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Periodic Processes for In Situ and On-Site Bioremediation of Leachates and

Soils

Article  in  Water Science & Technology · April 1993

DOI: 10.2166/wst.1993.0539

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Wat Sci. Tech. Vol. 27, No. 7-8, pp. 97-104, 1993. 0273-1223/93 SU-OO
Printed in Great Britain. All rights reserved. CopyrigbtC 19931AWQ

PERIODIC PROCESSES FOR IN SITU AND

ON-SITE BIOREMEDIATION OF
LEACHATES AND SOILS

Robert L. Irvine, Paul S. Yocum, James P. Early

and Robert Chozick
Center for Bioengineering and Pollution Control, P. O. Box G, University of Notre
Dame, Notre Dame, IN 46556, USA

ABSTRACf

Investigators at the University of Notre Dame's Center for Bioengineering and Pollution Control
have conducted research and development studies since 1980 in the broad area of hazardous
waste management. These efforts have been primarily directed at the use of periodic processes.
Many of the findings have been applied to the construction and operation of full scale bioreclama-
tion facilities.

Early research and development activities were directed at the suspended growth, Sequencing
Batch Reactor (SBR). The SBR is an activated sludge-like, periodic process that has been used
effectively for the treatment of both domestic and industrial wastewaters (Irvine and Busch, 1979;
and Irvine and Ketchum, 1989). Due to the time-oriented nature of the SBR, simple operational
modifications have allowed for nutrient removal (Alleman and Irvine, 1980a; Alleman and Irvine,
1980b; Ketchumel. al., 1987; Irvine et. al., 1979; Manning and Irvine, 1985; and Palis and Irvine,
1985) and the control of bulking sludge (Brenner et. al., 1992; Chiesa and Irvine, 1985; Chiesa et.
al., 1985; and Dennis and Irvine, 1979). The SBR has been shown to be a cost effective and
energy efficient means of removing hazardous organic compounds found in industrial wastes and
leachates from landfills (Brenner et. al., 1992; Herzbrun er. al., 1985; Irvine et. al., 1984; Irvine
and Wllderer, 1988; Smith and Wllderer, 1987; and; Ymg er, al., 1987).

The Soil Slurry-Sequencing Batch Reactor (SS-SBR) described by Irvine et. al. (1993) and the
Sequencing Batch Biofilm Reactor (SBBR), a fixed film periodic system that can be used in con-
junction with granular activated carbon (Chozick and Irvine, 1991), were developed in the late
1980's and early 1990's. Recent efforts have been directed at periodically operated in situ biore-
mediation systems. This paper provides a brief overview of how such systems can be used to
bioremediate contaminated leachates and soils.

Key Words: bioremediation, periodic processes, Sequencing Batch Reactor. Sequencing Batch
Biofilm Reactor, Soil Slurry-Sequencing Batch Reactor. in situ treatment

INTROD!!CUQN

Virtually all bioremediation schemes are directed at the enrichment and maintenance of a micro-
bial consortium that will degrade organic contaminants present in leachate and/or soils. This is
usually accomplished by providing the microorganisms naturally present at the site with condi-
tions that are conducive for growth. Often times this involves the aggressive alteration of site con-
ditions. Typically. some combination of water. nutrients, electron acceptors. co-substrates,
surfactants, and. sometimes, additional biomass, are added to encourage the degradation of
organic contaminants. Treatment is carried out either in situ or ex situ (i.e., in reactors). The
ground serves as the reactor for in situ bioremediation. The amendments needed are delivered to
97
 K. L. iK V 1I'1ji::.ellll.

the contaminated source, eliminating the need for soil or groundwater removal. The phrase "pump
and treat" usually describes above-ground reactors that are used for the ex situ bioremediation of
recovered contaminated groundwaters and leachates. Periodic processes developed for the man-
agement of hazardous wastes are described in the next section.

PERIODIC PROCESSES

Reactor based periodic systems consist of one or more identically operated tanks that provide for
the time sequencing of two or more processes or operations (e.g., equalization, biological conver-
sions, and clarification) during a complete reactor cycle. Each cycle may include up to five peri-
ods: fill, react, settle, draw, and idle. Some periodic systems (e.g. those utilizing suspended
cultures or slurried soils) employ mixing and/or aeration to keep the microorganisms in suspen-
sion during fill and react. Mixing and/or aeration are normally turned off to allow for clarification
during the settle period in suspended growth systems. This allows a clear supernatant to be
removed from the reactor during draw and an active culture to be maintained within the reactor
for the beginning of the next cycle. A settle period is not necessary for a fixed film system and
inappropriate for many slurry reactor systems because the resuspension of settled slurries may be
difficult In way of contrast, periodically operated in situ bioremediation systems utilize the
ground as the reactor and involve the periodic addition of the amendments.

