Antimony and arsenic partitioning during Fe 2þ -induced transformation of jarosite under acidic conditions Niloofar Karimian * , Scott G. Johnston, Edward D. Burton Southern Cross GeoScience, Southern Cross University, Lismore, NSW 2480, Australia highlights graphical abstract At pH 4.0, the addition of Fe 2þ (aq) resulted in no signicant trans- formation in jarosite. At pH 5.5, 60 min was sufcient for partial transformation of jarosite to green rust. Formation of green rust and goethite under pH 5.5, sequestered dissolved antimony. Arsenic was mostly repartitioned to the surface of green rust and goethite. article info Article history: Available online 27 December 2017 Keywords: Antimony Arsenic Jarosite Fe 2þ Green rust pH abstract Jarosite [KFe 3 (SO 4 ) 2 (OH) 6 ] is considered a potent scavenger for arsenic (As) and antimony (Sb) under oxidizing conditions. Fluctuations in water levels in re-ooded acid sulfate soils (ASS) can lead to high Fe 2þ (aq) concentrations (~10e20 mM) in the soil solution under acidic to circumneutral pH conditions. This may create favorable conditions for the Fe 2þ -induced transformation of jarosite. In this study, synthetic arsenate [As(V)]/antimonate [Sb(V)]-bearing jarosite was subjected to Fe 2þ (aq) (20 mM) at pH 4.0 and 5.5 for 24 h to simulate the pH and Fe 2þ (aq) conditions of re-ooded freshwater ASS/acid mine drainage (AMD)-affected environments at early and mid-stages of remediation, respectively. The addi- tion of Fe 2þ at pH 5.5 resulted in the formation of a metastable green rust sulfate (GR- SO 4 ) phase within ~60 min, which was replaced by goethite within 24 h. In contrast, at pH 4.0, jarosite underwent no signicant mineralogical transformation. Although the addition of Fe 2þ (aq) induced the dissolution/ transformation of jarosite at pH 5.5 and increased the mobility of Sb during the initial stages of the experiment (Sb (aq) ¼ ~0.05 mmol L 1 ), formation of metastable green rust (GR-SO 4 ) and subsequent transformation to goethite effectively sequestered dissolved Sb. Aqueous concentrations of As remained negligible in both pH treatments, with As being mostly repartitioned to the labile (~10%) and poorly crystalline Fe(III)-associated phases (~10e30%). The results imply that, under moderately acidic condi- tions (i.e. pH 5.5), reaction of Fe 2þ (aq) with jarosite can drive the dissolution of jarosite and increase Sb mobility prior to the formation of GR-SO 4 and goethite. In addition, repartitioning of As to the labile * Corresponding author. E-mail address: niloofar.karimian@scu.edu.au (N. Karimian). Contents lists available at ScienceDirect Chemosphere journal homepage: www.elsevier.com/locate/chemosphere https://doi.org/10.1016/j.chemosphere.2017.12.106 0045-6535/© 2017 Elsevier Ltd. All rights reserved. Chemosphere 195 (2018) 515e523