Environmental Pollution 212 (2016) 366e373

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Environmental Pollution
journal homepage: www.elsevier.com/locate/envpol

Mercury remediation in wetland sediment using zero-valent iron and

granular activated carbon
Ariel S. Lewis a, Thomas G. Huntington b, Mark C. Marvin-DiPasquale c, Aria Amirbahman a, *
a
Department of Civil and Environmental Engineering, University of Maine, Orono, ME, USA
b
The US Geological Survey, Augusta, ME, USA
c
The US Geological Survey, Menlo Park, CA, USA

a r t i c l e i n f o a b s t r a c t

Article history: Wetlands are hotspots for production of toxic methylmercury (MeHg) that can bioaccumulate in the food
Received 5 August 2015 web. The objective of this study was to determine whether the application of zero-valent iron (ZVI) or
Received in revised form granular activated carbon (GAC) to wetland sediment could reduce MeHg production and bioavailability
25 November 2015
to benthic organisms. Field mesocosms were installed in a wetland fringing Hodgdon Pond (Maine, USA),
Accepted 26 November 2015
Available online xxx
and ZVI and GAC were applied. Pore-water MeHg concentrations were lower in treated compared with
untreated mesocosms; however, sediment MeHg, as well as total Hg (THg), concentrations were not
significantly different between treated and untreated mesocosms, suggesting that smaller pore-water
Keywords:
Mercury
MeHg concentrations in treated sediment were likely due to adsorption to ZVI and GAC, rather than
Zero valent iron inhibition of MeHg production. In laboratory experiments with intact vegetated sediment clumps,
Granular activated carbon amendments did not significantly change sediment THg and MeHg concentrations; however, the mean
Wetlands pore-water MeHg and MeHg:THg ratios were lower in the amended sediment than the control. In the
Remediation laboratory microcosms, snails (Lymnaea stagnalis) accumulated less MeHg in sediment treated with ZVI
or GAC. The study results suggest that both GAC and ZVI have potential for reducing MeHg bio-
accumulation in wetland sediment.
© 2015 Elsevier Ltd. All rights reserved.

1. Introduction et al., 1994; Ullrich et al., 2010; Windham-Myers et al., 2009).

Mercury (Hg) contamination can negatively affect the health
of many faunal species in ecosystems. In natural systems,
methylmercury (MeHg) is the Hg species of greatest concern
because of its ability to bind to muscle tissue and thereby bio-
accumulate in food webs, potentially to the point of toxicity
(Chen et al., 2008; Liu et al., 2008; Patra and Sharma, 2000;
Watras et al., 1998; Wolfe et al., 1998). MeHg is primarily
formed by the methylation of inorganic divalent mercury (Hg(II))
by anaerobic bacteria (Benoit et al., 1999; Compeau and Bartha,
1985; Hamelin et al., 2011; Kerin et al., 2006). Recent studies
suggest that plant activity may enhance Hg(II) methylation;
therefore, wetlands can be important sources of MeHg contam-
ination to adjacent water bodies (Bowles et al., 2003; Cosio et al.,
2014; Hall et al., 2008; Marvin-Dipasquale et al., 2007; St. Louis
* Corresponding author.
E-mail address: ariaa@maine.edu (A. Amirbahman).
Low-cost, low-impact, in situ treatment of these potential MeHg
hotspots is desirable to reduce Hg toxicity in these wetland
ecosystems.
Zero-valent iron (ZVI) is an inexpensive material commonly
used in permeable reactive barriers to treat ground-water
contamination. ZVI treatment has been shown to lower the
toxicity of arsenic and chromium through reductive and sorptive
mechanisms (Fu et al., 2014). Research on the use of iron (Fe)
species for Hg remediation has largely focused on Fe(II) that was
shown to reduce Hg(II) methylation in pure culture of sulfate-
reducing bacteria (SRB), non-vegetated wetland sediment slur-
ries, and intact wetland sediment clumps (Mehrotra et al., 2003;
Mehrotra and Sedlak, 2005; Ulrich and Sedlak, 2010). The effect
of ZVI on Hg has been studied in synthetic aerobic and anaerobic
systems, where reductions in dissolved Hg concentrations were
attributed to adsorption by ZVI (Gibson et al., 2011; Vernon and
Bonzongo, 2014; Weisener et al., 2005; Wilkin and McNeil, 2003).
To our knowledge, the effect of ZVI on in situ MeHg production, and
the potential of ZVI as a remediation tool to reduce MeHg uptake by
biota have not been studied.

