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Management of hydrocarbon-contaminated soil through bioremediation and landfill disposal at a remote location in Northern Canada1 David Sanscartier, Kenneth Reimer, Barbara Zeeb, and Karen George

Abstract: Northern communities often have limited resources to resolve petroleum hydrocarbon (PHC) contamination. This project investigated an innovative approach for the management of diesel-contaminated soil in a remote community in Labrador. The soil was first treated in a passively aerated biopile to reduce the concentrations of mobile PHCs. The treated soil was then disposed of in the local landfill. Maximum total petroleum hydrocarbon (TPH) concentrations in soil, concentrations of PHCs with less than 16 carbons in soil, and TPH in leachate decreased during the 1 year field treatment. Microcosms incubated at 7 and 22 8C in the laboratory showed the potential for biodegradation of the PHCs. However, volatilization was likely the predominant PHC removal mechanism in the field. Disposal of treated soil to landfills has the advantage of transforming waste (i.e., soil) into a valued product (i.e., cover for the refuse). The development of risk-based guidelines for the disposal of PHC-contaminated soil into landfills in Canada appears to be needed and is discussed in this paper. Guidelines should be protective of the environment while prevent over-treatment of the soil, which may result in unnecessary spending and environmental impacts. The cost of the system tested was compared to that of treating soil in an off-site facility. Key words: bioremediation, biopile, petroleum hydrocarbons, diesel, north, contaminated sites, remote location, landfill disposal, cost estimate, soil management practices. Re´sume´ : Les communaute´s du Nord ont souvent peu de ressources pour assainir la contamination aux hydrocarbures pe´troliers (HCP). Ce projet a examine´ une approche innovatrice pour la gestion de sol contamine´ au die´sel dans une communaute´ e´loigne´e au Labrador. Le sol a d’abord e´te´ traite´ par biopile passivement ae´re´e pour re´duire les concentrations de HCP mobiles. Le sol traite´ a ensuite e´te´ e´tendu dans le de´potoir de la communaute´. Les concentrations maximales d’hydrocarbures pe´troliers totaux (HPT) dans le sol, les concentrations d’HCP ayant moins de 16 carbones dans le sol et les HPT dans le lixiviat ont diminue´s durant le traitement d’un an sur le terrain. Des microcosmes incube´s a` 7 et 22 8C en laboratoire ont de´montre´s le potentiel de biode´gradation des HCP. Cependant, la volatilisation a pu eˆtre le me´canisme pre´dominant de re´duction des HCP. L’e´limination de sol traite´ dans un de´potoir a comme avantage de transformer un de´chet (c.-a`-d., le sol) en un produit de valeur (c.-a`-d., recouvrement pour les de´chets). Le de´veloppement de normes base´es sur le risque pour l’e´limination de sol contamine´ aux hydrocarbures au Canada semble eˆtre requis et est couvert dans cet article. Les normes devraient prote´ger l’environnement tout en e´vitant le traitement excessif du sol, pouvant re´sulter en des de´penses et des impacts environnementaux superflus. Le couˆt du syste`me teste´ a e´te´ compare´ a` celui de traiter le sol hors-site. Mots-cle´s : bioreme´diation, biopile, hydrocarbures pe´troliers, die´sel, nord, site contamine´s, location e´loigne´e, e´limination en de´potoir, e´valuation des couˆts, approches de gestion de sol. [Traduit par la Re´daction]

1. Introduction In Canada, approximately 60% of contaminated sites involve petroleum hydrocarbon (PHC) contamination (CCME 2008a), including sites in the North. Treating PHC contamination in cold remote regions is difficult due to the short summers, suboptimal environmental conditions, remoteness,

and limited local infrastructure (Aislabie et al. 2006; Schiewer and Niemeyer 2006). In Northern Canadian communities, the lack of financial resources and technical knowledge makes it difficult to initiate remediation projects. Contaminants are often left in the ground where they can pose risks to human health and the environment (CCME 2008a). When resources are available,

Received 3 April 2009. Revision accepted 8 September 2009. Published on the NRC Research Press Web site at cjce.nrc.ca on 26 January 2010. D. Sanscartier, K. Reimer,2 B. Zeeb, and K. George. Environmental Sciences Group, Department of Chemistry and Chemical Engineering, Royal Military College of Canada, PO Box 17000 Stn Forces, Kingston, ON K7K 7B4, Canada. Written discussion of this article is welcomed and will be received by the Editor until 31 May 2010. 1A

paper submitted to the Journal of Environmental Engineering and Science. author (e-mail: [email protected]).

