Sensitive determination of glyoxal, methylglyoxal and hydroxyacetaldehyde in environmental water samples by using dansylacetamidooxyamine derivatization and liquid chromatography/fluorescence

被引:19
|
作者
Houdier, Stephan [1 ]
Barret, Manuel [1 ]
Domine, Florent [1 ]
Charbouillot, Tiffany [2 ]
Deguillaume, Laurent [3 ]
Voisin, Didier [1 ]
机构
[1] Univ Grenoble 1, Lab Glaciol & Geophys Environm, CNRS, UMR 5183, F-38041 Grenoble, France
[2] Univ Blaise Pascal, CNRS, Lab Photochim Mol & Macromol, UMR 6505, F-63000 Clermont Ferrand, France
[3] Univ Blaise Pascal, CNRS, Lab Meteorol Phys, UMR 6016, F-63000 Clermont Ferrand, France
关键词
HPLC; Fluorescence; Dicarbonyl compounds; Hydroxyaldehydes; Water samples; Environment; WEIGHT CARBONYL-COMPOUNDS; DICARBOXYLIC-ACIDS; AQUEOUS PHOTOOXIDATION; ATMOSPHERIC CHEMISTRY; OLIGOMER FORMATION; WET PRECIPITATION; FLUORESCENT-PROBE; POLAR COMPOUNDS; METHYL GLYOXAL; RAIN SAMPLES;
D O I
10.1016/j.aca.2011.08.002
中图分类号
O65 [分析化学];
学科分类号
070302 ; 081704 ;
摘要
In this study we improved the dansylacetamidooxyamine (DNSAOA)-LC-fluorescence method for the determination of aqueous-phase glyoxal (GL), methylglyoxal (MG) and hydroxyacetaldehyde (HA). As derivatization of dicarbonyls can potentially lead to complex mixtures, a thorough study of the reaction patterns of GL and MG with DNSAOA was carried out. Derivatization of GL and MG was shown to follow the kinetics of successive reactions, yielding predominantly doubly derivatized compounds. We verified that the bis-DNSAOA structure of these adducts exerted only minor influence on their fluorescence properties. Contrary to observations made with formaldehyde, derivatization of GL, MG and, to a lesser extent of HA, was shown to be faster in acidic (H2SO4) medium with a maximum of efficiency for acid concentrations of ca. 2.5 mM. Concomitant separation of GL, MG, HA and of single carbonyls was achieved within 20 min by using C-18 chromatography and a gradient of CH3CN in water. Detection limits of 0.27, 0.17 and 0.12 nM were determined for GL, MG and HA, respectively. Consequently, low sample volumes are sufficient and, unlike numerous published methods, neither preconcentration nor large injection volumes are necessary to monitor trace-level samples. The method shows relative measurement uncertainties better than +/- 15% at the 95% level of confidence and good dynamic ranges (R-2 > 0.99) from 0.01 to 1.5 mu M for all carbonyls. GL, MG and HA were identified for the first time in polar snow samples, but also in saline frost flowers for which unexpected levels of 0.1-0.6 mu M were measured. Concentrations in the 0.02-2.3 mu M range were also measured in cloud water. In most samples, a predominance of HA over GL and MG was observed. (C) 2011 Elsevier B.V. All rights reserved.
引用
收藏
页码:162 / 173
页数:12
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