Environmental Toxicology and Chemistry, Vol. 23, No. 10, pp.

2282–2289, 2004
q 2004 SETAC
Printed in the USA
0730-7268/04 $12.00 1 .00

Special Issue Honoring Don Mackay

FINDING FUGACITY FEASIBLE, FRUITFUL, AND FUN

DON MACKAY*
Canadian Environmental Modelling Centre, Environmental Studies, Trent University, Peterborough, Ontario K9J 7B8, Canada

( Received 18 August 2003; Accepted 16 January 2004)

Abstract—A review is presented concerning the evolution of the fugacity concept as applied to environmental science. The series
of serendipitous events that ultimately resulted in publication of the paper ‘‘Finding Fugacity Feasible’’ in 1979 is described. The
use of fugacity as a surrogate for concentration is shown to facilitate the compilation and solution of mass-balance equations. It
has proved to be valuable in a number of contexts, notably the description of chemical fate in unit worlds at various levels of
complexity. More complex systems can be simulated as sets of connected unit worlds. The fugacity approach enables the multimedia
character of organic chemicals to be deduced, thus contributing to the evaluation of chemical properties that impact persistence
and long-range transport. It has proved to be especially insightful for describing bioconcentration, bioaccumulation, and pharma-
cokinetic phenomena. Applications to the sensing and monitoring of chemical presence in the environment are described. Suggestions
are made for subject areas in which the fugacity concept may prove to be particularly valuable in the future. Finally, the many
colleagues who have contributed to the use of fugacity when quantifying chemical behavior in the environment are acknowledged.

Keywords—Fugacity Model Bioaccumulation Unit world Persistence

INTRODUCTION THE SERENDIPITOUS JOURNEY TO FFF

First, let me express my deep appreciation for the honor of
having this special issue of Environmental Toxicology and
Chemistry devoted to celebrating my career in environmental
science. In particular, I am very grateful to Herb Ward, Frank
Gobas, Derek Muir, and the editorial board for suggesting and
organizing this issue. It is humbling to see contributions from
so many colleagues whose work over the years I have admired
and who have been my collaborators and friends. The Society
of Environmental Toxicology and Chemistry (SETAC) has
played a major role in my career; thus, it is particularly sat-
isfying to receive this acknowledgment of my small contri-
butions. I welcome this opportunity to share some thoughts
on my rather disorganized but enjoyable and rewarding re-
search career, particularly as it relates to the concept of fu-
gacity.
In 1979, I published a feature article, ‘‘Finding Fugacity
Feasible’’ (FFF), in Environmental Science and Technology
[1]. It was, I believe, the first mention of fugacity in the context
of the environmental behavior of chemicals. Since then, nu-
merous papers have been published in which the fugacity con-
cept has been applied to a variety of contexts in environmental
science, and it is now accepted as being a useful tool for the
interpretation of monitoring data, for assembling and solving
sets of mass-balance equations, and in general, for contributing
to a fuller understanding of the quantitative aspects of envi-
ronmental fate. In the present article, I reminisce on the ser-
endipitous journey to FFF, review briefly some of the appli-
cations of the fugacity concept, and propose some promising
future directions. This also provides me with a welcome op-
portunity to acknowledge many of the individuals who have
guided and assisted me on this journey and to note some les-
sons I have learned on the way.
* dmackay@trentu.ca.
2282
My training was as an applied chemist and chemical en-
gineer at what is now the University of Strathclyde in Glasgow
(UK). After postdoctoral research on chemical gas-phase re-
actions in shock waves at the University of Toronto (Toronto,
ON, Canada), I returned to the United Kingdom to work in
the petrochemical industry for Imperial Chemical Industries
in Billingham (Co. Durham, UK). This provided the invaluable
experience of practical research into hydrocarbon reactions and
separations. One technical challenge facing this industry is to
understand, design, and simulate mathematically the diverse
processes that occur in the controlled conditions of a chemical
plant so that the operations can be accomplished safely, ef-
fectively, and economically. Chemical engineering has a rich
and often underappreciated history of successful design, op-
eration, simulation, and control of industrial chemical pro-
cesses.
On returning to the University of Toronto in 1967, I sought
to build a research program in which I could exploit my un-
derstanding of hydrocarbon properties and processing. The
environmental movement was well underway following pub-
lication of Rachel Carson’s Silent Spring [2]. Increasingly, the
public was realizing that it was possible to have both profitable
industrial activity and a clean environment. The principal is-
sues included air and water pollution, acid rain, pesticides,
hazardous wastes, and marine oil spills. At that time, proposals
had been made to transport oil from the Arctic by what is now
the Trans-Alaska Pipeline and in Canada from the Beaufort
Sea down the Mackenzie Valley to Alberta. The obvious en-
vironmental concerns resulted in a number of enlightened re-
search programs that had the general objective of understand-
ing the fate of hydrocarbons in cold climates, developing re-
medial technologies for spills, and mitigating adverse effects.