2Corresponding

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the contaminated soil is often shipped off-site instead of being treated on-site for lack of facilities for treating the soil in the community. Unfortunately, off-site treatment may have greater overall environmental impacts than onsite treatment due to transport of the soil over long distances (Sanscartier et al. 2010). Bioremediation is now recognized as possibly the most attractive and cost-effective clean-up approach for PHCcontaminated soil in Polar Regions (Aislabie et al. 2006). Ex-situ bioremediation (e.g., biopile, landfarm) is likely to be the strategy of choice in cold regions due to the difficulty of properly controlling limiting conditions with in situ bioremediation (e.g., bioventing) (Aislabie et al. 2006). Studies have shown the potential of a simple passively aerated biopile system (i.e., perforated pipes protruding from soil) to remediate diesel-contaminated soils in the Arctic (Mohn et al. 2001; Thomassin-Lacroix et al. 2002) and southern Canada (Sanscartier et al. 2009a). Once treated below environmentally-safe levels, PHCcontaminated soils can be disposed of in local landfills. This approach has been used at locations in Northern Canada (THR 2004; Pouliot et al. 2007).There are numerous benefits of using this approach: (i) it transforms the waste soil into a valued product (i.e., cover for the refuse), (ii) it avoids consumption and transport of material needed as cover (e.g., gravel, sand) and destruction of land (i.e., quarries), (iii) it avoids the transport of the contaminated soil over long distances, and (iv) it can reduce the cost and the pressures on the environment of both remediation and waste disposal. The main objective of the current study was to investigate this innovative practice for the management of soil contaminated with weathered diesel fuel at a remote community in Labrador. The soil was first treated in a passively aerated biopile to reduce levels of the low-molecular-weight mobile PHCs, thereby preventing their migration to the nearby ocean once the soil was disposed of in the unlined local landfill. The pilot-scale project was complemented with a laboratory study. PHC-contaminated soil collected in the field was incubated at 7 and 22 8C. Cost estimates were calculated for this remediation option and that of an alternative option (i.e., off-site treatment). Finally, the current ban on the disposal of PHC-contaminated soil to landfills in Newfoundland and the need for risk-based guidelines for this practice in Canada are discussed. Another goal of the project was to share knowledge on the remediation of the PHC contamination with the local governments and community members of the Labrador coast by involving them in the project.

2. Methods and materials 2.1 Case-study description Soil contaminated with weathered diesel was identified in a residential–commercial area of Hopedale, Labrador, Canada (55827’N, 60813’W). A risk assessment showed that the soil ingestion exposure pathway posed unacceptable risks to on-site residents (Jacques Whitford Environment 2003). A decision was made to remove the contaminated soil from the site to eliminate risks. Hopedale (pop. ~600) is a remote community only accessible by air or boat via Goose Bay, Labrador. It is character-

