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ENVIRONMENTAL FATE OF HEAVY METALS AND HYDROCARBONS IN ASH FROM MUKAH POWER GENERATION
PLANT
Azzudin Shebli
Master of Science (Environmental Science)
2014
ENVIRONMENTAL FATE OF HEAVY METALS AND HYDROCARBONS IN ASH FROM MUKAH POWER GENERATION PLANT
Azzudin Shebli
A thesis submitted in fulfillment of the requirement for The degree of Master of Science
In Environmental Science
Department of Chemistry Faculty of Resource Science and Technology
UNIVERSITY MALAYSIA SARA W AK 2014
A.SHEBLI
DECLARATION
No portion of the work referred to in this thesis has been submitted in support of an
application for another degree or qualification to this or any other university or institution of
higher learning.
Azzudin Shebli
09021510
Department of Chemistry Faculty of Resource Science and Technology Universiti Malaysia Sarawak
ACKNOWLEDGEMENTS
First, I would like to thank ALLAH the most merciful and most beneficent for His blessing
and guidance throughout this journey of my life.
I am greatly indebted to my principal supervisor Prof Dr Zaini Bin Assim for kindly
providing untiring guidance throughout the development of this study. His comments,
stimulating suggestion, encouragement and support have been of greatest help at all times in
this study and thesis writing. Thank you also goes to Prof Dr Zin Zawawi Bin Zakaria for his
academic assistance and moral support. Nonetheless, I also gratefully acknowledge the
General Manager of MPG Sdn Bhd for giving the permission to conduct this study within his
premise and the Jabatan Perkhidmatan Awam Malaysia for granting the scholarship that has
made this study possible.
I offer my heartfelt thank you to my parents, my wife, siblings and friends for their
everlasting encouragement support and for always being with me during high and low times
in my life.
Finally, very special thank you is extended to the laboratory assistant, Mr. Benedict, Mr.
Rajuna Tahir, Mdm. Dayang Fatimahwati Awang Ali and all supporting staff at Faculty of
Resource Science and Technology for their assistance and kindness throughout the duration of
my studies.
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ABSTRACT
Coal power generation plant emits several pollutants linked to the environmental problems.
Ash produced during coal combustion is partitioned into bottom ash and flyash. A study has
been undertaken to investigate the environmental fate of heavy metals and hydrocarbons in
ash from Mukah Power Generation Plant (MPG). Soil and sediment samples collected from
seven sampling locations at the vicinity of MPG were analysed for aliphatic hydrocarbons,
polycyclic aromatic hydrocarbons (PAHs) and heavy metals. The hydrocarbons were
extracted from core samples by Soxhlet extraction method and analysed using gas
chromatography equipped with flame ionisation detector (GC-FID). Heavy metals were
extracted by digestion with aqua regia solution and analysed on the inductively coupled
plasma optical emission spectrometer (ICP-OES). The total concentrations of total aliphatic
hydrocarbons (TAHs) and PAHs in core samples ranged between 2512.4 to 6566.0 mg/kg and
518.0 to 1210.4 mg/kg dry weight, respectively. Relatively elevated concentration of the
hydrocarbons and heavy metals concentrations were found at sampling sites located near to
the plant and at the top layers of sample cores suggesting of anthropogenic inputs. Molecular
indices and distribution patterns of hydrocarbons were used to predict the sources of
hydrocarbons. The diagnostic indices showed the hydrocarbons are petrogenic (fossil fuel)
and pyrogenic in characters. The hydrocarbons were resulted from incomplete combustion of
coal from the plant. Total organic carbon (TOC) is one of the most important factors that can
influence the concentration of hydrocarbons in soils. The concentration of T AHs and total
PAHs in the core samples of MPG found to be significantly correlated with the Toe of soil.
The distribution patterns of heavy metals in the study area were also used to predicting their
sources. The dominant heavy metals in core samples were Mn, Zn, V and Pb. The fate and
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dispersal pathways of hydrocarbons and heavy metals in the sample from study area were
predicted using simple correlation analysis. High correlation of both hydrocarbons and heavy
metals with fly ash suggests the fly ash is the pollution source. Spatial distribution trend of the
hydrocarbons and heavy metals showed the meteorological condition have influenced the
pollutants distribution in the study area. The pollution index values (PI) for most sampling
sites within vicinity of MPG area showed the study area was contaminated with aliphatic
hydrocarbons, PAHs and heavy metals from the plant discharge. The results of this study can
be used as baseline data in health risks assessment associated with coal-fired power plant
impacts toward environment.