http://dx.doi.org/10.1016/j.envpol.2015.11.047
0269-7491/© 2015 Elsevier Ltd. All rights reserved.
 A.S. Lewis et al. / Environmental Pollution 212 (2016) 366e373
Several experimental and laboratory microcosm studies have
shown that GAC can effectively remove inorganic Hg(II) and MeHg
from contaminated sediment (Ghosh et al., 2011; Gilmour et al.,
2013; Gomez-Eyles et al., 2013; Hollerman et al., 1999; Zhu et al.,
2009). Gilmour et al. (2013) tested the effect of a range of GAC
treatment levels on sediment pore-water partitioning of inorganic
Hg(II) and MeHg in homogenized sediment microcosms repre-
senting a range of salinity and contamination levels. In most in-
stances GAC resulted in a decrease in pore-water MeHg
concentration that led to an increase in MeHg partition coefficient
(KD,MeHg; defined as the ratio of sediment to pore-water MeHg
concentrations) and a decrease in MeHg biotic uptake. These results
suggest that GAC addition may also be a promising treatment for
reducing MeHg uptake by biota.
In this study we evaluated the use of ZVI and GAC as treatment
amendments in in situ vegetated wetland mesocosms, and in intact
vegetated laboratory microcosms. The field mesocosm experiments
were conducted to study the effect of ZVI and GAC on in situ sedi-
ment total Hg (THg) and MeHg concentrations, and on pore-water
MeHg concentrations. Additional microcosm experiments were
conducted to study the effect of these amendments on the uptake
of MeHg by a freshwater snail (Lymnaea stagnalis).
2. Materials and methods
2.1. Materials
Zero-valent iron was obtained from Connelly-GPM, Inc. (Chi-
cago, IL), and sieved to <2 mm before application to ensure high
surface area. GAC was mix coal/coconut powder, obtained from
Siemens Industry Inc., USA, and used as received. Table S1 shows
the particle size distribution for the ZVI and GAC. All other chem-
icals were trace metals grade.
2.2. Site description
This field study was conducted at a fringing wetland of Hodgdon
Pond (Tremont, Maine, USA; Fig. S1), located on the western border
of Acadia National Park on Mount Desert Island. This pond has a
surface area of 18.2 ha, a perimeter of 3300 m and reaches a
maximum depth of 6.7 m. Fish (pickerel) in Hodgdon Pond had an
average Hg body burden of 1.4 ppm, one of the highest concen-
trations among 125 studied lakes and ponds in Maine (Linda Bacon,
personal communication, 2014). The pond's eastern shore is part of
Acadia National Park and the western shore is privately owned
residential land. There are several fringing wetlands and other
wetlands in the pond's catchment (Nielsen, 2006). The southern
fringing wetland, where this study was conducted, is dominated by
grass and sedge vegetation. Water temperature and relative water
level in the lake during the sampling period are shown in Fig. S2.
There is no known point source of Hg contamination for this
pond; as such, Hg within the pond is derived almost exclusively
from atmospheric deposition. The high fish Hg body burden in
Hodgdon Pond is thought to be a result of conditions that are
conducive to high Hg(II)-methylation rates in this ecosystem,
namely the presence of wetlands.
2.3. Field mesocosms
Twelve mesocosms were established along an 18 m transect on
the waters edge of the southern fringing wetland of Hodgdon Pond
on 8/12/2013 (Fig. S3). Care was taken to locate the mesocosms
such that they contained a similar mass of the same plant material.
Mesocosms were isolated in the wetland by driving a ~38 cm
diameter ~39 cm long PVC pipe to a depth of ~15 cm. Treatments
367
were randomly assigned such that four mesocosms received ZVI (at
5
estimated sediment total Fe in the top 3 cm), four received GAC
(at 1.7% estimated sediment dry weight in the top 0e3 cm interval)
and four were left untreated. In the pristine environment of a Na-
tional Park, any amendments to the sediment should have minimal
effects on the background geochemical characteristics and on bio-
logical activity of the native flora and fauna. Therefore, the ZVI
concentration was based on preliminary experiments in which a
range of ZVI concentrations (5e50
native sediment acid-soluble
Fe) were added to the top 3 cm of homogenized wetland sediment
(Lewis, 2014). The results showed that the lower end ZVI dosage
had the least effect on pore-water chemistry, especially with
respect to pH and Fe(II) concentrations, while lowering the pore-
water MeHg concentration; in the top ~4 cm, the pore-water pH
ranges were 5.6e5.8, 5.8e6.0, and 6.3e6.5 for the control, 5
and
50
ZVI, respectively, and the pore-water Fe(II) ranges were
43e53, 80e83, and 229e269 mM for the three treatments,
respectively. The added GAC concentration was close to the lowest
concentration used in a recent study by Gilmour et al. (2013) on Hg
remediation of contaminated sediment. The ZVI and GAC were
gently mixed into the surface sediment (top ~0e3 cm interval for
~3 min) of the mesocosms using a plastic spoon taking care not to
damage the plants; the surface sediment of the reference treat-
ments was also similarly mixed. The water level was ~4 cm above
the sediment surface when the mesocosms were installed (Fig. S2).
Sediment samples were collected as a composite of 3e5 samples
from the top 0e3 cm of sediment immediately before treatment
applications in August (8/12/2013), and 25 days on September (9/6/
2013), and 91 days on November (11/11/2013) after treatment ap-
plications. Samples were flash frozen in the field using dry ice until
analysis; prior to analysis, they were thawed, homogenized and
freezeedried.
Pore water was sampled in two mesocosms of each treatment in
September and November. Equilibrium dialysis samplers (peepers)
were used to sample pore water. Peepers are acrylic frames with
5 mL cells on 1.5 cm centers and 0.45 mm Tuffryn HT polysulfone
(Gelman Sciences dialysis membranes). Peepers were assembled in
the laboratory and bubbled with N2 for two weeks prior to
deployment. They were modified with fittings to allow for in situ
pore water collection without having to withdraw the peepers and
disturb the sediment. Pore-water samples were withdrawn twice
from the peepers; the first draw of >3 mL was allocated to ancillary
chemistry (including Fe(II), hydrogen sulfide and dissolved organic
carbon; Table S2) and the second was allocated to MeHg analysis;
total Hg was not analyzed in field samples due to the low sample
volume. Following collection, pore-water samples collected for
MeHg analysis were transferred into pre-weighed falcon tubes and
kept on ice in the dark. Upon return to the lab, samples were pre-
served with 0.5% HCl (final concentration) by weight and frozen
until analysis.
2.4. Laboratory microcosms
Twelve microcosms were established in 1 gal glass aquaria. The
aquaria were established using intact sediment clumps containing
macrophytes collected on 10/14/2013 from the same wetland
where mesocosms were installed. Care was taken to establish mi-
crocosms so that they all had approximately the same amount of
sediment and plants. Microcosms were maintained at room tem-
perature with overlying water from Hodgdon Pond at a depth of
8e10 cm (Fig. S4). Similar to the field mesocosms, treatments were
assigned randomly with four for each treatment (ZVI or GAC) and
four untreated microcosms; added ZVI mass was similar to that in
field mesocosms, and GAC was added at 1.0% estimated sediment
dry weight in the top 0e3 cm interval. Peepers were inserted in two
368 A.S. Lewis et al. / Environmental Pollution 212 (2016) 366e373

