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Saranya Kuppusamy
Naga Raju Maddela
Mallavarapu Megharaj
Kadiyala Venkateswarlu
Total
Petroleum
Hydrocarbons
Environmental Fate, Toxicity, and
Remediation
Total Petroleum Hydrocarbons
Saranya Kuppusamy • Naga Raju Maddela
Mallavarapu Megharaj • Kadiyala Venkateswarlu
Total Petroleum
Hydrocarbons
Environmental Fate, Toxicity,
and Remediation
Saranya Kuppusamy Naga Raju Maddela
Centre for Environmental Studies Facultad de Ciencias de la Salud y
Anna University Departamento de investigación
Chennai, Tamil Nadu, India Universidad Técnica de Manabí
Portoviejo, Manabí, Ecuador
Mallavarapu Megharaj
Global Centre for Environmental Kadiyala Venkateswarlu
Remediation Nellore, Andhra Pradesh, India
The University of Newcastle
Newcastle, NSW, Australia
ISBN 978-3-030-24034-9 ISBN 978-3-030-24035-6 (eBook)
https://doi.org/10.1007/978-3-030-24035-6
© Springer Nature Switzerland AG 2020
This work is subject to copyright. All rights are reserved by the Publisher, whether the whole or part of
the material is concerned, specifically the rights of translation, reprinting, reuse of illustrations, recitation,
broadcasting, reproduction on microfilms or in any other physical way, and transmission or information
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now known or hereafter developed.
The use of general descriptive names, registered names, trademarks, service marks, etc. in this publication
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protective laws and regulations and therefore free for general use.
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in published maps and institutional affiliations.
This Springer imprint is published by the registered company Springer Nature Switzerland AG
The registered company address is: Gewerbestrasse 11, 6330 Cham, Switzerland
Preface
Hydrocarbons are made of the elements carbon and hydrogen and are the most
abundant organic compounds in the bio-geosphere. Hydrocarbons are formed bio-
synthetically through living organisms or through the transformation of biogenic
organic matter in the geosphere. The exploitation of hydrocarbon-based fossil fuels
as energy resources has played an important role in the evolution of industrial revo-
lution and the present modern life of humans. The term “total petroleum hydrocar-
bons (TPHs)” is used for any mixture of several hundreds of hydrocarbons that are
found in crude oil. Thus, TPHs represent the sum of volatile and extractable petro-
leum hydrocarbons (PHs). Environmental pollution by PHs, as a result of industri-
alization and anthropogenic activities, is one of the major growing concerns in the
world today due to its potential harms to both terrestrial and aquatic ecosystems. In
fact, there are more than five million potentially contaminated lands worldwide
which represent, in general, a lost economic opportunity and threat to the health and
well-being of humans and the environment. Also, petroleum-contaminated sites
constitute almost one-third of the total contaminated sites around the world. The
land contamination was recognized as early as the 1960s due to the legacy of indus-
trialization, but less than a tenth of potentially contaminated lands have only been
remediated due to the challenging nature of contamination, cost, technical imprac-
ticability, insufficient land legislation, and enforcement. As such, there is no avail-
ability of a single source that provides a complete information on the different
aspects of TPHs such as sources and range of products, methods of analysis, fate
and bioavailability, ecological implications including their impacts on human
health, various potential bioremediation approaches, and regulatory assessment pro-
cedures for TPHs-contaminated sites.
