Engineered passive bioreactive barriers: risk-managing the
legacy of industrial soil and groundwater pollution
Robert M Kalin
Permeable reactive barriers are a technology that is one decade
old, with most full-scale applications based on abiotic
mechanisms. Though there is extensive literature on engineered
bioreactors, natural biodegradation potential, and in situ
remediation, it is only recently that engineered passive
bioreactive barrier technology is being considered at the
commercial scale to manage contaminated soil and groundwater
risks. Recent full-scale studies are providing the scientific
confidence in our understanding of coupled microbial (and
genetic), hydrogeologic, and geochemical processes in this
approach and have highlighted the need to further integrate
engineering and science tools.
Addresses
Environmental Engineering Research Centre, School of Civil
Engineering, The Queen’s University of Belfast, Belfast BT9 5AG,
Northern Ireland, UK
e-mail: r.kalin@qub.ac.uk
Current Opinion in Microbiology 2004, 7:227–238
This review comes from a themed issue on
Ecology and industrial microbiology
Edited by Elizabeth Wellington and Mike Larkin
Available online 10th May 2004
1369-5274/$ – see front matter
ß 2004 Elsevier Ltd. All rights reserved.
DOI 10.1016/j.mib.2004.04.014
Abbreviations
MNA monitored natural attenuation
NA
natural attenuation
PRB
permeable reactive barrier
‘Environmental Engineering is the integration of the
built environment within the natural environment using
science and engineering to meet the principles of social,
economic and environmental sustainability’ Prof. Robert
M. Kalin
There are three primary strategies used separately or in
conjunction to reduce or eliminate the risk of contaminants in soil and groundwater:
1. Destruction or alteration of contaminants.
2. Extraction or separation of contaminants from environmental media.
3. Immobilization of contaminants.
There is a variety of both in situ and ex situ treatment
technologies capable of contaminant destruction by altering the chemical structure including thermal, biological
and chemical treatment methods. Highly engineered
treatment technologies that are commonly used for
extraction and separation of contaminants from environmental media include soil treatment by thermal desorption, soil washing, solvent extraction, soil vapour
extraction and ground water treatment by either phase
separation, carbon adsorption, air stripping, ion exchange,
or by some combination of these technologies. Immobilization technologies are generally only applied to soilbased contamination and include stabilization, solidification and containment technologies, such as placement in
a secure landfill or construction of cement-bentonite
slurry walls. However, the contaminants have not been
treated and it is now realized that no immobilization
technology is permanently effective.
The development of our current societal infrastructure
and standard of living has produced a legacy of land and
groundwater that is contaminated with potentially harmful inorganic and organic compounds. At the turn of the
new millennium much of the developed world turned its
attention to ‘sustainability’ where emphasis is now
placed on a balance between economic, social and environmental issues. This change in emphasis on integration
of the natural and anthropogenic environments is summarized in the following two quoted mission statements:
To this end, it has been realized over the past three
decades of environmental remediation that it is not
possible to use engineering to completely degrade all
contaminants that have been released to the environment. Thus, the development of remediation technologies to degrade these compounds has moved from
strongly intensive in situ and ex situ treatments to combined engineered and passive/natural approaches (treatment train) that manage the risks associated with the
‘source’ of the contaminants, the ‘pathways’ of flux and
contaminant transport and impact on the ‘receptor’
which may either be human health related or additional
environmental impact.
‘We will be recognized as the leading source of knowledge
and skills required to create a sustainable natural and
built environment for the benefit of future generations’
Institution of Civil Engineers (ICE) UK Vision Statement
One of the main obstacles to implementation of this
‘sustainable’ approach to dealing with contaminants in
soil and groundwater is the added costs, in time and
money, required to manage the risks of contaminants
Introduction
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Current Opinion in Microbiology 2004, 7:227–238
228 Ecology and industrial microbiology
in the environment. As a generalisation, the dominant
ex situ method for dealing with contaminated soil has
involved digging up much of the contamination and
disposing it in landfills. However, both legislative pressure and the increased costs of land-filling (both in the
UK, the EU and other countries) and a world-wide move
towards more sustainable remedial technologies are
prompting developers to consider alternative in situ and
ex situ methods of dealing with organic contaminants.
