Distribution and diagenetic fate of synthetic surfactants and their metabolites in sewage-impacted estuarine sediments

Surfactants are high production volume chemicals used in numerous domestic and industrial applications and, after use, the most abundant organic contaminants in wastewater. Their discharge might jeopardize the receiving aquatic ecosystems, including sediments, where they tend to accumulate. This is the first comprehensive study on their distribution and fate in this environmental compartment as we performed simultaneous analysis of the three main classes of surfactants (anionic: LAS; nonionic: NPEO and AEO; cationic: DTDMAC, DADMAC, BAC, and ATMAC) and some of their transformation products (SPC, NP, NPEC, and PEG). To account for spatial and time trends, surface sediments and dated cores were collected from Jamaica Bay, a heavily sewage-impacted estuary in New York City. The concentrations of surfactants in surface sediments were between 18 and > 200 μg g⁻¹ and showed slight variation (<10%) over different sampling years (1998, 2003 and 2008). Cationic surfactants were found at the highest concentrations, with DTDMAC accounting for between 52 and 90% of the total sum of target compounds. Vertical concentration profiles in dated cores from the most contaminated station, in the vicinity of the biggest local sewage treatment plant (STP), indicated two sub-surface surfactant peaks in the mid-1960s (469 μg g⁻¹) and late 1980s (572 μg g⁻¹) coinciding with known STP upgrades. This trend was observed for most target compounds, except for DADMAC, C22ATMAC, and PEG, which showed a continuous increase towards the top of the cores. In-situ degradation was studied by comparing sediment core samples taken 12 years apart (1996 and 2008) and revealed a net decrease in PEG and specific surfactants (BAC, ATMAC, NPEO, and AEO) accompanied by growing concentrations of metabolites (SPC, NP, and NPEC). DTDMAC, DADMAC, and LAS, however, remained stable over this period, suggesting recalcitrant behavior under the anaerobic conditions in Jamaica Bay sediments.Chronology of major synthetic surfactants are illustrated in the dated sediment cores, as well as their different diagenetic fates.