Register      Login
Environmental Chemistry Environmental Chemistry Society
Environmental problems - Chemical approaches
RESEARCH ARTICLE

Characterisation of oil contaminated soils by comprehensive multiphase NMR spectroscopy

Hashim Farooq A , Denis Courtier-Murias B , Myrna J. Simspon A , Werner E. Maas C , Michael Fey C , Brian Andrew C , Jochem Struppe C , Howard Hutchins C , Sridevi Krishnamurthy C , Rajeev Kumar D , Martine Monette D , Henry J. Stronks C and André J. Simpson A E
+ Author Affiliations
- Author Affiliations

A Department of Chemistry, University of Toronto, 1265 Military Trail, Toronto, ON, M1C 1A4, Canada.

B Universite Paris-Est, LaboratoireNavier (UMR 8205 IFSTTAR-ENPC-CNRS), Physics of Porous Media group, 2 alleKepler, F-77420 Champs sur Marne, France.

C Bruker Biospin Corporation, 15 Fortune Drive, Billerica, MA 01821-3991, USA.

D Bruker Ltd. Canada, 555 Steeles Avenue East, Milton, ON, L9T 1Y6, Canada.

E Corresponding author. Email: andre.simpson@utoronto.ca

Environmental Chemistry 12(2) 227-235 https://doi.org/10.1071/EN14129
Submitted: 12 July 2014  Accepted: 25 September 2014   Published: 18 March 2015

Environmental context. Novel technology is used to examine oil contaminated soil to better understand this longstanding problem. The data indicate that oil forms a non-discriminant layer over all the soil components, which in their natural state would be exposed to water, and that it retains certain polar compounds while contributing other oil contaminants to the surrounding porewater and groundwater. Such molecular level information helps to better understand the reoccurrence of hydrophobicity in remediated soil, and could lead to novel clean-up methods.

Abstract. Comprehensive multiphase (CMP) NMR spectroscopy is a novel NMR technology introduced in 2012. CMP NMR spectroscopy permits the analysis of solid, gel and liquid phases in unaltered natural samples. Here the technology is applied to control and oil contaminated soils to understand the molecular processes that give rise to non-wettable soils. 13C solid-state NMR spectroscopy is found to be excellent for studying the bulk rigid components of the soils whereas 1H solution and gel-state NMR provide a complimentary overview to subtleties occurring at the soil–water interface. Considered holistically the NMR data support the finding that the oil forms a non-discriminant layer over all the soil components, which in the natural state, would be exposed to water. Specifically, the oil was found to preferentially coat aliphatics and carbohydrates that normally stick out at the soil–water interface. In addition, it was shown that the oil forms a barrier that keeps small polar molecules such as formic acid inside the soil. At the soil–water interface selective oil components, such as asphaltenes, were found to exhibit unrestricted diffusion, suggesting that these components could leach into surrounding groundwater.


References

[1]  S. H. Doerr, R. A. Shakesby, R. P. D. Walsh, Soil water repellency: its causes, characteristics and hydro-geomorphological significance. Earth Sci. Rev. 2000, 51, 33.
Soil water repellency: its causes, characteristics and hydro-geomorphological significance.Crossref | GoogleScholarGoogle Scholar |

[2]  P. Kostecki, M. Behbehani, Assessment and Remediation of Oil Contaminated Soils 1999 (New Age International Ltd.: New Delhi).

[3]  M. R. Guerin, I. B. Rubin, T. K. Tao, B. R. Clark, J. L. Epler, Distribution of mutagenic activity in petroleum and petroleum substitutes. Fuel 1981, 60, 282.
Distribution of mutagenic activity in petroleum and petroleum substitutes.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaL3MXitVemu70%3D&md5=f9f76223d31126042093154483404f35CAS |

[4]  R. G. Harvey, Mechanisms of carcinogenesis of polycyclic aromatic hydrocarbons. Polycyclic Aromat. Compd. 1996, 9, 1.
Mechanisms of carcinogenesis of polycyclic aromatic hydrocarbons.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK2sXjt1Kltr8%3D&md5=035cccb3472d13f0a96c8a7fe6fa1e74CAS |

[5]  F. A. Leighton, The toxicity of petroleum oils to birds. Environ. Rev. 1993, 1, 92.
The toxicity of petroleum oils to birds.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK2cXivFWnur0%3D&md5=7f548c115008d967801731547d240687CAS |

[6]  N. Mahmoudi, Assessing in situ degradation of petroleum hydrocarbons by indigenous microbial communities 2013, Ph.D. thesis, McMaster University, Hamilton, ON.

[7]  D. R. Thakker, H. Yagi, W. Levin, A. W. Wood, A. H. Conney, D. M. Jerina, Polycyclic Aromatic Hydrocarbons: Metabolic Activation to Ultimate Carcinogens in Bioactivation of Foreign Compounds (Ed. M. W. Anders) 1985, pp. 177–242 (Academic Press: New York).

