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Density
Density of spilled oil increases as evaporation removes the lighter
constituents, but only rarely does the density reach that of seawater.
This effect is partially balanced by a density decrease with increasing
temperature. The effective density of a slick tends to increase due to
weathering, but more significant increases are attributable to (~) the
uptake of water by many oils to form emulsions (~moussen), which have
higher densities (approaching that of seawater), and (2) association
with suspended minerals or organic matter. Oxidation also may cause a
density increase, but the products may be quite water soluble and will
thus migrate out of the oil.
Density plays an obviously important role in the fate of spilled
oil, for the density difference between oil and water determines the
extent to which the slick is submerged and the residence time of oil
droplets which may be propelled downward in the water column by breaking
waves. Following the Kurdistan spill there were anecdotal but unsub-
stantiated accounts of submerged or neutrally buoyant oil (Vandermeulen,
1981~. It is generally accepted that the density of most weathered
oils does not become great enough for neutral buoyancy to occur and
result in significant amounts of particles and pancakes in suspended
equilibrium in the water column.
Viscosity and Pour Point
Spill viscosity (resistance to flow) increases with weathering and
decreases with increasing temperature. This is important, as it
controls the rate of spreading in the gravity-viscous regime. A
related property is pour point temperature for oils which is often
invoked as an Equivalent to melting point" for organic chemicals.
Phenomena associated with the rapid increase in viscosity as the pour
point is approached are not well understood. Probably more important
is the effect of emulsified water on the bulk viscosity of emulsions.
Oils usually have non-Newtonian theologies (flow) characteristics;
thus a viscosity measurement is meaningful only in the context of a
particular Theological model if the shear conditions are defined. It
is appropriate to measure and record low shear rate viscosities using,
for example, an Ostwald viscometer.
Vapor Pressure
Vapor pressure controls evaporation rate and air concentrations of
hydrocarbons and, therefore, the fire hazard in the vicinity of
spills. Vapor pressures can be estimated using Raoult's law (vapor
pressure of a solution equals the product of the vapor pressure of the
solvent and the mole fraction of the solvent) if the composition of the
mixture is known--which is usually not the case. The use of
pseudo-components or analytical expressions for vapor pressure is
discussed in the Evaporation section below.
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273
TABLE 4-1 Henry 's Law Constants for Selected Hydrocarbonsa
Molecular Vapor or Aqueous Henry 's Law
Weight Partial Pressure Solvability Constant
Compound (at 25°C) (g/mol) (atm) (g/m3) (atm m3/mol )
Methane 16 1.0 24 .1 0 .67
e-Butane 58 1.0 61.4 0.95
n-Hexane 86 0 .2 9.5 1. 81
e-Octane 114 0.019 0.66 3.28
n-Decane 148 0.0017 0.052 4. 83
Cyclohexane 84 0.13 55 0.19
1-Hexane 84 0.24 50 0.41
Benzene 78 0.13 1780 0.0055
Toluene 92 0.038 515 0.0067
o-Xylene 106 0.0087 175 0.0052
Naphthalene 128 0.00011 34 0.00043
Biphenyl 154 0 .000013 7 .5 0 .0002 7
aFor gaseous solutes the solohil ity is at 1.0 atm pressure.
SOURCE: Af ter McKay, 1981.
Aqueous Solub il ity
Henry's law, CP=HC, where p is pressure in atmospheres, C is concentra-
tion in solution, and H is Henry' s law constant, can be invoked,
although some er ror may be introduced because there is ev idence that
mixtures are more soluble than is expected from a direct mole fraction
dependence (Leionen et al., 1971), a phenomenon that is at least
partially due to the presence of dissolved natural humic-like matter in
seawater (Boehm and Quinn, 19731. Henry's law constants for selected
hydrocarbons in distilled water are given in Table 4-1.
The solubilities of hydrocarbons in seawater are generally some
60-809s of the distilled vrater values owing to the "salting out"
effect. ThiS can be character ized by the Setchenow equation
(Aquan-Yuen et al ., 1979 ~ .
