期刊论文详细信息
Chemistry Central Journal
Online solid phase extraction liquid chromatography tandem mass spectrometry (SPE-LC-MS/MS) method for the determination of sucralose in reclaimed and drinking waters and its photo degradation in natural waters from South Florida
Piero R Gardinali1  Venkata R Panditi1  Natalia Quinete1  Sudha Rani Batchu1 
[1]Southeast Environmental Research Center (SERC), Florida International University, Miami, FL, USA
关键词: High resolution mass spectrometry;    Degradation products;    Photo degradation;    Drinking water;    Reclaimed waters;    Online SPE;    Artificial sweetener;    Sucralose;   
Others  :  787852
DOI  :  10.1186/1752-153X-7-141
 received in 2013-06-26, accepted in 2013-08-15,  发布年份 2013
PDF
【 摘 要 】

Background

Sucralose has gained popularity as a low calorie artificial sweetener worldwide. Due to its high stability and persistence, sucralose has shown widespread occurrence in environmental waters, at concentrations that could reach up to several μg/L. Previous studies have used time consuming sample preparation methods (offline solid phase extraction/derivatization) or methods with rather high detection limits (direct injection) for sucralose analysis. This study described a faster and sensitive analytical method for the determination of sucralose in environmental samples.

Results

An online SPE-LC–MS/MS method was developed, being capable to quantify sucralose in 12 minutes using only 10 mL of sample, with method detection limits (MDLs) of 4.5 ng/L, 8.5 ng/L and 45 ng/L for deionized water, drinking and reclaimed waters (1:10 diluted with deionized water), respectively. Sucralose was detected in 82% of the reclaimed water samples at concentrations reaching up to 18 μg/L. The monthly average for a period of one year was 9.1 ± 2.9 μg/L. The calculated mass loads per capita of sucralose discharged through WWTP effluents based on the concentrations detected in wastewaters in the U. S. is 5.0 mg/day/person. As expected, the concentrations observed in drinking water were much lower but still relevant reaching as high as 465 ng/L. In order to evaluate the stability of sucralose, photodegradation experiments were performed in natural waters. Significant photodegradation of sucralose was observed only in freshwater at 254 nm. Minimal degradation (<20%) was observed for all matrices under more natural conditions (350 nm or solar simulator). The only photolysis product of sucralose identified by high resolution mass spectrometry was a de-chlorinated molecule at m/z 362.0535, with molecular formula C12H20Cl2O8.

Conclusions

Online SPE LC-APCI/MS/MS developed in the study was applied to more than 100 environmental samples. Sucralose was frequently detected (>80%) indicating that the conventional treatment process employed in the sewage treatment plants is not efficient for its removal. Detection of sucralose in drinking waters suggests potential contamination of surface and ground waters sources with anthropogenic wastewater streams. Its high resistance to photodegradation, minimal sorption and high solubility indicate that sucralose could be a good tracer of anthropogenic wastewater intrusion into the environment.

【 授权许可】

   
2013 Batchu et al.; licensee Chemistry Central Ltd.

【 预 览 】
附件列表
Files Size Format View
20140702204411267.pdf 1690KB PDF download
Figure 9. 39KB Image download
Figure 8. 31KB Image download
Figure 7. 49KB Image download
Figure 6. 69KB Image download
Figure 5. 49KB Image download
Figure 4. 79KB Image download
Figure 3. 149KB Image download
Figure 2. 45KB Image download
Figure 1. 81KB Image download
【 图 表 】

Figure 1.

Figure 2.

Figure 3.

Figure 4.

Figure 5.

Figure 6.

Figure 7.

Figure 8.

Figure 9.

