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  • 1.
    Cheng, Wei
    et al.
    College of Resources and Environmental Science, South-Central Minzu University, Wuhan, China.
    Li, Jiabin
    College of Resources and Environmental Science, South-Central Minzu University, Wuhan, China.
    Sun, Jie
    College of Resources and Environmental Science, South-Central Minzu University, Wuhan, China.
    Luo, Tao
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Université de Rennes, Ecole Nationale Supérieure de Chimie de Rennes, CNRS, ISCR-UMR 6226, Rennes, France.
    Marsac, Rémi
    Université de Rennes, CNRS, Géosciences Rennes─UMR 6118, Rennes, France.
    Boily, Jean-Francois
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Hanna, Khalil
    Université de Rennes, Ecole Nationale Supérieure de Chimie de Rennes, CNRS, ISCR-UMR 6226, Rennes, France.
    Nalidixic acid and Fe(II)/Cu(II) coadsorption at Goethite and Akaganéite surfaces2023Ingår i: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 57, nr 41, s. 15680-15692Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Interactions between aqueous Fe(II) and solid Fe(III) oxy(hydr)oxide surfaces play determining roles in the fate of organic contaminants in nature. In this study, the adsorption of nalidixic acid (NA), a representative redox-inactive quinolone antibiotic, on synthetic goethite (α-FeOOH) and akaganéite (β-FeOOH) was examined under varying conditions of pH and cation type and concentration, by means of adsorption experiments, attenuated total reflectance-Fourier transform infrared spectroscopy, surface complexation modeling (SCM), and powder X-ray diffraction. Batch adsorption experiments showed that Fe(II) had marginal effects on NA adsorption onto akaganéite but enhanced NA adsorption on goethite. This enhancement is attributed to the formation of goethite-Fe(II)-NA ternary complexes, without the need for heterogeneous Fe(II)-Fe(III) electron transfer at low Fe(II) loadings (2 Fe/nm2), as confirmed by SCM. However, higher Fe(II) loadings required a goethite-magnetite composite in the SCM to explain Fe(II)-driven recrystallization and its impact on NA binding. The use of a surface ternary complex by SCM was supported further in experiments involving Cu(II), a prevalent environmental metal incapable of transforming Fe(III) oxy(hydr)oxides, which was observed to enhance NA loadings on goethite. However, Cu(II)-NA aqueous complexation and potential Cu(OH)2 precipitates counteracted the formation of ternary surface complexes, leading to decreased NA loadings on akaganéite. These results have direct implications for the fate of organic contaminants, especially those at oxic-anoxic boundaries.

  • 2.
    Luo, Tao
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Univ Rennes, Ecole Nationale Supérieure de Chimie de Rennes, CNRS, ISCR-UMR 6226, Rennes, France.
    Chen, Tao
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Univ Rennes, Ecole Nationale Supérieure de Chimie de Rennes, CNRS, ISCR-UMR 6226, Rennes, France.
    Boily, Jean-Francois
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Hanna, Khalil
    Univ Rennes, Ecole Nationale Supérieure de Chimie de Rennes, CNRS, ISCR-UMR 6226, Rennes, France; Department of Chemistry, Durham University, Mountjoy Site, South Road, Durham, United Kingdom.
    Mobility and transport of pharmaceuticals nalidixic acid and niflumic acid in saturated soil columns2024Ingår i: Soil and Environmental Health, E-ISSN 2949-9194, Vol. 2, nr 1, artikel-id 100060Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Pharmaceutical compounds often coexist in mixtures rather than as individual entities. However, little is known about their co-adsorption and co-mobility in soil and groundwater. In this study, we investigated the adsorption of a quinolone antibiotic (nalidixic acid, NA) and an anti-inflammatory agent (niflumic acid, NFA) onto two soils from France and Sweden in water-saturated soil columns. Despite its lower hydrophobicity, adsorption of NA is much greater than NFA, which can be ascribed to the presence of both carbonyl and carboxylic groups in NA molecule. The data suggest that adsorption to soil components can mainly take place through hydrogen bonding and surface complexation mechanisms, prevailing over hydrophobic interactions. Accordingly, more sorption of NA and NFA was observed in the Swedish soil because it contains more clay content, and much higher Al and Fe contents than the French soil. Injection of NA/NFA mixture in the column did not modify the breakthrough behavior compared to single systems, although cooperative adsorption was observed under static batch conditions. Ca2+ inhibited NA adsorption by forming a soluble NA-Ca2+ complex but promoted NFA adsorption both in single and binary systems. The mobility in soil columns was well predicted using a new transport model that accounts for both kinetics and binding reactions of NA and NFA to soil constituents. This work will help in accurately predicting the mobility of coexisting pharmaceutical compounds in soils.