Processes
Advection and Spreading
Transport of oil spilled onto the sea surface is due to two processes:
advection and spreading. Advection is due to the influence of over-
lying winds and/or underlying currents. ThiS process may be subdivided
further depending on the causes of motion. For example, there may be
advection by Stokes drift, Ekman currents, Langmoir circulation,
geostrophic currents, or even turbulent flow. Descriptions and
mathematical treatments of these various advection processes can be
found in texts on general and physical oceanography.
The other transport process is spreading, a phenomenon resulting
from a dynamic equilibrium between the forces of gravity, inertia,
frict ion, v iscosity, and surface tension.
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274
1cm
1mm
1 00,um
1 OlJm
1pm
J
0.11Jm
0.01pm
l
DDULL BROWN
6
~NIFIC ANT
4~ SURFACE CONCENTRATIONS
~ DARKER BROWNS TO BLACK
IRIDESCENCE
- SILVERY SHEEN
/OLORLESS SLICK CAPILLARY WAVES DAMPED
/ MONOMOLECULAR LAYER
I I I ~ I I I
10 102 103 104 10S 106 107
SURFACE CONCENTRATION OF SPILL
tLITERS PER SQUARE KILOMETER)
FIGURE 4-2 Sur face concentration of spill .
SOURCE: Barger et al . ( 1974 ~ .
Oil on the sea surface manifests itself as slicks of var table
thickness. An approximate classif ication of these slicks is "thin"
slicks, less than 10 um thick, to "thick" slicks, often millimeters
or even centimeters thick. Generally, the area of thin slick exceeds
that of the thick, but most of the oil volume usually resides in the
thick slick. Figure 4-2 is a labeled plot of thickness versus surface
concentr at ion .
Observations of water may show f irst the evidence of oil by damping
of capillary waves: the sur face becomes less ~ rough ~ and more
"glassy," but no oil is visible. As the slick thickens to 1 Em,
light interference effects become apparent, often giving irridescent
colors. Further increase in thickness to approximately 10 Em gives
darker films.
The behavior of thin films is dominated by surface tension (or
interracial energy) effects; spreading is promoted when the sum of the
oil-water and oil-air infer facial tensions is less than that of the
water-air infer facial tension. Behavior in this regime is complicated
by the presence of natural organic surface layers on the ocean surface,
especial ly in quiescent and biologically productive areas. Although
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275
these infer facial tensions can be measured, reliable deduction of
behavior is not possible because (1 ) as the oil spreads it evaporates
and dissolves, and the infer facial tension changes; (2) oxidation
(probably photolytic in or igin) alters the composition of the oil,
especially by forming oxygenated compounds with low inter facial
tensions; (3 ~ as hydrocarbons dissolve in water they alter the water-air
infer facial tension; and (4 ~ spreading induces a change in composition
of the o il by select ive d issolut ion and evapor at ion of cer ta in
components .
Under relatively quiescent conditions, slicks of thickness greater
than 10 Am tend to be surrounded by thin slicks; thus, they do not
experience a surface tension force to induce spreading. Accordingly,
the thick slicks tend to spread more slowly, at a rate controlled by a
balance of hydrostatic, viscous, and inertial forces. This fluid flow
process can be described mathematically if certain simplifying assump-
tions are made. However, the results probably will not have general
utility because (1) solutions are very complex; (2) the rheology (flow)
of the oil is often complex, i.e., the viscosity is not constant; (3)
wave action stretches and compresses the oil slick; (4) water-in-oil
emulsions may form; (5) usually the slick is wind driven relative to
the water ; (6) the presence of natural surface convergences or diver-
gences will cause the oil slick to separate or accumulate; (7) oil
composition (as distinct from viscosity or sur face properties) appear s
to influence spreading (Fazal and Milgram, 1979~; and (8) the entire
spreading process is likely to be profoundly influenced by sea state,
especially under rough conditions in which oil may be carr fed by spray.