[8]  W. L. Xue, D. Warshawsky, Metabolic activation of polycyclic and heterocyclic aromatic hydrocarbons and DNA damage: a review. Toxicol. Appl. Pharmacol. 2005, 206, 73.
Metabolic activation of polycyclic and heterocyclic aromatic hydrocarbons and DNA damage: a review.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2MXlt1Gnsrc%3D&md5=0293259cd7773c65770d2eaf6dcc7305CAS |

[9]  J. G. Speight, K. K. Arjoon, Bioremediation of Petroleum and Petroleum Products 2012 (Scrivener Publishing: Beverly, MA).

[10]  A. Quyum, Water Migration through Hydrophobic Soils 2000 (University of Calgary: Calgary, AB).

[11]  A. Bhandari, R. Y. Surampalli, P. Champagne, S. K. Ong, R. D. Tyagi, I. M. C. Lo, Remediation technologies for Soils and Ground Water 2007 (American Society of Civil Engineers: Reston, VA, USA).

[12]  E. Moliterni, R. G. Jimenez-Tusset, M. V. Rayo, L. Rodriguez, F. J. Fernandez, J. Villasenor, Kinetics of biodegradation of diesel fuel by enriched microbial consortia from polluted soils. Int. J. Environ. Sci. Technol. 2012, 9, 749.
Kinetics of biodegradation of diesel fuel by enriched microbial consortia from polluted soils.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC38Xht1OrurbL&md5=e88d2c3633441cab771d9d664ccd2f47CAS |

[13]  M. Litvina, T. R. Todoruk, C. H. Langford, Composition and structure of agents responsible for development of water repellency in soils following oil contamination. Environ. Sci. Technol. 2003, 37, 2883.
Composition and structure of agents responsible for development of water repellency in soils following oil contamination.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3sXktFyhs7s%3D&md5=6f47068692c17160a3e8bbe71e489575CAS | 12875390PubMed |

[14]  A. J. Simpson, M. J. Simpson, R. Soong, Nuclear Magnetic Resonance Spectroscopy and Its Key Role in Environmental Research. Environ. Sci. Technol. 2012, 46, 11488.
Nuclear Magnetic Resonance Spectroscopy and Its Key Role in Environmental Research.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC38Xht1aqsrjM&md5=42be655f71089b2eff5824b944965537CAS | 22909253PubMed |

[15]  M. A. Wilson, NMR Techniques and Applications in Geochemistry and Soil Chemistry 1987 (Pergamon Press: Oxford).

[16]  J. L. Roy, W. B. McGill, M. D. Rawluk, Petroleum residues as water-repellent substances in weathered nonwettable oil-contaminated soils. Can. J. Soil Sci. 1999, 79, 367.
Petroleum residues as water-repellent substances in weathered nonwettable oil-contaminated soils.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK1MXkslOnt74%3D&md5=20ebe82eb973b6cc11f5b65bde9723c4CAS |

[17]  A. J. Simpson, D. J. McNally, M. J. Simpson, NMR spectroscopy in environmental research: from molecular interactions to global processes. Prog. Nucl. Magn. Reson. Spectrosc. 2011, 58, 97.
NMR spectroscopy in environmental research: from molecular interactions to global processes.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3MXjtVKruro%3D&md5=67198e1e649c5d44e22b4a297b982945CAS | 21397118PubMed |

[18]  D. Courtier-Murias, H. Farooq, H. Masoom, A. Botana, R. Soong, J. G. Longstaffe, M. J. Simpson, W. E. Maas, M. Fey, B. Andrew, J. Struppe, H. Hutchins, S. Krishnamurthy, R. Kumar, M. Monette, H. J. Stronks, A. Hume, A. J. Simpson, Comprehensive multiphase NMR spectroscopy: basic experimental approaches to differentiate phases in heterogeneous samples. J. Magn. Reson. 2012, 217, 61.
Comprehensive multiphase NMR spectroscopy: basic experimental approaches to differentiate phases in heterogeneous samples.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC38XkvFyls7s%3D&md5=dab9894db04a79088707984224f629b5CAS | 22425441PubMed |

[19]  J. A. Toogood, The Reclamation of Agricultural Soils after Oil Spills, Part 1: Research 1977 (University of Alberta: Edmonton).

[20]  J. L. Roy, W. B. McGill, Characterization of disaggregated nonwettable surface soils found at old crude oil spill sites. Can. J. Soil Sci. 1998, 78, 331.
Characterization of disaggregated nonwettable surface soils found at old crude oil spill sites.Crossref | GoogleScholarGoogle Scholar |

[21]  T. R. Todoruk, M. Litvina, A. Kantzas, C. H. Langford, Low-field NMR relaxometry: a study of interactions of water with water-repellant soils. Environ. Sci. Technol. 2003, 37, 2878.
Low-field NMR relaxometry: a study of interactions of water with water-repellant soils.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3sXktFymur0%3D&md5=7b07855a6591e9b20a560116fbf9b870CAS | 12875389PubMed |

[22]  H. Farooq, D. Courtier-Murias, R. Soong, W. Bermel, W. M. Kingery, A. J. Simpson, HR-MAS NMR spectroscopy: a practical guide for natural samples. Curr. Org. Chem. 2013, 17, 3013.
HR-MAS NMR spectroscopy: a practical guide for natural samples.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC2cXjtVKquw%3D%3D&md5=7c6afd29406d9c8f2dd9cea373f2dc4aCAS |