Keywords: Hydrocarbons, heavy metals, soil, gas chromatography-flame ionisation detector
(GC-FID), inductively couple plasma optical emission spectrometry, source identification.
IV
TABURAN SEKITARAN LOGAM BERAT DAN HIDROKARBON DALAM ABU DARI
LOJI JANAKUASA MUKAH
ABSTRAK
Loji janakuasa arang batu melepaskan beberapa bahan cemar yang berkaitan dengan
masalah alam sekitar. Abu yang dihasilkan semasa pembakaran arang batu dibahagikan
kepada abu bawah dan abu terbang. Satu kajian telah dijalankan untuk menyiasat taburan
sekitaran logam berat dan hidrokarbon dalam abu dari Loji Janakuasa arang batu Mukah
(MPG). Sampel teras tanah dan enapan dari tujuh lokasi persampelan dalam lingkungan
MPG telah dianalisis untuk menentukan kandungan hidrokarbon alifatik. hidrokarbon
aromatik polisiklik (HAP) dan logam berat. Hidrokarbon diekstrak dari sampel teras
menggunakan kaedah pengekstrakan Soxhlet dan dianalisis menggunakan kromatograji gas
pengesan pengionan nyalaan (KG-PPN). Logam berat diekstrak secara pencernaan dengan
larutan aqua regia dan seterusnya dianalisis dengan aruhan gandingan plasma-spektrometer
pancaran optik (A GP-SPO). Jumlah kepekatan hidrokarbon alifatik dan HAP dalam sampel
teras adalah dalam julat 2512.4 - 6566.0 mg/kg dan 518.0 - 1210.4 mg/kg berat kering.
masing-masingnya. Kepekatan agak tinggi bagi hidrokarbon dan logam berat yang dicerapi
pada tapak persampelan berhampiran loji dan pada lapisan atas sampe/ teras mencadangkan
input antropogenik. Indek molekul dan corak taburan hidrokarbon telah digunakan untuk
meramal sumber hidrokarbon. Indek diagnostik menunjukkan hidrokarbon tersebut adalah
bersifat pelrogenik (bahan api fossil) dan pirogenik. Hidrokarbon ini terhasil dari
pembakaran tidak fengkap arang batu dari foji janakuasa. Jumlah karbon organik
merupakan salah satu faktor penting yang mempengaruhi kepekatan hidrokarbon dalam
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tanah. Kepekatan jumlah hidrokarbon alifatik dan HAP dalam sampel teras dari kawasan
kajian berkait dengan jumlah karbon organik tanah. Corak taburan logam berat dalam
kawasan kajian juga digunakan untuk meramal sumber logam berat. Logam bera! yang
dominan dalam sampel teras adalah Mn, Zn, V dan Pb. Taburan dan tapalgalan
penyelerakan hidrokarbon dan logam berat dalam tanah di kawasan kajian diramal
menggunakan analisis korelasi mudah. Korelasi yang tinggi untuk kedua-dua hidrokarbon
dan logam berat terhadap abu terbang arang batu mencadangkan bahawa abu terbang
adalah sumber pencemaran. Corak taburan spatial hidrokarbon dan logam berat
menunjukkan keadaan cuaca mempengaruhi taburan pence mar di kawasan kajian. Nilai
indek pencemaran untuk kebanyakan tapak persampelan di sekitar kawasan MPG
menunjukkan bahawa kawasan kajian adalah tercemar dengan hidrokarbon alifatik, HAP
dan logam berat dari pelepasan loji. Hasil kajian ini boleh digunakan sebagai data garis
dasar dalam penilaian risiko kesihatan berkait dengan kesan loji janakuasa arang batu
terhadap persekitaran.
Kata kunci: Hidrokarbon, logam berat, tanah, kromatograji gas-pengesan pengionan
nyalaan (KG-PPN), aruhan gandingan plasma-spektrometer pancaran optik (A GP-SPO),
pengenalpastian sumber.