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  • 3.
    Luo, Tao
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Université de Rennes, École Nationale Supérieure de Chimie de Rennes, CNRS, ISCR-UMR 6226, Rennes, France.
    Le Crom, Sébastien
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Luong, N. Tan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Hanna, Khalil
    Université de Rennes, École Nationale Supérieure de Chimie de Rennes, CNRS, ISCR-UMR 6226, Rennes, France.
    Boily, Jean-Francois
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Goethite-bound copper controls the fate of antibiotics in aquatic environments2024Ingår i: ACS - ES & T Water, E-ISSN 2690-0637, Vol. 4, nr 2, s. 638-647Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Ciprofloxacin (CIP), a commonly used antibiotic, is today found in natural waterways and terrestrial environments alongside trace heavy metal contaminants. CIP however has a weak affinity for iron (oxy)hydroxide minerals, which often control contaminant transport in nature. This weak affinity is caused by the electrostatic repulsion between positively charged mineral surfaces and the CIP piperazine ring. Using goethite (α-FeOOH), a representative iron (oxy)hydroxide nanomineral, we show that the presence of Cu(II) greatly enhances CIP adsorption while at the same time catalyzes CIP oxidation to byproducts, which are new to nature. The CIP uptake was greatest at circumneutral pH and in saline conditions, where Cu(II), CIP, and mineral surface charges were the least repulsive. Vibrational spectroscopy and molecular simulations revealed that the enhanced uptake of CIP was caused by the the coordination of metal-bonded Cu(II)-CIP surface complexes on goethite. The inner-sphere Cu(II)-CIP complex also facilitated CIP oxidation into a series of new products, which we identified by mass spectrometry. Finally, to predict Cu(II) and quinolone loadings prior to redox-driven reactions, we propose a multisite surface complexation model using Cu(II)-CIP ternary surface complexes, alongside an ion pair to account for the ionic strength dependence on loadings. The information developed in this work will help tracking the fate of CIP in contaminated aquatic environments.

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  • 4.
    Luo, Tao
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Université de Rennes, Ecole Nationale Supérieure de Chimie de Rennes, CNRS, ISCR-UMR 6226, Rennes, France.
    Pokharel, Rasesh
    Department of Earth Sciences, Utrecht University, Utrecht, Netherlands.
    Chen, Tao
    Université de Rennes, Ecole Nationale Supérieure de Chimie de Rennes, CNRS, ISCR-UMR 6226, Rennes, France.
    Boily, Jean-François
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Hanna, Khalil
    Université de Rennes, Ecole Nationale Supérieure de Chimie de Rennes, CNRS, ISCR-UMR 6226, Rennes, France; Institut Universitaire de France (IUF), MESRI, 1 rue Descartes, Paris, France.
    Fate and transport of pharmaceuticals in iron and manganese binary oxide coated sand columns2023Ingår i: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 57, nr 1, s. 214-221Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Predicting the fate and transport of pharmaceuticals in terrestrial environments requires knowledge of their interactions with complex mineral assemblages. To advance knowledge along this front, we examined the reactivity of pipemidic acid (PIP), a typical quinolone antibiotic, with quartz particles coated with a mixture of manganese oxide (MnO2) and goethite (α-FeOOH) under static and dynamic flow conditions. Batch and dynamic column experiments showed that PIP binding to MnO2 proceeded through a heterogeneous redox reaction, while binding to goethite was not redox-reactive. Mixed columns of aggregated goethite-manganese particles however enhanced redox reactivity because (i) goethite facilitated the transport of dissolved Mn(II) ion and increased the retention of PIP oxidation products, and (ii) MnO2 was protected from passivation. This mobility behavior was predicted using transport models accounting for adsorption and transformation kinetics of PIP on both goethite and MnO2. This work sheds new light on reactivity changes of mixtures of Fe and Mn oxides under flow-through conditions and will have important implications in predicting the fate and transport of redox-active organic compounds as well as development of new geomedia filters for environmental remediation.

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