Sources and Fate of Cyclic Phenylmethylsiloxanes in One Municipal Wastewater Treatment Plant and Biosolids-Amended Soil

Abstract

cis-/ trans-2,4,6-Triphenyl-2,4,6-trimethylcyclotrisiloxanes ( cis-P3 and trans-P3) and cis-/ trans-2,4,6,8-tetraphenyl-2,4,6,8-tetramethylcyclotetrasiloxanes ( cis-P4 and trans-P4a,b,c) were detected in personal care products [<LOD-54.2 μg/g, detection frequencies (df) = 14.5-15.5%, n = 110] collected from a Chinese city, suggesting their potential release to local municipal wastewater treatment plant (WWTP). In the local WWTP, per capita mass loadings of P3 and P4 were 43.4-340 μg/d in influents, while neither P3 nor P4 was detected in effluents. Due to large solid/water distribution coefficients (apparent Log Kd = 3.42-3.99), sorption to sludge had a dominant contribution (95.6-99.2%) to phenylmethylsiloxanes removal in the WWTP. As amended by biosolids containing phenylmethylsiloxanes [66.2 ng/g to 2.63 μg/g dw (dry weight)] from this WWTP, concentrations (<LOD -255 ng/g dw, df = 27.5-52.5%, n = 120) of six phenylmethylsiloxane isomers in soils from one commercial forest were significantly higher than those (<LOD) in the reference area without biosolids application, but no increasing trend was found at six sampling events during July 2015 to February 2017. Simulated experiments indicated that hydrolysis half-lives of phenylmethylsiloxanes (1.50-6.50 d for P3, 16.5-65.4 d for P4) in soil were 4.74-46.3 times shorter than volatilization half-lives (51.9-120 d for P3, 158-376 d for P4). For both cyclic phenylmethylsiloxanes, their trans-isomers had lower (1.14-1.82 times) degradation rates than their cis-isomers.