I was fortunate to be involved in this research for some 20
years. In late 1988, I decided that no further large oil spills
would occur and that further research was not really needed.
In March 1989, the Exxon Valdez ran aground.
Finding fugacity feasible, fruitful, and fun
During this fruitful period of research, we devoted consid-
erable effort to modeling the behavior of spilled oil as it ex-
periences natural weathering processes, including evaporation,
dissolution, and emulsification to form water-in-oil and oil-in-
water emulsions. With my colleagues, especially Tom Hutch-
inson and Michael Charles, we explored the behavior of oil
spills on Arctic tundra, taiga, rivers, snow, and ice, doing field
work in that fascinating environment with its remarkable peo-
ples and ecosystems. This fascination with cold climates was
to be revisited in later years. We became convinced—and we
remain so—that the best oil spill countermeasure (after pre-
vention) is chemical dispersion using surfactants that emulsify
the oil, thus preventing organisms such as birds from being
smothered and mitigating adherence to shorelines and sedi-
ments. Admittedly, there is probably a greater pelagic pulse
of toxicity, but it is expected to be transient and, hence, a
logical environmental trade-off. Debate on this issue continues
to this day. I learned a great deal about the principles and
practice of toxicity from my collaboration with Peter Wells on
dispersant toxicity [3]. Later, Alice Bobra was able to assign
toxic effects separately to the dissolved and emulsified oil and
to the dispersant [4]. This work continues, with Debbie French-
McCay having recently developed a ‘‘state of the science’’
model describing the toxicity of this complex system [5].
Hydrocarbons tend to be toxic to organisms by two prin-
cipal routes. Oil can smother surfaces, resulting in respiratory
failure, loss of insulation in the case of birds, and direct in-
gestion of the oil. More subtle is the effect of hydrocarbons
that dissolve in water, then partition from water to the organism
by the respiratory route, possibly resulting in lethality. Most
hydrocarbons are sparingly soluble in water; for example, n-
octane has a solubility of only 0.66 mg/L or ppm [6], which
seemed to be too low to cause toxicity. Indeed, little infor-
mation was available in the literature regarding hydrocarbon
solubility in water, the notable exception being the pioneering
work of Clayton McAuliffe of Chevron (La Habra, CA, USA),
who devised an elegant headspace technique for measuring
low solubilities. I met McAuliffe and later enjoyed a fruitful
collaboration with him for many years. A colleague in botany
at the University of Toronto, Tom Hutchinson (who is now
also at Trent University), had the idea of measuring the toxicity
of a variety of hydrocarbon solutions in water to algae. We
discovered a remarkably good correlation between toxicity and
the hydrocarbon’s octanol–water partition coefficient [7]. This
work provided one of the first environmental structure–activity
relationships, or quantitative structure–activity relationships
(QSARs), for the prediction of aquatic toxicity.
I became convinced, both by this work and by the emerging
science of bioaccumulation as developed by Brock Neely and
colleagues at Dow Chemical (Midland, MI, USA) [8], that a
fruitful research area was the link between hydrocarbon prop-
erties, environmental partitioning (especially bio-uptake), and
toxicity. In reality, the environmental community had been
slow to recognize the pioneering contributions of workers such
as Overton and Ferguson, who first pointed out this relation-
ship. We thus set out to measure and correlate physicochemical
properties of organic chemicals, especially hydrophobic chem-
icals. This is experimentally demanding and requires metic-
ulous techniques, but I was fortunate to work initially with
Aaron Wolkoff and then for over 30 years with Wan Ying Shiu
on such measurements. This evolved into a series of handbooks
and a CD-ROM on physicochemical properties [6] authored
Environ. Toxicol. Chem. 23, 2004 2283
by Wan Ying Shiu; her husband, Kuo Ching Ma (University
of Toronto); and myself.
We, in common with others, experienced difficulty main-
taining constant concentrations of hydrocarbons in solution.
Although octane is less volatile than water, a solution of octane
in water will lose most of its octane in an hour or two by
evaporation. A similar effect had been noted for evaporation
of DDT from water and soils. These observations were in-
correctly explained by a nonexistent ‘‘codistillation’’ effect.
The fast evaporation is, in fact, attributable to the high activity
coefficient of the octane in solution (i.e., high hydrophobicity),
which counteracts the dilution and the low vapor pressure.
Based on these insights, we published a paper in 1973 that
explained how this phenomenon could be taken into account
when quantifying volatilization rates of hydrophobic substanc-
es from solution [9].
Peter Liss, the UK chemical oceanographer, kindly wrote
to me and pointed out that he had addressed this issue for
gases in seawater and had invoked the Whitman two-resistance
model to quantify the volatilization rate [10]. Since we had
incorrectly used a one-resistance model, we shortly published
a corrected version [11].
This work came to the attention of George Baughman of
the U.S. Environmental Protection Agency lab at Athens (GA,
USA), who suggested a three-year grant to measure these re-
sistances in terms of mass-transfer coefficients. The intent was
to build up the predictive capability of what is now the U.S.