【 参考文献 】
  • [1]Brorström–Lundén E, Svenson A, Viktor T, Woldegiorgis A, Remberger M, Kaj L, Dye C, Bjerke A, Schlabach M: Measurements of Sucralose in the Swedish Screening Program 2007-PART 1; Sucralose in surface waters and STP samples IVL B1769. Stockholm: IVL Swedish Environmental Research Institute Ltd; 2008.
  • [2]Mead RN, Morgan JB, Avery GB Jr, Kieber RJ, Kirk AM, Skrabal SA, Willey JD: Occurrence of the artificial sweetener sucralose in coastal and marine waters of the United States. Mar Chem 2009, 116:13-17.
  • [3]Loos R, Gawlik BM, Boettcher K, Locoro G, Contini S, Bidoglio G: Sucralose screening in European surface waters using a solid-phase extraction-liquid chromatography-triple quadrupole mass spectrometry method. J Chromatogr A 2009, 1216:1126-1131.
  • [4]Scheurer M, Brauch H-J, Lange FT: Analysis and occurrence of seven artificial sweeteners in German waste water and surface water and in soil aquifer treatment (SAT). Anal Bioanal Chem 2009, 394:1585-1594.
  • [5]Ferrer I, Thurman EM: Analysis of sucralose and other sweeteners in water and beverage samples by liquid chromatography/time-of-flight mass spectrometry. J Chromatogr A 2010, 1217:4127-4134.
  • [6]Mawhinney DB, Young RB, Vanderford BJ, Borch T, Snyder SA: Artificial Sweetener Sucralose in U.S. Drinking Water Systems. Environ Sci Technol 2011, 45:8716-8722.
  • [7]Brown KD, Kulis J, Thomson B, Chapman TH, Mawhinney DB: Occurrence of antibiotics in hospital, residential, and dairy, effluent, municipal wastewater, and the Rio Grande in New Mexico. Sci Total Environ 2006, 366:772-783.
  • [8]Minten J, Adolfsson-Erici M, Bjorlenius B, Alsberg T: A method for the analysis of sucralose with electrospray LC/MS in recipient waters and in sewage effluent subjected to tertiary treatment technologies. Int J Environ Anal Chem 2011, 91:357-366.
  • [9]Oppenheimer J, Eaton A, Badruzzaman M, Haghani AW, Jacangelo JG: Occurrence and suitability of sucralose as an indicator compound of wastewater loading to surface waters in urbanized regions. Water Res 2011, 45:4019-4027.
  • [10]Grice HC, Goldsmith LA: Sucralose - An overview of the toxicity data. Food Chem Toxicol 2000, 38:1-6.
  • [11]Lubick N: Artificial sweetener persists in the environment. Environ Sci Technol 2008, 42:3125-3125.
  • [12]Wiklund A-KE, Breitholtz M, Bengtsson B-E, Adolfsson-Erici M: Sucralose - An ecotoxicological challenger? Chemosphere 2012, 86:50-55.
  • [13]Soh L, Connors KA, Brooks BW, Zimmerman J: Fate of Sucralose through Environmental and Water Treatment Processes and Impact on Plant Indicator Species. Environ Sci Technol 2011, 45:1363-1369.
  • [14]Hjorth M, Hansen JH, Camus L: Short-term effects of sucralose on Calanus finmarchicus and Calanus glacialis in Disko Bay, Greenland. Chem Ecol 2010, 26:385-393.
  • [15]Lillicrap A, Langford K, Tollefsen KE: Bioconcentration of the intense sweetener sucralose in a multitrophic battery of aquatic organisms. Environ Toxicol Chem 2011, 30:673-681.
  • [16]Lappin-Scott HM, Holt G, Bull AT: Microbial transformation of 1,6-dichloro-1,6-dideoxy-β, D-fructofuranosyl-4-chloro-4-deoxy-α, D-galactopyranoside (TGS) by soil populations. MIRCEN J Appl Microb 1987, 3:95-102.
  • [17]Labare MP, Alexander M: Microbial cometabolism of sucralose, a chlorinated discaccharide, in environmental-samples. Appl Microbiol Biotechnol 1994, 42:173-178.
  • [18]Labare MP, Alexander M: Biodegradation of sucralose, a chlorinated carbohydrate, in samples of natural environments. Environ Toxicol Chem 1993, 12:797-804.
  • [19]Lange FT, Scheurer M, Brauch HJ: Artificial sweeteners-a recently recognized class of emerging environmental contaminants: a review. Anal Bioanal Chem 2012, 403:2503-2518.