In recent years there have been many attempts to model the fate of
oil spills. For example, more than 35 different models are described
in a comprehensive repor t by Huang and Monastero (1982~. Because
advective processes are the principal controls for the fate of a spill,
they are the most frequently modeled. The general consensus of
modeling experts is that there is no one universal model that will
generally yield predictions that are real istic or undistorted . The
modell ing of the many d isper sed smaller sl icks is a ma jor unsolved
problem.
Wind causes surface water dr if t at a velocity of a few percent of
the wind speed . Oil behaves s imilar ly, the consensus be ing that the
drift velocity is 3-4% of the wind speed. G.L. Smith (1977) has
treated this in some detail, err iving at a dr if t factor of 3 .64 ~
O . 51% . An important observation is that the dr if t factor of the thick
slick exceeds that of the thin; thus, the thicker region tends to
accumulate at the leading edge of the sl ick, with the th inner reg ion
trail ing .
Calculation of dr if t is essential in oil spill tra jectory models,
but is compl icated by (1 ) the possible influence of Cor iol is forces on
the slick (tending to cause diversion to the "right" in the northern
hemisphere and "left" in the southern hemisphere), (2 ~ by residual and
tidal ocean currents which provide an additional vector, (3) by Stokes
surface drift associated with gravity waves (Lange and Hufner fuss,
1978), and (4) the reduction by floating oil of wind stress transmitted
to the sea.
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276
Comparison of computed and actual trajectories of slicks such as
those from the Argo Merchant, Ixtoc blowout, Kurdistan, or Amoco Cadiz
suggests that the major sources of uncertainties are (1) lack of reli-
able data on wind speed and direction (due to distance from weather
stations) and (2) lack of detailed ocean surface current data.
Evaporation
Evaporation, which may be responsible for the loss of from one- to
two-thirds of an oil spill mass in a per lad of a few hour s or a day
(Jordan and Payne, 1980), causes considerable changes in chemical com-
position and physical properties of the oil. Calculation of evapo-
ration rates is cliff icult because the rate depends on a number of
factors, all of which may change with time. Observations of evapora-
tion rate and attempts to predict that rate have been reported by
Kreider (1971), McAuliffe (1977), Mackay et al. (1980b), Butler (1976),
and Harrison et al. (1975) and are generally reviewed by Jordan and
Payne (1980~.
The rate of evaporative loss from a given volume of oil depends on
(1) the area exposed, which tends to increase continuously as the slick
spreads; (2) the oil phase component vapor pressures, which are a
function of oil temperature and composition, and which fall as the
lighter components are depleted from the slick; (3) the oil-air mass
transfer coeff icient, which depends primarily on the wind speed but
also on the hydrocarbon vapor diffusivity; and (4) the possible presence
of diffusive barriers such as a water-in-oil emulsion or a "skin" on
the oil surface.
Thus the "half-lives. for the various hydrocarbon components in the
slick cannot be determined, although approximate values can be suggested
for defined conditions. The rate of evaporation from a thick, cold
slick under calm conditions may be orders of magnitude slower than from
a thin, warm slick under stormy conditions.
There are two general approaches to calculating evaporation rates.
First is a pseudocomponent approach in which the oil is postulated to
consist of a number of components or pseudocomponents of defined
volatility and with proportions selected to give a mixture with volatil-
ity characteristics similar to that of the oil. As evaporation pro-
ceeds, the change in oil composition is computed and the falling vapor
pressure is calculated from Raoult's law at the desired temperature.
This approach has been used by Mackay and Leionen (1975), Yang and Wang
(1977), and Mackay and Paterson (19811.
The second approach is to postulate an analytical expression for
the amount evaporated as a function of time and composition as attempted
by Butler (1976) and Mackay et al. (1980b). In the latter case, a
method was proposed by which oil distillation data could be used to
predict vapor pressures and, hence, evaporation rates.