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TABLE OF CONTENT
Pages
DECLARATION
ACKNOWLEDGEMENTS ii
ABSTRACT iii
ABSTRAK v
TABLE OF CONTENT VII
LIST OF FIGURES xiii
LIST OF TABLES xvi
LIST OF ABBREVIATIONS xviii
CHAPTER ONE: INTRODUCTION
1.1 General Introduction
1.2 Coal in Malaysia 3
1.3 Significance of Studies 5
1.4 Objectives 6
1.5 Scope of the Study 7
CHAPTER TWO: LITERATURE REVIEW
2.1 Coal Formation 8
2.2 Classification of Coal to
2.3 Heavy Metals in Coal 13
2.3.1 Occurrence and distribution 13
2.3.2 Enrichment of heavy metals in coal 15
VII
2.3.3 Mode of occurrence of heavy metals in coal 16
2.4 Hydrocarbons in Coal 17
2.4.1 Aliphatic hydrocarbons in coal 17
2.4.2 Aliphatic hydrocarbons molecular indices 19
2.4.3 Aromatic hydrocarbons in coal 21
2.4.4 P AHs molecular indices 25
2.5 Coal Ash 27
2.5.1 Bottom ash 28
2.5.2 Fly ash 29
2.5.3. Chemical composition of coal ash 30
2.5.3.1 Heavy Metals in Coal Ash 31
2.5.3.2 Hydrocarbons in Coal Ash 33
2.6 Ash Disposal Area 34
2.7 Environmental Impacts of Coal-Fired Power Plant 35
2.7.1 Soil pollution 36
2.7.2 Sediment pollution 37
2.8 Anthropogenic Organic Pollutants: PAHs 38
2.8.1 PAHs in soils 38
2.8.2 PAHs in sediments 42
2.8.3 PAHs causitive agent associated with cancer 44
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CHAPTER THREE: DISTRIBUTION OF ALIPHATIC AND POLYCYCLIC
AROMATIC HYDROCARBONS (PAHs) IN ASH FROM MUKAH POWER
GENERATION PLANT
3.1 Introduction 45
3.2 Materials and Methods 47
3.2.1 Sampling sites and samples collection 47
3.2.2 Soil extraction and lipid fractionation 50
3.2.3 Gas chromatographic analysis of aliphatic hydrocarbons and P AHs 50
3.2.4 Total organic carbon (TOC) analysis 51
3.2.5 Particle size analysis 51
3.2.6 Coal quality testing 53
3.2.6.1 Proximate Analysis 53
3.2.6.1.1 Determination of moisture (Mq) 54
3.2.6.1.2 Determination of ash 55
3.2.6.1.3 Determination of volatile matter (VM) 55
3.2.6.1.4 Determination of fixed carbon (FC) 56
3.2.6.2 Ultimate Analysis 57
3.2.6.2.1 Determination of the percentage carbon, hydrogen 57 and nitrogen (CHN)
3.2.6.2.2 Determination of sulphur (S) 58
3.2.6.2.3 Determination of oxygen (0) 58
3.2.6.3 Determination of Gross Calorific Value (GCV) 58
3.3 Results and Discussion 60
3.3.1 Quality of feeds coal for MPG 60
3.3.2 Characteristics of soils and sediment sample 61
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3.3.3 Aliphatic hydrocarbons 63
3.3.3.1 Spatial Distribution of n-Alkanes 63
3.3.3.2 Vertical Distribution of n-Alkanes 66
3.3.3.3 Sources of n-Alkanes 69
3.3.4 Polycyclic aromatic hydrocarbons 80
3.3.4.1 Spatial Distribution of PAHs 80
3.3.4.2 Vertical Distribution of PAHs 82
3.3.4.3 Sources of P AHs 85
3.3.5 Fossil fuel derived n-alkanes versus TPAHs relationship 107
3.3.6 The role of total organic carbon (TOC) 108
3.3.7 Assessment of hydrocarbons contamination III
3.4 Conclusions 114
CHAPTER FOUR: HEAVY METALS IN ASH FROM MUKAH POWER
GENERATION PLANT
4.1 Introduction
4.2 Materials and Methods
4.2.1 Sampling sites and sample collection
4.2.2 Extraction of heavy metals
4.2.3 Inductively couple plasma-optical emission spectrometer (ICP-OES)
4.2.4 Determination of pH
4.2.5 Particle size distribution and total organic carbon (TOC)
4.3 Results and Discussion
4.3.1 Spatial distribution of heavy metals in MPG area
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4.3.2 Vertical distribution of heavy metals in MPG area 129
4.3.3 Correlation coefficient analysis 135
4.3.4 Source identification 138
4.3.5 Environmental assessment of heavy metals 139
4.4 Conclusions 145
CHAPTER FIVE: GENERAL CONCLUSIONS AND RECOMMENDATIONS
5.1 General Conclusions 146
5.2 Recommendations 149
REFERENCES 151
APPENDICES
Appendix 1: ASTM test methods for coal proximate analysis (ASTM, 2007c, d, e and f).
