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subzones ofinfluence was suggested. This separation is confinned by Figure 5.23 and can be attributed to different relative importance ofpetroleum sources in the PAH assemblage generally dominated by combustion-produced compounds. The highest overall contribution from petroleum sources within this zone is demonstrated by station 953. Stations affected bv the Detroit River: As stations 357, 358, 969, 974, 1012, and 961 were shown to be affected by the outflow ofthe Detroit River, they are characterized by fairly significant contribution ofpetroleum-related sources to the PAH assemblage typical of this signal. This is indicated by their position in the lower halfofFigure 5.2.3, characteristic ofpetroleum influence. The influence ofpetroleum-related sources is expressed in light isotopic values for all compounds (Fig. 4.2.19). These stations also show predominance ofPy over Fa (Fig. 4.2.1) characteristic ofpetroleurn input (e.g., Yunker and MacDonald, 1995; Yunker et al.; 1995). The isotopic value s for BeP, RaP and Fa for most stations fluctuate close to the characteristic petroleum range (Fig. 4.2.6). In addition. the mas s balance calculations also indicate that relative contribution of petroleum is very high at these sites (Fig. 4.2.7). The greatest contributionofpetroleum related sources is seen at station 969 (BeP!BaP=9O"/o; Fig. 4.2.7). This might be due to possible seepage ofcrude oil from the oil field located in this region (fig. 5.2.4). On the contrary, station 974 demonstrates the least contribution ofpetroleum in the region. It is worth noting that thi s station may, to some extent, be affected by the outflow ofthe Maumee River at Toledo. This outflow might be characterized by an increased 212
importance ofcombustion-derived PAR. Further, the location ofthis group ofstatioos on the graphs for mixing curves also conflrms the importance ofpctroleum in the fonnatioo of the PAH assemblage (Fig. 4.2.8-4.2.17). Finally, these statiOlLS occupy an intermediate position between petroleum and combustion sources on the third principal component for molecular data . responsible for their relative contribution (Fig. 4.2.5c). Stations atkctedby the outRow at Cleveland: The PAH assemblage from stations 961.84.1021.23 , and 935 demonstrate similarities to the pollution signa) introduced by Cleveland in which combustion sources entirely dominate over petroleum. This is first indicated by the location orthis group in the shaded zone in Figure 5.2.3. This position is explained by relativel y heavy isotopic composition for all compounds (Fig. 4.2.19a). The characteristic ratios ofkinelic compounds to their thennodynamic isomers demonstrate predominance ofthe less stable compounds for almost all the stations (Fig. 4.2.1). Only at station 84 the ratio FaIPy is less than unity. This and somewhat lighter isotopic composition for Pa (Fig. 42 .6) show that this site might still be affected by the petroleum signal introduced by the Detroit River. The minimum contribution ofpetroleum at most stations is also shown by their position on the mixing curve graphs (Fig. 4.2.8-4.2.17). Only the relative abundance of Py vs. Chy and BaP indicated possible minor influence of petroleum related sources (Fig. 4.2.5c). The isotopic composition ofStation 1021 is somewhat different from the other stations withinthis subcluster. It demonstrates very light isotopic values for Fa while the composition ofBAIChy is enriched with respect to IlC (Fig. 4.2.8, 4.2.9, 4.2.15-4.2.17). None ofthe sources employed in the present study 213
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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
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hexane. 2) the unsaturated aliphati
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this problem. Ratios ofthe two stab
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Figure 3. 1.4 Configuration ofIsoch
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3.2.1 UNl- AND BIVAJUATE METHODS Th
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f igure 3.2. 1 Mean and range (± s
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utilized the same instrument (Isoch
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Selecting lIt1J'iahlu: It was demon
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w- _ 71
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seven variables with fewer missing
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analysis also employed a greate r n
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description. The second cluster ana
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elationships between different site
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Figure 4.1.3 Regression ofthree fir
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Figure 4.[.5 Isotopic composition (
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Figure 4.1.6 Weights ofvariables (c
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Figure 4.1.8 Distri bution ofsample
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those at the majority ofstations. S
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Ion, 969, 971, 357, 358). In additi
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Figure 4.2.3 Samples and prominent
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analysis supported some ofthc previ
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, ", Is , , >\ ryr " II ,- - , I ,
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11'
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sources (Fi g. 4.2 .5c). This compo
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Figure 4.2.7 The relative contribut
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".1.1.2 Miring CllrIIU (isotopic co
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Figure 42.9 Samples and promin ent
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Figure 4.2. 13 Samples and prominen
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It is difficult to differentiate be
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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 (
Page 184: Figure 5.1.4 Zones (clusters) in th
Page 187: Figure 5.1.5 Direction ofthe mean s
Page 191 and 192: The location ofthe third station at
Page 193: Figure 5.1.7 Station locations and
Page 201 and 202: 5.1.4 and Section 4.1.2). This clus
Page 204: Figure 5.1.1 1 Statioo locations an
Page 208 and 209: unaffected by the contaminated flow
Page 211 and 212: this station is die clo$esf to the
Page 213 and 214: samples and sources (Fig. 52.1 and
Page 216 and 217: There is yet another observation po
Page 218 and 219: with the relative contribution ofdi
Page 221 and 222: Table S.l.1 Six dusters identified
Page 224 and 225: the three previous ly identified zo
Page 229 and 230: contribution from petroleum related
Page 231 and 232: (Fig. 4.2.7). Finally. this site co
Page 233: Snow melt and sewer releases seem t
Page 237 and 238: Intens ity o(degradation (the South
Page 239 and 240: where this importance is somewhat r
Page 241: Figure 5.2.5 Station tocatices andz
Page 244 and 245: :2 for molecular composition assume
Page 247 and 248: ange of Slatistica1 variat ion of t
Page 249: Figure 5.].1 Descriptive model ofso
Page 252 and 253: conveyed into the river through dir
Page 254 and 255: molecular composition. Its applicat
Page 256 and 257: Canton L. and Grimal t 1. O. (1992)
Page 258 and 259: Howell E. T., Marvin C. H., Bilyea
Page 260 and 261: Olson F. C. W. (l950) The currents
Page 263 and 264: Willett P. (1981) Similarity and cl
Page 266: t Apprndb AI. [cout.) bl S,.lioD A<
Page 271 and 272: Appendill A6. The two-component mas
Page 273: Appendix A7. (cont.) Xl. = X llVt r
Page 277: • ass
Page 281: 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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