Evaporation rates and composition changes can be measured by simple
pan evaporation experiments, either outdoors or in wind tunnels, with
an attempt to extrapolate the results to oceanic conditions. There
remains a need to improve the prediction of oil evaporation rates and
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277
to characterize oil volatility characteristics more accurately by means
of information obtained from pan evaporation experiments, distillation
temperature data, and evaporation by a controlled air flow bubbled
through the oil. Such information probably can be used to estimate the
oil fractions evaporated under various defined conditions and to calcu-
late the fractional retention of specific hydrocarbons at various times.
Such a capability would be invaluable as a means of calculating changes
in dens ity or v iscos ity, assess ing changing toxicity, and improving
identif ication of slick samples for legal purposes. Although parts of
this overall capability are in place, a comprehensive treatment is
s til 1 lack ing .
Hydrocarbons may evaporate from true solution in sur face water quite
rapidly--often with half-lives of an hour or less. This is illustrated
by the analytical data reported for samples collected under dispersed
oil slicks in which there was evidence of substantial removal of vola-
tiles from the water column (McAulif fe et al ., 1980 ~ . In the case of
high-molecular-weight hydrocarbons of low Volubility, most may be in
colloidal or accommodated form and are not immediately available for
evaporation. This topic has been reviewed recently by Mackay et al.
(1981a), using calculations based on previous work by Mackay and
Leionen (1975) and L'ss and Slater (1974~.
Dissolution
Dissolved hydrocarbon concentrations in water are particularly important
because of their potentiality for exerting a toxic effect on biological
systems.
They are less important from the viewpoint of the mass lost by the
spill, for dissolution of even a few percent of the spill is unlikely.
Dissolution is bet ieved to be directly from the slick to the water
column and from dispersed oil drops to the water column. In analyzing
spill behavior a prediction of dissolution rate is unnecessary because
the mass dissolved is negligible compared with that removed by droplet
entrainment and can be subsumed in the dispersion rate expression.
The extent of dissolution is obviously influenced by the oil's
aqueous Volubility which, for a crude oil, is typically 30 mg/L. Most
of the dissolved hydrocarbons are the more soluble low molecular weight
aromatics such as benzene, toluene, and the xylenes. As the oil evapo-
rates, these hydrocarbons are removed; thus the oil Volubility drops
and the dissolution rate falls to a negligible value. Some illustrative
Volubility data for fresh and weathered crude oils are given by Mackay
and Shiu (1975~.
Calculations of the rate of dissolution are imprecise, and only
Cohen et al. (1980) and Butler (1976) have attempted to make estimates.
The most soluble hydrocarbons, which are also the most volatile, are
likely to be preferentially removed by evaporation, which is typically
orders of magnitude faster. Even when hydrocarbons do dissolve, many
are likely to be removed by subsequent evaporation from the water ,
provided they have sufficient volatility.
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278
It should be reemphasized that in the subsequent chapter on Effects
the simplest aromatic compounds are shown to be among the most toxic
compounds of crude and refined oil, and as they are also the most
soluble, their impact on the marine environment is greater than simple
mass balance considerations would imply.
Dispersion/Vertical Tr anspor t
The lifetime of an oil slick on an ocean surface is often controlled by
the dispersion or vertical transport of small particles of oil or
oil-in-water emulsions into the water column (}lackey et al., 1980a).
This 1 if etime usually determines whether a given sl ick is 1 ikely to
impact on a particular shoreline that may be, for example, several days
drift time from the site of the spill. Dispersion also results in
exposure of subsurface marine organisms to particulate and dissolved
oil. These organisms, in turn, may mediate the sedimentation of some
of the oil through incorporation into fecal pellets.
The nature of the fluid mechanics of the event resulting in natural
vertical dispersion is not well understood and is undoubtedly complex.
Breaking or surface turbulence waves probably cause the oil to be
driven into the water column, thus forming a swarm of oil droplets.