Environmental Protection Agency EXAMS model of chemical
fate in aquatic systems. During this work, I was privileged to
visit Athens and was exposed to the thinking of George Baugh-
man, Ray Lassiter, Larry Burns, Richard Zepp, Sam Karick-
hoff, Dave Brown, and Dotty Paris as well as that of their
collaborators, Ted Mill, Bill Mabey, and Jim Smith. It was a
wonderful education to be associated with these pioneers.
I was deeply influenced by George Baughman’s concept of
‘‘evaluative environments’’ and by his conviction that it was
essential to strive for environmental mass balances for con-
taminants [12]. The assembly of mass-balance equations in
models such as EXAMS was similar to those used by chemical
engineers simulating chemical behavior in chemical plants. So,
why not use one of the tools from these simulations, namely
the concept of fugacity? Fugacity simplifies and clarifies the
relationship between equilibrium concentrations in various flu-
ids and solids. Rather than relate two concentrations using a
partition or distribution coefficient, such as Kow or Koa, each
concentration is independently related to a fugacity, and the
two fugacities are equated. The fugacity–concentration rela-
tionship is usually linear at low concentrations, further sim-
plifying the calculations.
This approach has problems, but they can be solved. The
correct concentration to use is a mole fraction, but what is the
mole fraction of DDT in a fish? Calculating this quantity re-
quires the molecular weight of a fish—a very doubtful quantity.
The simple expedient is to use concentrations in units of mol/
m3, which leads to the simple relationship
C (concentration mol/m3) 5 Z (mol/m3·Pa) · f (fugacity Pa)
The proportionality constant Z (with units of mol/m3·Pa) or
fugacity capacity is analogous to a heat capacity (J/m3·K) in
that fugacity (Pa) is analogous to temperature (K) and chemical
concentration (mol/m3) is analogous to a concentration of heat
(J/m3). Doing heat-transfer calculations without the use of tem-
perature is unthinkable, yet environmental calculations of mass
2284 Environ. Toxicol. Chem. 23, 2004
transfer and partitioning did not use the analogous quantity,
fugacity. It seemed to me that by reformulating equations in
terms of fugacity, environmental mass balances could be done
more easily, especially for systems involving disparate phases
such as air and soil. With this in mind, I wrote what was to
become FFF [1]. It received a deservedly cool reception.
The original research paper, which had a longer and very
dull title, was soundly criticized by reviewers. Why use fu-
gacity when concentration can do the same task? The editor
of Environmental Science and Technology, Russ Christman,
rightly rejected the paper, but in a gesture of remarkable ed-
itorial insight and generosity, he suggested that I rewrite it as
a feature article in collaboration with Stanton Miller, the man-
aging editor. Stan changed the title to ‘‘Finding Fugacity Fea-
sible’’ and reworked the graphics, and the paper was published
in 1979. Sequels coauthored with Sally Paterson, ‘‘Calculating
Fugacity’’ [13] and ‘‘Fugacity Revisited’’ [14], appeared later
as the concept developed. The book Multimedia Environmen-
tal Models: The Fugacity Approach was published by Lewis
Publishers in 1991, with the most recent edition being pub-
lished in 2000 [15].
Two other concepts were developed in FFF. George Baugh-
man had conceived of using the evaluative or hypothetical
environment. I borrowed this idea and, in collaboration with
Brock Neely of Dow Chemical, developed the concept of ‘‘unit
worlds,’’ in which fugacity can be used to deduce chemical
partitioning [16]. The second was the idea of performing en-
vironmental partitioning and fate calculations in ‘‘levels’’ of
increasing complexity and, thus, fidelity to real systems. Se-
lecting an appropriate level of complexity for environmental
simulation remains problematic, but a strong case can be made
that it is best to start with a simple model and then build in
more complexity only when needed. Introducing models in a
progression of increasing complexity also has an obvious ed-
ucational advantage.
THE BASICS OF FUGACITY
It was G.N. Lewis who introduced the equilibrium criterion
of fugacity ( f ) as a concept in 1901. It is really a corrected
partial pressure and, thus, has units of Pascals (Pa). For cal-
culation purposes, it is much more convenient than chemical
potential, because in dilute solutions, it is linearly related to
concentration. The key texts on the subject were those of Van
Ness and Abbot [17] and Prausnitz et al. [18], which have
been subject to more recent revisions and have been ther-
modynamic ‘‘bibles’’ to me and to a generation of chemical
engineers.
As indicated earlier, f can be related to concentration C
using the proportionality constant Z, which can be viewed as
a kind of solubility or capacity of the phase to absorb the
chemical. Chemicals thus tend to migrate into phases in which
Z is large, such as lipids of fish for dissolved DDT or aerosol
particles for gaseous benzo[a]pyrene. Calculation procedures
or recipes are available for estimating Z values using either
measured or correlated partition coefficients and other phys-
icochemical properties.
