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ABSTRACT: Mercury is a naturally occurring metal found in air, water and soil.
Mercury exists in any of three valence states: Hg0 (elemental mercury), Hg2+2 (mercurous
mercury) and Hg+2 (mercuric mercury). These forms can be organized under three
headings: metallic mercury, inorganic mercury, and organic mercury. Metallic mercury is
present at liquid state in room temperature, and is used in thermometers and some
electrical switches. Inorganic mercury compounds occur when mercury combines with
elements such as chlorine, sulfur, or oxygen. These mercury compounds are also called
mercury salts. Most inorganic mercury compounds are white powders or crystals, except
for mercuric sulfide (also known as cinnabar), which is red and turns black after exposure
to light. Organic mercury compounds (or organomercurials) occur when mercury
combines with carbon. In the environment there is a large number of organic mercury
compounds; however, by far the most common organic mercury compound in the
environment is methyl mercury (or MeHg+). Methyl mercury is of particular concern
because it can build up in certain edible freshwater and saltwater fish and marine
mammals to levels that are many times greater than levels in the surrounding water.
INTRODUCTION
Mercury has been well known as an environmental pollutant for several decades. As
early as the 1950’s it was established that emissions of mercury to the environment could
have serious effects on human health. These early studies demonstrated that fish and
other wildlife from various ecosystems commonly attain mercury levels of toxicological
concern when directly affected by mercury-containing emissions from human-related
activities. Mercury in the air may settle into water bodies and affect water quality. This
airborne mercury can fall to the ground in raindrops, in dust, or simply due to gravity
(known as “air deposition”). After the mercury falls, it can end up in streams, lakes, or
estuaries. Over time, the mercury mostly precipitates to the red mineral cinnabar, HgS,
which is responsible for soil contamination. With the aid sulfate-reducing bacteria (SRB)
or iron-reducing bacteria (IRB), the cinnabar is converted to methyl mercury under
anaerobic and acidic conditions, which are typical of the well-buried muddy sediments of
rivers, lakes, and oceans. SRB and IRB use sulfur rather than oxygen as their cellular
energy-driving system.
HgS(s) ⎯SRB
⎯/⎯
IRB
⎯→ CH 3 Hg(II)X (aq ) + H 2 S(g )
Where X is a ligand (an ion, a molecule, or a molecular group that binds to another
chemical entity to form a larger complex), typically Cl- or OH-, are the most toxic forms.
Upon methylation,
€ the SRB transport the new mercury complex back to the aquatic
environment, where it is taken up by other microorganisms. The conversion of inorganic
mercury to methyl mercury is important for two reasons:
(1) Methyl mercury is much more toxic than inorganic mercury.
(2) Organisms require a considerably longer period to eliminate methyl mercury.
At this point, the next higher level in the food chain may consume the methyl mercury-
containing bacteria, or the bacteria may release the methyl mercury to the water where it
can quickly adsorb to plankton. Plankton may also be consumed by the next level in the
food chain, or after dying, settle to the bottom of the lake and are incorporated into
bottom sediments. Studies of sediment cores show that younger sediments deposited
since industrialization have mercury concentrations that are about 3-5 times that of
historical sediments.
Mercury in aquatic environment
Most of the mercury entering aquatic environments is Hg+2. Methyl mercury
accumulates in fish at levels that may harm the fish and the other animals that eat them
via bioaccumulation and biomagnification. Bioaccumulation is the process by which
organisms (including humans) can take up contaminants more rapidly than their bodies
can eliminate them, thus the amount of mercury in their body accumulates over time. If
for a period of time an organism does not ingest mercury, its body burden of mercury will
decline. However, if an organism continually ingests mercury, its body burden can reach
toxic levels. The rate of increase or decline in body burden is specific to each organism.