[23]  A. Simpson, Multidimensional solution state NMR of humic substances: a practical guide and review. Soil Sci. 2001, 166, 795.
Multidimensional solution state NMR of humic substances: a practical guide and review.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3MXovVertr0%3D&md5=f7f5bf6d5ab64cef47de78374ead5a5bCAS |

[24]  B. Lam, A. J. Simpson, Direct 1H NMR spectroscopy of dissolved organic matter in natural waters. Analyst 2008, 133, 263.
Direct 1H NMR spectroscopy of dissolved organic matter in natural waters.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD1cXhtVGnur0%3D&md5=4b444b0b946378fb7346ac74dff15623CAS | 18227951PubMed |

[25]  M. J. Duer, Essential Techniques for Spin-1/2 Nuclei 2002 (Blackwell Science: Oxford, UK).

[26]  P. Conte, R. Spaccini, A. Piccolo, State of the art of CPMAS 13C-NMR spectroscopy applied to natural organic matter. Environ. Sci. Technol. 2004, 44, 215.
| 1:CAS:528:DC%2BD2cXkvVSkurg%3D&md5=86e4aa99c36ce6b3eda5dd61fb560b08CAS |

[27]  H. Masoom, D. Courtier-Murias, H. Farooq, R. Soong, M. J. Simpson, W. Maas, R. Kumar, M. Monette, H. Stronk, A. J. Simpson, Rapid estimation of nuclear magnetic resonance experiment time in low-concentration environmental samples. Environ. Toxicol. Chem. 2013, 32, 129.
Rapid estimation of nuclear magnetic resonance experiment time in low-concentration environmental samples.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3sXhtFSrs7o%3D&md5=d8408db3caf70bad752e669fbf9c131aCAS | 23065696PubMed |

[28]  A. Yamazawa, T. Iikura, A. Shino, Y. Date, J. Kikuchi, Solid-, solution-, and gas-state NMR monitoring of 13C-cellulose degradation in an anaerobic microbial ecosystem. Molecules 2013, 18, 9021.
Solid-, solution-, and gas-state NMR monitoring of 13C-cellulose degradation in an anaerobic microbial ecosystem.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3sXht1GksbzI&md5=45813de45fd2e760a922b2f705909719CAS | 23899835PubMed |

[29]  A. J. Simpson, Determining the molecular weight, aggregation, structures and interactions of natural organic matter using diffusion ordered spectroscopy. Magn. Reson. Chem. 2002, 40, S72.
Determining the molecular weight, aggregation, structures and interactions of natural organic matter using diffusion ordered spectroscopy.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD38XpsVOiurg%3D&md5=5746be3c5255c1543ab98a575684e409CAS |

[30]  K. Paudyn, A. Rutter, R. Kerry Rowe, J. S. Poland, Remediation of hydrocarbon contaminated soils in the Canadian Arctic by landfarming. Cold Reg. Sci. Technol. 2008, 53, 102.
Remediation of hydrocarbon contaminated soils in the Canadian Arctic by landfarming.Crossref | GoogleScholarGoogle Scholar |

[31]  W. L. Straube, C. C. Nestler, L. D. Hansen, D. Ringleberg, P. H. Pritchard, J. Jones-Meehan, Remediation of polyaromatic hydrocarbons (PAHs) through landfarming with biostimulation and bioaugmentation. Acta Biotechnol. 2003, 23, 179.
Remediation of polyaromatic hydrocarbons (PAHs) through landfarming with biostimulation and bioaugmentation.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3sXntVCju7o%3D&md5=f7405928e2cedf3537cae86e31ba21d5CAS |

[32]  M. P. Maila, T. E. Cloete, Bioremediation of petroleum hydrocarbons through landfarming: are simplicity and cost-effectiveness the only advantages? Rev. Environ. Sci. Biotechnol. 2004, 3, 349.
Bioremediation of petroleum hydrocarbons through landfarming: are simplicity and cost-effectiveness the only advantages?Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2MXkvVGitb4%3D&md5=689e6b7210986f32964b2dacaf77d5b1CAS |

[33]  A. J. Simpson, W. L. Kingery, D. R. Shaw, M. Spraul, E. Humpfer, P. Dvortsak, The application of 1H HR-MAS NMR spectroscopy for the study of structures and associations of organic components at the solid–aqueous interface of a whole soil. Environ. Sci. Technol. 2001, 35, 3321.
The application of 1H HR-MAS NMR spectroscopy for the study of structures and associations of organic components at the solid–aqueous interface of a whole soil.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3MXkvFKqsLc%3D&md5=8e6ed63fb3bdab712b38bd991156da43CAS | 11529571PubMed |

[34]  R. L. Malcolm, The uniqueness of humic substances in each of soil, stream and marine environments. Anal. Chim. Acta 1990, 232, 19.
The uniqueness of humic substances in each of soil, stream and marine environments.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK3cXkslCms7w%3D&md5=e7e0503be088902fcbe7099fc0b40e85CAS |