microcosms of each treatment and untreated sediment; ZVI and
GAC were added four days after collection on 10/18/2013.
Sediment from the microcosms was sampled 121 days after
application of treatments on 2/20/2014 as described above; pore-
water samples were collected on that day (post-treatment) using
peepers as described above. Pore-water volume was sufficient for
analysis of both THg and MeHg. After MeHg analysis, pore-water
samples were oxidized with 0.5 mL bromine monochloride for
THg analysis.
2.5. Lymnaea stagnalis
On 2/7/2014, 108 days after application of treatments, ten Great
Pond Snails (L. stagnalis; ~10e15 mm in length) were added to each
microcosm. Upon the addition of the snails, the microcosms were
covered with breathable plastic wrap (Saran) to prevent escape.
L. stagnalis were raised from eggs to a length of approximately
10e15 mm, in synthetic moderately hard water (USEPA, 2002) on a
diet of romaine lettuce, prior to incubation in the microcosms. This
species was chosen as a test organism because of their vast natural
range, flexible detritus and periphyton diet, and ease of non-
destructive sampling.
On 3/20/2104, after an exposure period of 41 days, L. stagnalis
were removed from the aquaria, frozen wet and subsequently
removed from their shells. Prior to analysis, the snails from each
microcosm were freeze dried, composited and homogenized by
grinding manually with an acid cleaned spatula inserted into the
falcon tube.
2.6. Mercury and methylmercury analyses
three months (November) after the treatments. There were no
significant differences in sediment concentrations of THg
(p ¼ 0.249) or MeHg (p ¼ 0.157) among mesocosms in August, prior
to the ZVI and GAC treatment applications (Fig. 1). For all sampling
dates, sediment THg ranged from 76 to 131 ng g1 dw (Fig. 1a). Using
repeated measures analysis, date was found to be a significant
factor for variation in sediment THg (Table 1). Post hoc Tukey's HSD
determined that November sediment THg was significantly higher
than those in September and August. The highest mean sediment
THg concentration for the aggregate of all treatments (109.0 ng g1 dw)
occurred in November compared to September (101.8 ng g1 dw), and
August (98.4 ng g1dw) (Fig. 1a).
In the field mesocosms, sediment MeHg concentrations for all
dates ranged from 1.98 to 8.25 ng g1 dw (Fig. 1b). Using repeated
measures analysis, date was found to be a significant factor for
variation in sediment MeHg (Table 1). November sediment MeHg
concentrations were found to be statistically lower than sediment
MeHg in August and September using post hoc Tukey's HSD. Higher
mean sediment MeHg concentrations for all treatments were
observed in August (5.43 ng g1 1
dw) and September (6.02 ng gdw) than
1
in November (3.12 ng gdw). There was no significant difference in
sediment MeHg from August to September. Over this time span the
mean sediment MeHg concentrations increased by 0.05, 1.00, and
0.70 ng g1dw for the control, ZVI-treated and GAC-treated meso-
cosms, respectively.
140
(a) Sediment THg Ctrl
GAC
130 ZVI