The larger particles probably rise and coalesce with the slick, while
the smaller oil droplets are conveyed with water eddies vertically
downward to become permanently incorporated into the water column.
These smaller droplets, which do not r ise to the surface, and their
associated water medium may be classified as an oil-in-water emulsion.
This emulsion formation is only a part of the overall dispersion
process .
Expressions for natural dispersion rates have been assembled by
Mackay et al. ~1980a), Spaulding et al. ~1978), Carver and Williams
(1978), and Aravamudan et al. (19811. The simplest approach for includ-
ing dispersion in an oil spill model is that used in the SLICKTRAC
model by Blaikley et al. (1978), who tabulated estimated vertical
dispersion rates expressed as a percentage of the oil per day as a
function of sea state and duration of the spill. This tabulation is
undoubtedly an oversimplification of a complex phenomenon. A similar
approach has been used by Audunson et al. (1980~.
Experimental wind-wave tank measurements and a mathematical
treatment of this process have been made by Mackay et al. (1981a).
Equations were proposed for transport rates as a function of the oil
slick thickness, the oil-water infer facial tension, the sea state, and
in particular, the fraction of the sea covered by breaking waves.
Although there are some data on this fraction, it is only for seas in
the absence of oil. As is well known, oil reduces the incidence of
breaking waves. Also, the dispersion process is believed to occur even
when there are no breaking waves, a possible mechanism being Folding n
of the oil when short waves of relatively high amplitude and short
wavelength pass through the oil layer.
When the surface layer of water is well mixed, vertical eddy diffu-
sion presumably causes further transport downward, and hypothetically,
OCR for page 279
279
Langmair circulation cells may be even more important. Sutcliffe et
al. (1963) reported sinking rates of water in the convergences of
2.7-5.7 cm/s with moderate wind speeds . This should be suff icient to
overcome the buoyancy of some oil droplets that otherwise would not
sink, but direct observations are lacking.
Further research on the problem of vertical dispersion is justified.
An adequate set of equations cannot be developed until the basic
mechanisms are better understood.
Emulsification/Mousse Formation (Water-in-Oil)
Laboratory studies to evaluate water-in-oil emulsion fornication for
different crude oils and petroleum products have demonstrated a depen-
dence on the unique chemical compositions of each of the mater ials
tested (Payne, 1984, and references therein) . Heavier crudes with high
viscosities are, in general, found to form the more stable emulsions
(Bocard and Gatellier, 1981), and the presence of asphaltenes and
higher-molecular-weight waxes have been found to be positively cor-
related with mousse stability (Berridge et al., 1968a,b; Davis and
Gibbs, 1975; MacGregor and McLean, 1977; Mackay et al., 1979, 1980a;
Twardus, 1980; Bocard and Gatellier, 1981; Bridie et al., 1980~.
Slightly differ ing results have been obtained in different investiga-
tions, but generally these materials act together in the emulsif ication
process, although the asphaltenes do appear to play a more s ignificant
role (Bridle et al., 1980; Berridge et al., 1968a,b). The crystallizing
properties of the component waxes (near the pour points of the oils
tested) are believed to be important in affecting the internal oil-
mousse structure and viscosity, and the asphaltenes are believed to act
as surfactants, preventing water-water coalescence in the more stable
mixtures (Berridge et al., 1968c; Canevari, 1969; Mackay et al., 1973;
Bridie et al., 1980; Cairns et al., 1974~. Other indigenous surface-
active agents such as metalloporphyrins and nitrogen, sulfur, and
oxygen compounds are believed to be equally important.
The products of photochemical and microbial oxidation have also
been identif fed as having an impor tent role as stabiliz ing agents
(Bocard and Gatellier, 1981; Klein and Pilpel, 1974; Burwood and
Spears , 1974 ; Zaj ic et al ., 1974 ; Fr iede , 1973 ; Guire et al ., 1973 ~ .