Appendix 2: ASTM test methods for coal ultimate analysis (ASTM, 2007i and j).
Appendix 3: Gas chromatogram from GC-FID analysis of n-alkanes in standard mixture.
Appendix 4: Typical GC-FID chromatograms for aliphatic fractions of core samples from MPG area.
Appendix 5: Concentrations (mg/kg dw) of individual n-alkanes in the soils and sediments from study area.
Appendix 6: Gas chromatogram from GC-FID analysis ofPAHs in a standard mixture.
Appendix 7: Typical GC-FID chromatograms ofPAHs fractions of core samples from MPG area.
Appendix 8: Concentrations (mg/kg dw) of 16 US EPA priority PAHs in the soils and sediments from study area.
Appendix 9: The results of the selected heavy metals contents (mg/kg dw) in nine core samples and flyash analysed in this study (n=3).
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LIST OF FIGURES
Figures Titles Pages
Figure 1.1 Electricity generation mix in Malaysia in 2010 (APEC, 2012) 5
Figure 2.1 Simplified coal genesis (Haenel, 1992). 10
Figure 2.2 Some structures of PAHs according to rings number 22
Figure 2.3 The molecular structures of benzopyridine, benzoquinone and 23 benzotropolone
Figure 2.4 Molecular structures of some carcinogenic PAHs (IARC, 1983) 40
Figure 3.1 The study area and the location of sampling sites. 48
Figure 3.2 Soil textural triangle ofthe USDA classification scheme (Starr et aI., 53 2000).
Figure 3.3 Distribution ofTNA in soil and sediment collected from study area. 65
Figure 3.4 Vertical profiles ofTNA in the cores soil from study area (SS1 - 68 SS5 and CSS).
Figure 3.5 Vertical profiles ofTNA in the core sediments from study area 69 (SD 1, SD2 and CSD).
Figure 3.6 Distribution of individual n-alkanes in soils near the plant chimney 71 from study area (SS 1, SS4 and SS5).
Figure 3.7 Distribution of individual n-alkanes in soils far from the plant 72 chimney in study area (SS2 and SS3).
Figure 3.8 Distribution of individual n-alkanes in sediments from study area 73 (SO 1 and SD2).
Figure 3.9 The vertical distribution of the ratio ofLMW/HMW n-alkanes in the 75 core soil samples from MPG area (SS 1 - SS5).
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Figure 3.10 The vertical distribution of the ratio ofLMW/HMW n-alkanes in the 76 core sediment samples from MPG area (SD 1 and SD2).
Figure 3.11 The vertical distribution of the CPI in the core soil from MPG area 77 (SSI- SS5).
Figure 3.12 The vertical distribution of the CPT in the core sediment from MPG 78 area (SD 1 and SD2).
Figure 3.13 The spatial distribution ofTPAHs in surface soils and sediments 81 from study area.
Figure 3.14 Vertical profiles of TPAHs in the cores soil from study area (SS 1 - 84 SS5 and CSS).
Figure 3.15 Vertical profiles of TPAHs in the cores sediment from study area 85 (SDl, SD2 and CSD).
Figure 3.16 Distribution of individual PAHs In soils near the chimney from 87 MPG area (SS 1, SS4 and SS5).
Figure 3.17 Distribution of individual PAHs in soils far from the chimney in 88 MPG area (SS2 and SS3).
Figure 3.18 Distribution of individual PAHs in sediments from MPG area (SDI 89 and SD2).
Figure 3.19 Percentage of PAHs in soils collected from MPG area according to 90 their benzene ring number.
Figure 3.20 Percentage of PAHs in sediments collected from MPG area 90 according to their benzene ring number.
Figure 3.21 Relative amount of PAHs from different sources in the soil and 92 sediment of MPG area.
