Skip to main content
Log in

Long-term simulation of in situ biostimulation of polycyclic aromatic hydrocarbon-contaminated soil

  • Original Paper
  • Published:
Biodegradation Aims and scope Submit manuscript

Abstract

A continuous-flow column study was conducted to evaluate the long-term effects of in situ biostimulation on the biodegradation of polycyclic aromatic hydrocarbons (PAHs) in soil from a manufactured gas plant site. Simulated groundwater amended with oxygen and inorganic nutrients was introduced into one column, while a second column receiving unamended groundwater served as a control. PAH and dissolved oxygen (DO) concentrations, as well as microbial community profiles, were monitored along the column length immediately before and at selected intervals up to 534 days after biostimulation commenced. Biostimulation resulted in significantly greater PAH removal than in the control condition (73% of total measured PAHs vs. 34%, respectively), with dissolution accounting for a minor amount of the total mass loss (~6%) in both columns. Dissolution was most significant for naphthalene, acenaphthene, and fluorene, accounting for >20% of the total mass removed for each. A known group of PAH-degrading bacteria, ‘Pyrene Group 2’ (PG2), was identified as a dominant member of the microbial community and responded favorably to biostimulation. Spatial and temporal variations in soil PAH concentration and PG2 abundance were strongly correlated to DO advancement, although there appeared to be transport of PG2 organisms ahead of the oxygen front. At an estimated oxygen demand of 6.2 mg O2/g dry soil and a porewater velocity of 0.8 m/day, it took between 374 and 466 days for oxygen breakthrough from the 1-m soil bed in the biostimulated column. This study demonstrated that the presence of oxygen was the limiting factor in PAH removal, as opposed to the abundance and/or activity of PAH-degrading bacteria once oxygen reached a previously anoxic zone.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6

Similar content being viewed by others

References

  • Adams JA, Reddy KR (2003) Extent of benzene biodegradation in saturated soil column during air sparging. Ground Water Monit Rem 23:85–94

    CAS  Google Scholar 

  • Alexander M (2000) Aging, bioavailability, and overestimation of risk from environmental pollutants. Environ Sci Technol 34:4259–4265

    Article  CAS  Google Scholar 

  • Bamforth SM, Singleton I (2005) Bioremediation of polycyclic aromatic hydrocarbons: current knowledge and future directions. J Chem Technol Biotechnol 80:723–736

    Article  CAS  Google Scholar 

  • Bodour AA, Wang JM, Brusseau ML, Maier RM (2003) Temporal change in culturable phenanthrene degraders in response to long-term exposure to phenanthrene in a soil column system. Environ Microbiol 5:888–895

    Article  PubMed  CAS  Google Scholar 

  • Borchert S, Mueller J, Alesi E, Leins C, Haninger V (1995) In situ bioremediation application strategies for soil and groundwater impacted by PAHs. Land Contam Reclam 3:6-1–6-4

    Google Scholar 

  • Bouchez M, Blanchet D, Vandecasteele J (1995) Substrate availability in phenanthrene biodegradation: transfer mechanism and influence on metabolism. Appl Microbiol Biotechnol 43:952–960

    Article  PubMed  CAS  Google Scholar 

  • Breedveld GD, Karlsen DA (2000) Estimating the availability of polycyclic aromatic hydrocarbons for bioremediation of creosote contaminated soils. Appl Microbiol Biotechnol 54:255–261

    Article  PubMed  CAS  Google Scholar 

  • Breedveld GD, Sparrevik M (2000) Nutrient-limited biodegradation of PAH in various soil strata at a creosote contaminated site. Biodegradation 11:391–399

    Article  PubMed  CAS  Google Scholar 

  • Chi FH, Amy GL (2004) Transport of anthracene and benz(a)anthracene through iron-quartz and three aquifer materials in laboratory columns. Chemosphere 55:515–524

    Article  PubMed  CAS  Google Scholar 

  • Enell A, Reichenberg F, Warfvinge P, Ewald G (2004) A column method for determination of leaching of polycyclic aromatic hydrocarbons from aged contaminated soil. Chemosphere 54:707–715

    Article  PubMed  CAS  Google Scholar 

  • Eriksson M, Dalhammar G, Borg-Karlson AK (2000) Biological degradation of selected hydrocarbons in an old PAH/creosote contaminated soil from a gas work site. Appl Microbiol Biotechnol 53:619–626