Transport and transformation processes can be expressed
using D values that are essentially rate constants in fugacity
format. Whereas a chemical reaction rate is VCk, where V is
volume, C is concentration, and k is a rate constant, the cor-
responding rate is Df in terms of fugacity. A convenient feature
of D is that it can be applied to reactions, diffusion processes,
and advection processes; thus, all competitive rates are ex-
D. Mackay
pressed in terms of a dimensionally identical quantity. This
facilitates interpretation of the complex behavior of chemicals
in the environment and, especially, in biological systems.
With a toolbox containing f, Z, and D, the modeler has the
key tools to quantify chemical fate in a vast variety of situ-
ations from transport across a cell membrane to estimating
global distribution of chemicals of commerce. As with all
tools, some practice is needed, but the rewards are consider-
able.
UNIT WORLDS
The concept of a ‘‘unit world’’ consisting of at least air,
water, soil, and sediment compartments has proved to be very
valuable for assessing chemical fate. I was very fortunate in
having a long-term collaboration with Sally Paterson, who was
instrumental in applying and testing these models of chemical
fate [19]. As time has progressed, the concept has been applied
internationally, notably at the National Institute of Public
Health and the Environment in The Netherlands by Dik van
de Meent and Jaap Strujs in their SimpleBox and SimpleTreat
models, which are now an integral part of the EUSES system
[20]. Other applications have included the ChemCAN model
[21], the ChemFrance model by Devillers and Bintien [22] and
as part of Tom McKone’s CalTOX model [23] of chemical
fate and exposure in regions of California (USA). Katsuya
Kawamoto collaborated with Matt MacLeod to apply it to
Japan [24]. Kevin Jones and Andy Sweetman have applied a
version to the United Kingdom [25].
Two further developments were of note. In 1994, SETAC
sponsored workshops at Leuven (Belgium) and Denver (CO,
USA), resulting in a monograph on multimedia modeling,
largely thanks to the efforts of Christina Cowan-Ellsberry and
Tom Feijtel of the Procter & Gamble Company of Cincinnati
(OH, USA) [26]. Also in collaboration with Christina Cowan-
Ellsberry and Antonio DiGuardo, then of the University of
Milan, the Equilibrium Criterion or EQC model was developed
and made widely available as a user-friendly Visual Basic
program to provide a rational, tiered assessment of chemical
fate [27–29]. It contains level 1, 2, and 3 programs and is
applicable to involatile and insoluble substances as well as to
conventional organic chemicals. Miriam Diamond successfully
devised methods of applying the fugacity tool to metals [30]
and speciating substances [31].
The EQC program (Trent University Environmental Mod-
eling Centre) was developed at an opportune time, because
international efforts were underway to identify persistent,
bioaccumulative, and toxic chemicals as well as those with
potential for long-range transport (LRT). This issue has been
the subject of considerable attention in both the scientific and
regulatory communities, resulting in UN Environment Progam
actions to regulate or ban the ‘‘dirty dozen’’ [32]. In various
countries, a large number of chemicals of commerce are being
reviewed for their persistence, bioaccumulation, toxicity, and
LRT characteristics, and this list of a dozen likely will increase
in number in the future. Unit world models, using either fu-
gacity or concentration, can play a key role in assessing overall
environmental persistence and LRT, because partitioning prop-
erties and mode of entry to the environment are taken into
account. The issue of quantifying the persistence of organic
substances remains a challenge both in obtaining reliable es-
timates of media-specific half-lives and in combining these
estimates to assess overall persistence. Eva Webster and Todd
Gouin have shown that level 2 and 3 fugacity unit world mod-
Finding fugacity feasible, fruitful, and fun
els can play a key role in this important assessment [33,34].
Likewise, LRT cannot be measured; it must be obtained using
a model in either lagrangian coordinates, as suggested by Van
Pul et al. [35] and Bennett et al. [36], or in eulerian or unit
world coordinates, as suggested by Beyer et al. [37].
By providing a quantitative depiction of chemical fate, unit
world models can help with assessment of the large number
of chemicals of commerce. They can also contribute to edu-
cation about the wide differences in fate, persistence, and trans-
port experienced by these substances.
Connected unit worlds
An obvious extension of the unit world concept is to apply
it to multiple connected unit worlds, thus increasing the ability
of the model to address spatial variability. This approach is
routinely applied in water-quality modeling. My education in
water-quality modeling was largely the result of reading the
works by pioneers such as Steve Chapra, Ken Reckow, and
Jerry Schnoor, but most enjoyably the result of listening in
fascination as Dominic Di Toro expounded on this subject.
That group at Manhattan College, including Donald O’Connor,
Bob Thomann, and John Connolly, raised environmental mod-
eling to a new level of credibility, practicality, and effective-
ness.
