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A high-resolution record of polycyclic aromatic hydrocarbon (PAH) deposition in Rhode Island over the past ∼180 years was constructed using a sediment core from the anoxic Pettaquamscutt River basin. The record showed significantly more structure than has hitherto been reported and revealed four distinct maxima in PAH flux. The characteristic increase in PAH flux at the turn of the 20th century was captured in detail, leading to an initial maximum prior to the Great Depression. The overall peak in PAH flux in the 1950s was followed by a maximum that immediately preceded the 1973 Organization of Petroleum Exporting Countries (OPEC) oil embargo. During the most recent portion of the record, an abrupt increase in PAH flux between 1996 and 1999 has been found to follow a period of near constant fluxes. Because source-diagnostic ratios indicate that petrogenic inputs are minor throughout the record, these trends are interpreted in terms of past variations in the magnitude and type of combustion processes. For the most recent PAH maximum, energy consumption data suggest that diesel fuel combustion, and hence traffic of heavier vehicles, is the most probable cause for the increase in PAH flux. Systematic variations in the relative abundance of individual PAHs in conjunction with the above changes in flux are interpreted in relation to the evolution of combustion processes. Coronene, retene, and perylene are notable exceptions, exhibiting unique down-core profiles.

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Petroleum-derived hydrocarbons continue to persist in Wild Harbor, West Falmouth, MA, following a spill of No. 2 fuel oil in 1969 from the barge Florida. Recent analysis of marsh sediments revealed that residues of degraded oil are present with concentrations of total petroleum hydrocarbons as high as approximately 9 mg g(-1). Polycyclic aromatic hydrocarbons (PAHs) constitute only a minor fraction of these residues with maximum concentrations of 134 mirog g(-1), but their fate is of interest because of their potential toxicity to organisms. As compared to typical unweathered No. 2 fuel oil, the current distribution of PAHs in the sediments reflects substantial weathering by abiotic and biotic processes, specifically a preferential loss of naphthalenes relative to phenanthrenes, as well as isomer-specific biodegradation of alkylated PAHs. Based on comparison to results from an earlier study, it appears that little or no change has occurred to the distribution of PAHs since 1989, indicating that weathering at this site has stalled or is now proceeding at a significantly slower rate. To assess whether sediment-water partitioning and molecular diffusion in the interstitial medium are now the dominant processes controlling the vertical distribution of PAHs, downcore profiles were compared to a numerical model. While in some cases the model accurately reproduced the measured data, there were instances where the distribution of PAHs was slightly under or overestimated. Reasons for these discrepancies are discussed and are likely due to bioturbation, colloid-facilitated transport, or both. Assessment of the influence of these processes on the spilled oil expands our understanding of the overall fate of these compounds and their potential long-term effects on the environment.

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