    Article  PubMed  CAS  Google Scholar 

  • Groves MR (1976) Preliminary Report on Groundwater Resources in Rowan County, North Carolina, pp 46–52

  • Gustavson KE, Harkin JM (2000) Comparison of sampling techniques and evaluation of semipermeable membrane devices (SPMDs) for monitoring polynuclear aromatic hydrocarbons (PAHs) in groundwater. Environ Sci Technol 34:4445–4451

    Article  CAS  Google Scholar 

  • Jones MD, Crandell DW, Singleton DR, Aitken MD (2011) Stable-isotope probing of the polycyclic aromatic hydrocarbon-degrading bacterial guild in a contaminated soil. Environ Microbiol 13:2623–2632

    Article  PubMed  CAS  Google Scholar 

  • Khalil MF, Ghosh U, Kreitinger JP (2006) Role of weathered coal tar pitch in the partitioning of polycyclic aromatic hydrocarbons in manufactured gas plant site sediments. Environ Sci Technol 40:5681–5687

    Article  PubMed  CAS  Google Scholar 

  • Kim H, Lindsay K, Pfaender F (2008) Enhanced mobilization of field contaminated soil-bound PAHs to the aqueous phase under anaerobic conditions. Water Air Soil Pollut 189:135–147

    Article  CAS  Google Scholar 

  • Lahlou M, Harms H, Springael D, Ortega-Calvo JJ (2000) Influence of soil components on the transport of polycyclic aromatic hydrocarbon-degrading bacteria through saturated porous media. Environ Sci Technol 34:3649–3656

    Article  CAS  Google Scholar 

  • Li J, Pignatello JJ, Smets BF, Grasso D, Monserrate E (2005) Bench-scale evaluation of in situ bioremediation strategies for soil at a former manufactured gas plant site. Environ Toxicol Chem 24:741–749

    Article  PubMed  CAS  Google Scholar 

  • Liebeg EW, Cutright TJ (1999) The investigation of enhanced bioremediation through the addition of macro and micro nutrients in a PAH contaminated soil. Int Biodeterior Biodegrad 44:55–64

    Article  CAS  Google Scholar 

  • Lundstedt S, Haglund P, Oberg L (2003) Degradation and formation of polycyclic aromatic compounds during bioslurry treatment of an aged gasworks soil. Environ Toxicol Chem 22:1413–1420

    Article  PubMed  CAS  Google Scholar 

  • Luthy RG, Aiken GR, Brusseau ML, Cunningham SD, Gschwend PM, Pignatello JJ, Reinhard M, Traina SJ, Weber WJ, Westall JC (1997) Sequestration of hydrophobic organic contaminants by geosorbents. Environ Sci Technol 31:3341–3347

    Article  CAS  Google Scholar 

  • Madsen EL, Mann CL, Bilotta SE (1996) Oxygen limitations and aging as explanations for the field persistence of naphthalene in coal tar-contaminated surface sediments. Environ Toxicol Chem 15:1876–1882

    Article  CAS  Google Scholar 

  • Millette D, Butler BJ, Frind EO, Comeau Y, Samon R (1998) Substrate interaction during aerobic biodegradation of creosote-related compounds in columns of sandy aquifer material. J Contam Hydrol 29:165–183

    Article  CAS  Google Scholar 

  • Mohan SV, Kisa T, Ohkuma T, Kanaly RA, Shimizu Y (2006) Bioremediation technologies for treatment of PAH-contaminated soil and strategies to enhance process efficiency. Rev Environ Sci Biotechnol 5:347–374

    Article  CAS  Google Scholar 

  • Murarka I, Neuhauser E, Sherman M, Taylor BB, Mauro DM, Ripp J, Taylor T (1992) Organic substances in the subsurface: delineation, migration, and remediation. J Hazard Mater 32:245–261

    Article  CAS  Google Scholar 

  • Reemtsma T, Mehrtens J (1997) Determination of polycyclic aromatic hydrocarbon (PAH) leaching from contaminated soil by a column test with on-line solid phase extraction. Chemosphere 35:2491–2501

    Article  CAS  Google Scholar 

  • Richardson SD, Aitken MD (2011) Desorption and bioavailability of polycyclic aromatic hydrocarbons in contaminated soil subjected to long-term in situ biostimulation. Environ Toxicol Chem 30(12):2674–2681