Freeze-dried sediment and tissue total Hg was analyzed

120
following the EPA method 7473 using a Milestone DMA-80 that
THg (ng gdw-1)

employs thermal decomposition, amalgamation, and detection

110
using atomic absorption. The method detection limit (MDL) for this
instrument is 50 ng g1.
100
Pore-water total Hg analyses were carried out following the EPA
method 1631 using the cold vapor atomic fluorescence spectros-
90
copy techniques (CVAFS; Tekran 2600). The MDL for this was
2.2 ng L1.
80
Pore-water MeHg was analyzed using a Tekran 2700 and
L. stagnalis tissue MeHg using a Brooks Rand MERX. Pore-water
70
MeHg samples were distilled prior to analysis. Sediment and tis- 10
sue MeHg were extracted using 25% KOH in MeOH in a 60  C oven for (b) Sediment MeHg Ctrl
4 h. All MeHg samples were ethylated, purged onto Tenex traps, GAC
ZVI
separated using GC, and detected using CVAFS following EPA 8
method 1630. The MDL values for these samples were sample spe-
cific, and are not reported. Any result below the MDL is reported as
MeHg (ng gdw-1)

<X, with X being the MDL for that sample, in the SI section (Table S2). 6

2.7. Statistical analysis

4

Differences among the field mesocosms were assessed using

repeated measures analysis and post-hoc Tukey's HSD with p-
2
values 0.1. Differences among treatments in the laboratory mi-
crocosms were assessed by analysis of variance (ANOVA), with p-
values 0.1 and post-hoc Tukey's HSD using JMP 12 (SAS Institute 0
Inc.). Aug Sept Nov
Pre-treatment
Sampling Date
3. Results
Fig. 1. (a) Sediment THg and (b) MeHg concentrations in the field mesocosms as a
3.1. Field mesocosms function of time and treatment. The August data represent the pre-treatment, and
September and November data represent post-treatment conditions. Each bar repre-
sents the average concentration for each treatment, and the error bars indicate one
Sediment was sampled from field mesocosms before the treat- standard deviation. The individual data points represent concentrations in each mes-
ments (August), and approximately one month (September) and ocosm (four per treatment).
 A.S. Lewis et al. / Environmental Pollution 212 (2016) 366e373
Table 1
p-values of analyzed parameters as they are affected by date and treatment for the
field mesocosms. p-values represent between-subject factors of repeated measures
analysis of variance.
Date Treatment Date
treatment
Degrees of freedom 2 2 4 November.
Sediment THg 0.0029 0.2849 0.1944
Sediment MeHg <0.0001 0.5325 0.1113
MeHg:THg ratio <0.0001 0.9246 0.2383
Given the small sample size for the field mesocosm pore-water
MeHg measurements (i.e., two peepers per treatment), we
considered the relative mean concentrations for each treatment
versus the control instead of attempting statistical analysis. Pore-
water non-detectable values were substituted with half the mini-
mum detection limit as reported in the SI section (Table S2). Field
mesocosm pore-water data are presented as the average of samples
taken at four depths (~1, 3, 5, and 7 cm below sediment-water
interface; Fig. S5). We observed a higher mean pore-water MeHg
concentration in the control (2.08 ± 1.36 ng L1) than either GAC-
(0.65 ± 0.48 ng L1) or ZVI- (1.21 ± 0.85 ng L1) treated mesocosms
in September (Fig. 2). The reported numbers are the means of all
eight sampling ports of each treatment, that is two peepers per
treatment at four depths ± the pooled standard deviation. We also
observed a seasonal reduction in the average pore-water MeHg
concentration in the control mesocosms from September
(2.08 ± 1.36 ng L1) to November (0.72 ± 0.35 ng L1) (Fig. 2). The
November pore-water MeHg concentrations for the GAC- and ZVI-
treated mesocosms were 0.44 ± 0.31 and 0.79 ± 0.62 ng L1,
respectively.
A higher average pore-water Fe(II) concentration was observed
in the control than either GAC or ZVI mesocosms in September
(Fig. S6). The high average Fe(II) concentration in the control
mesocosms was due to the especially high concentrations in one
mesocosm (Table S2b). A higher average pore-water DOC concen-
tration was also observed in the control than either GAC or ZVI
mesocosms in September; this difference was brought about by
high concentrations in the same mesocosm (Fig. S7). In the control
mesocosms, pore-water Fe(II) and DOC concentrations correlated
strongly (r2 ¼ 0.95); such correlations were not observed for the
GAC and ZVI mesocosms. All mesocosms showed a seasonal
