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 significant trans-
formation in jarosite.
At pH 5.5, 60 min was sufficient 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-flooded 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-flooded 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
significant 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