(Na, Pb)-Jarosite nucleation and growth on anglesite: Implications for inhibition of Pb releasing.

The mobility and bioavailability of Pb can be significantly reduced by Pb-bearing minerals encapsulation in jarosite-group minerals, especially in sulfate-rich environments. However, the kinetic pathways and mechanisms of jarosite-group minerals formations on Pb-bearing mineral surfaces are not well understood. Here, time-resolved heterogeneous (Na, Pb)-jarosite nucleation and growth on anglesite were explored to gain insights into the encapsulation mechanisms. The initial dissolution of anglesite were clearly distinguished, and for the first time, the facet-specific heterogeneous nucleation of (Na, Pb)-jarosite on anglesite was demonstrated. Density functional theory calculations revealed higher adsorption energies and electronic interactions of FeSO complex on anglesite (020), (140), (110) facets, attributed to the preferential nucleation of (Na, Pb)-jarosite on these facets, which resulted in effective passivation of the facets resistant to dissolution. An interpretation was proposed where (Na, Pb)-jarosite grew via a particle-attachment pathway involving the formation of amorphous intermediate, and subsequently, it transformed to the crystalline phase by solid-state conversion. These observations might improve the mechanistic understanding of interface interactions between slightly soluble Pb-bearing minerals and iron minerals, with implications for Pb immobilization in sulfate-rich environments.