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The processes ofdegradation might play an important role at station 971. This is shown by its position in the left part of the graph in Figure 5.2.3. 1be location indicates predominance ofhigher molecular weight compounds (OFI, BeP, BaP) over lower molecular weight PAH (Fa, Py; Fig. 4.2.5a). The ratio/ratio mixing curves for molecular com position also demonstrate that station 971 is shifted away from primary sources and thei r mixing arrays towards predominance ofhigher molecular weight compoWlds (Fig. 4.2.2. 4.2.3). The process ofweathering could be enhanced here due to increased microbial activity resulting from possible presence ofoil in sedime nts (Lee and Takahashi. 1977: Neff. 1979). The laner is indicated by the increased relative importance of petroleum-related sources in PAM supp ly. In addition, well oxygenated shallow water column (Fig. 5.1.11) and increased water temperatures in summer (Fig. 2.1.8) might also ha ve facilitated various processes ofdecomposition at this site (payne and Phillips, 1985: Mille et al.• 1988: Kelly et 01.. 1991). FinaJly this station is located as far as 30 kilometers downstream from the City of Detroit and thus the PAH assemblage might undergo significant changes during irs transport. prior to deposition in lake sediments. Cleveland (Station 955): Petroleum sources seem to be less important at Cleveland than at Detroit. However they may still influence the formation ofcertain compounds. The overa ll predominance ofcombustion sources is indicated by the position ofstation 955 within the shaded (com bustion) zone in Figure 5.2.3. This position is determined by relatively heavy isotopic values ofall compounds as indicated by PC 1 for isotopic composition (Fig. 4.2.19a). [n addition, none ofthe characteristic ratios indicates 206
contribution from petroleum related sources at this site (F ig. 4.2.1). The comparison with characteristic ranges for Sl3C also demonstrates complete absence ofpetroleum influence in the assemblage (Fig. 4.2.6). However, mass balance calculations showed that as much as 10% ofPy. 30% ofChy and 40% ofBePIBaP could stiU have been derived from petroleum related sources (Fig. 4.2.7). Further, the mixing curves for isotopic composition also indicate that 10-30% ofme higher molecular weight compounds (Chy BaP) might originate from petroleum (Fig. 4.2.9, 4.2.12 - 4.2.14). Both wood burning and fossil fuel combustion sources have almost equaUy contributed to the formation ofthe PAH assemblage at Cleveland. This is first shown by PC 3 for molecular composition which demonstrates almost equivalent contribution of car em issions and fife soots to the formation ofcompounds (Fig. 4.2.5c). In addition, the isotopic composition of Py also indicates that PAH at this site are almost equally supplied by the two prominent contributors (Fig. 4.2.19c). The PAH produced by the city might be further directed to the aquatic environment through city runoffand releases ofsewers. The importance ofthese two pathways is indicated by the relative contribution ofPy vs. ChyfBaP to the PAH assemblage at station 955 (Fig. 4.2 .5c). In the mixing curves for slle values, this station is also often shifted towards the road sweep end member (Fig. 4.2.8, 4.2.10, 4.2.11, 4.2.15). The lattcragain indi cates the possible importance ofdirect city runoffas a pathway ofPAH into the lake. The increased role ofsurface runoffas compared to that at Detroit may possibly be attributed to somewhat different precipitation regime ofthe two areas (Fig. 2.1.9). ]JJ7
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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
Page 177: f igure 5.1.1 Zones coinciding with
Page 180: 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 231 and 232: (Fig. 4.2.7). Finally. this site co
Page 233 and 234: Snow melt and sewer releases seem t
Page 235 and 236: importance ofcombustion-derived PAR
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
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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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