Weathering of metallurgical slags : a comprehensive study on the importance of chemical and biological contributions

par Nang Htay Yin

Thèse de doctorat en Sciences et Techniques de l'Environnement

Sous la direction de Eric Van Hullebusch.

Soutenue le 02-12-2014

à Paris Est en cotutelle avec l'Erasmus Mundus ETeCoS3 , dans le cadre de École doctorale Sciences, Ingénierie et Environnement (Champs-sur-Marne, Seine-et-Marne ; 2010-2015) , en partenariat avec Laboratoire Géomatériaux et Environnement (Champs-sur-Marne, Seine-et-Marne) (laboratoire) et de Laboratoire Géomatériaux et Environnement / LGE (laboratoire) .

Le président du jury était Marc Benedetti.

Le jury était composé de Eric Van Hullebusch, Yann Sivry, François Guyot, Piet N. L. Lens, Giovanni Esposito.

Les rapporteurs étaient Cécile Quantin, Vojtech Ettler.

  • Titre traduit

    L'altération des scories métallurgiques : une étude approfondie sur l'importance des contributions chimiques et biologiques


  • Résumé

    Le crassier du site MetalEurop (Noyelles-Godault) a accueilli des scories de première fusion entre les années 1936 à 2003. Il est actuellement constitué de 4 millions de tonnes de ces matériaux générés par les deux procédés pyrométallurgiques les plus usités dans le monde pour la production du plomb et du zinc : le procédé Lead Blast Furnace (LBF) et le procédé Impérial Smelting Furnace (ISF). L'utilisation de ces scories en tant que matériau de substitution dans les ciments et dans les routes a été envisagée et a fait l'objet de recherches, mais présente des risques environnementaux, c'est-à-dire, essentiellement la dissémination de polluants (Pb et Zn)


  • Résumé

    Primary smelting slags, known as Lead Blast Furnace (LBF) and Imperial Smelting Furnace (ISF), were generated by the former pyrometallurgical industries located in Noyelles-Godault, Northern France. Following its closure in 2003, 4 million tons of primary slags have been landfilled as a heap in the vicinity of the Deûle River, near the industrial basin of Nord-Pas-de-Calais. These slag materials are often enriched in particular metals (Pb, Zn) that can be released into the environment through alteration processes and leaching. Many biological and chemical processes might take place within these tailings and thus affect significantly the slag weathering. Predicting the environmental impact of these wastes requires an understanding of the mineral-water interactions as well as the influence of the biological activities (the involvement of microorganisms). Thus, this research is designed to simulate the natural weathering of slag by simulating different weathering conditions with or without the involvement of the microorganisms as well as by varying several chemical parameters. Chemical weathering of both LBF and ISF slags was studied by as a function of pHs (4, 5.5, 7, 8.5 and 10) as well as under two atmospheres (open air and nitrogen). Significant amounts of Ca, Fe and Zn were released under acidic conditions (pH 4) with a decrease towards the neutral to alkaline conditions (pH 7 and 10) for both slags. The concentrations of all elements increased gradually after 216 h compared to initial 24 h of leaching period. The presence of oxygen under open-air atmosphere not only enhanced oxidative weathering but also encouraged formation of secondary oxide and carbonate phases. In addition, Zn dissolution was related to extremes zinc isotopic signatures in the leachate; heavier δ66Zn values at low pH than at high pH for both slags under open-air atmosphere. On the other hand, bioweathering of both slags was studied in the presence of a pure heterotrophic bacterial strain (Pseudomonas aeruginosa) in a bioreactor operated in batch conditon as well as in a semi-flow through reactor with intermittent leachate renewal conditions. P. aeruginosa is shown to play a significant role in slags weathering by enhancing the leaching and solubility of Zn and Pb. In addition, the cumulative bulk release of dissolved Fe, Si, Ca and Mg doubled in the presence of bacteria, probably due to the release of soluble complexing organic molecules (e.g. siderophores). Bacterial biomass served as the bioadsorbent for Pb, Fe and Zn as 70-80% of Pb and Fe, 40-60% of Zn released are attached to and immobilized by the bacterial biomass. Oxides, hydroxides and carbonates were predicted as secondary phases during chemical weathering of slags whereas carbonates and phosphates were dominant phases during bioweathering. These predictions were in agreement with the observations by Scanning Electron Microscopy (SEM) with Energy Dispersive X-Ray Analysis (EDS), Transmission Electron Microscopy (TEM) analysis, and X-ray Photoelectron Spectroscopy (XPS) analysis


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