Molecular and isotopic records of the combustion inputs to the environment over the last 250 yrs

The most ubiquitous source of polycyclic aromatic hydrocarbons (PAHs) to the environment is incomplete combustion. This study generated a high-resolution historical record of pyrogenic PAH emissions since pre-industrial times from anoxic aquatic sediments, allowing for detailed comparison with energy consumption data. We show that an increase in PAH concentrations over the last decade may be due to a rise in emissions from diesel-powered vehicles. Compound-specific radiocarbon measurements demonstrated unequivocally that the proportion of PAHs derived from fossil fuel combustion has increased substantially during the 20th century. [delta]¹³C and [delta]¹⁴C measurements were also used to constrain the relative importance of combustion versus in situ production as sources of perylene. In addition, a comparison of the down-core concentration and isotopic profiles of black carbon (BC) generated by a combination of chemical and/or thermal oxidation methods highlighted the limitations of these methods when applied to sedimentary matrices. Finally, parallel lead and cesium isotopic records revealed two new potential stratigraphic markers in North American sedimentary records. ²⁰⁶Pb/²⁰⁷Pb profiles show a distinct peak in the mid-19th century, while a ¹³⁷Cs peak was found to coincide with the 1986 Chernobyl accident.

Department dc:contributor.department

Joint Program in Oceanography

Grantor dc:publisher

Massachusetts Institute of Technology

Year dc:date.issued

2004

Author dc:creator

• Lima, Ana Lúcia Cessel de, 1969-

Advisor dc:contributor.advisor

• Timothy I. Eglinton and Christopher M. Reddy.

• Joint Program in Oceanography.
• Earth, Atmospheric, and Planetary Sciences.
• Woods Hole Oceanographic Institution.

Statement dc:rights

• M.I.T. theses are protected by copyright. They may be viewed from this source for any purpose, but reproduction or distribution in any format is prohibited without written permission. See provided URL for inquiries about permission.

Licence dc:rights.uri

• http://dspace.mit.edu/handle/1721.1/7582

Language dc:language.iso

eng

Handle dc:identifier.uri

http://hdl.handle.net/1721.1/39413

OAI identifier oai:identifier

oai:dspace.mit.edu:1721.1/39413