In several instances, mousse could only be formed with photochemically
or microbially weathered oils which were also subject to evaporation/
d issolution processes . Brega, Niger fan, Zar zatine, and 1 ight Arabian
crude oils have all been shown to exhibit this behavior in laboratory
studies (Berridge et al., 1968b; Bocard and Gatellier, 1981) . The
formation of a stable mousse at the Ixtoc I wellhead was also observed
to be delayed until after these processes had been operative for 24-48
hours on the oil released during that blowout (Payne , 1981 ) .
No stable mousses could be formed in laboratory studies at any
temperature with light petroleum distillates such as gasoline, kerosenes
and several diesel fuels (Berridge et al., 1968a,b; Twardus, 1980) and
could only be obtained with several 1 ight lube oils when they are
fortif fed with wax and asphaltene mixtures obtained from known mousse
OCR for page 280
280
forming oils such as Kuwait crude (Bridle et al., 1980~. This
asphaltene mixture could also contain other surface-active agents of
higher molecular weights.
Temperature is also a factor in mousse formation, and in several
instances at low temperatures approaching the pour point of the heavier
oils, stable emulsions have been generated regardless of wax or
asphaltene content. Conversely, if stable water-in-oil emulsions are
repeatedly exposed to freeze-thaw cycles, some destabilization and
separation of water and oil have been noted (Dickens et al., 1981; and
Twardus, 1980~. Similar results have been obtained when laboratory
generated and real spill water-in-oil emulsions were subjected to
prolonged heating or removal from the water column.
The absolute amount of water content and the size of water droplets
incorporated into various mixtures of mousse also significantly affect
their stability and viscosity (8erridge et al., 1968a,b; Mackay et al. ,
1980a; Twardus, 1980; Bocard and Gatellier, 1981) . Positive correla-
tions of percent water versus mousse stability and viscosity have been
noted for several of the crude oils studied (Mackay et al., 1979,
1980a) . In general, with many oils, maximum stability is achieved with
a water content in the range of 20-80%; however, at an oil-specific
critical point, significant destabilization of the emulsions occurred
(Berridge et al., 1968a,b; Twardus, 1980~. Presumably, this reflects
enhanced water-water contact and coalescence resulting in ultimate
phase separation.
In most of the laboratory studies, the presence and/or absence of
bacteria and suspended particulate material did not appear to affect
emulsion behavior (Berridge et al., 1968a,b; Davis and Gibbs, 1975~.
Bacterial growth was generally limited to the surface of the mousse
products tested, and is believed to have been inhibited by limited
oxygen and nutrient diffusion into the mousse. Toxic materials inher-
ent to the oils themselves may also be responsible for these observa-
tions, although water content (and in particular the size of the water
droplets encapsulated within the mixtures) has also been correlated
with the presence of bacteria in the less stable mousses (Berridge et
al., 1968a,b). In several laboratory studies significant bacterial
utilization of the mousse only occurred after treatment with disper-
sants, resulting in the break-up of the material, with concomitant
increased surface-to-volume ratios (Bocard and Gatellier, 19811.
Physical Properties of Water-in-Oil Emulsions The physical properties
of stable emulsions are different from those of the starting crudes,
and increases in specific gravity and viscosity have been observed to
affect spreading, dispersion, and solution rates (Berridge et al.,
19685; Davis and Gibbs, 1975; MacGregor and McLean, 1977; Mackay et
al., 1979, 1980a; Twardus, 1980~. Some evidence has also suggested
that evaporation of hydrocarbons of lower molecular weight (Cg-C12)
is af fected by the emulsion (Twardus, 1980; Nagata and Rondo, 19771.
In general, these effects are most significant in the emulsions con-
taining greater than 50% water. Water-in-oil emulsions with less water
usually have pour points, spreading properties, and viscosities which
proportionately resemble those of the starting oils (Twardus , 1980 ;
Mackay et al., 1980a).
OCR for page 358
358
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Representative terms from entire chapter:
aromatic hydrocarbons
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