Alternative remediation technologies that permanently
destroy or detoxify contaminants are becoming commonplace in the USA, Australasia and European countries.
natural carbon substrates. Other complicating factors
whereby natural degradative processes are limited
include nutrient availability, redox conditions, substrate
competition, bioavailability, toxicity and a combination of
geologic, geotechnical and hydrogeologic factors that
make the subsurface an immensely complex environment. An evolution of approach is needed which develops
a conceptual understanding of all elements and identifies
knowledge gaps. There is also a need for further development/refinement of tools for site study that will provide
an understanding of the rate controlling mechanisms for
natural biodegradative processes [23–25].
The complete degradation of man-made or xenobiotic
chemicals by microorganisms in the environment is universally considered to be beneficial. In particular, those
high priority pollutants of soils and groundwater’s that are
regarded as carcinogenic and toxic (EU Council Directive
2000/60/EC). The concept of ‘microbial infallibility’ with
respect to biodegradation has long been the assumption.
Indeed, Stanley Dagley concluded in his introduction to
the text ‘Microbial Degradation of Organic Compounds’ that
‘On thermodynamic grounds, no organic compound can
be excluded from serving as a possible energy source for
aerobic microorganisms’.
In this review, I have chosen to write from the ‘engineering’ perspective and briefly touch upon a wide range of
both engineering and science issues that must be considered for implementation of passive bioreactive barrier
technology. This includes not only the microbiological
biotransformations, but also where the technology has
come from (including abiotic transformations), the wide
scope of issues that are needed to design the engineering
of a bioreactor that must operate with little or no maintenance for decades, and cost effective and rapid ways of
monitoring the ‘health’ of the system.
Engineered passive bioreactive barriers
Some of the most promising alternative technologies are
based therefore on bioremediation [1–3]. When considered from an ‘engineering’ perspective, there are two
general approaches to microbial biodegradation i) those
that use engineered or inoculated microorganisms [4–6],
or ii) those that use natural microbial biodegrative potential [7–17,1819] in technologies such as bio-sparging,
bio-slurping and natural attenuation (NA) [20–22]. Of
these biological technologies, NA has received significant
attention. NA relies on the indigenous microbial population and aquifer nutrients to biodegrade contaminants.
Monitored natural attenuation (MNA) can be used for
risk management and as a remediation method for contaminant plumes. The application of MNA can be limited
by nutrient availability and/or high risks associated with
contaminant movement, hence at some sites the potential
to use NA as a risk management strategy is poor and
intervention is necessary.
There is a plethora of publications in the literature that
describe microbial species, populations and mechanisms
for biotransformation of potentially hazardous compounds, but many of these publications focus on a very
limited number of substrates. ‘Real’ sites may have many
hundreds or thousands of contaminants partitioned
between soil, water and vapour phases, and for which
bioremediation is expected to provide a successful reduction in risk. Engineering a sustainable bioremediation
solution depends on long-term microbial populations that
will biotransform a significant number of contaminant
substrates and metabolites as well as a superfluity of
Current Opinion in Microbiology 2004, 7:227–238
Permeable reactive barriers (PRBs) are a passive intervention remediation technology [26–31] that have been
used for risk-management in even the most extreme
environments found on earth [32,33,34,35,36]. In
PRB systems contaminated groundwater passes through
an in situ reactive material that either biotically or abiotically degrades the contaminants. PRBs are unique
because they can be engineered to prevent contaminant
movement across site boundaries before risk receptors, or
simply to cut-off the source of a contaminant plume that
then dissipates via NA processes. By far the most successful PRB technology to date is barriers of zero-valent iron
[37–43,44,45]. The laboratory, pilot scale and full-scale
experience, of which there are nearly 80 installations
world-wide, have been shown to abiotically degrade
chlorinated solvents such as trichloroethene and tetrachloroethene, trace metals and radionuclides, and inorganic contaminants such as nitrate and sulphate/sulphide
[46–56]. Microorganisms have a greater scope for transformation of a wide range of compounds and recent
studies are examining synergetic degradation between
abiotic zero-valent iron and biologic processes [57,58].