Conventional concentration-based water-quality models
contain a diverse set of expressions for advection, diffusion,
evaporation, deposition, resuspension, degrading reactions,
and partitioning from water to solids and biota. These ex-
pressions can be written in fugacity format, simplifying the
mathematics and enabling the modeler to more easily com-
prehend the characteristics of the system. Any fugacity cal-
culation can equally be done using concentrations and partition
coefficients, so no new knowledge is generated. It is just or-
ganized in a more easily assimilable form. Accordingly, we
developed simple, single-segment water-sediment-air models
for lakes and rivers [38,39], then expanded them to multis-
egment systems. The acronym QWASI (quantitative water, air,
sediment interaction) model was coined for this ‘‘aquatic unit
world.’’ Indeed, using the QWASI model as a basis, Susan
Sang and Penny Vlahos developed a ‘‘rate constant’’ version
that has been applied to the Great Lakes [40] and is currently
being applied to San Francisco Bay (CA, USA). Much of the
incentive was to describe the fate of chemicals in the Great
Lakes and their areas of concern [41,42]. One of the most
publicized examples was the project that Michael McLachlan
undertook to model toxic emissions from the mists of Niagara
Falls [43]. Michael, in collaboration with Otto Hutzinger, be-
came a leading dioxin analyst in Bayreuth and is now at Stock-
holm University (Stockholm, Sweden).
More ambitious examples of connected unit world models
include the GloboPOP model of Frank Wania [44] that divides
the Earth’s surface into 10 meridional unit worlds and can be
used to explore and predict chemical fate on a global scale.
The BETR North America model developed by Matt MacLeod
divides that continent into 24 connected regions [45], whereas
the BETR World model developed by Liisa Toose and David
Woodfine uses the same approach but on a global scale [46].
Martin Scheringer has quantified the spatial and temporal rang-
es in chemical transport globally using a number of connected
unit worlds [47]. Efforts are underway to apply these concepts
in a variety of regions and continents, especially with the
incentive of determining how chemical usage in one jurisdic-
tion results in exposure in other regions. This issue is of par-
Environ. Toxicol. Chem. 23, 2004 2285
ticular concern in the Canadian Arctic, in which residents are
subject to food advisories about consuming local fish and
mammals that are contaminated with substances originally
used thousands of kilometers away.
PHYSICOCHEMICAL PROPERTIES AND
ENVIRONMENTAL PARTITIONING
The unit world calculations demonstrate that environmental
fate is primarily controlled by a chemical’s physicochemical
properties. The accuracy of any model simulation or prediction
depends on the availability of accurate physicochemical data
for the substance of interest. Regrettably, regulatory agencies
often fail to appreciate these relationships, and determination
of properties is left to a few underfunded enthusiasts. A major
effort of our group at the University of Toronto was deter-
mining and correlating these properties. I was very fortunate
in my 30-year association with Wan Ying Shiu, who made
meticulous determinations of these properties, guided many
students, and saw her work culminate in the compilation of a
series of handbooks on chemical properties [6].
In the 1970s, largely as a result of the pioneering efforts
of individuals such as Steve Eisenreich, Anders Andren, and
Dave Armstrong, along with their talented students, such as
Deb Swackhamer and Joel Baker, at the Universities of Min-
nesota and Wisconsin (USA), a realization emerged that sub-
stantial cycling of substances such as polychlorinated biphenyl
(PCB) was occurring between the atmosphere and the waters
of the Great Lakes. Sally Paterson, Steve Eisenreich, Mila
Simmons, and I edited a book on this topic [48] that convinced
me of the compelling need for accurate air–water partition
coefficients that control both the direction and rate of air–water
transfer. Measurements of other coefficients followed. A very
enjoyable collaboration with Davide Calamari of the Univer-
sity of Milan, Eros Bacci of the University of Sienna, and
Sally Paterson showed the importance of vegetation in con-
trolling chemical fate. We suggested use of the octanol–air
partition coefficient, Koa, as a descriptor of air-to-foliage trans-
fer of organic substances [49]. It has been satisfying to see
continued measurement and use of this parameter, especially
by Tom Harner, who devised the first method of experimental
determination [50], and by Andreas Beyer and Frank Wania,
who clarified the relationship between Koa and Kow/Kaw [51].
Tony Finizio, working under the guidance of Terry Bidleman,
later showed that Koa is an excellent descriptor of air–aerosol
partitioning [52].
A particularly elegant application of fugacity to environ-
mental partitioning has been by Terry Bidleman and Lisa Jan-
tunen, who have shown that the ratio of air and ocean water
fugacities of a-hexachlorocyclohexane has changed signifi-
cantly over the years as northern oceans acted first as a sink
and then as a source for this substance [53]. Similar approaches
have been applied to substances such as PCBs in the Great
Lakes, in which there has been a probable reversal of net air–
water exchange. As water bodies such as the Great Lakes
respond to reduced loadings, the levels of persistent contam-
inants such as PCB in various media tend to approach equi-
librium or equifugacity [54]. Identifying the key processes and
their rates likely will require assessment of the contaminant’s
dynamic behavior using both concentration and fugacity as
criteria of presence. To make such assessments requires con-
tinued effort to measure and correlate partition coefficients,
especially as a function of temperature.