The Sequencing Balch Reactor

Conventional suspended growth SBRs are currently being used extensively for the treatment of
both domestic and industrial wastewaters. As is described in detail by Irvine and Ketchum (1989), \
the SBR is uniquely suited for the selection and enrichment of desired microbial populations
because of the ease with which a diverse array of operating conditions and selective pressures can
be implemented. The convenience in its operation stems from the time-oriented nature of the pro-
cess. Specifically, each tank in the SBR system is filled during a distinct period of time. During
this fill period, organism selection can be controlled by manipulating the actual specific growth
rates of the microbes and by regulating the oxygen tension in the reactor (e. g., from anaerobic to
anoxic to aerobic). After a tank is filled, treatment continues with the SBR operating as a batch
reactor. During this react period, further selective pressures are applied by controlling the length
of time the organisms are subjected to starvation conditions. Other activated sludge like periodic
processes, such as the intermittent cycle extended aeration system, do not have the distinct settle
and draw periods of the SBR and are not described in this paper.

The first full-scale application of the SBR was a demonstration study sponsored by the United
States Environmental Protection Agency (U.S. EPA) in 1979. This demonstration involved the
conversion of an existing 0.3 MGD municipal wastewater treatment facility at Culver, Indiana, to
SBR operation (Irvine et. al., 1983). The conversion was based on results obtained from both the-
oretical analyses and bench scale studies. After two years of successful full-scale operation, the
U.S. EPA described the SBR as an innovative and alternative technology.

During the study at Culver, Hooker Chemical Company (now Occidental Chemical Corporation
[DCC]) funded a biological treatment study to investigate the biodegradability of hazardous
organics present in leachate collected from their Hyde Park Landfill. Bench scale and pilot scale
studies using organism selection control strategies which had been previously developed on rather
simple substrates demonstrated that over 90% of the total organic carbon could be removed bio-
logically (Irvine et. al., 1984). DCC used the technology developed by Notre Dame faculty to
construct a full-scale SBR for the biological treatment of Hyde Park leachates.

Based on the experience gained at Culver and early promising results from the DCC study,
CECOS International was able to secure co-funding from the New York State Energy Research
and Development Authority (NYSERDA) to construct a full-scale SBR at their hazardous waste
disposal site in Niagara Falls, NY (Herzbrun er, al., 1985). With on-going direction from Notre
Dame faculty, the utility of biological treatment of hazardous organics was demonstrated. These
were recognized by the Office of Technology Assessment in its April 1985 report titled Superfund
Strategy, which described the SBR as an innovative technology for the treatment of hazardous
wastes. Since this time, over 300 full scale SBRs have been designed and constructed world-wide.
 Bioremediation of Ieacbates and soils 99

The Sequencing Batch Biofilm Reactor

The SBR system has been found to be effective in the treatment of a wide variety of organic con-
taminants present in waters and wastewaters. The SBBR, however, was developed to treat con-
taminated leachates and groundwaters that have low concentrations of organic contaminants and/
or contain volatile organics that can be readily stripped during treatment (Chozick and Irvine,
1991).

The SBBR shown below is a fixed film, periodic process, which utilizes a submerged gas-perme-

OXYGEN
PROBE
EFFLUENT

FEED

OXYGEN
SUPPLY

OXYGEN
PURGE
VALVE

able membrane for both aeration and support of a biofilm. By allowing the biomass to attach to the
silicone coil, the SBBR offers operational and performance advantages associated with attached
growth systems. These include: enhanced biological treatment of organics present at low concen-
trations; maintenance of large numbers of slow-growing organisms; maintenance of organisms
with poor settling characteristics which would wash out of a suspended growth system; elimination
of the need for a settle period in the operation of the SBR, allowing for longer react periods (or
shorter overall cycle times); and minimization of fugitive emissions. While the tubing is primarily
used to supply oxygen as the electron acceptor (Wilderer er. aI., 1985), it can also supply alterna-
tive electron donors (e.g., methane) that may be necessary for the cometabolism of an organic
contaminant (e.g., trichloroethylene). Contaminated gas streams, like those associated with soil
venting described later, may be introduced and treated in a similar manner.

During the past three years emphasis has been placed on the biological treatment of lightly con-
taminated groundwaters containing benzene, toluene, ethyl benzene, and xylenes (BTEX), both
with and without granular activated carbon (i.e., in the GAC-SBBR). All studies to date have been
limited to the bench and pilot scale.

