New insights into spatiotemporal source apportionment of n-alkanes under mixed scenario: A pilot study on Lake Chaohu, China

Sci Total Environ. 2020 Nov 10:742:140517. doi: 10.1016/j.scitotenv.2020.140517. Epub 2020 Jun 27.

Abstract

N-alkanes are ideal molecular markers for the source apportionment of organic matter. However, the estimation of both biogenic and anthropogenic sources under mixed scenario using n-alkanes and their related proxies still remains an issue. In this study, we investigated spatiotemporal variations of n-alkanes in suspended particulate matter of Lake Chaohu for their source apportionment. Overall, Σ29 n-alkanes ranged from 324.1 to 113685 ng·L-1. C17H36 was the most abundant homologue and was followed by C18, C27 and C29 homologues. Carbon preference indexes (CPIs) in most samples (at least 85%) were < 3, indicating mixed sources of n-alkanes in Lake Chaohu. Therefore, biogenic and anthropogenic n-alkanes were separated by subtraction to avoid potential bias. Our results showed Σ biogenic and Σ anthropogenic n-alkanes ranged from 14.8 to 3531.6 ng·L-1 and 257.6 to 4938.5 ng·L-1, respectively. For biogenic n-alkanes, their carbon-chain distributions posed a preponderant peak at C17, indicating algae were the main contributors to biogenic n-alkanes in Lake Chaohu. Biogenic average chain length (ACLbio) was developed to quantify the contributions of different biogenic sources. We recommended ACLbio < 21 for algae dominance and ACLbio > 26 for terrestrial plant dominance. For anthropogenic n-alkanes, their carbon-chain distribution presented obviously spatiotemporal variations. The sources of anthropogenic n-alkanes in summer and winter were typical dominances of light petroleum and incomplete fossil fuel burning/heavy oil emission, respectively. New developed proxies, anthropogenic average chain length (ACLanthro) and the ratio of unit short- to long-carbon anthropogenic n-alkanes (L/H), are effective for quantifying the relative contributions of different anthropogenic sources. We recommend log10L/H > 0.5 and ACLanthro < 20.5 for light petroleum input dominance, log10L/H < -0.5 and ACLanthro > 26.5 for incomplete fossil fuel burning at high temperature/heavy oil emission dominance.

Keywords: Carbon–chain distribution; Lake Chaohu; N–alkanes; Proxy; Source apportionment; Spatiotemporal variations.