2286 Environ. Toxicol. Chem. 23, 2004
BIOACCUMULATION AND TOXICITY
It is perhaps when elucidating the phenomena of biocon-
centration, bioaccumulation, and biomagnification that the fu-
gacity concept is of greatest value. The early views that bio-
accumulation resulted from fast intake and slow loss of chem-
ical have proved to be unsatisfactory, because slow loss is the
result rather than the cause of bioaccumulation. Jerry Hamelink
first conceived that bioaccumulation was basically a partition-
ing phenomenon, and the pioneering studies by Brock Neely
and his colleagues at Dow [8] revealed the relationship with
Kow for organic substances.
When viewed in terms of concentrations, it seems strange
that a PCB achieves a concentration in fish approximately 1
million-fold that of the water it respires. When viewed in terms
of fugacity, however, the reason is obvious. The chemical is
merely seeking to achieve equal fugacities in fish and water.
The high concentration factor is caused by the ratio of the
large Z value in fish and the low Z value in water. The success
of the correlations with Kow reflect the near-equivalence of
chemical Z values in lipids and octanol [55]. Slopes of plots
of log bioconcentration factor versus log Kow are often less
than the expected 1.0, an effect the late Amy Hughes showed
was attributable both to the long equilibration time and to
reduced bioavailability when Kow is large [56].
The phenomenon of biomagnification, in which a fish or
other animal achieves a fugacity greater than that of its food,
was first clearly demonstrated in the field, for the Great Lakes,
by John Connolly and Chrissa Pedersen [57]. Aspects of this
process remain incompletely understood. Frank Gobas and Ka-
thy Clark undertook demanding and meticulous laboratory de-
terminations of bioaccumulation at the University of Toronto
(Toronto, ON, Canada) and devised a model that quantifies
these processes [58]. Later, Frank Gobas and his colleagues at
Simon Fraser University (Burnaby, BC, Canada) refined this
model [59] and performed elegant experiments showing that
a fugacity increase occurs in the gut as the ‘‘solvent’’ lipids
in food are digested—that is, the Z value decreases, and this
drives chemical into the body, achieving high concentrations
[60] They have recently applied these concepts to terrestrial
food chains, notably the lichen-caribou-wolf sequence [61].
Alison Fraser has shown that the fugacity concept can provide
a very clear and satisfying picture of this complex and fas-
cinating phenomenon [62].
Clearly, there is a continuing, high-priority need for lab-
oratory and field research into the factors that control the con-
centration of toxic substances in an organism as a function of
concentration in food and the respired media of air or water.
The extension to food webs that treat multiple organisms is a
logical sequel. Ultimately, these food webs must include plants
as well as animals. It seems likely that fugacity can contribute
significantly to this task of establishing comprehensive de-
scriptions of chemical migration in vegetable and animal food
webs [63].
Another exciting avenue of research is the use of physio-
logically based pharmacokinetic (PBPK) models to elucidate
the disposition of chemicals in the compartments of the body.
Fugacity models seem to be ideal for this purpose, as Sally
Paterson showed for styrene [64] and Tom Cahill showed for
phthalate esters [65].
For many years, I offered an evening course on fugacity
modeling at the University of Toronto during the winter term.
Two enthusiastic biology students from George Dixon’s tox-
D. Mackay
icology group at the University of Waterloo (Waterloo, ON,
Canada) braved the weather and traffic of the 300-km weekly
journey to attend this course. I always felt guilty, because I
learned more from Lynn McCarty and Brendan Hickie than
they learned from me. They paid fees; I was paid! Both became
valued colleagues, including Brendan’s wife, Ellen Bentzen,
who had worked in the internationally recognized limnology
group at McGill University (Montreal, PQ, Canada) with the
late Rob Peters.
Lynn McCarty’s exhaustive analysis of bioaccumulation
and toxicity data convinced me that the future of environmental
risk assessment lies in the combination of PBPK models and
the critical body residue approach, in which toxicity is ex-
pressed as a concentration applicable to a defined mode of
toxic action at the target tissue rather than as external con-
centrations, such as the median lethal concentration [66]. This
idea, which is routine in pharmacology, is slowly being ac-
cepted in environmental science, which traditionally has relied
on external concentrations as metrics of toxicity. If modes of
toxic action can be identified and quantified in terms of tissue
concentration ranges, it should become possible to link exter-
nal concentrations to internal levels using PBPK and bioac-
cumulation models and, thus, to toxic responses. This concept
underlies the advocacy of the critical body residue approach
[67], a concept elegantly demonstrated experimentally by Rob
Peters at McGill University and Joop Hermens and his col-
leagues at the University of Utrecht (Utrecht, The Nether-
lands).
Brendan Hickie has successfully demonstrated the appli-
cation of fugacity-based PBPK models to marine mammals
[68]. The lower observed fugacities in female whales are el-
egantly accounted for by reproduction and lactation losses,
which provide a loss D value that is unavailable to males. The
PBPK modeling of the 30-year lifetime of these animals re-
veals their extreme vulnerability to persistent hydrophobic
chemicals.
