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Scientific publication · Applied Geochemistry · Volume 163

Antimony isotope fractionation during Sb(V) and Sb(III) adsorption on secondary Fe-minerals (schwertmannite, ferrihydrite) typical of mine waters

Sb Isotope fractionation Adsorption Fe minerals Mine waters 2024
Graphical abstract showing antimony isotope fractionation during Sb adsorption on ferrihydrite and schwertmannite
Experimental study of Sb(III) and Sb(V) adsorption onto ferrihydrite and schwertmannite, two secondary Fe minerals commonly formed in acid mine drainage environments.
Key points

What the study shows

Adsorption of Sb onto ferrihydrite and schwertmannite produces measurable equilibrium isotope fractionation.
The lighter 121Sb isotope is preferentially retained on the mineral surfaces, leaving the dissolved Sb relatively enriched in 123Sb.
Fractionation is similar for Sb(III) and Sb(V) and for both Fe mineral phases under the experimental conditions.
Neither pH nor the initial Fe:Sb ratio produced a significant change in the measured isotope fractionation factors.
Summary

Understanding how adsorption modifies Sb isotope signatures

Adsorption onto secondary Fe minerals is one of the main processes controlling the mobility of antimony in acid mine drainage and mine-impacted streams. Ferrihydrite and schwertmannite can efficiently retain dissolved Sb as acidic drainage waters evolve downstream.

For Sb isotopes to be used as tracers of environmental transport, it is therefore necessary to determine whether this retention process changes the isotope composition of the dissolved and adsorbed pools.

This study experimentally investigated the equilibrium isotope fractionation produced during adsorption of both Sb(III) and Sb(V) onto ferrihydrite and schwertmannite. Experiments were carried out under controlled pH and solid-to-liquid conditions, allowing the effect of mineral phase, Sb oxidation state and Fe:Sb ratio to be compared.

All experimental systems showed preferential retention of the lighter 121Sb isotope on the solid phase. Consequently, dissolved Sb becomes relatively enriched in the heavier 123Sb isotope as adsorption proceeds.

The similar isotope response observed for both Sb oxidation states and both Fe minerals indicates a relatively consistent equilibrium fractionation associated with this adsorption process under the investigated conditions.

Main result

Adsorption onto ferrihydrite and schwertmannite preferentially removes the lighter 121Sb isotope from solution. The resulting Δ123Sbsolid–solution values range from approximately −0.25 to −0.36‰. The direction and magnitude of the fractionation are broadly similar for Sb(III) and Sb(V), and no significant effect of pH or initial Fe:Sb ratio was detected under the experimental conditions.

Experimental results

Similar isotope fractionation across both minerals and oxidation states

The four experimental systems produce negative Δ123Sbsolid–solution values, confirming preferential adsorption of the lighter Sb isotope onto the Fe-bearing solid phase.

Ferrihydrite · Sb(III) −0.25 ± 0.08‰ Δ123Sbsolid–solution measured for Sb(III) adsorption onto ferrihydrite.
Ferrihydrite · Sb(V) −0.34 ± 0.08‰ Equilibrium isotope fractionation measured for Sb(V) adsorption onto ferrihydrite.
Schwertmannite · Sb(III) −0.36 ± 0.06‰ Largest negative fractionation measured among the four experimental conditions.
Schwertmannite · Sb(V) −0.27 ± 0.03‰ Equilibrium fractionation measured during Sb(V) adsorption onto schwertmannite.
Experimental evidence

The isotope response is linked to the adsorption process

The negative Δ123Sbsolid–solution values consistently indicate enrichment of 121Sb on the adsorbing mineral phase. The similarity between experiments suggests that this fractionation reflects a common change in the local bonding environment of Sb when it moves from the aqueous phase to an Fe-bearing surface.

Isotope direction

The solid phase is isotopically lighter than the remaining dissolved Sb because 121Sb is preferentially adsorbed.

Mineral independence

Ferrihydrite and schwertmannite generate comparable fractionation factors despite their different mineral structures.

Limited pH effect

Within the tested experimental range, pH and the initial Fe:Sb ratio do not significantly alter the equilibrium isotope fractionation.

Environmental significance

Why this matters for isotope tracing in mine waters

Sb isotope signatures measured downstream from mining areas do not reflect only the initial source of antimony, but also the processes affecting it after release. Understanding the fractionation induced by adsorption therefore helps distinguish changes produced during environmental transport from differences directly inherited from the contamination source.

Publication

Scientific reference

Citation

Ferrari, C., Resongles, E., Freydier, R., Casiot, C. (2024). Antimony isotope fractionation during Sb(V) and Sb(III) adsorption on secondary Fe-minerals (schwertmannite, ferrihydrite) typical of mine waters. Applied Geochemistry, 163, 105935.

DOI: 10.1016/j.apgeochem.2024.105935
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