Can. J. Civ. Eng. Vol. 37, 2010

ized by a cold and moist climate with relatively short summers and long winters (EC 2008). Two options were considered to handle the contaminated soil: (1) building a temporary treatment facility on site or (2) packaging the contaminated soil into 1 m3 bags and shipping them ~800 km by barge to a permanent treatment facility in Goose Bay, the regional center for Labrador. Treatment in the off-site facility involves windrows of soil periodically turned with a front-end loader. In both options, the treated soil is ultimately disposed of in an unlined local landfill. Option 1 was chosen. A biopile was built at the landfill site located 1.3 km from the community and ~200 m from the Atlantic Ocean. There is no infrastructure (i.e., power and fresh water) at the landfill. Landfarming was considered for on-site treatment but was rejected due to the very limited level ground at Hopedale. The soil on site is coarse-grained with 46% gravel, 52% sand, and 2% particles < 0.075 mm. It is characterized by  low inorganic nitrogen (NO 3 þ NO2 : 2.1 mg/kg and NH3: 3.2 mg/kg) and orthophosphates (20 mg/kg), low total organic matter content (0.7%), and a pH of 7.8. 2.2 Microcosms A microcosm experiment was conducted in the laboratory with soil collected in the field, stored at –20 8C until used in the experiment, to assess the bioremediation potential of the soil and PHC removal mechanisms (i.e., biodegradation and volatilization). Individual microcosms were composed of 50 g of sieved (1 cm) contaminated soil (equivalent dry weight) in sealed 500 mL Mason jars. The contaminated soil was incubated for 110 d in four treatments: (1) amended with fertilizers at 7 8C (A7), (2) amended with fertilizers at 22 8C (A22), (3) poisoned control at 7 8C (C7), and (4) poisoned control at 22 8C (C22). Microcosms amended with fertilizers received urea and diammonium phosphate (DAP) to concentrations of ~0.120 mg N/g soil and ~0.017 mg P/g soil. The control microcosms were poisoned with 3 mg sodium azide (NaN3)/g dry soil to inhibit microbial activity (as per Thomassin-Lacroix et al. 2002) and did not receive fertilizers. Fertilizers and NaN3 were added as solutions. Biostimulation has been found to enhance bioremediation in numerous studies; recommended nutrient application rates vary widely but low rates appear to be optimal in coarse-grained soils (Braddock et al. 1997; Schiewer and Niemeyer 2006). Application rates used in the current study were chosen based on the results of previous experiments in our laboratory with soils from other locations in Northern Canada (Reimer et al. 2003). Incubation at 7 8C simulated the average temperature at the site during the warm months while incubation at 22 8C evaluated bioremediation in more suitable conditions. Moisture content was adjusted to 18% moisture by weight. Each treatment was tested in triplicate microcosms (total of 12 jars). Soil respiration (CO2 evolution) was monitored based on Alef (1995). Petroleum hydrocarbon concentrations were measured from triplicate soil samples prior to start of the experiment and from one sample collected from each of the 12 jars at the end of the experiment. 2.3 Field biopile The biopile was constructed over a 10 cm layer of clean sand within a bermed area lined with 0.76 mm XR5 8130 Published by NRC Research Press

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Fig. 1. The passively aerated biopile. The locations of the soil gas probes (SG) and the direction of prevailing wind are indicated.

reinforced geomembrane (Seaman Corp.) in August 2006 (Fig. 1). The pile measured 7.8 m wide  16 m long  1.2 m high giving a volume of ~112 m3. Vertical and horizontal aeration pipes made of 3@ polyvinyl chloride (PVC) and 4@ perforated high-density polyethylene (HDPE) pipes, were laid out in the direction of prevailing winds and left protruding from the soil pile, to promote air circulation within the pile (Fig. 1). Treatment ended in September 2007. The same types of fertilizers as in the microcosm study were applied to the soil in dry granular form at the same application rates. Small portions of each fertilizer were mixed into each dump truck load of soil. Once the biopile was built, urea was spread on top of the pile and mixed into the soil manually. Totals of 40 kg of urea and 13.6 kg of DAP were applied. During treatment, leachate water that collected in the containment area was sprayed onto the surface of the biopile. This served to redistribute water, nutrients, and PHCs. In case of excessive wastewater and saturated soil, the water was pumped through a filter before being released to the environment. Thirty and 35 samples were collected from the biopile in August 2006 and July 2007, respectively, in 125 mL amber jars with Teflon lined lids and stored at –20 8C until analysis. Samples were collected from the soil surface (0–10 cm) and at depth (70–80 cm). Soil-gas CO2 levels were measured during a period of 24 h at the last visit on site (3–4 September 2007) with a portable gas analyzer (ATX-620, Industrial Scientific) from three soil-gas probes installed in the soil to a depth of 80 cm during construction of the biopile. A fourth probe was initially installed on the same side of the pile as SG1 but was inadvertently damaged and could not be used. The ends of the aeration pipes were sealed during CO2 monitoring. 2.5 Analytical methods Hydrocarbon concentrations in soil were measured using the Canada-Wide Standard for petroleum hydrocarbons in soil (PHC-CWS) reference method (CCME 2001). This method defines four PHC fractions based on boiling point of n-alkanes as follows: F1, nC6-nC10; F2, >nC10 to nC16; F3, >nC16 to nC34; and F4, >nC34. For F1, a purge and