Biomagnification is the incremental increase in concentration of a contaminant at each
level of a food chain. This phenomenon occurs because the food source for organisms
higher on the food chain is progressively more concentrated in mercury and other
contaminants, thus magnifying bioaccumulation rates at the top of the food chain. The
bioaccumulation effect is generally compounded the longer an organism lives, so that
larger predatory fish will likely have the highest mercury levels. In addition, unlike
organic contaminants (such as dioxin and PCBs) that concentrate in the skin and fat
tissues, mercury concentrates in muscle tissues. This implies that mercury cannot be
filleted or cooked out of consumable fish. Figure 1 illustrates the aquatic mercury cycle.
In the reactions above, under light of wavelength of 254 nm light, elemental mercury
is excited in reaction (1). The excited mercury reacts with oxygen in reaction (2) to
€
produce elemental mercury and an oxygen molecule in an excited state. The species
responsible for oxidation of elemental mercury are formed in reactions (3) and (4)
through the reaction of excited state oxygen with oxygen to form ozone and oxygen
radical, which also reacts with oxygen to form ozone. Both ozone and oxygen radicals
react with elemental mercury to form mercuric oxide (HgO) as shown in (5) and (6).
Most of the mercuric oxide is formed through the thermal reaction with ozone. The
overall reaction is obtained by adding reactions (1) through (5):
583 500
Melting Point (0C) -38.87 277 sublimation decomposition - 170
Water Solubility
(g/L) 56.1*10-6 66 2*10-24 5.3*10-2 2.95 <0.1
Atomic Properties:
Formal Oxidation Number: +1 +2
Electronegativity: 1.9 (Pauling scale)
Atomic radius / pm: 150.3
Covalent radius / pm: 132±5
Van der Waals radius / pm: 155±5
Physical Properties:
Phase at room temperature: Liquid
Appearance: Silver-white, heavy, mobile, liquid metal. When heated it becomes a
colorless, odorless gas.
Odor: Odorless
pH: No information found
Melting point / °C: -38.83
Boiling point / °C: 356.73
Critical point / °C: 1476.85
Density / g*cm-3: 13.55 (293 K)
Molar volume / cm3*mol-1: 14.81 (293 K)
Electrical resistivity / μ*Ω*cm: 95.8 (20 °C)
Speed of sound / m/s: 1451.4 (liquid, 20°C)
Thermal Properties:
Thermal conductivity / W m-1K-1: 8.34
Thermal expansion / µm m-1K-1: 60.4 --> constant rate over wide temperature range, thus
is used in thermometers and barometers
Heat of fusion / kJ mol-1: 2.331
Heat of vaporization / kJ mol-1: 59.11
Heat of atomization / kJ mol-1: 64.463
Ionization Energy:
1st ionization energy / kJ mol-1: 1007.07
2nd ionization energy / kJ mol-1: 1809.69
3rd ionization energy / kJ mol-1: 3299.82
Isotopes:
Isotope Relative atomic mass Mass percent Stable with
196
Hg 195.965815(4) 0.15(1) 116 neutrons
198
Hg 197.966752(3) 9.97(8) 118 neutrons
199
Hg 198.968262(3) 16.87(10) 119 neutrons
200
Hg 199.968309(3) 23.10(16) 120 neutrons
201
Hg 200.970285(3) 13.18(8) 121 neutrons
202
Hg 201.970626(3) 29.86(20) 122 neutrons
204
Hg 203.973476(3) 6.87(4) 124 neutrons
Dissolved Hg0 in cloud droplets is oxidized by O3, hydroxyl radical (HO•) and
chlorine (HOCl/OCl−), leading to the formation of Hg+2 in rain or cloud water, which may
then be removed from the atmosphere on shorter time scales due to the increase in water
solubility. After oxidized by Ozone, elemental mercury in cloud droplets mainly forms
HgO(aq), which reacts further to divalent mercury, Hg2+2 or Hg+2. Another oxidant of
potential significance is OH(aq), which is also capable of oxidizing elemental mercury in
cloud droplets to divalent mercury. A modeling study involving known atmospheric
reactions of mercury concluded that the two most important oxidation reactions of
elemental mercury in aqueous phase involve hydroxyl group (OH) in daytime and
chlorine atom (Cl) at nighttime.
