Multi-Proxy Approach on Black Carbon Characterization and Combustion Products Source Discrimination in Environmental Media



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Environmental applications of pyrogenic carbon, aka black carbon (BC), have been hampered due to the poor characterization and quantification of environmental BC. This dissertation was dedicated to the better characterization of environmental char/charcoal BC (char-BC), the most heterogeneous and the less identifiable group in the BC continuum. The analytical approach developed for char-BC was further incorporated with other BC methods in environmental samples for a comprehensive assessment of combustion-derived carbon inputs in different environmental systems. The present study firstly evaluated the feasibility of using levoglucosan, a marker derived from cellulose/hemocellulose combustion, to characterize and quantify char-BC in the environment. Levoglucosan was found exclusively in BC materials derived from biomass combustion albeit in highly variable yields across different char-BC. A further examination of synthetic chars showed that temperature is the most influential factor affecting levoglucosan yield in char. Notably, levoglucosan was only detectable in low temperature char samples (150-350 degrees C), regardless of plant species. These results demonstrated that levoglucosan could serve as a good qualitative indicator for the presence of char produced under low temperature conditions in soil, sediments, and aerosols. Results of lignin analysis on the synthetic chars further reveal that combustion can greatly decrease the yield of the eight major lignin phenols with no lignin phenols detected in any synthetic char produced at greater than or equal to 400 degrees C. The values of all lignin parameters show significant shifts with increasing combustion severity (temperature and/or duration), indicating that thermal alteration is an important abiotic lignin degradation process. Hence the input of char-BC in the environments represents a terrestrial organic matter source with highly altered lignin signatures. Finally, a multi-proxy approach, including elemental (soot-BC) and molecular (levoglucosan, polycyclic aromatic hydrocarbons (PAHs), and lignin oxidation products) proxies, was adopted to investigate the centennial-scale temporal distribution of combustion products in four sediment cores from Puget Sound basins, WA. The observed temporal trends of soot-BC and combustion PAHs fluxes reflect the evolution of energy consumption and the positive effects of environmental regulations. The distinct temporal patterns of soot and PAHs among cores demonstrate that urbanization is a crucial factor controlling the inputs of combustion byproducts to the environment. On the other hand, the trends of levoglucosan may be more relevant to the climate oscillation and thus show a regional distribution pattern. Our results demonstrate that environmental loading of combustion byproducts is a complex function of urbanization and land use, fuel usage, combustion technology, environmental policies, and climate changes.