ENVIRONMENTAL MODELING
To those of us who view chemical fate in the environment
in terms of fugacity as well as concentration, a compelling
incentive exists to measure and monitor fugacity directly in
concert with concentration. This is widely practiced in the form
of headspace analysis by agencies such as the police when
using breathalyzer tests for alcohol. The partial pressure or
fugacity of ethanol in exhaled air is measured, but the result
is expressed in terms of blood concentration. The widespread
use of biota for water-quality monitoring exploits the relative
ease of measuring high concentrations in lipids relative to those
in water. There also exists a degree of integration of concen-
tration over time that damps out short-term fluctuations. As
contaminant concentrations in the environment fall below 1
ng/L in water or 1 ng/m3 in air, analysis becomes very de-
manding. Meticulous and expensive quality control becomes
essential. In this regime, the amplification and integration of
concentrations become advantageous by sensing fugacity in a
medium of high Z value that approaches or is brought into
equilibrium with the environmental phase of concern.
Notable in this area has been the pioneering work of Jim
Huckins and his colleagues [69] in developing semipermeable
membrane devices for water analysis. Such devices have been
successfully applied to air by Kevin Jones and his group at
Lancaster (UK) [70]. The technique is currently the subject of
considerable research, especially to tailor the sensor’s response
Finding fugacity feasible, fruitful, and fun
time to meet specific requirements. Philipp Mayer, Johannes
Tolls, and Joop Hermens [71] have recently reviewed these
equilibrium sampling devices and have suggested novel ap-
plications, including their use in reverse to deliver desired,
constant concentrations in toxicity tests. Essentially, they de-
fine the exposure fugacity and determine the corresponding
response of the organism to that fugacity.
An elegant and innovative monitoring, sensing, and mod-
eling application has been regarding airborne contaminants in
urban environments by Miriam Diamond and her colleagues
[72]. Dirty windows naturally become coated with a thin, oily
film that absorbs gaseous substances and can trap aerosols.
Washing dirty urban windows and sampling the washwater
throws much needed light, both figuratively and literally, on
the presence of chemicals in urban air. It is often forgotten
that from a public health viewpoint, most human exposure
occurs in these urban regions and, especially, indoors. A no-
table contribution regarding indoor exposure has been made
by Yoshihide Matoba of the Sumitomo Chemical Company
(Takarazuka, Japan), who has successfully developed and val-
idated fugacity models of pesticide fate in the indoor envi-
ronment [73]. Kevin Jones and his colleagues have pioneered
much needed, global-scale monitoring of persistent organics
in soils [74] and even in local butter [75], exploiting the high
Z values in these integrating media.
THE FUTURE
What, then, is the future of fugacity in environmental sci-
ence? Let me suggest a number of areas.
The unit world concept and fugacity calculations in their
various forms provide an insightful method for characterizing
aspects of the behavior of chemicals as influenced by parti-
tioning and degradation properties. These aspects include per-
sistence, bioaccumulation, and LRT potentials, which are key
attributes in selecting priority substances from among the mul-
titude of chemicals of commerce.
I am convinced that the future of environmental science
lies in being increasingly quantitative about sources, fate, and
effects. The mass-balance approach provides a sound basis for
estimating exposure and for making decisions about acceptable
emissions that will translate into an acceptable risk of toxic
effects. Fugacity models can be invaluable in this context,
especially when applied to both the abiotic and biotic com-
partments of our complex, multimedia environment.
Ultimately, a primary concern of environmental science is
the uptake of chemicals in organisms, their distribution and
conversions within the organism, and the adverse effects that
result from the multitude of possible modes of interaction be-
tween the chemical and the sites of actions. I believe that
viewing these phenomena through the lens of fugacity will
help in the vital process of understanding and quantifying these
pharmacokinetic and toxicokinetic processes.
The important task of monitoring chemicals in the envi-
ronment and interpreting the findings can be assisted by as-
sessing contaminant levels as both concentrations and fugac-
ities. Particularly attractive are monitoring devices that mea-
sure fugacity as a surrogate for concentration.
Perhaps one of the most useful and educationally illumi-
nating aspects of fugacity is that it clearly expresses the con-
cept that all chemicals have the potential to migrate and seek
equilibrium throughout all parts of the environment. This par-
adigm is readily accepted by students. It helps them to accept
the inherent, multimedia nature of the environment and the
Environ. Toxicol. Chem. 23, 2004 2287
need to establish the big picture of chemical fate. As tomor-
row’s regulators, theirs will be the responsibility to manage
chemicals in our environment.