Anthropogenic mercury emission has been a global issue, forcing the leading countries
to innovate new technologies in order to reduce the environmental effect resulted to
aquatic environments. In Canada, anthropogenic mercury emissions were reduced from
approximately 32 to 8 metric tons from 1990 to 2000. The largest source of mercury prior
to 1995 was base metal mining industry. From 1995 to 2000, electricity generation and
metal smelting were equally the largest sources of mercury into the atmosphere, each
accounting for 25% of Canadian emissions. In the US, emissions of mercury to the air
from anthropogenic sources have fallen by more than 45% since passage of the 1990
Clean Air Act Amendments, which provided new authority to EPA to reduce emissions
of mercury and other toxic pollutants to the air (U.S. EPA, 2006). Figure 8 shows the
anthropogenic mercury emissions in the US over the past decade.
Figure 8. U.S. anthropogenic mercury emissions over past decades (U.S. EPA, 2006)
Anthropogenic emissions from a number of major sources have been estimated to be
decreasing in North America and Europe due to reduction efforts during the last decade,
while the anthropogenic emissions from some developing countries have been increasing
dramatically over past ten years (Figure 9). In recent years, Asia was the biggest
anthropogenic mercury emission region, accounting for about 52% of the global
anthropogenic emission.
Hg0 measurements
The gaseous elemental mercury vapor exits in the largest portion in the atmosphere
(95-99%), making the measurement techniques crucial to protect the welfare of the public
and the environment. Measurements of elemental mercury are conducted by using CEMS
(continuous emission monitoring systems) as of the beginning of the third millennia. The
measurement of elemental mercury is done by “gold trap”. Gold traps consist of a wafer
thin ceramic tube, which has been carefully crafted to achieve minimum thermal inertia.
The tube has been packed with pure gold and supports a heating coil on its outside. The
mercury gold trap reveals sharp and high peaks and an excellent long-term stability. As
air is used for purging the trap during the heating step, possible contaminations are
oxidized and swept off thus preventing from passivation.
The primary reason why gold traps work is because mercury sticks to gold at room
temperature. A flue gas used in the measurement of elemental mercury is carrying
gaseous mercury (mostly elemental mercury and mercuric chloride). In order to convert
the other mercury species into an elemental form, there is a use in thermo-catalytic
converter that uses wet chemical reactions that converts mercuric chloride to elemental
mercury vapor. Commonly used reagents to accomplish the conversion to elemental
mercury were Stannous Chloride, Sodium Tetrahydroborate and Ascorbic Acid. Due to
the presence of reactors and tubings associated with wet chemistry, first generations of
the CEMS suffered from problems related to tubing pluggage, corrosion and inefficient
conversion of mercuric chloride to mercury.
Once solely elemental mercury is present in the flue gas (typically between 50C and
0
35 C), it is then pulled through the trap, the gas continues to flow through the trap but the
mercury stays behind since it got trapped on the gold. After the mercury is captured, the
gold trap is rapidly heated to approximately 2000C. As a result, the mercury is released as
a gas (thermal desorption). The gaseous mercury is then swept by the flow of purified
mercury free air (composed of a very high content of nitrogen gas) into the optical cell of
the detector, which measures the mercury in a UV Atomic Absorption Spectrometry
(AAS) operating at 253.7 nm.
It is essential that the trap is free of mercury before sampling. This is ensured by a
cleaning step, which is automatically performed. To keep particles out of the system and
to protect the trap from passivation, an easily replaceable filter is installed upstream the
sample inlet. The filter is made of low-interactive material; the filter membrane has a
porosity of 0.45 µm and is made of PTFE. It is possible to control sample volume based
on the expected mercury concentration. An illustration of the measurement of elemental
mercury is shown in figure 10.
