Roles of polydadmacs, dithiocarbamates and activated carbons in formation of N-nitrosamine contaminants in water
Padhye, Lokesh Pradeep
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N-Nitrosamines are an emerging group of disinfection byproducts characterized by high carcinogenic risks at ng/L levels and by their frequent detection in water and wastewater treatment systems in the U.S. and other parts of the world. The overall goal of this research is to achieve a better understanding of the roles of common nitrosamine precursors in leading to N-nitrosamine formation in water and wastewater treatment systems. The specific objectives of this research are: (a) To probe the mechanisms of nitrosamine formation from commonly employed water treatment polymers, particularly polyDADMACs, during ozonation, (b) To evaluate the role of dithiocarbamate compounds as nitrosamine precursors in reaction with common water disinfection oxidants, and (c) To investigate the potential enhancement effect of activated carbons (AC) to promote transformation of amines to nitrosamines and identify the involved reaction mechanism. Results of this research show that, upon ozonation, polyDADMACs may yield N-nitrosodimethylamine (NDMA) at levels up to two orders of magnitude higher than current advisory guidelines for NDMA. Radical pathways may be responsible for the degradation of the quaternary ammonium ring groups in polyDADMACs to release of dimethylamine (DMA). Detection of significant amounts of nitrite after ozonation of polyDADMACs and DMA suggests the potential role of nitrosation pathway in NDMA formation. Study results also reveal dithiocarbamates as potent nitrosamine precursors with significant nitrosamine yields upon ozonation and monochloramination. Identification and quantification of reaction products suggest nitrosation and chlorinated-UDMH oxidation as primary reaction mechanisms in nitrosamine formation from ozonation and monochloramination of dithiocarbamates compounds, respectively. This research also demonstrates that many commercial AC materials may catalyze transformation of secondary amines to yield trace levels of N-nitrosamines under ambient aerobic conditions. This is a novel discovery with far-reaching implications because of the widespread usage of AC materials in numerous analytical and environmental applications. The study results show that the properties of AC materials and reaction conditions play a crucial role in the catalyzed nitrosamine formation and should be carefully selected to minimize analytical errors and undesirable nitrosamine formation in water samples. Overall, the mechanistic information obtained in this research will be useful for the water industry and research communities to develop more effective strategies to control undesirable nitrosamine formation in water and wastewater treatment systems and thus better protect the public health.