This book, intended to cover all the above different aspects of TPHs contamina-
tion, is organized into nine chapters. Chapter 1 introduces the readers to the produc-
tion of TPHs, their environmental release, extent of contamination, and environmental
concerns of TPHs contamination. It also provides an overview of TPHs with
description about the different range of TPHs products and their physico-chemical
properties. Chapter 2 describes the chemical analytical methods used to detect and
measure different types of TPHs from varied environmental matrices. Chapter 3
v
vi Preface
focuses on the fate of TPHs in different environments of air, terrestrial, and aquatic
(marine vs freshwater vs sediments). Chapter 4 describes the bioavailability of
TPHs and the methods used to measure the bioavailability, i.e., chemical vs biologi-
cal. Chapter 5 provides the ecological impacts of TPHs that include the nontarget
effects of TPHs toward terrestrial organisms (microbes, plants, invertebrates, verte-
brates) and aquatic organisms − marine vs freshwater (microbes, plants, inverte-
brates, vertebrates). Chapter 6 describes the potential impacts of TPHs on human
health with emphasis on the routes of exposure (dermal vs inhalation) and their
potential toxicity and carcinogenicity. Chapter 7 deals with the approaches for
remediation of TPHs-contaminated sites which includes the risk-based, traditional,
and modern emerging remediation technologies. Chapter 8 focuses on the environ-
mental regulations across the world and the available ecological-/health-based regu-
latory guidelines adopted by different countries. Finally, Chapter 9 describes several
available case studies on successful remediation of sites contaminated with TPHs
all over the world because of historical oil spills. Thus, this state-of-the-art book is
the first compilation of all the critical information and updated knowledge required
for understanding the TPHs fate, behavior, and their remediation in contaminated
environments. We believe that this comprehensive book will be a good source of
reference for graduate students, researchers, technicians of oil industries, remedia-
tion practitioners of contaminated sites, as well as policy-makers who are interested
in working on the sites contaminated with TPHs.
Chennai, Tamil Nadu, India Saranya Kuppusamy
Portoviejo, Ecuador Naga Raju Maddela
Newcastle, NSW, Australia Mallavarapu Megharaj
Nellore, Andhra Pradesh, India Kadiyala Venkateswarlu
Acknowledgments
Dr. Saranya Kuppusamy gratefully acknowledges the Science and Engineering
Research Board of the Department of Science and Technology for the award of
DST-SERB Ramanujan Fellowship (Sanction Order No. SB/S2/RJN-182/2017) and
the Centre for Environmental Studies, Anna University, Chennai, India, for provid-
ing facilities during this fellowship period.
Dr. Naga Raju Maddela greatly acknowledges the Universidad Téchnica de
Manabi, Portoviejo, Ecuador, for the facilities and encouragement and his col-
leagues in the Faculty of Health Science, Department of Investigation, for their help
in literature collection.
vii
Abbreviations
AAL Arizona Action Levels
ACGIH American Conference of Governmental Industrial Hygienists
ADD Average Daily Dose
AFB Air Force Base
AIS Alveolar Interstitial Syndrome
API American Petroleum Institute
ASTM American Society for Testing and Materials
ASTM American Society of Testing and Materials
BAAQMD Bay Area Air Quality Management District
BaP Benzo(a)Pyrene
BER Bioelectrochemical Remediation
BES Bioelectrochemical System
BOD Burden of Disease
BTEX Benzene, Toluene, Ethylbenzene, and Xylenes
CCEH Center for Children’s Environmental Health
CCME Canadian Council of Ministers of the Environment
CERCLA Comprehensive Environmental Response, Compensation and Liability
Act
CEV Critical Exposure Values
CHD Coronary Heart Disease
CNS Central Nervous System
CoNPs Cobalt Nanoparticles
CPT Cone Penetrometer Technology
CYPs Cytochrome P450 Monooxygenases
DOI Department of Interior
DRO Diesel Range Organics
DUS Dynamic Underground Striping
DWH Deepwater Horizon
EA Environment Agency
ECIA Electrochemical Immunoassay
EFR Enhanced Fluid Recovery
ix
x Abbreviations
EK Electrokinetic
ELISA Enzyme-Linked Immunosorbent Assay
EPA Environmental Protection Agency
EPHs Extractable Petroleum Hydrocarbons
ESLs Ecological Screening Levels
EU European Union
F Fractions
FHCs Fuel Hydrocarbons
FID Flame Ionization Detector
FLTG French Limited Task Group
FPAC Fine Particle Associated Carbon
GAC Granular Activated Carbon
GC-MS/FID Gas Chromatography-Mass Spectrometry/Flame Ionization Detector
GE Genetic Engineering
GMOs Genetically Modified Microorganisms
GRO Gasoline Range Organics
GSA Gasoline Spill Area
HC Hazardous Concentration
HEPA High-Efficiency Particulate Air
HEWAF High-Energy WAF
HI Hazard Index
HIP Health Information Products
HMW High-Molecular-Weight
HPCD Hydroxypropyl-β-Cyclodextrin
HPLC High-Performance Liquid Chromatography
HQ Hazard Quotient
HRH High-Range Hydrocarbons
