several transport models, including the dual-continuum model (DCM) and the fractional derivative equation (FDE) model.

Comprehensive Multi-compartment Sampling for Quantification of Long-Term Accumulation of PAHs in Soils.

Long-term accumulation in the soils of ubiquitous organic pollutants such as many polycyclic aromatic hydrocarbons (PAHs) depends on deposition from the atmosphere, revolatilization, leaching, and degradation processes such as photolysis and biodegradation. Quantifying the phase distribution and fluxes of these compounds across environmental compartments is thus crucial to understand the long-term contaminant fate. The gas-phase exchange between soil and atmosphere follows chemical fugacity gradients that can be approximated by gas-phase concentrations, yet which are difficult to measure directly.

Legacy pollutants in fractured aquifers: Analytical approximations for back diffusion to predict atrazine concentrations under uncertainty.

We present novel analytical approximations for the estimation of travel distance and relative height of solute concentration peaks within a single fracture system for pollutants that have been temporarily applied at a constant rate in the past. These approximations are used to investigate the spatiotemporal evolution of the concentration of atrazine, as an example for many other so-called legacy compounds that are still found in the groundwater of fractured rock aquifers even decades after their application has stopped. This is done in a stochastic framework to account for the uncertainty in relevant parameters, focusing on probabilities of exceeding the given legal concentration limit and the expected length of the recovery period.

Spatial origin analysis on atmospheric bulk deposition of polycyclic aromatic hydrocarbons in Shanghai.

Atmospheric deposition of polycyclic aromatic hydrocarbons (PAHs) onto soil threatens terrestrial ecosystem. To locate potential source areas geographically, a total of 139 atmospheric bulk deposition samples were collected during 2012-2019 at eight sites in Shanghai and its surrounding areas. A multisite joint location method was developed for the first time to locate potential source areas of atmospheric PAHs based on an enhanced three dimensional concentration weighted trajectory model.

Travel time-based modelling of nitrate reduction in a fractured limestone aquifer by pyrite and iron carbonates under pore size limitation.

We investigate denitrification in a ferric iron-containing fractured micritic limestone aquifer (Triassic Upper Muschelkalk) in south-west Germany by numerical simulations. Low porosity values (average value of 1%), partly small pore sizes of the rock matrix (~ 0.1 μm), and thus potential absence of microbial activity in the rock matrix suggest that denitrification is taking place solely in the fracture.

First order approximation for coupled film and intraparticle pore diffusion to model sorption/desorption batch experiments.

A simple first order approximation was derived to model sorption/desorption kinetics of hazardous compounds in batch experiments based on a coupled film and intraparticle diffusion model. The solution is accurate enough to replace infinite series expansions needed in analytical solution for intraparticle diffusion and it accounts for the mass transfer shift from diffusion in the external aqueous boundary layer to the intraparticle pore space. With increasing distribution coefficient (K) and intraparticle particle porosity (ε) or decreasing Sherwood number (Sh) this mass transfer shift from film diffusion to intraparticle pore diffusion is delayed.

Dilution of concentrations of PAHs from atmospheric particles, bulk deposition to soil: a review.

Polycyclic aromatic hydrocarbons (PAHs) are emitted to the atmosphere by various anthropogenic activities as well as natural sources, they undergo long-range transport, are degraded (e.g., by photolysis) and finally they are deposited onto the surface and potentially accumulate in topsoil.

Long-Term Leaching Behavior of Organic and Inorganic Pollutants after Wet Processing of Solid Waste Materials.

The recycling of mineral materials is a sustainable and economical approach for reducing solid waste and saving primary resources. However, their reuse may pose potential risks of groundwater contamination, which may result from the leaching of organic and inorganic substances into water that percolates the solid waste. In this study, column leaching tests were used to investigate the short- and long-term leaching behavior of "salts", "metals", and organic pollutants such as PAHs and herbicides from different grain size fractions of construction & demolition waste (CDW) and railway ballast (RB) after a novel treatment process.

Dilution of PAHs loadings of particulate matter in air, dust and rivers in urban areas: A comparative study (Tehran megacity, Iran and city of Tübingen, SW-Germany).

PAHs (polycyclic aromatic hydrocarbons) in urban areas are usually bound to particles. Concentrations are different in different compartments (airborne particles, street dust, suspended sediments in rivers and channels). This study follows concentrations of PAHs from particles in air to street dust and finally suspended sediments in the city of Tehran, Iran compared to Tübingen, Germany.

Mass Transfer Principles in Column Percolation Tests: Initial Conditions and Tailing in Heterogeneous Materials.

