Fresenius' Journal of
Fresenius J Anal Chem (1994) 350:403-409 ....
© Springer-Verlag 1994
Determination of trace amounts
of highly hydrophilic compounds in water by direct derivatization
and gas chromatography - mass spectrometry
Claudio Minero, Marco Vincenti, Stefania Lago, Ezio Pelizzetti
Dipartimento di Chimica Analitica, Universit~ di Torino, Via Pietro Giuria 5, 1-10125 Torino, Italy
Received: 7 February 1994/Accepted: 18 March 1994
Abstract. A new procedure has been developed to de-
rivatize a large set of highly hydrophilic substances ((poly)
hydroxy and/or (poly)carboxylic acids, glycols and dihyd-
roxybenzenes) directly in water. The key element of the
method is the derivatizing agent used, n-hexyl chlorofor-
mate, which proved to be much more effective than other
alkyl and aryl chloroformates. Detection limits in the low
gg/L range were found for most of the compounds
studied, using positive ion chemical ionization mass spec-
trometry as the detection technique. Calibration curves
exhibited a good linearity over 2-3 orders of magnitude,
so that quantitative determinations were possible. Among
the experimental parameters tested, it was found crucial
to introduce the chloroformate slowly and under sonica-
tion. The whole derivatization procedure takes only
2-3 rain from sample collection to injection into the gas
chromatograph.
Introduction
Few analytical procedures deal with the determination
of highly hydrophilic organic substances, such as poly-
hydroxy and/or (poly)carboxylic acids, in water, parti-
cularly when they are present at trace levels [1, 2]. In
contrast, the determination of hydrophobic organic sub-
stances in aqueous solutions is a widely investigated field
of analytical chemistry, particularly in environmental ap-
plications [3-7]. Analytical procedures for this purpose
include a preliminary extraction step, where the hydro-
phobic substances are transferred from water to an or-
ganic solvent, followed by clean-up and concentration
steps and, lastly, injection into a chromatographic device,
possibly a capillary column gas chromatograph interfaced
to a mass detector [8, 9].
The problems for determining hydrophilic com-
pounds are due, at least in part, to the difficulties encoun-
tered in the two fundamental steps mentioned above,
Correspondence to: C. Minero
namely (i) the extraction of hydrophilic substances from
the aqueous matrix and (ii) their chromatographic separ-
ation and detection. Compounds exhibiting some am-
phiphilic character (i.e. alkyl monocarboxylic acids) can
be extracted from water with difficulty [10] but substan-
ces such as polyalcohols and polycarboxylic acids have
such a high water affinity that they do not partition into
the organic phase to any extent.
Derivatization chemically modifies the polar groups
that prevent the extraction into a non-polar organic sol-
vent. However reactions using the most common de-
rivatizing agents (polyalkylsilanes, diazoalkanes, alkyl
halides and perfluoroalkyl halides) must be performed
under rigorously anhydrous conditions since the reagents
are instantly hydrolyzed in water [11-13]. Thus these
derivatizations require a preliminary step, in which the
solvent is evaporated to dryness, before the reaction can
be carried out on the residue or in a subsequently added
organic solvent [14-16]. This procedure can lead to par-
tial or total loss of some analytes and it is also time-
consuming. Alternatively, extractive derivatizations can
be utilized [ 17, 18].
Alkyl chloroformates have been used since 1976 to
derivatize amino acids and amines in aqueous solution
[19-22]. More recently, Hugek developed a series of inter-
esting methodologies, which tolerate quite high percent-
ages of water in the solvent, to derivatize alkyl carboxylic
acids [23], 2-hydroxyalkyl carboxylic acids [24-26],
amino acids [27, 28], amines [29] and phenolic acids [30]
with alkyl chloroformates. It was found that the reaction
occurring between 2-hydroxyalkyl carboxylic acids and
methyl, ethyl or propyl chloroformates, transforms the
carboxylic group into the corresponding ester (or into the
alkoxycarbonyl ester, depending on the reaction condi-
tions) and the hydroxyl group into the corresponding
carbonate. The reaction can be carried out in a mixed
solvent composed by acetonitrile, water, pyridine and an
alcohol, although it was claimed that the highest derivat-
ization yields were obtained using anhydrous solutions
[24]. Hydroxyls which were not located in the c~position
to a carboxylic group could not be derivatized with this
procedure [24].