There is a considerable research effort to continually find
new abiotic methods for destruction of contaminants
using passive techniques [59–61,62,63]. PRBs using
activated carbon can remove many organic contaminants
from groundwater through sorption (non-destructive process), but some compounds may not be removed, or if
inappropriately designed, the effect of ‘roll-up’ may end
in chromatographic effects that release concentrations of
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Engineered passive bioreactive barriers: risk-managing the legacy of industrial soil and groundwater pollution Kalin 229
contaminants in higher concentration than was originally
observed [64–67,68,69,70,71].
tion of contaminated soil and groundwater for most compounds of concern [91–103,104,105,106,107].
The recent advancement on this technology is to use
engineered passive bioreactors in situ to take advantage of
the potential for microbial biotransformation of potentially hazardous compounds. Bioreactive ‘zones’ have
been engineered to change redox conditions or provide
substrates/nutrient that facilitate the natural biodegradative system [72–81]. Current biological reactive zones rely
on either dissolved nutrients or injected nutrients to
support the biodegradation of contaminants passing
through the ‘barrier’. Delivery of nutrients throughout
a barrier has been shown to be hydrologically difficult and
can add considerable expense to a remediation project.
Additionally, there is the potential that media must be
replenished periodically.
The engineering challenge was therefore to take existing
knowledge and expertise and apply it passively using only
the inertia of natural groundwater systems to transport a
flux through the bioreactive barrier, and design systems
capable of operation for years to decades with little or no
maintenance. The overall performance of a bioreactive
PRB must also balance the rate of contaminant degradation with the flux of contaminants entering the reactive
zone. Laboratory batch and column studies using real site
water and microbial populations can provide an estimate
of the rate of biotransformation [108–112,113,114,115,
116,117]. However, there are a large number of variables
that could be examined and it often takes significant
research to elucidate the major factor(s) that control
the occurrence and rate of biodegradation. Figure 1 presents a flow diagram of the decision making and design
process for implementation of a PRB. An integral part of
evaluation is laboratory and pilot scale experiments that
study, under site conditions, the operational windows for
in situ bioreactive barrier methods [118–121,122] before
Given the complexity of the subsurface, passive bioreactive barriers have applied the principles and knowledge
used in the biotransformation of potentially hazardous
compounds with bioreactor technology [82–89,90]. Ex
situ bioreactors have been used successfully for remedia-
Figure 1
Risk assessment
Solution identification
Site investigation
Hydrogeology
Flux
Biogeochemistry
Microbiology
Identification
of knowledge
gap
Pilot scale
trial studies
Microbiology
Geochemistry
Evaluation of
pilot scale
Modelling
Design and
implementation
Scale up to
design
criteria
Engineering
Evaluation
Full scale PRB
evaluation
Evaluation
Microbiology
Geochemistry
Current Opinion in Microbiology
In situ passive remediation of contaminants in soil and groundwater (e.g. Permeable Reactive Barrier, PRB) must integrate the rate flux of
substrate transport or availability, rates of natural or enhanced biodegradation with evaluation of the temporal uncertainty in each of these parameters
to allow design and implementation. It will be essential that large complex genetic databases are easily available (at minimal cost) so that the
emerging array technology can reach its ultimate potential and provide rapid and detailed feedback for remediation science and technology.
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Current Opinion in Microbiology 2004, 7:227–238
230 Ecology and industrial microbiology
design and full-scale implementation of bioreactive PRB
systems [123–132,133,134,135,136]. One of the most
significant single-use sources of contaminated soil and
groundwater in the UK and Europe is former coal gasification sites. The long and complex history of these
activities has resulted in a wide range of compounds
in soil and groundwater that require risk-management.