Figure 13. Global anthropogenic emission of atmospheric mercury in 1990 (Dastoor and
Larocque, 2003)
The three major source areas are Europe, China and North America but, There are also
significant emissions in South Africa. The total global anthropogenic emission for 1990,
according to EPA, was 1881 tons/year which approximately 33% was from Europe, 38%
from China and Japan and 14% from North America. More recent global emissions are
being compiled and they show that the geographical distribution is changing. However,
the total global emissions of atmospheric mercury are not declining. Figure 14 shows the
distribution of the total gaseous mercury on the surface in 1997 at the North Hemisphere
(NH), the South Hemisphere (SH) and globally.
Figure 14. Monthly mean total gaseous mercury surface average air concentrations in
1997 (Dastoor and Larocque, 2003)
Figure 14 shows an average seasonal cycle in Northern and Southern Hemispheres with
higher concentrations in fall and winter due to the increase in coal combustion to provide
electricity and heat. Conversely, during the spring and summer there are lower
concentrations, as the weather gets warmer.
From table 2 previously presented, the major anthropogenic sources of atmospheric
mercury were medical waste incineration (26%), municipal waste collection (22%),
electric utility boilers (22%) and power & heat generation plants (13%). Figures 14-16
illustrate the emission of elemental mercury, RGM and particulate mercury into the
atmosphere across the US in 1990, respectively:
Figure 13. Elemental mercury emissions (tons per year) from anthropogenic sources at
the US in 1990 (EPA: 1997)
Figure 14. Reactive gaseous mercury emissions (tons per year) from anthropogenic
sources at the US in 1990 (EPA: 1997)
Figure 15. Particulate mercury emissions (tons per year) from anthropogenic sources at
the US in 1990 (EPA: 1997)
From observation of figures 13, 14 and 15, it is evident that the eastern side of the US
contains more point sources of atmospheric mercury emission. This is due to the presence
of coal-burning power plants that generate electricity that are mostly at the northeastern
side of the US. Most of the emission of reactive gaseous mercury and particulate mercury
are due to medical waste incineration facilities and municipal waste collections.
The EPA model, IEM-2M, was presented to the congress in 1997. The model divided
the US into Western and Eastern halves along the line of 90 degrees west longitude. IEM-
2M is composed of two integrated modules that simulate mercury fate using mass
balance equations describing watershed soils and a shallow lake. The results of these
terrestrial and aquatic models were used to predict mercury exposure to hypothetical
humans through inhalation, consumption of drinking water, and ingestion of soil, farm
products (e.g., beef products and vegetables), and fish. These models were also used to
predict mercury exposure in hypothetical fish-eating birds and mammals through their
consumption of fish. The model compared pre-industrialized atmospheric mercury
emission with industrialized ones. It was estimate that pre-industrial (starting
approximately around the 17th century) atmospheric mercury levels were roughly one
third of current levels. Table 3 presents the inputs to the IEM-2M models on both the
Western and Eastern sides of the 90 degrees west longitude, comparing the emission of
mercury from the pre-industrial and the industrial eras. Once the input to the model has
been inserted, an atmospheric model for mercury transportation can be made.
Table 3. Inputs to IEM-2M model obtained from atmospheric mercury measurements
As expected, once the industrial era started, all measurement parameters across the US
have increased considerably. From the atmospheric modeling analyses of mercury
deposition and on a comparative basis, a facility located in a humid climate has a higher
annual rate of mercury deposition than a facility located in an arid climate. Precipitation
removes various forms of mercury from the atmosphere and deposits mercury to the
surface of the earth. Of the species of mercury that are emitted, divalent mercury is
predicted to generally deposit to local environments near sources. Elemental mercury is
predicted to generally remain in the atmosphere for longer periods until atmospheric
conversion to divalent species occurs.
Given the simulated deposition efficiencies for each form of mercury air emission
(elemental mercury – 1%, divalent mercury vapor – 70%, and particulate mercury – 38%)
the relative source contributions to the total anthropogenic mercury deposited to the
continental U.S. are strongly and positively correlated to the mass of emissions in
oxidized form. This oxidized mercury occurs in both gaseous (Hg+2) and particulate (Hgp)
forms. While coal combustion is responsible for more than half of all emissions of
mercury in the inventory of U.S. anthropogenic sources, the fraction of coal combustion
emissions in oxidized form is thought to be less than that from waste incineration and
combustion. The true speciation of mercury emissions from the various source types
modeled is still uncertain and is thought to vary, not only among source types, but also
for individual plants as feedstock and operating conditions change. With further research,
it may be possible to make a confident ranking of relative source contributions to
mercury deposition in the continental U.S. Table 4 shows a comparison of mercury
concentrations between rural and urban areas.