Figure 3.22 Un burnt coal particles scattered in the ash ponds due to incomplete 93 combustion from MPG.
Figure 3.23 Plots ofLMW/HMW PAHs ratios versus TPAHs for the surface soil 99 and sediment of MPG area.
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Figure 3.24 Plots of Ant/(Ant + Phe) ratios versus TPAHs for the surface soil 100 and sediment ofMPG.
Figure 3.25 Plots of Flua/(Flua + Pyr) ratios versus TPAHs for the surface soil 101 and sediment of MPG area.
Figure 3.26 Plots of B[a]Ant/(B[a]A + Chry) ratios versus TPAHs for the 103 surface soil and sediment ofMPG area.
Figure 3.27 Concentration ofPAHs in flyash samples from MPG area. 105
Figure 3.28 Concentration ofPAHs in soil samples from MPG area. 106
Figure 3.29 Concentration ofPAHs in sediment samples from MPG area. 106
Figure 3.30 Relationship of TPAHs versus fossil fuel n-alkanes in the soil and 108 sediment of MPG area.
Figure 3.31 The correlation between the concentrations of TNA with percentage 109 ofTOC.
Figure 3.32 The correlation between the concentrations of TPAHs with 110 percentage ofTOC.
Figure 3.33 Distribution of PIs for TNA and TPAHs in the surface soils and 113 sediments collected from MPG area.
Figure 4.1 Concentrations of individual heavy metals (Cr, Mn, Co, Ni and V) 125 in class I at surface soil and sediment of the study area.
Figure 4.2 Concentrations of individual heavy metals (Cu, Zn, Cd, As and Pb) 126 in class II at surface soil and sediment of the study area.
Figure 4.3 Distribution of heavy metals in the surface soils of study area (SS 1 - 127 SS5 and CSD).
Figure 4.4 Distribution of heavy metals in the surface sediments of study area 128 (SD 1, SD2 and CSD).
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Figure 4.5
Figure 4.6
Figure 4.7
Figure 4.8
Vertical profile of heavy metals (Cr, Mn, Co, Ni and V) concentration within class I in core soils collected from MPG area.
Vertical profile of heavy metals (Cu, Zn, Cd, As and Pb) concentration within class II in core soils collected from MPG area.
Vertical profile of heavy metals (Mn, Co and V) concentration within class I in core sediments collected from MPG area.
Vertical profile of heavy metals (Cu, Zn, Cd, As and Pb) concentration within class II in core sediments collected from MPG area.
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Figure 4.9 Plots of heavy metals concentration in soils and sediments relative 140 to the heavy metals concentration in flyash released from MPG.
Figure 4.10 Plots of heavy metals pollution index (PI) in the soil and sediment 142 within vicinity of MPG.
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LIST OF TABLES
Tables Titles Pages
Table 1.1 List of the coal-fired power plants in the Malaysia (Jaffar, 2009). 4
Table 2.1 The classification of coal by rank according to ASTM (2007a). 12
Table 2.2 Enrichment factor of heavy metals in coal with respect to the average 16 composition of the earth's crust (USNCG, 1980).
Table 3.1 Location of nine sampling sites within study area. 49
Table 3.2 ASTM test methods for coal proximate analysis. 54
Table 3.3 ASTM test methods for coal ultimate analysis. 57
Table 3.4 MPG feeds coal quality. 61
Table 3.5 Distribution of particle size, total organic carbon, total nitrogen and 62 mole ratio of carbon over nitrogen in samples.
Table 3.6 TNA concentration (mg/kg dw) in soil and sediment cores collected 64 from study area.
Table 3.7 The grouping of the sampling sites for soil samples into two zones at 70 MPG area.
Table 3.8 The average value of CPI in core soils and sediments from MPG area. 78
Table 3.9 Comparison of CPI values with the reported values in other cities of 79 China.
Table 3.10 Diagnostic ratios of PAHs in the soil of MPG area. 94
Table 3.11 Diagnostic ratios ofPAHs in the sediment ofMPG area. 95
Table 3.12 The plant wax n-alkanes in the soil and sediment ofMPG area. 107
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Table 3.13 The concentration of TNA and TPAHs in the surface soil and 112 sediment of the study area.
Table 4.1 The concentration of the selected heavy metals (mg/kg dw) in surface 124 soil from study area (n=3).