6
Pore water Ctrl
GAC
5 ZVI
4
MeHg (ng L )
-1
3 respectively. No correlations were observed between pore-water
2
1
0 The field mesocosm results are complicated by the effects of
September November
Sampling Date
Fig. 2. Pore-water MeHg concentrations in the field mesocosms as a function of time
and treatment. Each bar represents the average concentration for each treatment, and
the error bars indicate one standard deviation. The individual data points represent
concentrations in individual peeper cells (four per peeper) in each mesocosm (two per
treatment, shown as open and filled circles).
369
reduction in the average pore-water Fe(II) and DOC concentrations
from September to November (Figs. S6 and S7). No significant dif-
ferences in average pore-water S(-II) concentrations were observed
among mesocosms in September (Fig. S8); the average concentra-
tions did not diminish in any treatments from September to
3.2. Laboratory microcosms
In the laboratory microcosms, sediment THg and MeHg con-
centrations were in the range of 83e112 and 2.09e6.63 ng g1 dw,
respectively (Fig. 3a). Both concentrations were analyzed using
ANOVA, and no significant differences were found in sediment THg
(p ¼ 0.272) or sediment MeHg (p ¼ 0.202) between treated mi-
crocosms and controls.
Laboratory microcosm pore water was only sampled at one
depth (~2 cm below sediment-water interface). The mean pore-
water THg concentrations were 7.18 ± 1.00, 5.25 ± 1.12 and
10.11 ± 2.09 ng L1 in the two control, ZVI-treated, and GAC-treated
microcosms, respectively (Fig. 3b). The mean pore-water MeHg
concentrations were 4.00 ± 1.32, 2.48 ± 0.52 and 3.05 ± 0.14 ng L1
in the two control, ZVI-treated, and GAC-treated microcosms,
respectively (Fig. 3b). The reported numbers are the means of two
microcosms sampled at one depth ± one standard deviation. The
mean pore-water MeHg:THg ratios were 0.55, 0.49, and 0.31 in the
two control, ZVI-treated, and GAC-treated microcosms, respec-
tively. The observed pore-water MeHg concentrations and the
MeHg:THg ratios in the two control mesocosms were similar to
those reported in other freshwater stream and lake sediment pore-
water systems (Hines et al., 2004; Marvin-DiPasquale et al., 2009;
Chalmers et al., 2013).
The differences in the THg in snail tissues were found to be non-
significant using ANOVA (p ¼ 0.320). The differences in snail tissue
MeHg concentrations (Fig. 3c), however, were found to be signifi-
cant using ANOVA (p ¼ 0.045). Subsequent Tukey's HSD deter-
mined that the tissue MeHg from snails in control mesocosms
(103.1 ± 44.7 ng g1 dw) was significantly greater than tissue from
snails raised in ZVI-treated mesocosms (41.8 ± 20.6 ng g1 dw;
p ¼ 0.047). Comparing snail tissue MeHg between GAC-treated
(64.6 ± 12.7 ng g1 dw) and control microcosms, Tukey's HSD
showed a p-value ¼ 0.110. The reported numbers are the means of
approximately 40 snails; ten per each of the four microcosms of
each treatment ± one standard deviation (Table S3).
The pore-water concentrations for Fe(II), S(-II) and DOC are
shown in Fig. S9. The average Fe(II) concentrations were higher in
the ZVI (660 mM) than in either the GAC (354 mM) or control
(569 mM) mesocosms. The average S(-II) concentrations, however,
were lower in the ZVI (6.0 mM) than in GAC (9.0 mM) or control
(8.1 mM) mesocosms. The average DOC concentrations in the con-
trol, GAC and ZVI mesocosms were 40.0, 40.3 ppm and 35.0 ppm,
MeHg and Fe(II), S(-II) and DOC concentrations.
4. Discussion
4.1. Seasonality in the field
seasonality. Maine is a temperate region of the USA with August
and September being substantially warmer and having higher plant
activity than November. By November the mesocosm plants had
visibly died back as they began senescence. We attribute the major
difference in sediment THg and MeHg, and pore-water MeHg in the
control mesocosms between summer (August and September) and
fall (November) (Figs. 1 and 2a) to the effects of seasonality (i.e.,
370 A.S. Lewis et al. / Environmental Pollution 212 (2016) 366e373

115 10 higher water temperature in summer; Fig. S2) and plant senes-
(a) Sediment cence. In November we observed overall lower sediment and pore-
110
8 water MeHg, as well as pore-water Fe(II) and DOC (Figs. S6 and S7),

)
-1
which we attribute to a decrease in microbial activity driven by the
)

105
-1

dw
dw

decrease in temperature in combination with plant senescence.