The Soil Slurry-Sequencing Batch Reactor

The treatment of soils in reactors requires significant consideration of materials handling. Screen-
ing and pre-mixing tank systems are needed to remove oversized materials and to prepare a slurry
prior to addition to the SS-SBRs. Final dewatering of the treated soil slurry, either by mechanical
means (e.g., filter presses, vacuum drum filters, centrifugation) or by natural evaporation and per-
colation, must be considered. Complex laboratory studies must be conducted in reactors similar to
the one shown below to determine the desired soil to water ratio, nutrient requirements, contami-
l()() R. L. IRVINE et at.

Air supplied lhrough carbon adsorbers to

microimpinger tube when vacuum appliod
Control valve
Control valve

t=::::::::<=~l:JlII~1:~ V~mn

ubon adsorbers
Sample valve

Magnetic stirrer or orbital mixer

nant destruction rates, and the need for co-substrates. Difficult, time consuming analytical proce-
dures often produce uncertain results. However, the potential cost savings associated with the use
of slurry bioreactors has resulted in considerable attention to these systems in the United States.

Functionally, the SS-SBR system is simply a set of tanks that are operated on a fill and draw basis.
As with the SBR system, each tank is filled during a discrete period of time and then operated as a
batch reactor during react. A notable difference between the SBR and the SS-SBR is that the time
required for react in the SS-SBR is typically in the order of days as opposed to hours for the SBR.
Several possible SS-SBR operating strategies can be employed dependent on the nature of the
contan.inants, the physical properties of the soil and slurry, and on-site factors such as the avail-
ability of process water and the need for recycle. For example, when process water is readily
available and extensive additional treatment of the effluent slurry water will not be required. a
complete reactor cycle includes only three operating periods: fill - time during which slurry is
added to the reactor; react - period where most of the contaminants are biologically removed; and
draw - time in which the treated slurry is withdrawn from the reactor. After draw, a small portion
of the treated slurry would remain in the reactor as an acclimated seed material for the next cycle.
During all periods, agitation and aeration, often provided with a mechanical mixer, are used to
keep the reactor contents mixed. An activated carbon air scrubber coupled to a blower system is
used to provide a continuous supply of fresh air in the reactor headspace. If process water is not
readily available, system operation must be modified to include the immediate reuse of process
water. This water could either be captured during slurry dewatering or obtained as a supernatant
by adding a short quiescent settle period to the reactor cycle before draw.

Bench scale studies have been conducted for soils contaminated with bis-(2-ethylhexyl) phthalate
(BEHP), gasoline, diesel oil, and trinitrotoluene (Irvine et. al., 1993). Results from the BEHP
study will be provided in this paper.

In Situ Bioremediation

Economic delivery of required nutrients and electron acceptors to any subsurface system is lim-
ited by a number of soil properties including permeability, heterogeneity, and ion exchange capac-
ity. For example, because of the ion exchange properties of some soils, the transport of nitrogen
(e.g., as the ammonium ion) to contamination zones remote from the injection sites may be much
less than predicted by convection and diffusion. Similarly, the demand for oxygen may be so great
in soils that contain high concentrations of contaminants that alternative systems of oxygen sup-
ply may be needed. The rate of microbial degradation (i.e., of remediation) is often controlled by
the delivered mass flux of electron acceptors and/or nutrients.
 Bioremediation of teachates and soils 101

Oxygen 'has been delivered for the in situ aerobic biological treatment of contaminated soil by
using either water or air as the carrier, When water is used, air or pure oxygen are bubbled through
fresh or recirculated water prior to the injection of water into the ground. Alternatively, hydrogen
peroxide can be added to the injected water. In any case, the produced water may require treat-
ment in above-ground reactors.

The delivery of oxygen in the water phase may be costly and could increase the potential for
migration of contaminants. Recently air has been used to supply oxygen directly. These in situ
operations are often referred to as "bioventing." Air, drawn through the soil in these bioventing
systems, results in the simultaneous volatilization and in situ biological destruction of the organic
contaminants. Infiltration galleries are often used (especially with sandy soils) to supply water
needed to maintain biological activity. The volatilized or stripped organics may require treatment
in above-ground reactors. As would be expected, the rate of remediation slows as the volatility
and solubility of the residual targeted contaminants decreases with the time.

The periodic operation of in situ bioremediation systems involves the use of both water and air. In
this case the contaminated zone is isolated by multi purpose injection and extraction wells. Ini-
tially, nutrients and moisture are supplied to the targeted area with water. After the injection of
water is terminated, liquid extraction wells remain operational so that contaminants concentrated
in and around the capillary fringe will be exposed to oxygen delivered by air drawn through the
site by suction pumps. When degradation rates diminish (typically determined by the monitoring
of off-gas oxygen concentrations) water is reinjected to provide additional nutrients, moisture,
and other needed amendments. The sequencing of the injection of water and the withdrawal of air
constitutes the periodic in situ bioremediation system.

