Inferring Black Carbon Concentrations in Particulate Organic Matter by Observing Pyrene Fluorescence Losses

Abstract

Black carbon (BC), the soot and char formed during incomplete combustion of fossil and biomass fuels, is ubiquitous, participates in diverse environmental processes, and has adverse effects on human health. However, uncertainty persists regarding how accurately the present measurement methods quantify total BC or even defined subportions of the BC continuum. Hence, we sought to improve this situation by developing a new, low-sample manipulation methodology that does not require any oxidative or pyrolytic treatments but rather differentiates BC from other non-BC organic carbon (OC) using its sorbent properties. The procedure, referred to as the pyrene fluorescence loss (PFL) method, infers BC concentrations in particulate organic matter (POM) by observing the decrease in fluorescence from pyrene spiked into aqueous POM suspensions. The method was first tested using diverse materials previously utilized in an international BC method intercomparison study, and then its effectiveness (e.g., sensitivity and geochemical reasonableness) was tested by applying itto sediment and seawater POM samples collected from a coastal area downwind of important BC sources. Parallel evaluation of BC, using the PFL method and CTO-375 procedure, suggested we can characterize the predominant BC in a given sample as (i) thermally recalcitrant and highly sorptive per mass (e.g., soot), (ii) thermally labile and highly sorptive per mass (e.g., char), or (iii) thermally recalcitrant but not highly sorptive (e.g., lignite coal).