MeHg (ng g
6
TH g (n g g

100
Increased MeHg production in waters with high wetland inputs
95
4 have been documented extensively (Bowles et al., 2003; Cosio et al.,
2014; Regier et al., 2012; St. Louis et al., 1994; Tessier et al., 2007).
90
Windham-Myers et al. (2009) showed a positive correlation be-
2
85 tween the concentration of a plant exudate, acetate, and Hg(II)
methylation rate in the wetland rhizosphere. We similarly hy-
80 0
14 6
pothesize that plant activity may positively affect Hg(II)
(b) Pore water methylation through the influence of the redox cycle in the rhizo-
12 5 sphere and/or the production of labile carbon exudates that are
available as a food source to sediment microbes (Blossfeld et al.,

MeHg (ng L )
10

-1
TH g (n g L )

4 2011; Neubauer et al., 2005; Nikolausz et al., 2008; Revsbech

-1

8 et al., 1999).
3
6
The same seasonal reduction in our mesocosm sediment MeHg
2
concentrations is also observed in mesocosm pore-water MeHg
4 concentrations (Fig. 2). These results correspond to seasonal trends
1 observed in studies of pore-water MeHg in an Allequash Creek
2
wetland, Wisconsin, USA (Creswell et al., 2008), and a seepage lake
0 0 in Minnesota, USA (Hines et al., 2004); both studies observed the
180 180
(c) L. stagnalis tissue highest pore-water MeHg concentrations during the summer. The
160 160
authors of these studies also attributed the seasonal change in
140 140 pore-water MeHg concentrations to changes in plant activity.
)
-1
THg (ng gdw )
-1

dw

120 120
MeHg (ng g

100 100 4.2. Treatment effects on sediment and pore-water MeHg

80 80
We did not observe any statistically significant differences in
60 60
sediment MeHg due to ZVI and GAC additions in either field mes-
40 40
ocosms (Table 1) or laboratory microcosms (p ¼ 0.202). Gilmour
20 20 et al. (2013) observed an increase in sediment MeHg following
0 0 GAC application exceeding 4.8% of sediment dry weight to estua-
28000 2800 rine sediment, and at 5% of sediment dry weight to freshwater
(d) Partition coefficient sediment. At lower GAC application rates, they did not observe an
24000 2400
increase in sediment MeHg. The authors attributed this increase to
KD, MeHg (L kg )
-1
KD, THg (L kg )
-1

MeHg adsorption onto GAC reducing its availability for demethy-

20000 2000
lation. The GAC dosages used in our field mesocosms and labora-
16000 1600 tory microcosms were 1.7% and 1.0%, respectively, below a level at
which Gilmour et al. (2013) observed any significant increase in
12000 1200 sediment MeHg concentrations.
To our knowledge, ZVI has not been used for Hg remediation in
8000 800
wetland sediment. ZVI removes inorganic Hg(II) from water via
adsorption (Gibson et al., 2011; Vernon and Bonzongo, 2014;
4000 400
Weisener et al., 2005) involving the formation of HgeO bonds on
1.6 60
the Fe(III) (oxy)hydroxide species formed on the surface of ZVI
(e) Bioaccumulation factor
1.4 (Gibson et al., 2011). In the absence of dissolved oxygen, a layer of
50
1.2
mixed Fe(II)/Fe(III) oxide may be formed on ZVI surfaces (Huang
40 and Zhang, 2005) that can facilitate Hg(II) removal. Microbially-
BAF, MeHg
BAF, THg