HSLs Health Screening Levels
HTTD High-Temperature Thermal Desorption
IARC International Agency for Research on Cancer
IC Internal Combustion
IR Infrared Spectroscopy
IRIS Integrated Risk Information System
IUR Inhalation Unit Risks
IVOCs Intermediate-Volatile Organic Compounds
KOC Kuwait Oil Company
LC Lethal Concentration
LLNL Lawrence Livermore National Laboratory
LMW Low-Molecular-Weight
LOEC Lowest Observed Effect Concentration
LRH Low-Range Hydrocarbons
LTA Land Treatment Area
LTTD Low-Temperature Thermal Desorption
LTU Land Treatment Unit
M Modules
Abbreviations xi
MBC Microbial Biomass Carbon
MCL Maximum Contaminant Level
MEK Methyl Ethyl Ketone
MFCs Microbial Fuel Cells
MGP Manufactured Gas Plants
MnNPs Manganese Nanoparticles
MOS Marine Oil Snow
MPC Maximum Permissible Concentration
MPPS Multiprocess Phytoremediation System
MRH Midrange Hydrocarbons
MS Mass Spectrometry
MtBE Methyl Tertiary Butyl Ether
NAPL Nonaqueous Phase Liquid
NCP National Contingency Plan
NCQA National Committee for Quality Assurance
NEPC National Environment Protection Council
NEPMs National Environment Protection Measures
NLM National Library of Medicine
NOAA National Oceanic and Atmospheric Administration
NOEC No Observed Effect Concentration
NPL National Priorities List
O&M Operations and Maintenance
OECD Organization for Economic Cooperation and Development
ONGC Oil and Natural Gas Corporation
OPA Oil Particulate Aggregates
ORO Oil Range Organics
OSPM Oil Soil Particulate Matter
OWP Oil Weathering Processes
PAHs Polycyclic Aromatic Hydrocarbons
PBMC Peripheral Blood Mononuclear Cells
PCA Principal Component Analysis
PED Polyethylene Device
PGPR Plant Growth-Promoting Rhizobia
PH Petroleum Hydrocarbon
PHC CWS Canada-Wide Standards for Petroleum Hydrocarbons
PHs Petroleum Hydrocarbons
PIC Petrochemical Industrial Complexes
PM Particulate Matter
PNEC Predicted No-Effect Concentration
PRGs Preliminary Remediation Goals
PRPs Potentially Responsible Parties
PVA Polyvinyl Alcohol
PYR Pyrene
RACER Remedial Action Cost Engineering and Requirements
RBCA Risk-Based Corrective Action
xii Abbreviations
RBCLs Risk-Based Clean-Up Levels
RBR Risk-based Remediation
RCLs Recommended Clean-Up Levels
RCRA Resource Conservation and Recovery Act
ReTec Remediation Technologies, Inc.
RfC Inhalation Reference Concentrations
RfDo Oral Reference Doses
RME Reasonable Maximum Exposure
ROD Record of Decision
ROS Reactive Oxygen Species
ROS-LIF Rapid Optical Screening Tool Laser-Induced Fluorescence
RSLs Regional Screening Levels
RVIM The National Institute for Public Health and the Environment
S/S Stabilization/Solidification
SDWA Safe Drinking Water Act
SEPA State Environmental Policy Act
SIM Selected Ion Monitoring
SMCs Splenic Melano-macrophage Centers
SMRT Single-Molecule Real Time
SOA Secondary Organic Aerosols
SPM Suspended Particulate Materials
SPMD Semipermeable Membrane Device
SPME Solid-Phase Microextraction
SQGE Soil Quality Guidelines for Environmental Health Protection
SRC Serious Risk Concentration
SRCs Serious Risk Concentrations
SSD Species Sensitivity Distribution
SVE Soil Vapor Extraction
SVOCs Semi-volatile Organic Carbons
SW Soil Washing
TCE Trichloroethylene
TCICs Total Carcinogenic Indicator Chemicals
TCLP Toxicity Characteristic Leaching Procedure
TD Thermal Desorption
TDI Tolerable Daily Intake
TERI The Energy and Resources Institute
TLC Thin-Layer Chromatography
TOC Total Organic Carbon
TOFMS Time-of-Flight Mass Spectrometry
TPHs Total Petroleum Hydrocarbons
TRPHs Total Recoverable Petroleum Hydrocarbons
UCMs Unresolved Complex Mixtures
UFPs Ultrafine Particles
US EPA United States Environmental Protection Agency
USAF United States Air Force
Abbreviations xiii
USTs Underground Storage Tanks
UT Ultrasound Technology
UVIF Ultraviolet-Induced Fluorescence
VOCs Volatile Organic Compounds
VPHs Volatile Petroleum Hydrocarbons
WAFs Water Accommodated Fractions
WHP Wellness and Health Promotion
Contents
1 An Overview of Total Petroleum Hydrocarbons���������������������������������� 1
1.1 Introduction�������������������������������������������������������������������������������������� 1
1.2 Definitions���������������������������������������������������������������������������������������� 3
1.2.1 Hydrocarbon ������������������������������������������������������������������������ 3
1.2.2 Crude Oil������������������������������������������������������������������������������ 3
1.2.3 Petroleum������������������������������������������������������������������������������ 3
1.2.4 PHs���������������������������������������������������������������������������������������� 4
1.2.5 TPHs ������������������������������������������������������������������������������������ 5
1.3 Sources of TPHs������������������������������������������������������������������������������� 6
1.4 Carbon Ranges in TPHs�������������������������������������������������������������������� 6
1.5 Components of TPHs������������������������������������������������������������������������ 7