Initial conditions (pre-equilibrium or after the first flooding of the column), mass transfer mechanisms and sample composition (heterogeneity) have a strong impact on leaching of less and strongly sorbing compounds in column percolation tests. Mechanistic models as used in this study provide the necessary insight to understand the complexity of column leaching tests especially when heterogeneous samples are concerned. By means of numerical experiments, we illustrate the initial concentration distribution inside the column after the first flooding and how this impacts leaching concentrations.

Anaerobic Neutrophilic Pyrite Oxidation by a Chemolithoautotrophic Nitrate-Reducing Iron(II)-Oxidizing Culture Enriched from a Fractured Aquifer.

Neutrophilic microbial pyrite (FeS) oxidation coupled to denitrification is thought to be an important natural nitrate attenuation pathway in nitrate-contaminated aquifers. However, the poor solubility of pyrite raises questions about its bioavailability and the mechanisms underlying its oxidation. Here, we investigated direct microbial pyrite oxidation by a neutrophilic chemolithoautotrophic nitrate-reducing Fe(II)-oxidizing culture enriched from a pyrite-rich aquifer.

Long-term behavior of PFAS in contaminated agricultural soils in Germany.

PFAS contaminated compost materials have been applied over the last few decades to agricultural fields in Germany, resulting in large-scale diffuse PFAS plumes. The leaching behavior of PFAS from the first two identified contaminated agricultural sites in Germany were investigated, one at Brilon-Scharfenberg, North Rhine-Westphalia Site (BS-NRW), and the other at Rastatt/Mannheim, Baden-Württemberg. The specific objectives of this study were to assess the longevity of the PFAS agricultural sources and compare standardized column percolation tests to long-term leaching of PFAS from contaminated sites.

Nitrate Removal by a Novel Lithoautotrophic Nitrate-Reducing, Iron(II)-Oxidizing Culture Enriched from a Pyrite-Rich Limestone Aquifer.

Nitrate removal in oligotrophic environments is often limited by the availability of suitable organic electron donors. Chemolithoautotrophic bacteria may play a key role in denitrification in aquifers depleted in organic carbon. Under anoxic and circumneutral pH conditions, iron(II) was hypothesized to serve as an electron donor for microbially mediated nitrate reduction by Fe(II)-oxidizing (NRFeOx) microorganisms.

In-situ and ex-situ measurement of hydrophobic organic contaminants in soil air based on passive sampling: PAH exchange kinetics, non-equilibrium correction and comparison with traditional estimations.

It is a great challenge to accurately estimate chemical activity of hydrophobic organic contaminants in field soils. Ex-situ and in-situ determinations were developed for this purpose based on low-density polyethylene (LDPE) passive sampling and non-equilibrium correction by release of performance reference compounds (PRCs) previously spiked to the samplers. This work investigated kinetic processes of target contaminants' uptake into and PRCs' release from the sampler in an ex-situ soil suspension incubated for 100 days.

Impact of trophic levels on partitioning and bioaccumulation of polycyclic aromatic hydrocarbons in particulate organic matter and plankton.

The distribution and bioconcentration of polycyclic aromatic hydrocarbons (PAHs) in water, suspended particulate material (SPM), algae, and zooplankton samples from the Pearl River Delta (PRD), South China, were investigated. The PAHs in the water and SPM samples is significantly associated with chlorophyll a (Chl a), implying the important role of the aquatic productivity on PAH distribution. PAHs in the water or SPM samples were strongly correlated to dissolved organic carbon (DOC) or algal particulate organic carbon (A-POC).

Air-soil diffusive exchange of PAHs in an urban park of Shanghai based on polyethylene passive sampling: Vertical distribution, vegetation influence and diffusive flux.

Compared with dry and wet deposition rates, air-soil exchange fluxes cannot be directly measured experimentally. Polyethylene passive sampling was applied to assess transport directions and to measure concentration gradients in order to calculate diffusive fluxes of polycyclic aromatic hydrocarbons (PAHs) across the air-soil interface in an urban park of Shanghai, China. Seven campaigns with high spatial resolution sampling at 18 heights between 0 and 200 cm above the ground were conducted in 2017-2018.

Microplastic-Contaminant Interactions: Influence of Nonlinearity and Coupled Mass Transfer.

Microplastic particles are ubiquitously detected in the environment. Despite intensive public and scientific discussions, their potential to transport contaminants in rivers and oceans under environmental conditions is still under assessment. In the present study we measured sorption isotherms and kinetics in batch experiments using phenanthrene (as a typical hydrophobic wastewater contaminant) and microplastic particles of different sizes and materials.