1.0
mediated Hg(II) methylation may be inhibited by Hg(II) sorption
0.8 30 to ZVI; therefore, we might expect a reduction in sediment MeHg
0.6
following treatment with ZVI. However, we did not observe a sig-
20
nificant change in sediment MeHg in ZVI-treated compared to
0.4
control mesocosms and microcosms in this work, and believe that
10
0.2 this is a result of any adsorption being below the statistically sig-
0.0 0
nificant detectable levels relative to background concentrations.
Ctrl ZVI GAC The pore-water concentrations for both the September field
mesocosms (Fig. 2) and laboratory microcosms (Fig. 3b) show that
Fig. 3. Laboratory microcosm (a) sediment THg and MeHg concentrations, (b) pore- both ZVI and GAC reduce pore-water MeHg concentrations relative
water THg and MeHg concentrations, (c) L. stagnalis tissue THg and MeHg concen-
trations, (d) sediment-water distribution coefficients (KD) for THg and MeHg, and (e)
to the control. For the mesocosms in November (Fig. 2), no pore-
the bioaccumulation factor (BAF) for THg and MeHg. THg data are in squares on the left water MeHg reduction was observed among treatments, poten-
axis, and MeHg data are in triangles on the right axis. Square and triangle points tially due to a lack of plant and/or microbial activity.
represent individual mesocosm results;
represents the average result for the treat- The results of this study corroborate those of Gilmour et al.
ment and the bars are one standard deviation.
(2013) who observed a consistent decrease in pore-water MeHg
 A.S. Lewis et al. / Environmental Pollution 212 (2016) 366e373
concentrations in sediment treated with GAC, although this
decrease was not always statistically significant. Direct Fe(II)
addition to wetland sediment has also been shown to decrease
MeHg concentrations (Ullrich and Sedlak, 2010); ZVI is a source of
Fe(II).
The fact that there are no significant differences in sediment
MeHg concentrations between the control and the treated meso-
cosms and microcosms, but that there is reduction in pore-water
MeHg concentrations means that both ZVI and GAC likely
decrease the MeHg concentration via adsorption and not deme-
thylation or inhibition of Hg(II) methylation. GAC is a strong sorbent
and its effect on MeHg removal from water via adsorption is known
(Gomez-Eyles et al., 2013). However, ZVI can not only act as a sor-
bent, but is a significant source of Fe(II) that may inhibit MeHg
production via shifting the inorganic Hg(II) speciation (Mehrotra
and Sedlak, 2005), or reducing inorganic Hg(II) to Hg(0)
(Amirbahman et al., 2013). Our results suggest that net MeHg
production was probably not affected by ZVI since the MeHg
sediment concentration was not reduced following application of
ZVI. The reduction in pore-water MeHg concentration following
application of ZVI leads us to hypothesize that sorption was the
primary method of action for both ZVI and GAC in our experiments.
A higher KD value suggests an increased tendency for the species
to partition into the sediment; in many instances this leads to a
decreased bioavailability of that species. For the field mesocosms,
KD,MeHg (in L kg1) was calculated using the average pore-water
concentration (Fig. 4). In the field mesocosms, we observed a
lower mean KD,MeHg for the control (2900) than either ZVI (5700) or
GAC (8200) in September (Fig. 4). We also observed a weak but
significant correlation between pore-water MeHg and DOC
(r2 ¼ 0.359, p ¼ 0.002) in the field mesocosms, suggesting associ-
ation of MeHg with DOC; a higher average DOC concentration in the
control mesocosms (Fig. S7) contributes to the higher pore-water
MeHg concentration and lower KD,MeHg.
The same trend was also observed in the KD,MeHg values for
laboratory microcosms for the control (670), ZVI (1300) and GAC
(1800) (Fig. 3d). The increase in KD,MeHg values in treated compared
to control mesocosms and microcosms was effectively due to the
decrease in pore-water MeHg concentrations in treated sediment.
We hypothesize that the overall lower KD,MeHg observed in the
laboratory microcosms compared to the field microcosms may have
been due to higher pore-water MeHg cocentrations as a result of
Partition Coefficient
Ctrl
10000
GAC
ZVI
8000
KD, MeHg (L kg )
-1
6000
4000
2000
0
September November
Sampling Date
Fig. 4. Sediment-water distribution coefficients for MeHg (KD,MeHg) in the field mes-
ocosms as a function of time and treatment. Each bar represents the average KD,MeHg
values for each treatment calculated by averaging the KD,MeHg calculated from the
average pore-water MeHg from each mesocosms, and discrete data points represent
the KD,MeHg values calculated for each mesocosm using the average pore-water MeHg
concentration.
371
elevated temperatures in the microcosms that may have increased
microbial activity.
4.3. The effects of treatment on biotic uptake
The bioaccumulation factor (BAF) is defined as the tissue:sedi-
ment concentration ratio. BAF is used in many studies as an indi-
cation of how likely contaminants are to increase in tissues up a
trophic system (Bowles et al., 2001; Cosio et al., 2014; Gilmour et al.,
2013; Hammerschmidt et al., 2013; Harmon et al., 2005; Paller
et al., 2004). In the case of Hg, Lawrence and Mason (2001) found
in laboratory experiments that bioaccumulation is affected by fac-
tors such as sediment organic matter content and the organisms'
feeding methods. They also found that BAF is a more reliable in-
dicator of a system's toxicity with respect to Hg than other mea-
sures, such as sediment Hg concentration.
The BAFMeHg values (average ± one standard deviation) for the
control, ZVI- and GAC-treated microcosms were 34.0 ± 16.7,
16.0 ± 6.9 and 15.3 ± 4.3, respectively (Fig. 3e). These values were
analyzed using ANOVA and found to have significant differences.
Post hoc Tukey's HSD indicated that snails in ZVI- and GAC-treated
microcosms had significantly lower BAFMeHg than those in control
microcosms (p ¼ 0.093 and 0.072, respectively). The differences in
BAFTHg between treatments and control were not significant
(p ¼ 0.856).
The significant reduction in BAFMeHg in GAC-treated microcosms
agrees with the reduction observed in GAC-treated systems by
Gilmour et al. (2013), where they studied MeHg uptake by Lum-
briculus variegatus oligochaetes, even though our treatment (1.0%
GAC) is lower than the lowest treatment used in that study (2.4%
GAC). We observed a significant reduction in BAFMeHg in the GAC-
treated microcosms relative to the control, while we did not
observe a significant reduction in the snail tissue MeHg concen-
tration for GAC-treated microcosms relative to the controls. We
believe that this may have been due to a higher concentration of
sediment MeHg in one of the GAC-treated microcosms (Fig. 3a). We
are not aware of any previously published study on the role of ZVI in
MeHg uptake by biota.
The statistically significant reduction of BAFMeHg observed in
both GAC- and ZVI-treated microcosms relative to the control mi-
crocosms indicates that both treatments reduce MeHg uptake in
L. stagnalis. The snails served as an integrative way to sample the
microcosms over their deployment period, potentially resulting in
more representative data than the data provided by discrete sedi-
ment or pore-water sampling. The greatest bioaccumulative in-
crease of MeHg in the food chain takes place between water and
phytoplankton (Watras, 2009). Snails consume periphyton and
detritus, and are themselves consumed by higher trophic
organisms.
4.4. Correlation of MeHg partitioning and biotic uptake
Pore-water MeHg concentrations showed a positive correlation
to the snail tissue MeHg concentration (r2 ¼ 0.81, p ¼ 0.014; Fig. 5a).
This suggests that MeHg pore-water concentration may be a
reasonable measure of Hg toxicity to benthic macroinvertebrates,
such as L. stagnalis, with higher pore-water MeHg concentrations
corresponding to higher biological uptake. These data follow the
same trend observed by Gilmour et al. (2013) in L. variegatus oli-
gochaetes in GAC-treated microcosms.
The BAF is inversely correlated to the partition coefficient,
KD,MeHg (r2 ¼ 0.65; p ¼ 0.053; Fig. 5b). This suggests that the greater
the MeHg partitioning into the sediment (i.e., higher KD,MeHg) the
lower the MeHg uptake by L. stagnalis. These data follow the same
trend observed by Gilmour et al. (2013). In a study of Hg
372 A.S. Lewis et al. / Environmental Pollution 212 (2016) 366e373