There is a significant body of literature on the biotransformation of many of these compounds [137,138,139–
141], the use of ex situ bioreactor techniques [142–144]
and recent applications of pilot-scale to full-scale PRBs
for risk management of these sites [145–151]. Significant
collaborative research on full-scale engineered bioreactive barrier systems at two UK Sites is on-going between
two research groups at the Queen’s University Belfast
(QUESTOR Centre and Environmental Engineering
Research Centre), Oxford University and the University
of Surrey, and two industrial partners, Second-Site
Property Holding Ltd, and Parsons Brinkerhoff.
Figure 2 shows the site and bioreactor layout for one
of the projects on Sequential REactive BARrier (SEREBAR) remediation of contaminated groundwater, the
results of this research has highlighted the need for
integration of science and engineering when implementing this technology.
Of particular note is the difficulty for prediction of not
only how a bioactive barrier might adapt and function
over timescales that range from days to decades, but also
how to measure temporal changes in microbial populations. Figure 3 depicts a conceptual/hypothetical series of
changes in microbial ecology or genetic diversity over
time or resulting from shocks to the bioreactive barrier.
Chemical monitoring of the system provides confirmatory
cause/effect information on the end-result of biotransformation, or lack thereof, but can provide little predictive
Figure 2
SEquenced
REactive
BARrier
(SEREBAR)
Abiotic
Anaerobic
Aerobic
Sorptive
Current Opinion in Microbiology
Site and design drawings of the engineered bioreactive barrier for project SEREBAR at a former coal gasification site in the UK combining site
groundwater flow and contaminant flux with abiotic, anaerobic biotransformation, aerobic biotransformation and abiotic sorption stages.
Current Opinion in Microbiology 2004, 7:227–238
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Engineered passive bioreactive barriers: risk-managing the legacy of industrial soil and groundwater pollution Kalin 231
Figure 3
Declining diversity
Increasing microbial diversity
or degradation potential
Increasing diversity
Adaptive diversity
Toxic event
Toxic event
Toxic event
Adaptive Biofilm
Toxic event
Biofilm not affected
Biofilm strongly affected
0
5
10
15
Time (months)
20
25
30
Current Opinion in Microbiology
In situ passive treatment of groundwater and soil is a process that takes months to decades and there is a lack of extant knowledge vis-à-vis the
long-term response of microbial biodegradation on these time scales. There are several potential changes in microbial biodegradative potential
over time, hypothetical variations shown here, which must be evaluated by the emerging body of research into this technology (e.g. the UK
BBSRC Link and CLAIRE project SEREBAR). Note: A toxic event may reflect an abrupt change in substrate, nutrients or concentration.
measure of the ‘health’ or ‘sustainability’ of the microbial
populations doing all the work.
There is a challenge to find cost effective and time
efficient ways to monitor these systems at the biofilm/
microbiological level. On-line automated measurement is
needed of toxicity, respiration, identification of metabolites, and potentially, direct methods [152–161,162]. The
increasing use of isotopes, either natural abundance or
labelled compounds provides direct evidence of substrate
Table 1
Typical time frames for PRB implementation.
Task
Timeframe
Technology selection
Preliminary site evaluation and risk assessment
Hydrogeologic study
Detailed biogeochemical site evaluation
Choice of technology generally 4 to 26 weeks
1 to 12 weeks
4 to 26 weeks
4 to 12 weeksa
PRB remediation validation
Hydrogeologic/contaminant flux modelling
Laboratory trials/kinetics of reactions
Conceptual design
Pilot scale studies and conceptual design period generally 5 to 19 weeks
2 to 12 weeks
5 to 15 weeksa
2 to 4 weeks
PRB tender and construction
Engineering design
Implementation/construction
Engineering design and implementation generally 14 to 30 weeks
2 to 4 weeks
10 to 26 weeks
PRB operation
Monitoring and maintenance
Years to decades
In general, is takes between 6 months and 1.5 years for implementation of passive PRB technology. aHowever, there is a limited window
of opportunity during which detailed microbial evaluation and results are able to provide specific design parameters. It is imperative that the
microbial genetics revolution develops a capability to provide detailed understanding of both site investigation soil and groundwater samples
and laboratory trials in a highly time efficient manner if this data are to be used in Engineering Design to its greatest potential.
