High-Resolution Historical Record of Plant Protection Product Deposition Documented by Target and Nontarget Trend Analysis in a Swiss Lake under Anthropogenic Pressure

A multiproxy workflow was used to assess >60 plant protection products (PPPs) in sediment samples from a Swiss lake under heavy agricultural pressure. The results show the appearance of PPPs for the first time in the early 1960s with an overall detection of 34 PPPs and with herbicides and fungicides found in equal proportions. Paleolimnological data [e.g., chronology, hyperspectral imaging of sedimentary green pigments, and semiquantitative elemental composition (μXRF scans)] suggest that PPP concentrations and fluxes to the sediment over time are not related to land surface processes such as soil erosion or lake biogeochemistry but are attributed mainly to PPP application (inferred from sales) or regulatory measures (bans). Additional compounds with similar sources of contamination as the target PPPs captured by nontarget trend analysis (≥2000 unknown profiles) reveal significant inputs of contaminants to the lake starting in the 1970s, followed by a decrease of contamination at the beginning of the 1990s and a constant increase by ∼28% of the unknown compounds since the year 2000. An ecological risk assessment conducted on detected PPPs indicates that since the 1980s, the sediment quality is insufficient with risk quotient values displaying maximum levels in the most recent sediments (∼2010) despite bans of specific PPPs and environmental regulations.