1.5.1 Gasolines������������������������������������������������������������������������������ 7
1.5.2 Kerosene ������������������������������������������������������������������������������ 8
1.5.3 Diesel Fuels�������������������������������������������������������������������������� 8
1.5.4 Jet Fuels�������������������������������������������������������������������������������� 12
1.5.5 Stoddard Solvent������������������������������������������������������������������ 13
1.5.6 Mineral-Based Motor Oils���������������������������������������������������� 14
1.5.7 Fuel Oils No. 5 and 6������������������������������������������������������������ 14
1.5.8 BTEX������������������������������������������������������������������������������������ 15
1.5.9 PAHs ������������������������������������������������������������������������������������ 16
1.6 Chemicals Included in TPHs������������������������������������������������������������ 17
1.7 Summary ������������������������������������������������������������������������������������������ 23
References�������������������������������������������������������������������������������������������������� 23
2 Methodologies for Analysis and Identification of Total Petroleum
Hydrocarbons ������������������������������������������������������������������������������������������ 29
2.1 Introduction�������������������������������������������������������������������������������������� 29
2.2 Methods for PHs Analysis���������������������������������������������������������������� 30
2.2.1 Collection and Preservation of Environmental
Samples �������������������������������������������������������������������������������� 31
2.2.2 Sample Extraction���������������������������������������������������������������� 31
xv
xvi Contents
2.2.3 Concentration of the Extract ������������������������������������������������ 35
2.2.4 Clean-Up of the Extract�������������������������������������������������������� 36
2.2.5 Detection and Quantification of PHs������������������������������������ 37
2.3 Resolving the Unresolved Complex Mixture in
TPHs-Impacted Media���������������������������������������������������������������������� 45
2.4 TPHs Levels in Environmental Samples������������������������������������������ 46
2.5 Summary ������������������������������������������������������������������������������������������ 50
References�������������������������������������������������������������������������������������������������� 50
3 Fate of Total Petroleum Hydrocarbons in the Environment���������������� 57
3.1 Introduction�������������������������������������������������������������������������������������� 57
3.2 Fate of TPHs in Air �������������������������������������������������������������������������� 60
3.3 Fate of TPHs in Land-Spillage���������������������������������������������������������� 62
3.4 Fate of TPHs in Aquatic Systems ���������������������������������������������������� 65
3.4.1 Marine Environment ������������������������������������������������������������ 65
3.4.2 Freshwater System���������������������������������������������������������������� 70
3.4.3 Sediments������������������������������������������������������������������������������ 72
3.4.4 Ice������������������������������������������������������������������������������������������ 73
3.5 Summary ������������������������������������������������������������������������������������������ 73
References�������������������������������������������������������������������������������������������������� 74
4 Bioavailability of Total Petroleum Hydrocarbons�������������������������������� 79
4.1 Introduction�������������������������������������������������������������������������������������� 79
4.2 Definitions of Bioavailability������������������������������������������������������������ 80
4.3 Importance of Bioavailability in Bioremediation ���������������������������� 82
4.4 Surfactants to Enhance TPHs Bioavailability ���������������������������������� 83
4.5 Assessing Bioavailability of TPHs���������������������������������������������������� 83
4.5.1 Chemical Assays ������������������������������������������������������������������ 84
4.5.2 Biological Assays������������������������������������������������������������������ 87
4.6 Summary ������������������������������������������������������������������������������������������ 91
References�������������������������������������������������������������������������������������������������� 91
5 Ecological Impacts of Total Petroleum Hydrocarbons ������������������������ 95
5.1 Introduction�������������������������������������������������������������������������������������� 96
5.2 Terrestrial Organisms������������������������������������������������������������������������ 98
5.2.1 Microorganisms and Their Activities������������������������������������ 99
5.2.2 Plants������������������������������������������������������������������������������������ 102