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Current Opinion in Microbiology 2004, 7:227–238
232 Ecology and industrial microbiology
utilization [162,163–167,168]. However, the greatest
potential lies with array techniques that elucidate large
amounts of genetic information on both expression and
potential of the microbial community [169–175,176,
177]. The challenge will be providing a rapid, cost
effective routine and reliable monitoring application of
this technology. In particular, there is need to model the
short-term and long-term behavior of engineered passive
systems. A significant research effort is needed to couple
predictive modeling of microbial behavior [178,179,180,
181,182], microbial transport and establishment
within the bioreactor [182,183–188,189], the formation and behavior of the resulting biofilm [190–193]
within the predictive design and modeling of full-scale
PRB systems [194–201], and the response of bioremediation to changes in operational parameters [202–204].
A further challenge is to provide this information within a
‘typical’ project management time-line for an engineered
PRB system such that the information can play a crucial
role in the conceptual model, design and implementation.
Table 1 presents recent experience on the evaluation,
design and implementation of engineered bioreactive
PRBs and the associated time-scales for sites in the
UK. There is often only a matter of weeks during which
sample collection, microbial evaluation and substrate
utilization, and predictive study can take place. For
detailed design, the results of microbial investigation
must also be interpreted side-by-side with hydrogeological, biogeochemical and engineering results. Without
readily available rapid and robust (inclusive and dependable) screening methods, there will continue to be a
limited ability for detailed microbiological study to provide predictive design input for full-scale engineering,
and thereby have the greatest benefit for implementation
and monitoring of novel ‘sustainable’ technology.
Conclusions
Sustainability, economic, social and environmental,
requires implementation of contaminated land and
groundwater risk-management on decadal time scales.
Although significant scientific understanding of natural
bioattenuative processes has emerged, there is a current
lack of knowledge or engineering experience that allows
the accurate prediction of the long-term sustainability of
passive engineered bioremediation systems for soil and
groundwater. The challenge for the future is to use the
potential of emerging microbial genetic methods to provide a prediction of long-term changes in microbial biodegradative potential in combination with hydrogeological,
biogeochemical, geotechnical and engineering understanding for effective design and implementation.
Acknowledgements
The author would like to acknowledge years of discussion and research with
collaborators at QUB and in the QUESTOR Centre, in particular Mike
Larkin, at Oxford University, at the University of Surrey, in particular
Stephan Jefferis, and members of PRB-Net, in particular Robert Puls
Current Opinion in Microbiology 2004, 7:227–238
of the US EPA. The research experience of the author has been supported
by the BBSRC, EPSRC, NERC, EA, and by industrial partners/collaborators,
in particular the QUESTOR Industrial Board, Second-Site Property
Holdings Ltd, Keller Ground Engineering, and Environmental
Technologies (ETI).
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32. Farrell RL, Rhodes PL, Aislabie J: Toluene-degrading Antarctic
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An example of using by-products from other processes (in this case
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This is a very recent paper clearly showing how laboratory data can
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A wonderful field demonstration of a bioreactive permeable reactive
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All who are interested in sequential treatment steps during passive
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providing the ‘whole’ picture for combined anaerobic/aerobic degradation of mixed chlorinated hydrocarbons and benzene, toluene, ethylbenzene and the xylenes.
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hydrocarbon (PAH) degradation. However, the relative rates of reactions
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A good candidate for application of molecular techniques.
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156. Franzmann PD, Zappia LR, Power TR, Davis GB, Patterson BM:
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