  • [20]Buerge IJ, Buser H-R, Kahle M, Mueller MD, Poiger T: Ubiquitous Occurrence of the Artificial Sweetener Acesulfame in the Aquatic Environment: An Ideal Chemical Marker of Domestic Wastewater in Groundwater. Environ Sci Technol 2009, 43:4381-4385.
  • [21]Torres CI, Ramakrishna S, Chiu C-A, Nelson KG, Westerhoff P, Krajmalnik-Brown R: Fate of sucralose during wastewater treatment. Environ Eng Sci 2011, 28:325-331.
  • [22]Ordonez EY, Benito Quintana J, Rodil R, Cela R: Determination of artificial sweeteners in water samples by solid-phase extraction and liquid chromatography-tandem mass spectrometry. J Chromatogr A 2012, 1256:197-205.
  • [23]Panditi VR, Batchu SR, Gardinali PR: Online solid phase extraction-liquid chromatography-electrospray-tandem mass spectrometric determination of multiple classes of antibiotics in environmental and treated waters. Anal Bioanal Chem 2013, 405:5953-5964.
  • [24]Quinete N, Wang J, Fernandez A, Castro J, Gardinali PR: Outcompeting GC for the detection of legacy chlorinated pesticides: online-SPE UPLC APCI/MSMS detection of endosulfans at part per trillion levels. Anal Bioanal Chem 405:5887-5899.
  • [25]Neset TSS, Singer H, Longree P, Bader HP, Scheidegger R, Wittmer A, Andersson JCM: Understanding consumption-related sucralose emissions - A conceptual approach combining substance-flow analysis with sampling analysis. Sci Total Environ 2010, 408:3261-3269.
  • [26]Heeb F, Singer H, Pernet-Coudrier B, Qi WX, Liu HJ, Longree P, Muller B, Berg M: Organic Micropollutants in Rivers Downstream of the Megacity Beijing: Sources and Mass Fluxes in a Large-Scale Wastewater Irrigation System. Environ Sci Technol 2012, 46:8680-8688.
  • [27]Ramirez CE, Batchu SR, Gardinali PR: High sensitivity Liquid Chromatography Tandem Mass Spectrometric (LC-MS/MS) methods for the analysis of dioctyl sulfosuccinate (DOSS) in different stages of an oil spill response monitoring effort. Anal Bioanal Chem 2013, 405:4167-4175.
  • [28]Zaikin VG, Halket JM: Derivatization in mass spectrometry - 8. Soft ionization mass spectrometry of small molecules. Eur J Mass Spectrom 2006, 12:79-115.
  • [29]Singh G, Gutierrez A, Xu KY, Blair IA: Liquid chromatography/electron capture atmospheric pressure chemical ionization/mass spectrometry: Analysis of pentafluorobenzyl derivatives of biomolecules and drugs in the attomole range. Anal Chem 2000, 72:3007-3013.
  • [30]Thurman EM, Ferrer I, Barcelo D: Choosing between atmospheric pressure chemical ionization and electrospray ionization interfaces for the HPLC/MS analysis of pesticides. Anal Chem 2001, 73:5441-5449.
  • [31]Chusaksri S, Sutthivaiyakit S, Sutthivaiyakit P: Confirmatory determination of organochlorine pesticides in surface waters using LC/APCI/tandem mass spectrometry. Anal Bioanal Chem 2006, 384:1236-1245.
  • [32]Maragou NC, Thomaidis NS, Koupparis MA: Optimization and Comparison of ESI and APCI LC-MS/MS Methods: A Case Study of Irgarol 1051, Diuron, and their Degradation Products in Environmental Samples. J Am Soc Mass Spectrom 2011, 22:1826-1838.
  • [33]King R, Bonfiglio R, Fernandez-Metzler C, Miller-Stein C, Olah T: Mechanistic investigation of ionization suppression in electrospray ionization. J Am Soc Mass Spectrom 2000, 11:942-950.
  • [34]Levine AD, Asano T: Recovering sustainable water from wastewater. Environ Sci Technol 2004, 38:201A-208A.
  • [35]Miamidade: About reclaimed water. 2013. http://www.miamidade.gov/water/reclaimed-water-about.asp webcite. Accessed on 7/10/2013
  • [36]MDWASD: Alternative water supply plan and reuse feasibility plan annual progress report. http://www.miamidade.gov/water/library/reports/water-use-permit-alternative-supply-reuse-2007.pdf webcite. Accessed on 10/1/2012; 2007