5.2.3 Invertebrates�������������������������������������������������������������������������� 106
5.2.4 Vertebrates���������������������������������������������������������������������������� 110
5.3 Aquatic Organisms���������������������������������������������������������������������������� 116
5.3.1 Microorganisms�������������������������������������������������������������������� 116
5.3.2 Plants������������������������������������������������������������������������������������ 120
5.3.3 Invertebrates�������������������������������������������������������������������������� 122
5.3.4 Vertebrates���������������������������������������������������������������������������� 124
5.4 Summary ������������������������������������������������������������������������������������������ 130
References�������������������������������������������������������������������������������������������������� 131
Contents xvii
6 Impact of Total Petroleum Hydrocarbons on Human Health ������������ 139
6.1 Introduction�������������������������������������������������������������������������������������� 139
6.2 TPHs Sources for Human Exposure ������������������������������������������������ 142
6.3 Routes of TPHs Entry ���������������������������������������������������������������������� 144
6.4 Effects of TPHs on Human Health��������������������������������������������������� 147
6.4.1 Effects on Mental Health������������������������������������������������������ 151
6.4.2 Effects on the Respiratory System���������������������������������������� 152
6.4.3 Effects on the Hematopoietic, Renal, and Digestive
Systems �������������������������������������������������������������������������������� 153
6.4.4 Carcinogenicity and Genotoxic Effects�������������������������������� 154
6.4.5 Teratogenic Effects �������������������������������������������������������������� 156
6.4.6 Immunotoxicity and Endocrine Toxicity������������������������������ 157
6.5 Health Risk Assessments������������������������������������������������������������������ 158
6.6 Summary ������������������������������������������������������������������������������������������ 161
References�������������������������������������������������������������������������������������������������� 162
7 Approaches for Remediation of Sites Contaminated
with Total Petroleum Hydrocarbons������������������������������������������������������ 167
7.1 Introduction�������������������������������������������������������������������������������������� 167
7.2 Risk-Based Clean-Up of TPHs-Contaminated Sites:
An Emerging Approach�������������������������������������������������������������������� 169
7.3 TPHs Risk Reduction������������������������������������������������������������������������ 169
7.3.1 Established Remediation Technologies�������������������������������� 170
7.3.2 Emerging Remediation Technologies ���������������������������������� 189
7.4 Summary ������������������������������������������������������������������������������������������ 196
References�������������������������������������������������������������������������������������������������� 196
8 Regulatory Guidelines for Total Petroleum Hydrocarbon
Contamination������������������������������������������������������������������������������������������ 207
8.1 Introduction�������������������������������������������������������������������������������������� 207
8.2 International Guidelines for TPHs Contamination �������������������������� 208
8.2.1 Canada���������������������������������������������������������������������������������� 208
8.2.2 New Zealand ������������������������������������������������������������������������ 212
8.2.3 Netherlands �������������������������������������������������������������������������� 214
8.2.4 United Kingdom������������������������������������������������������������������� 215
8.2.5 USA�������������������������������������������������������������������������������������� 217
8.2.6 Australia�������������������������������������������������������������������������������� 218
8.2.7 Asia �������������������������������������������������������������������������������������� 221
8.3 Suggestions for Improved Regulatory Regimes ������������������������������ 222
8.4 Summary ������������������������������������������������������������������������������������������ 223
References���������������������������������������������������������������������������������������������������������� 223
9 Case Studies on Remediation of Sites Contaminated with Total
Petroleum Hydrocarbons������������������������������������������������������������������������ 225
9.1 Introduction�������������������������������������������������������������������������������������� 225
9.2 Bioremediation of Oil Spill Site in Gujarat Oil Field in
Western India������������������������������������������������������������������������������������ 228
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