trap extraction technique was used, and for the other three fractions, solvent extraction was used. Extracts were analyzed by gas chromatography with flame ionization detection (GC/FID). A SPB-1 fused silica capillary column (30 m, 0.25 mm i.d.  0.25 mm film thickness) was used for F1 while a DB-1 capillary column (15 m, 0.53 mm diameter, 0.15 mm film thickness) was used for F2 to F4 fractions. For the microcosm study, PHC analysis was limited to the determination of the concentrations of F2 to F4 because fraction F1 only accounted for ~7% of the initial contamination in the biopile and was not detected at the end of treatment. The extracts of fractions F2 to F4 of field-collected samples were also analyzed with GC/FID fitted with a SPB1 fused silica capillary column (30 m, 0.25 mm i.d.  0.25 mm film thickness) allowing a better separation of PHCs than with the shorter column and quantification of the individual compounds nC17, nC18, pristane (2,6,10,14tetramethylpentadecane), and phytane (2,6,10,14-tetramethylhexadecane) (based on USEPA 2000). The PHC concentration in the leachate was determined with soil samples collected from the biopile before and after treatment to evaluate the effectiveness of treatment and potential migration of the contaminant to the nearby ocean after spreading the soil in the landfill. For each sampling event, samples were combined and homogenized. Leachates were produced in triplicate subsamples by tumbling 45 g of the homogenized soil in 1 L Teflon bottles filled with 900 mL of TCLP solution #1 for 24 h (USEPA 1992). For the analysis of PHC concentrations in leachate, 75 mL of the leachate sample was placed in a 125 mL glass separatory funnel. Hexane (5 mL) was added and the mixture shaken vigorously and allowed to separate. If emulsions formed, the funnel was briefly sonicated to ensure adequate phase separation. An aliquot of the extract was analyzed by GC/ FID and total petroleum hydrocarbons (TPH) was quantified (USEPA 2000). In this paper, the term ‘‘TPH’’ refers to the concentration of PHCs in both soil and leachate. For samples analysed by the CCME (2001) method, TPH is defined as the sum of F1 to F4 concentrations. Initial soil characteristics were determined with samples Published by NRC Research Press

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collected before adding fertilizers. The hydrocarbondegrading microbial population (PHC-degraders) was quantified by spread plate count using diesel fuel as the sole carbon source (Sanscartier et al. 2009b). Ammonia (NH3),  nitrate + nitrite (NO 3 þ NO2 ) (reported as one compound), 3 and orthophosphates (PO4 ) were determined on digested samples using colorimetric methods 4500-NH3 G, 4500NO3 H, and 4500-P (APHA 2005). Particle size distribution was carried out by sieve analysis (grains > 75 mm) and hydrometer analysis (grains < 75 mm) (ASTM 1998). Soil pH was carried out with ~10 g of soil mixed with 30 mL of distilled water. The slurry was left undisturbed for 2 h to allow settling of soil and pH was measured. Total organic carbon was determined using a combustion infrared gas analyzer (USEPA 1995). Soil moisture content was measured gravimetrically by weighing ~10 g of soil, drying overnight at 105 8C, and weighing it again. All concentrations are reported per dry weight. The PHC CWS method prescribes comprehensive quality assurance quality control procedures that were met (CCME 2001). For analysis of leachate PHC concentration, blanks were below detection limit ( 61 8C, and no free liquids are present (BRWMSC 2005). These two examples illustrate the need for developing risk-based guidelines for this practice in Canada. Guidelines should be protective of the environment while not resulting in unnecessary spending and environmental impacts. A criterion based on TPH does not consider the type of petroleum mixture present in soil, which is a key factor for proper management of risks associated with petroleum contamination (CCME 2008a). The PHC–CWS guidelines address this challenge by breaking down petroleum mixtures in broad PHC fractions (described in the analytical methods Published by NRC Research Press

