In one yearly cycle (2016), D4 and D5 were detected in biogas samples (n = 36, 0.105-2.33 mg/m) from a Chinese municipal landfill, while D4-D6 were detected in influents/effluents of leachate storage pond (n = 72, < LOQ-30.5 μg/L). Mass loads of cVMS in both biogas (591-6575 mg/d) and leachate influents (659-5760 mg/d) increased from January to July (summer), and then decreased from July to December (winter). Removal experiments indicated that 1) hydrolysis and volatilization were predominant removal mechanism for D4 and D5, respectively, in leachate storage pond, responsible for their more significant removal (94.5-100%) in August; 2) indirect phototransformation (t = 25.5-87.0 days), such as hydroxylation by OH radical generated in leachates, was the predominant (50.0-75.5%) removal pathway for D6, which led to the largest removal efficiencies (65.2-73.7%) in June, the month with the largest sun light intensity and highest photosensitizer (e.g., Fe and NO) concentrations. Monohydroxylated products of D5 and D6, D4TOH and D5TOH, were detected in leachate effluents (39.6-187 ng/L) during May-July. Compared to D5 and D6, volatilization half-lives of D4TOH (86.3 days) and D5TOH (177 days) in leachates were 2.9 and 1.4 times longer, while their hydrolysis half-lives (7.50 days for D4TOH and 21.5 days for D5TOH) were 7.1 and 10 times shorter, respectively.

Simulated experiments indicated that chlorinated volatile methylsiloxanes, detected by Q-TOF GC/MS, could be generated in a pulp-bleaching process, where poly(dimethylsiloxane)s fluids with volatile methylsiloxanes as impurities and molecular chlorine were used as a defoamer and bleaching agent, respectively. In the producing processes of one papermaking factory, the mean total concentrations of monochlorinated D4, D5, and D6, i.e., D3D(CHCl), D4D(CHCl), and D5D(CHCl), were 0.0430-287 μg/L in aqueous samples, while they were 0.0329-270 μg/g in solid samples. In the coupled papermaking-wastewater treatment processes, D3D(CHCl), D4D(CHCl), and D5D(CHCl) were detected in all water (0.113-8.68 μg/L) and solid samples (0.888-26.2 μg/g), with solid-water partition values (468-3982 L/kg) 1.08-4.82 times higher than those of their corresponding nonchlorinated analogs. The removing efficiencies of D3D(CHCl)-D5D(CHCl) in the whole wastewater treatment processes were 77.1-81.6%, and sorption to sludge (35.7-74.1%) and removal in the primary clarifier (7.19-32.5%) had major contributions to their total removal. Elimination experiments showed that 1) hydrolysis half-lives of D3D(CHCl)-D5D(CHCl) (0.9-346 h) in the primary clarifier (pH = 7.8-9.2) were 2.16-3.60 times shorter than those of their nonchlorinated analogs; 2) D3D(CHCl)-D5D(CHCl) were hardly degraded in oxic sludge treatment process, and their volatilization half-lives (7.38-21.1 h) in oxic sludge were 1.21-1.50 times longer than those of their nonchlorinated analogs.