Table 4. Summary of measures mercury concentrations in rural and urban areas
Table 4 shows that the measured U.S. atmospheric mercury concentrations are generally
very low. The dominant form in the atmosphere is vapor-phase elemental mercury,
although close to emission sources, higher concentrations of the divalent form may be
present due to its strong ability to dissolve in water. Small fractions of particulate
mercury and methyl mercury may also be measured in ambient air. The formation of
methyl mercury in the atmosphere still remains a great unknown. In rural areas, airborne
particulate mercury is typically 4% or less of the total (particulate + gas phase) mercury
in air
From the modeling analysis and a review of field measurement studies, it is concluded
that mercury deposition appears to be ubiquitous across the continental U.S. and at, or
above, detection limits when measured with current analytic methods. Due to the use of
atmospheric models to detect atmospheric mercury, it was discovered that of the total
amount of elemental mercury vapor that is emitted, about 1 percent (0.9 metric tons/yr)
may be atmospherically transformed into divalent mercury by tropospheric ozone and
adsorbed to particulate soot in the air and subsequently deposited in rainfall and snowfall
to the surface of the continental U.S. The vast majority of emitted elemental mercury
does not become part of the global mercury cycle due to the fact that it does not diffuse
vertically to the free atmosphere. However, nearly all of the elemental mercury vapor
emitted from other sources around the globe also enters the global cycle and can be
deposited slowly to the U.S. Over 30 times as much elemental mercury vapor is deposited
from these other sources than from stationary point sources and area sources within the
U.S.
ENVIRONMENTAL FATE OF ATMOSPHERIC MERCURY
Mercury is emitted to the environment by both anthropogenic and natural processes.
Due to its chemical properties, mercury is thought to move through various
environmental compartments, possibly changing form and species during process.
Mercury, like other elements such as nitrogen, sulfur and carbon, has a cycle that
describes its environmental fate. The mercury cycle has been studies by many scholars
over the years, and the understanding of it continues to undergo refinement. The
movement and distribution of mercury in the environment can be confidentially described
in general terms, since not all its details are agreed due to lack of information. Currently
it is estimated that about half of total anthropogenic mercury emissions eventually enter
the global atmospheric cycle. The remainder is removed through local or regional cycles.
An estimated 5 to 10 percent of primary RGM emissions are deposited within 100 km of
the point of emission and a larger fraction on a regional scale. Elemental mercury that is
emitted may be removed on a local and regional scale to the extent that it is oxidized to
RGM. Some elemental mercury may also be taken up directly by plants and trees.
However, most elemental mercury that is not oxidized will undergo long-range transport
due to its insolubility in water. In general, primary RGM emissions will be deposited on a
local and regional scale to the degree that wet deposition processes remove the soluble
RGM. The wet and dry deposition phenomena will be discussed in this section. Figure 16
below illustrates the mercury cycle, illustrating the natural and anthropogenic sources of
mercury in the environment.
Henry’s law governs the gas-liquid equilibriums of mercury species. The Henry’s law
constant for elemental mercury is quite small in the atmosphere, which lowers its partial
pressure; therefore it can travel for long distances. Although elemental mercury is the
dominant constitute of atmospheric mercury, the cloud-water concentration of elemental
mercury in Henry’s equilibrium with gaseous elemental mercury range only from 1.3 to
5.3 ×10-14 M, which is relatively low compared to the total dissolved and absorbed reactive
gaseous mercury. In contrast, the Henry’s law constants for Hg(OH)2 and HgCl2 are 4 and
6 orders of magnitude bigger than that for elemental mercury. Solid mercury species are
not likely present in atmospheric water given the low atmospheric concentration of
mercury. The quantitative description of gas-solid equilibriums is rather limited due to
uncertain nature of atmospheric particles.