Table 4.2 The concentration of the selected heavy metals (mgikg dw) in surface 124 sediment from study area (n=3).
Table 4.3 Values for the heavy metals concentration, total organic carbon 136 (TOC), PAHs and pH for soil cores collected from MPG area.
Table 4.4
Table 4.5
Table 4.6
Pearson correlation coefficients, r, between heavy metals concentrations, TOC, PAHs and pH.
Heavy metals pollution index (PI) for soil and sediment within vicinity of MPG.
Distribution of heavy metals concentrations compared to the Netherlands Soil Contamination Guidelines (DSPN, 1994).
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Acp
Acpy
Ant
ASTM
B[a]A
B[a]P
B[b]F
BCS
B[ghi]P
B[k]F
CCRs
CHN
Chry
CPI
CRM
DB [a,h]A
DCM
dw
EF
LIST OF ABBREVIATIONS
Acenapthene
Acenapthy lene
Anthracene
American Society for Testing and Materials
Benzo[ a ] anthracene
Benzo[ a ]pyrene
Benzo[b ]tluoranthene
British certified standard
Benzo[ghi]perylene
Benzo[k ]fluoranthene
Coal combustion residues
Carbon, Hydrogen and Nitrogen
Chrysene
Carbon preference index
Certified reference material
Dibenzo[a,h ]anthracene
Dichloromethane
Dry weight
Enrichment factor
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FC
Flua
Flu
GC
GC-FID
GCV
GPS
HMW
IARC
i.d.
I[ 1 ,2,3-cd]P
IPP
L
LMW
MPG
mL
mtpa
MW
Nap
Fixed carbon
Flouranthene
Fluorine
Gas chromatography
Gas chromatograph-flame ionisation detector
Gross calorific value
Global positioning system
High molecular weight
International Agency for Research on Cancer
Internal diameter
Indeno[l,2,3-cd]perylene
Independent Power Producer
Liter
Low molecular weight
Moisture
Total moisture
Mukah power generation plant
milliliter
Million tonne per annum
Megawatt
Naphthalene
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NIST
TNA
PAHs
PFA
Phe
PI
PIC
ppm
Pyr
RSD
SOC
TPAHs
RSD
TN
TOC
UCM
USEPA
USDA
J.lglml
J.l1
National Institute of Standard and Technology
Total n-alkanes
Polycyclic aromatic hydrocarbons
Pulverised fuel ash
Phenanthrene
Pollution index
Products of incomplete combustion
Part per million
Pyrene
Relative standard deviation
Soil organic carbon
Total PAHs
Relative standard deviation
Total nitrogen
Total organic carbon
Unresolved complex mixture
United States Environmental Protection Agency
United States Department of Agriculture
Microgram per millimeter
Microliter
Micrometer
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VM
WCA
WNA
Volatile matter
World coal association
Wax n-alkanes
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CHAPTER ONE
INTRODUCTION
1.1 General Introduction
Fossil fuels such as coal, petroleum and natural gas have supplied most of the world's
energy requirements. Energy is essential in transportation, agricultural and industrial and
constructional development, which are indispensable to the scientific, technical, cultural and
socio-economic progress of every nation. Coal represents the accumulation of organic
materials in sedimentary strata. In other words, coal is an organoc1astic sedimentary rock
composed essentially of lithified plant debris. The initial sediment formed by this process is a
moist, spongy material called peat. It becomes compressed, dried, and modified in both
texture and composition due to diagenesis associated with burial and tectonic activity. It is
more plentiful than oil and gas, at the current production rate with around 119 years of coal
remaining worldwide (WCA, 2011).
The energy crisis caused by the reduction of fuel oil availability and the consequent
continuous increase of the oil fuel prices contributes to the increase on the worldwide use of
coal. Global coal consumption has grown faster than any other fuel since 2000. The most
significant use of coals nowadays is in electricity generation. World net electricity generation
increases from 18.0 trillion kilowatt hours in 2006 to 23.2 trillion kilowatt-hours in 2015 and
31.8 trillion kilowatt hours in 2030 (Meawad et ai., 2010). Coal fired generation in 2006
accounted for 41 % of world electric supply and projected to be 43% by 2030. This reflects
coal continues to fuel the largest share of worldwide electric power production. In 2008, about
1