Fingerprinting pharmaceuticals of multiple sources at a provincial watershed scale

Pharmaceutical residues in the aquatic environment have increasingly attracted public concerns but their fingerprint of sources remain unclear at a watershed scale. This study systematically explored pharmaceutical residues in effluent of 8 different type of sources in a provincial watershed in China using a multi-category protocol of pharmaceutical quantification. Seventy-seven out of 94 target compounds from 6 categories were quantified in effluent, up to 71,318 ng L^-1 in total from urban hospital sources with 20 antibiotics and 32 others. The spectrum of the quantified compounds in effluent significantly differentiated the urban (hospitals, domestic sewages, and WWTPs), rural (health centers and domestic sewages), and agricultural production sources (poultry and swine breeding yards, aquaculture ponds, and paddy fields). Compounds of non-steroidal anti-inflammation drugs (NSAIDs), cardiovascular drugs (CVs), and central nervous drugs (CNs) could fingerprint the three groups of sources. However, the three categories contributed 7 out of 10 compounds with high risk (risk quotient >1.0) to the aquatic environment identified by the eco-environmental risk assessment. No high-risk compounds were identified in effluent of urban WWTPs. Findings of this study suggest source identification and compound spectrum fingerprinting are crucial for studies on pharmaceutical residues in the aquatic environment, especially the complexity of pharmaceutical residues in source effluents for exploring source-sink dynamics at a watershed scale.