In the aqueous phase, mercury compounds often remain as not disassociated
molecules, and the reported solubility values reflect this. Most organomercurics are not
soluble and do not react with weak acids or bases due to the low affinity of the mercury
for oxygen bonded to carbon. Hydroxy methyl mercury, CH3HgOH, however, is highly
soluble due to the strong hydrogen bonding capability of the hydroxide group. The
mercuric salts vary widely in solubility. For example HgCl2 is readily soluble in water,
and HgS is as unreactive as the organomercurics due to the high affinity of mercury for
sulfur.
The phenomenon of re-emission of deposited mercury results most significantly from
the evasion of elemental mercury from the oceans. In this process, anthropogenically
emitted mercury is deposited to the oceans as reactive gaseous mercury and then reduced
to volatile elemental mercury and re-emitted. According to one estimate, this process
accounts for approximately 30% (10 Mmol/year) of the total mercury flux to the
atmosphere. The slow release of mercury from terrestrial sinks to freshwater and coastal
waters will likely persist for much longer, though, effectively increasing the lifetime of
anthropogenic mercury further. This may be particularly significant considering that
surface soils currently contain most of the pollution-derived mercury of the industrial
period. However, recently published studies indicate that mercury in soil may be reduced
and re-volatilized, in that the capacity of soils to isolate airborne mercury must be
reconsidered. Thus, re-emissions of anthropogenic mercury will contribute to long-term
influences on the global biogeochemical cycle for mercury.
By considering the current global mercury budget and estimates of the preindustrial
mercury fluxes, it was estimated that total emissions have increased by a factor of
approximately 4.5 since preindustrial times, which has subsequently increased the
atmospheric and oceanic reservoirs by a factor of 3. The difference is attributed to local
deposition near anthropogenic sources. Although the estimated residence time of
elemental mercury in the atmosphere is about 1 year, the equilibrium between the
atmosphere and ocean waters results in a longer time period needed for overall change to
take place for reservoir amounts. Therefore, by substantially increasing the size of the
oceanic mercury pool, anthropogenic sources have introduced long-term perturbations
into the global mercury cycle. Modeled results estimated that if all anthropogenic
emissions were ceased today, it would take about 15 years for mercury pools in the
oceans and the atmosphere to return to pre-industrial conditions. However, The Science
Advisory Board concluded that it could take significantly longer.
CONCLUSION
Mercury is an element that is naturally present in the environment. Mercury is
persistent pollutant that is released to the atmosphere mostly by coal-burning power
plants. Atmospheric mercury is characterized into three types: elemental, reactive
gaseous and particulate. Elemental mercury is insoluble in water and can be transported
for long distances, whereas the reactive gaseous form is highly soluble in water and as a
result lands in nearby areas to the pollution sources via wet deposition.
When enters to aquatic systems, mercury is transformed by sulfur and iron reducing
bacteria to an organic form – methyl mercury, the most toxic form of mercury. In aquatic
systems, fish eat different foods that were contaminated with methyl mercury, staying in
their body for long periods of time. Human consuming fish containing methyl mercury
experience a biomagnification of methyl mercury in their body, resulting in severe
diseases and eventually - death. Up to date, it is still unknown how mercury is
transformed form its inorganic form to the organic one, in both aquatic and atmospheric
matrices.
Currently, mercury is monitored in many areas around the world, trying to predict or
model future transportation or behavior of the pollutant in the atmosphere. Understanding
the movement of mercury in the atmosphere will help to alert populations with different
health risks that are associated with mercury. Future research in the investigation of
mercury as an atmospheric pollutant can focus on understanding to greater details how to
analyze obtained data within three or four years since measurement dates instead of eight
or nine years as it stands now. In addition, more accurate equipments generating less
uncertainty per given measurement will greatly help in the future understanding and
prediction of atmospheric mercury pollution.
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