160 addition, changes in sediment nutrient availability, etc.). However,

L. stagnalis tissue MeHg (ng/gdw)

the results of this study are promising and suggest that ZVI or GAC
140 application may be considered in the establishment of engineered
wetlands to reduce the potential negative impact of benthic MeHg
120
production.
100
Acknowledgments
80
r² = 0.81
60 p = 0.014 Funding for this work was provided by a grant from the USGS-
National Park Service Water Quality Partnership Program. Addi-
40 Ctrl tional funding was provided by the USGS-Toxics Program. Clive
GAC Devoy, Karen Small and the staff of the Sawyer Environmental
20
ZVI Chemistry Research Laboratory at the University of Maine, and
(a) Evangelos Kakouros, Michelle Arias, Le Kieu and Jennifer Agee of
0
2.0 2.5 3.0 3.5 4.0 4.5 5.0 the US Geological Survey (Menlo Park, CA) are acknowledged for
their help with sample analysis. Daniel Cain of the US Geological
pore-water MeHg (ng/L) Survey (Menlo Park, CA) provided the L. stagnalis eggs and advice
on their handling. William Halteman is acknowledged for his
50 advice on the statistical treatment of data. Upal Ghosh and three
r² = 0.65 anonymous reviewers provided valuable critiques of the
p = 0.053 manuscript.
40
Appendix A. Supplementary data
BAF (MeHg)

30
20
10
(b)
0 Benoit, J.M., Gilmour, C.C., Mason, R.P., Heyes, A., 1999. Sulfide controls on mercury
500 1000 1500 2000
KD,MeHg (L/Kg)
Fig. 5. Correlation between MeHg uptake and sediment water partitioning from the
laboratory microcosm experiments. (a) L. stagnalis tissue MeHg versus pore-water
MeHg, and (b) BAF versus KD,MeHg. Each data point represents an individual microcosm.
bioaccumulation by several benthic vertebrate and epibenthic
macroinvertebrate species, Chen et al. (2009) observed a significant
inverse correlation between the BAF and sediment organic carbon
concentration. Their results are consistent with ours, given that
sediment organic carbon and KD,MeHg are strongly correlated
(Hammerschmidt and Fitzgerald, 2004). Interestingly, among the
species studied by Chen et al. (2009) was an omnivore fish (Fun-
dulus heteroclitus) whose Hg body burden was dependent on
sediment Hg partitioning. In the context of our study, this may be
interpreted as any remedial strategy that increases KD,MeHg can
result in a lower fish Hg body burden.
5. Conclusions
This work finds that sediment treatment with ZVI and GAC can
reduce the pore-water MeHg concentration in wetland sediment
containing active plants, leading to greater MeHg partitioning to
sediment. The dominant mechanism for this reduction in pore-
water concentration is likely MeHg adsorption and not inhibition
of Hg(II) methylation or MeHg demethylation. The reduction in
pore-water MeHg concentration resulted in lower MeHg uptake by
L. stagnalis. More study is needed to determine the longevity of a
given ZVI or GAC application, and if there are any negative chemical
and biological consequences associated with large-scale applica-
tions of either of these treatments (e.g., pH increase due to ZVI
Supplementary data related to this article can be found at http://
dx.doi.org/10.1016/j.envpol.2015.11.047.
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