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that at Cbeland. Conversely, Detroit samp le (97 1) is located among the major group of stat ions showing average:isotopic composition. Slatioos 961 and 84 seem to occupy intermediafe position between the two cities. The second component el(plains 21"'. ofvarianc:c and can be attributed to an op position in isotopic composition o f higher (> 228) and loWCl" « 202) molecular weight compounds (Fig. 4.I.gb). Most sta tions demonstrate isotopically balanced compounds. However. station 1021 shows heavy values forCby and BbF andlight values for Fa. The third PC aCCOWllS for 11.5% oftotal variance (Fig. 4.1.6). This component is most significan tly influenced by the isotopic composition of Py (72%). The interpretation is confirmed by sign ificanl correlation (FO.76; p
those at the majority ofstations. Station 1021 is distinct due to the relationship between isotopic co mpos ition oflower and higher molecular weight compounds. Finally, stations 953 and 951 are marked by unbalanced isotopic values for Pyand Pa, Per. 4.2 SOURCE IDENTlF1CAnON 4.2.1 MOLECUlAR COMPOSmON ".2.1.1 Characteristic ratios and mixing cutveS The ratios of kinetic to thennodynamic isomers have been found characteristic of the relative contribution of combustion and petroleum sources to the PAH assemblage (e.g., Yunker and Macdonald, 1995; see also Appendix. AS). In addition, Lipiatou and Saliot (1992) demonstra ted that PylPer ratio may serve as an indicator ofthe intensity of diagenetic processe s. Foll owing these ideas, three commonly used isomer ratios (FaIPy, BbFf8kF. BaP!BeP) and the Py/Per ratio were calculated and plotted against the longest axis of the lake (Fig. 4.2.1). The general pattern that emerges from the cons ideration of the ratio profiles is that combustion sources dominate over petroleum. input and anthropogenic produ ction ofPAH is more important than diagenetic so urces throughout the lake. However, there are a few sites where petroleum related sources can playa significant role and/or the process ofdiagenesis might be intensive. Although the isomer ratios may be ambiguo us in some cases, a few regions with an increased importance o f petroleum-related sources can be discerned across the lake. The ratio of Fa to Py consistently indicates petroleum. presence in the Western Basin. The affected sites seem to beconcentrated close to the mouth of tbe Detroit River (974, 973, 102
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POLYCYCLIC AROMATIC HYDROCARBONS IN
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composition. Portions ofthe lake th
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TABLE OF CONTENTS . ABSTRAcr._._ _
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6. CONCLUSIONS_._ _....._._._ _ ._
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FIGURE 3.104 CONfIGURATION OF ISOCH
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FIGURE 4 .2.12 SAMPLES AND PROMINEN
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fIGURE 5.3.1 DESCR1Pl1VE MODEL OF S
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APPENDIX B 3 _ T HEoerwt Of A PtUNC
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Ip » Ideno(l,2.3 cd)pyrene NIST =
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Figure L 1.1 The 16 parental polycy
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After release by the primary source
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decomposition processes (O'Malley e
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Figure 2.1.1 The Great Lakes draina
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;: Duluth Chicago 1 J Lake Superior
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are the Black River, the Cuyaho ga
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Figure 1.1.5 The pattern of permane
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sedimentary basins, Western. Centra
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Figure 2. 1.8 Summer (July) air and
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Natural Resources: The lower Great
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American waters under the current U
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continuously overflowed com bined s
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3.1 EXPERIMENTAL 3. METHODS 3.1.1 S
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Table 3,1.1 Locations and types ofs
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Figure 3.12 Extraction and purifica
Page 72 and 73: hexane. 2) the unsaturated aliphati
Page 75: this problem. Ratios ofthe two stab
Page 78: Figure 3. 1.4 Configuration ofIsoch
Page 82 and 83: 3.2.1 UNl- AND BIVAJUATE METHODS Th
Page 84: f igure 3.2. 1 Mean and range (± s
Page 87 and 88: utilized the same instrument (Isoch
Page 90 and 91: Selecting lIt1J'iahlu: It was demon
Page 92 and 93: w- _ 71
Page 95 and 96: seven variables with fewer missing
Page 97 and 98: analysis also employed a greate r n
Page 99: description. The second cluster ana
Page 104 and 105: elationships between different site
Page 107: Figure 4.1.3 Regression ofthree fir
Page 112: Figure 4.[.5 Isotopic composition (
Page 116: Figure 4.1.6 Weights ofvariables (c
Page 120: Figure 4.1.8 Distri bution ofsample
Page 126 and 127: Ion, 969, 971, 357, 358). In additi
Page 129: Figure 4.2.3 Samples and prominent
Page 132 and 133: analysis supported some ofthc previ
Page 135 and 136: , ", Is , , >\ ryr " II ,- - , I ,
Page 137 and 138: 11'
Page 139: sources (Fi g. 4.2 .5c). This compo
Page 143: Figure 4.2.7 The relative contribut
Page 146 and 147: ".1.1.2 Miring CllrIIU (isotopic co
Page 149: Figure 42.9 Samples and promin ent
Page 157: Figure 4.2. 13 Samples and prominen
Page 168 and 169: It is difficult to differentiate be
Page 170 and 171: Figure 4.2.18 Weights ofvariables (
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Figure 42.19 Distribution ofsamples
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5.1 SPATIAL DI STRIBUTION s. DISCUS
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f igure 5.1.1 Zones coinciding with
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f igure 5. 1.2 Average and range (
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Figure 5.1.4 Zones (clusters) in th
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Figure 5.1.5 Direction ofthe mean s
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The location ofthe third station at
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Figure 5.1.7 Station locations and
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5.1.4 and Section 4.1.2). This clus
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Figure 5.1.1 1 Statioo locations an
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unaffected by the contaminated flow
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this station is die clo$esf to the
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samples and sources (Fig. 52.1 and
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There is yet another observation po
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with the relative contribution ofdi
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Table S.l.1 Six dusters identified
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the three previous ly identified zo
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contribution from petroleum related
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(Fig. 4.2.7). Finally. this site co
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Snow melt and sewer releases seem t
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importance ofcombustion-derived PAR
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Intens ity o(degradation (the South
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where this importance is somewhat r
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Figure 5.2.5 Station tocatices andz
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:2 for molecular composition assume
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ange of Slatistica1 variat ion of t
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Figure 5.].1 Descriptive model ofso
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conveyed into the river through dir
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molecular composition. Its applicat
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Canton L. and Grimal t 1. O. (1992)
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Howell E. T., Marvin C. H., Bilyea
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Olson F. C. W. (l950) The currents
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Willett P. (1981) Similarity and cl
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t Apprndb AI. [cout.) bl S,.lioD A<
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Appendill A6. The two-component mas
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Appendix A7. (cont.) Xl. = X llVt r
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• ass
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Appendix 82. (cont.)
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Appendix IU. (cant.) oj Tue Dec 24
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AppendiI C3. (cont.) Coo c.eo lrati
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