Adsorption of hydrogen gas and redox processes in clays

Environmental Science & Technology
Mathilde DidierLaurent Charlet

Abstract

In order to assess the adsorption properties of hydrogen gas and reactivity of adsorbed hydrogen, we measured H(2)(g) adsorption on Na synthetic montmorillonite-type clays and Callovo-Oxfordian (COx) clayrock using gas chromatography. Synthetic montmorillonites with increasing structural Fe(III) substitution (0 wt %, 3.2 wt %, and 6.4 wt % Fe) were used. Fe in the synthetic montmorillonites is principally present as structural Fe(III) ions. We studied the concomitant reduction of structural Fe(III) in the clays using (57)Fe Mössbauer spectrometry. The COx, which mainly contains smectite/illite and calcite minerals, is also studied together with the pure clay fraction of this clayrock. Experiments were performed with dry clay samples which were reacted with hydrogen gas at 90 and 120 °C for 30 to 45 days at a hydrogen partial pressure close to 0.45 bar. Results indicate that up to 0.11 wt % of hydrogen is adsorbed on the clays at 90 °C under 0.45 bar of relative pressure. (57)Fe Mössbauer spectrometry shows that up to 6% of the total structural Fe(III) initially present in these synthetic clays is reduced upon adsorption of hydrogen gas. No reduction is observed with the COx sample in the present experimental conditions.

References

Apr 20, 2005·The Journal of Chemical Physics·Jenny G VitilloGabriele Ricchiardi
Mar 16, 2006·Journal of the American Chemical Society·Antek G Wong-FoyOmar M Yaghi
Nov 24, 2006·Angewandte Chemie·Michel LatrocheGérard Férey
Dec 21, 2006·Journal of the American Chemical Society·Mircea DincăJeffrey R Long
Jun 7, 2008·Journal of the American Chemical Society·Jenny G VitilloAdriano Zecchina
Sep 21, 2010·Journal of Colloid and Interface Science·C MansourS Zanna

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