Thanks to their adaptability and high efficiency compared to traditional carbon based surfactants, silicone surfactants are a success in many different applications, from pesticides to cosmetics, polyurethane foam, textile and car care products. In spite of those numerous applications, no analytical method existed for their trace determination in environmental samples and no data have been available regarding their environmental occurrence and fate.
An analytical method for the trace analysis of trisiloxane surfactants in the aqueous environment was developed and validated. The method, based on liquid-liquid extraction and HPLC-MS/MS, reaches limits of quantification in the ng L-1 range and allows an individual quantification of every homologue of the targeted trisiloxane surfactant. The newly developed analytical method was applied to analyze 40 river water samples. The targeted trisiloxane surfactant was detected in 14 samples, between 1 ng L-1 and 100 ng L-1. The results showed that the studied trisiloxane surfactant does not ubiquitously occur in the aquatic environment in measurable concentrations, but can reach surface waters on a local scale.
In order to assess the persistence of the trisiloxane surfactant in surface waters, its hydrolysis was studied in the lab, under various conditions (temperature, pH, and concentration). The half-lifes at pH 7 and 2 mg L-1 were found to be between 29 days and 55 days at 25°C and between 151 days and 289 days at 12°C. Taking only into account the hydrolysis, these results indicate that the trisiloxane surfactant could persist several weeks in surface waters. A degradation product of the trisiloxane surfactant was tentatively identified by high resolution mass spectrometry.
When used as agricultural adjuvants, trisiloxane surfactants may reach the soil compartment and might further leach to ground water. The behavior of the trisiloxane surfactant on soil was therefore investigated to assess the possibility to reach ground water. With a sorption batch equilibrium method, distribution coefficients between water and soil (Kd, Koc, and Kclay) were estimated for two standard soils (loam and sandy loam) and for every homologue of the trisiloxane surfactant. The obtained values for Kd were between 15 L kg-1 and 135 L kg-1, indicating that the trisiloxane surfactant is only slightly mobile in soil. To further investigate the possibility of leaching to ground water after application on agricultural fields, the leaching in soil was simulated in the lab in a soil column. The experimental settings were designed to simulate a worst case scenario where the application of the trisiloxane surfactant is done on quartz sand and is immediately followed by a heavy rainfall. Even in these conditions, less than 0.01 % of the initially applied trisiloxane surfactant leached through 20 cm of quartz sand. Based on the Kd values and the results of the leaching in soil column, the studied trisiloxane surfactant is considered to be unlikely to leach to ground water after application as an agricultural adjuvant.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa.de:bsz:14-qucosa-197541 |
| Date | 09 May 2016 |
| Creators | Michel, Amandine |
| Contributors | Technische Universität Dresden, Fakultät Umweltwissenschaften, Prof. Dr. Eckhard Worch, Prof. Dr. Heinz-Jürgen Brauch, Prof. Dr. Martin Jekel |
| Publisher | Saechsische Landesbibliothek- Staats- und Universitaetsbibliothek Dresden |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | doc-type:doctoralThesis |
| Format | application/pdf |
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