Society now demands that it enjoy the benefits of using a
multitude of chemicals of commerce, such as fuels, plastics,
solvents, coatings, adhesives, pesticides, biocides, and thera-
peutic drugs. It also demands that these chemicals be produced,
transported, and used safely, with minimal risk of adverse toxic
effects as a result of the inevitable occupational, consumer,
and environmental exposures. Mistakes have been made in the
past, largely from ignorance rather than malice. No doubt sur-
prises are in store, such as the recent concern about polyfluor-
inated compounds, but the best guarantee of safety is the ac-
quisition and application of a full and advanced, quantitative
understanding of chemical sources, fate, and effects, and with
an appropriate level of accuracy. This must involve industry,
governments, and academics—the three pillars of SETAC. The
challenge is immense, because chemicals of commerce are so
numerous and so very different in character. Undoubtedly, we
must rely on predictive techniques such as QSARs that relate
chemical structure to properties and on models that predict
chemical exposure and the risk of adverse effects. The fugacity
concept and fugacity models, I believe, can play a valuable
role in this task and, thus, in promoting the safe and sustainable
use of chemicals in our society.
LESSONS LEARNED AND ACKNOWLEDGEMENT
I cannot resist sharing some lessons I have learned on this
journey. First is the remarkable generosity of my colleagues
in environmental science. It is particularly notable, because I
have found such generosity lacking in other fields of science
and engineering. Competition can be so compelling that it
discourages collaboration and collegiality.
In retrospect, the journey to fugacity was tortuous, seren-
dipitous, and totally unplanned. There was never a grant or
contract proposal to develop the fugacity concept, nor could
there have been. That journey would not have been possible
without the unselfish help of individuals such as Brock Neely,
Peter Liss, George Baughman, and Russ Christman. Peter Liss
could have written a nasty letter to the editor, but instead, he
encouraged me to correct my mistake. Russ Christman took a
chance on a new, unproved idea. Promoting an idea such as
fugacity required a lot of help, generosity, and encouragement,
and I, as a young scientist, was indeed fortunate that these
were forthcoming. If one lesson is to be learned from this
journey, it is that we should be similarly generous to the new
breed of young scientists who bring their enthusiasms and
creativity to SETAC.
The founders of SETAC, individuals such as Gene Kenega,
Rich Kimerle, Herb Ward, and their colleagues, displayed re-
markable insight when they conceived of the centrality of the
three constituencies of industry, government, and academics
in environmental science. All three provide essential insights.
My industrial colleagues, especially at Dow, Dupont,
ExxonMobil, and Procter & Gamble, have shared with me their
deep understanding of and concern regarding their chemicals
and their safe use. It is essential to appreciate this attitude and
exploit this knowledge. Governments have the ultimate reg-
ulatory tools to protect the public and the environment. This
is an enormous responsibility that, I find, most individuals seek
to apply based on sound science, but often under difficult
conditions. Academics have the freedom to develop much of
the fundamental knowledge about environmental processes,
2288 Environ. Toxicol. Chem. 23, 2004
and they provide the essential training ground for tomorrow’s
scientists. By bringing these constituencies together and, es-
pecially, by encouraging young scientists, SETAC has made
an immense contribution worldwide. It has been a privilege
to be part of this remarkable movement.
As I reflect on my career, I am struck by how fortunate I
have been in my associations with students and colleagues,
often through SETAC. Many of these have already been men-
tioned, but space prevents me from naming them all. Notable
are my colleagues at UC Davis, Don Crosby and Jim Seiber;
Louis Thibodeaux and K.T. Valsaraj at LSU; and Klaus Kaiser,
who pioneered the QSAR conferences. Warren Lyman, Sam
Yalkowsky, and Gerrit Schüürman have been valued col-
leagues. Phil Howard has made a notable contribution to chem-
ical evaluation through the EPIWIN suite of QSAR models.
Bob Boethling and Bob Lipnick have accomplished so much
in both scientific and regulatory contexts. I have been fortunate
in my many colleagues at Environment Canada, Heath Canada,
and the Department of Fisheries and Oceans, especially Derek
Muir, Ross Nostrom, Ken Lee, Jocelyne Hellou, Dave Kane,
and Robie MacDonald. Otto Hutzinger has been a major in-
fluence on my career, and it was thanks to him that Frank
Gobas and Frank Wania joined our group. Finally, I have been
deeply indebted to my many colleagues at the University of
Toronto and Trent University
I have been incredibly fortunate to have had so many tal-
ented students as well. It has been very satisfying to see them
develop their own careers and enthusiasms. I have learned a
great deal from them, probably more than they learned from
me. The best way to learn environmental science is to teach
it to skeptical and critical students! Three colleagues have
made immense contributions to our research projects and have
been close friends over the years. Wan Ying Shiu did excellent,
meticulous physical chemistry at the University of Toronto for
over 30 years. Sally Paterson was instrumental in developing
the early fugacity and oil spill models at Toronto. Eva Webster
has been my Assistant Director at the Canadian Environmental
Modeling Centre at Trent University and has been responsible
for bringing our models to the Internet.
Finally, none of this would have been possible without the
support and contributions of my wife, Ness, my constant col-
league and companion, and of my sons, Neil and Ian, who
have tolerated my absences and preoccupations during this
long journey.
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