  • [37]Panditi VR: Assessment of the Occurrence and Potential Risks of Antibiotics and their Metabolites in South Florida Waters Using Liquid Chromatography Tandem Mass Spectrometry. FIU Electronic Theses and Dissertations 2013. Paper 916. http://digitalcommons.fiu.edu/etd/916 webcite
  • [38]Fernandez M, Pico Y, Manes J: Comparison of gas and liquid chromatography coupled to mass spectrometry for the residue analysis of pesticides in oranges. Chromatographia 2001, 54:302-308.
  • [39]Radjenovic J, Godehardt M, Petrovic M, Hein A, Farre M, Jekel M, Barcelo D: Evidencing Generation of Persistent Ozonation Products of Antibiotics Roxithromycin and Trimethoprim. Environ Sci Technol 2009, 43:6808-6815.
  • [40]Li DHW, Lam JC, Lau CCS: A Study of Solar Radiation Daylight Illuminance and Sky Luminance Data Measurements for Hong Kong. Archit Sci Rev 2002, 45:21-30.
  • [41]Diepens M, Gijsman P: Photodegradation of bisphenol A polycarbonate. Polym Degrad Stab 2007, 92:397-406.
  • [42]Wu ZR, Gao WQ, Phelps MA, Wu D, Miller DD, Dalton JT: Favorable effects of weak acids on negative-ion electrospray ionization mass spectrometry. Anal Chem 2004, 76:839-847.
  • [43]USEPA: Definition and procedures for the determination of the method detection limit. Revision 1.11. edition. Guidelines establishing test procedures for the analysis of pollutants. Appendix B, part 136. Definition and procedures for the determination of the method detection limit. U.S. Code of Federal Regulations, Title 40. Revision 1.11. 2010.
  • [44]USCB: State & County QuickFacts. 2011. http://quickfacts.census.gov/qfd/states/12/1249450.html webcite. Accessed on 10/1/2012
  • [45]Scheurer M, Storck FR, Graf C, Brauch HJ, Ruck W, Lev O, Lange FT: Correlation of six anthropogenic markers in wastewater, surface water, bank filtrate, and soil aquifer treatment. J Environ Monit 2011, 13:966-973.
  • [46]Brorstrom-Lunden E, Svensson A, Viktor T, Woldegiorgis A, Remberger M, Kaj L, Dye C, Bjerke A, Schlabach M: Measurements of Sucralose in the Swedish Screening program 2007. Part 2; Sucralose in Biota samples and regional STP samples. Sweden: IVL Swedish Environmental Research Institute Ltd, Stockholm; 2008.
  • [47]Morlock GE, Schuele L, Grashorn S: Development of a quantitative high-performance thin-layer chromatographic method for sucralose in sewage effluent, surface water, and drinking water. J Chromatogr A 2011, 1218:2745-2753.
  • [48]Berset JD, Ochsenbein N: Stability considerations of aspartame in the direct analysis of artificial sweeteners in water samples using high-performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS). Chemosphere 2012, 88:563-569.
  • [49]Gan Z, Sun H, Wang R, Feng B: A novel solid-phase extraction for the concentration of sweeteners in water and analysis by ion-pair liquid chromatography–triple quadrupole mass spectrometry. J Chromatogr A 2013, 1274:87-96.
  • [50]Imhoff K, Imhoff K: Taschenbuch der Stadtentwässerung (Pocketbook on Sewerage). 26th edition. Munich: R. Oldenbourg; 1985.
  • [51]UNEP: International Source Book on Environmentally Sound Technologies for Wastewater and Stormwater Management. 2000. http://www.unep.or.jp/Ietc/Publications/TechPublications/TechPub-15/main_index.asp webcite. Accessed on 2/20/2013
  • [52]Water supply & Treatment. http://www.miamidade.gov/water/water-supply-treatment.asp webcite. Accessed on 4/1/2013
  • [53]Scheurer M, Storck FR, Brauch H-J, Lange FT: Performance of conventional multi-barrier drinking water treatment plants for the removal of four artificial sweeteners. Water Res 2010, 44:3573-3584.
  • [54]Fujimaru T, Park JH, Lim J: Sensory Characteristics and Relative Sweetness of Tagatose and Other Sweeteners. J Food Sci 2012, 77:S323-S328.
  文献评价指标  
  下载次数:63次 浏览次数:26次