RESULTS

A laboratory scale SBBR using silicone membrane aeration and a iz-bour operating cycle was
used to treat a BTEX-contaminated groundwater containing between 0.6 and 3.5 mg/L of total
BTEX. This wastewater was typically treated to below 10 µgIL. A synthetic wastewater contain-
ing approximately 115 mgIL of total BTEX. used to examine the effect of higher BTEX concen-
trations on the performance of the SBBR, was typically treated to below 2 µg/L as is shown in the
figure below. Elevated concentrations of BTEX in the influent caused reduced dissolved oxygen

140

120 t Ti
100
::r
a,
.:!. 80
><
ur
60
Iii
~ 40
I-

2:~

0 4 8 12
TIme (hrs)

concentrations, but did not adversely affect the overall performance of the reactor. Accumulation
of biomass over extended operating periods, however, caused a steady decline in dissolved oxy-
gen concentrations in the reactor and eventually led to reduced reactor efficiency. The perfor-
mance of the reactor was improved by the removal of excess biomass after a decline in
performance was observed. A regular biomass wasting strategy is critical to long-term operation.
Total volatile losses from the system accounted for approximately 3.2% of the total voe's
treated, demonstrating the effectiveness of membrane aeration in minimizing fugitive emission
during treatment of wastewaters containing volatile components.
102 R. L. IRVINE <I al.

Laboratory scale SS-SBRs were used to evaluate the bioremediation potential of two soils, one
contaminated with a weathered gasoline, the other with bis-(2-ethylhexyl) phthalate (BEHP) and
total petroleum hydrocarbons (fPH). The weathered gasoline contaminated soil was used to
develop methodologies available to perform both remedy screening and selection studies (U.S.
EPA, 1991) that would potentially be applicable to a number of biologically based processes. An
open reactor system with biologically inhibited controls and a closed system similar to the one
shown previously allowed capture of volatilized organics, determination of evolved CO:!, and
consumption of 02. These systems were used to estimate biological hydrocarbon removal rates .
.Selected data from these studies are shown in the figure that follows.

12000 r----------------,
- Carbon Dioxide
10000 - ....- Oxygen

---&-- TPH
8000

6000

4000

2000

1 2 3 4 5 6 7
Time (Days)

The hydrocarbons contained in the soil were analyzed with several different GC columns and
detector configurations, and compared with GC/MS results. Methods were developed which
allowed determination of available nitrogen and phosphorus concentrations in the soil slurry envi-
ronment. The results of this investigation showed that greater than 95% of the aged gasoline
hydrocarbons could be biologically degraded in less than 7 days to a soil concentration of less
than 10 mg/kg.
The BEHP contaminated soil posed an interesting problem since no reference to the biodegrada-
tion of BEHP in a soil environment could be found in the literature. After demonstrating that the
indigenous microbial populations could mineratize BEHP, slurry reactors were used to determine
nutrient requirements and BEHP and TPH removal rates. Results obtained for BEHP removal are
shown in the figure that follows. .
 Bioremediation of leacbates and soils 103

30000

-
:s.,
.....
..
'0

.I<:
Oil
20000

1 \ -0-
Bioreactor
Control
E
.5 10000
~
::t::
=
r-l

0
0 10 20 30
Days
A bench scale soil-venting system has been employed to investigate bioremediation of a weath-
ered diesel fuel contaminated soil. Both air and amended water are circulated through the soil in
this system. Traps for water and volatilized organics allowed mass balance calculations on the
contained soil. To minimize spacial contaminant variations, initial studies used homogenized soil
that was recompacted to the initial measured value of air permeability, Following initial saturation
with nutrient solutions. moderate air flow rates (10 pore volumes/day) have resulted in removal of
1f3 of the initial contaminants in 30 days with minimal volatilization or leaching (less than 0.1 %
of the total removal), Results have also shown that the rates of remediation are increased appre-
ciably (as determined by the monitoring of off-gas carbon dioxide and oxygen concentrations)
after the reinjection of water. This suggests that the concentration of organic contaminants in the
liquid phase may be increased during the periodic wetting events.

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reactor operation. Water Res. 14. 1483.
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waste in an SBR. Water Environ. Res. 64, 128.
Chiesa, S. C., Irvine, R. L., and Manning, Jr., J. F. (1985) Feast/famine growth environments and
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