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section above) of similar physicochemical characteristics and consider land use, soil type, and exposure pathways. The PHC–CWS guidelines for industrial land use are used here for discussing the safe disposal of PHC-contaminated soil to landfills. The ‘‘ecological soil contact’’ and ‘‘protection of groundwater’’ pathways are not applicable as the ecological receptors of concern (plants and soil invertebrates) should not be present on the premises and drinking water wells should not be located near a landfill (Table 4). Numerous landfills in Northern communities are unlined sites often located close to the coast (sometimes surrounded by a fence). Considering the potential migration of contaminants is therefore essential. The ‘‘Protection of ground water for aquatic life’’ and ‘‘Off-site migration’’ pathways may be suitable for this matter (Table 4). These pathways are also protective of potential exposure to human receptors (i.e., lower criteria than the ‘‘direct contact’’ pathway). Regulators should also account for public perception of risks from contaminated soils when developing such guidelines, for example, by ensuring that the disposed soils do not contribute to formation of sheens. In the case of sanitary landfills, the impact of PHCs on the liner performance should also be considered. Studies suggested that geomembrane liner properties are less affected by contact with PHC contaminated soil than when in direct contact with the pure petroleum product (Bathurst et al. 2006; Rowe et al. 2007). The PHC-contaminated soil used as cover for the refuse should not be in direct contact with the liner. Consideration of liner performance should therefore focus on possible free product formation and migration. The ‘‘Management limit’’ pathway, which considers free phase formation, explosive hazards, and buried infrastructure effects, could be an interesting starting point for the consideration of this issue. During the current study, the initial average concentrations in the biopile were below F1, F3, and F4 criteria of the ‘‘Protection of ground water for aquatic life’’ pathway. The criterion for F2 was achieved with treatment suggesting that the soil could be safely disposed to the unlined landfill. Residual contamination by F3 and F4 fractions are less of a concern because these fractions tend to sorb to soil and are poorly soluble (CCME 2000), as shown by the higher values for these fractions’ criteria in the ‘‘Off-site migration’’ and ‘‘Management limit’’ pathways and lack of criteria for the ‘‘Protection of aquatic life’’ pathway (Table 4).

4. Conclusions The objective of the treatment (i.e., reducing the levels of the mobile PHC fractions) was achieved by the passively aerated biopile. The concentration of the F2 fraction was reduced to below the PHC–CWS criteria for protection of aquatic life and TPH in leachate were reduced significantly. Findings suggest that biodegradation may have played a role in the removal of F2 compounds but volatilization was likely the predominant removal mechanism. Treatment time was relatively short in the current study. It may vary depending with the initial PHC level in soil, type of petroleum product present, and environmental conditions at the site. This simple technology may be an interesting alternative to

153 Table 4. Generic criteria of the Canada-Wide Standard for Petroleum Hydrocarbon in soil for selected exposure pathways in coarse-grained soil, industrial land use (adapted from CCME 2008b). Hydrocarbon fractions Exposure pathway Human direct contacta Protection of potable GW Ecological soil contactb Protection of GW for aquatic lifec Offsite migration Management limitd

F1

F2

F3

F4

(mg/kg) 30 000 240

(mg/kg) 30 000 320

(mg/kg) 30 000 NA

(mg/kg) 30 000 NA

320 1800

260 600

1700 NA

3300 NA

NA 700

NA 1000

4300 3500

30 000 10 000

Note: NA, not applicable; GW, groundwater. a

Human direct contact = Ingestion + dermal contact. For the protection of vascular plants and soil invertebrates. c Assumes surface water body at 10 m from site. d Includes considerations such as free phase formation, explosive hazards, and buried infrastructure effects. b

landfarming where level ground is limited and when remediation time is not a concern. The reduction of the concentration of mobile PHC fractions, followed by disposal of the treated soil to a landfill may be a suitable management solution for fuel spills at remote communities in Canada’s North. The treated soil should achieve risk-based criteria before being disposed of in such a manner. There appears to be a need to develop PHC-fraction-based guidelines for this practice in Canada. The CCME PHC–CWS may be a suitable starting point. This project also served to build capacity and technical knowledge in the community. Ownership of the materials that made up the biopile facility was transferred to the Nunatsiavut Government (NG) — a regional Inuit government in Labrador. The NG will use the facility to treat other fuel spills in the community and as a demonstration project for the other Inuit communities in Labrador.

5. Acknowledgments This work was financially supported by the Royal Canadian Mounted Police, the Federal Contaminated Sites Action Plan, the Natural Sciences and Engineering Research Council of Canada, and the Northern Scientific Training Program. The following organizations and persons deserve special thanks: the Analytical Services Group, Royal Military College (RMC), Kingston, Ont., for help and guidance for data analysis; the Department of Civil Engineering, RMC, for logistical support; D. Loock for overall management of the project and insight; and N. Schaffer for help with the field work.

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