    Google Scholar 

  • Richardson SD, Lebron BL, Miller CT, Aitken MD (2011) Recovery of phenanthrene-degrading bacteria after simulated in situ persulfate oxidation in contaminated soil. Environ Sci Technol 45:719–725

    Article  PubMed  CAS  Google Scholar 

  • Ringelberg DB, Talley JW, Perkins EJ, Tucker SG, Luthy RG, Bouwer EJ, Fredrickson HL (2001) Succession of phenotypic, genotypic, and metabolic community characteristics during in vitro bioslurry treatment of polycyclic aromatic hydrocarbon-contaminated sediments. Appl Environ Microbiol 67:1542–1550

    Article  PubMed  CAS  Google Scholar 

  • Singleton DR, Powell SN, Sangaiah R, Gold A, Ball LM, Aitken MD (2005) Stable-isotope probing of bacteria capable of degrading salicylate, naphthalene, or phenanthrene in a bioreactor treating contaminated soil. Appl Environ Microbiol 71:1202–1209

    Article  PubMed  CAS  Google Scholar 

  • Singleton DR, Hunt M, Powell SN, Frontera-Suau R, Aitken MD (2007) Stable-isotope probing with multiple growth substrates to determine substrate specificity of uncultivated bacteria. J Microbiol Methods 69:180–187

    Article  PubMed  CAS  Google Scholar 

  • Talley JW, Ghosh U, Tucker SG, Furey JS, Luthy RG (2002) Particle-scale understanding of the bioavailability of PAHs in sediment. Environ Sci Technol 36:477–483

    Article  PubMed  CAS  Google Scholar 

  • Talley JW, Zhang X, Waisner S, Ringelberg D, Hansen L (2004) Study of the potential for bioremediation of petroleum hydrocarbons within smear zone soils. J Environ Eng 130:1401–1407

    Article  CAS  Google Scholar 

  • Tiehm A, Stieber M, Werner P, Frimmel FH (1997) Surfactant-enhanced mobilization and biodegradation of polycyclic aromatic hydrocarbons in manufactured gas plant soil. Environ Sci Technol 31:2570–2576

    Article  CAS  Google Scholar 

  • U.S. Environmental Protection Agency (USEPA) (1996) Method 3535: solid phase extraction in Test methods for evaluating solid waste physical/chemical methods, SW-846 annual

  • Viñas M, Sabate J, Espuny MJ, Solanas AM (2005) Bacterial community dynamics and polycyclic aromatic hydrocarbon degradation during bioremediation of heavily creosote-contaminated soil. Appl Environ Microbiol 71:7008–7018

    Article  PubMed  Google Scholar 

  • Volkering F, Breure AM, Sterkenburg A, Andel JG (1992) Microbial degradation of polycyclic aromatic hydrocarbons: effect of substrate availability on bacterial growth kinetics. Appl Microbiol Biotechnol 36:548–552

    Article  CAS  Google Scholar 

  • Wehrer M, Totsche KU (2005) Determination of effective release rates of polycyclic aromatic hydrocarbons and dissolved organic carbon by column outflow experiments. Eur J Soil Sci 56:803–813

    CAS  Google Scholar 

  • Zamfirescu D, Grathwohl P (2001) Occurrence and attenuation of specific organic compounds in the groundwater plume at a former gasworks site. J Contam Hydrol 53:407–427

    Article  PubMed  CAS  Google Scholar 

  • Zhang Y, Zhu S, Xiao R, Wang J, Li F (2008) Vertical transport of polycyclic aromatic hydrocarbons in different particle-size fractions of sandy soils. Environ Geol 53:1165–1172

    Article  CAS  Google Scholar 

Download references

Acknowledgments

We thank Randall Goodman and Glenn Walters for their help in the design and construction of the columns. We also thank Dr. Wei Sun and Joe Rigdon of the UNC Department of Biostatistics for assistance with statistical analyses. This work was supported by the National Institute of Environmental Health Sciences (Grant No. 5 P42 ES005948).

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Stephen D. Richardson.

Electronic supplementary material

Below is the link to the electronic supplementary material.

Supplementary material 1 (DOC 1457 kb)

Rights and permissions

Reprints and permissions

About this article

Cite this article

Richardson, S.D., Jones, M.D., Singleton, D.R. et al. Long-term simulation of in situ biostimulation of polycyclic aromatic hydrocarbon-contaminated soil. Biodegradation 23, 621–633 (2012). https://doi.org/10.1007/s10532-012-9538-9

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10532-012-9538-9

Keywords

Navigation