161

Graphite-Ethylene=Propylene=Diene Terpolymer Composite

Electrodes. A New Electrode Material for Electrochemical
Detection
Luis Alonso, ConcepcioÂn Parrado, MarõÂa Pedrero, Lourdes AguÈÂõ, and Jose M. PingarroÂn*
Departamento de QuõÂmica AnalõÂtica, Facultad de Ciencias QuõÂmicas, Universidad Complutense de Madrid, E-28040 Madrid, Spain

Received: September 30, 1998

Final version: November 18, 1998

Abstract
The preparation and electroanalytical performance of a new composite electrode material, fabricated by mixing graphite and the
ethylene=propylene=diene (EPD) terpolymer is reported. The voltammetric and ¯ow-injection with amperometric detection responses at this
composite electrode of several substances of different solubilities in water are discussed and compared with those obtained at graphite-
Te¯on composite and glassy carbon electrodes. An EPD content around 2% ensures good compactness of the material and an adequate
conductivity. Under ¯owing conditions, these electrodes show better signal-to-background ratios than those obtained with the other
electrode materials tested. Furthermore, the new electrodes show very good resistance to fouling with no need of electrode surface pre-
treatment. The presence of a high content of organic solvent in the carrier solution produces a sharp decrease in the amperometric current
thus limiting the advantageous use of the graphite-EPD composite electrodes to predominantly aqueous media.
Keywords: Graphite, Ethylene=propylene=diene terpolymer, Composite electrodes, Flow-injection with amperometric detection

1. Introduction electrode and compared with those obtained at graphite-Te¯on

The development of new electrode materials capable of
improving the functional characteristics of conventional electro-
des such as renewability, manageability, versatility, sensitivity
and low price has attracted great attention during the past [1],
mainly in connection with the wider and wider use of electro-
chemical detectors in ¯owing systems.
In this context, carbon-based materials have been extensively
studied, and, besides the well-known carbon paste electrodes [2],
materials such as reticulated vitreous carbon [3, 4], and compo-
sites fabricated by mixing graphite with Te¯on [5, 6], Kel-F [7],
PVC [8, 9], zeolites [10], sol-gel matrices [11] or paraseal wax
[12] have been employed with analytical purposes.
In particular, and besides other important advantages, it has
been claimed that composite electrodes exhibit current density
enhancement when they are used for electrochemical detection in
¯owing streams [1]. Recently, we have critically compared par-
af®n carbon paste and graphite-Te¯on composite electrodes
concerning the voltammetric and ¯ow-injection amperometric
behavior of several antioxidants of different hydrophobicity [13].
This article reports on the preparation and electroanalytical
performance of a new composite electrode material, constructed
by mixing graphite and the ethylene=propylene=diene (EPD)
terpolymer (poly(ethylene-co-propylene-co-5-methylene-2-nor-
bornene)), a rubbery material with a 70 wt. % ethylene and a 4 wt
% 5-methylene-2-norbornene content, used in the construction of
secondary lithium ion batteries [14] offering a good bending and
impact resistance with improved surface properties. No ante-
cedents were found in the literature regarding the use of this
polymer as binding agent for the fabrication of composite vol-
tammetric electrodes. Various substances, differing in their
solubility in water, were chosen as analytical probes. Thus, the
voltammetric and ¯ow-injection with amperometric detection
responses of potassium ferrocyanide, ascorbic acid, penta-
chlorophenol and the herbicide thiram (tetramethyl-thiur-
amdisul®de) were examined at the graphite-EPD terpolymer
composite and glassy carbon electrodes.
2. Experimental
2.1. Apparatus and Electrodes
The measurements were performed on a Eco Chemie Autolab
PSTAT 10 potentiostat using the software packages GPES 3.1
and 3.4.
A Metrohm 6.0805.010 glassy carbon electrode as well as
graphite (Ultra F purity, Carbon of America)-PTFE (polytetra-
¯uorethylene)(Aldrich) and graphite-EPD (ethylene=propylene=
diene terpolymer, Aldrich) composite electrodes were used as
working electrodes. A Ag=AgCl BAS MF2063 reference elec-
trode, and a platinum wire counter electrode were also used in
batch experiments, while a Ag=AgCl=KCl 3 mol Lÿ1 Metrohm
6.0727.000 reference electrode, and a Au 6.0333.010 counter
electrode were used for ¯ow injection measurements.
The ¯ow-injection arrangement consisted of a Gilson Mini-
puls-3 peristaltic pump, and a Rheodyne Model 5020 injection
valve with variable injection volumes. Detection was accom-
plished by using a Metrohm EA-1096 wall-jet cell, and potentials
were controlled by means of the Eco Chemie Autolab mentioned
above.
A P-Selecta ultrasonic bath and a Carver pellet press were also
used.
2.2. Composite Electrodes Preparation
Graphite-PTFE pellets were prepared following the procedure
previously described [15]. Then, several 3.5 mm diameter disk
portions of the pellet were bored, and each disk was press-®tted
into a 3.5 mm i.d. Te¯on holder. Electrical contact was made
through a stainless steel screw.

Electroanalysis 1999, 11, No. 3 # WILEY-VCH Verlag GmbH, D-69469 Weinheim, 1999 1040±0397/99/0303±0161 $17.50‡:50=0
162
Graphite-EPD pellets were prepared by thoroughly hand-
mixing the appropriate amounts of graphite and a 1255 mg Lÿ1
solution of the terpolymer in cyclohexane (Panreac), depending
on the ®nal EPD percentage required, until cyclohexane was
completely evaporated. Next, the mixture was pressed into pellets
with a 5.0 mm diameter Carver pellet press at 2000 Kg cmÿ2 for
10 min. Afterwards, each pellet was press-®tted into a 3.5 mm i.d.
te¯on holder where electrical contact, as occurred with graphite-
PTFE pellets, was made through a stainless steel screw.
2.3. Reagents and Solutions
Pentachlorophenol, and thiram (Aldrich) stock solutions
(1.0610ÿ3 mol Lÿ1 ) in methanol (Panreac), and potassium fer-
rocyanide (Sigma), and ascorbic acid (Merck) stock solutions
(1.0610ÿ3 mol Lÿ1 ) in water, were prepared weekly by weigh-
ing. More dilute standards were obtained by suitable dilution
with 0.1 mol Lÿ1 HClO4 (ascorbic acid), 0.1 mol Lÿ1 HCl
(potassium ferrocyanide), and 0.1 mol Lÿ1 HPO4 2ÿ =H2 PO4 ÿ
(pentachlorophenol and thiram). All chemicals were of analytical
reagent grade, and the water used was obtained from a Millipore
Milli-Q puri®cation system. Acetonitrile (Panreac) was also used.
2.4. Procedures
The graphite-PTFE and graphite-EPD composite electrodes
were polished daily, ®rst for 5 s on a 150 grit SiC paper, and then
on weighing paper until a shiny surface was obtained. This
procedure was the same as that previously used for graphite-
PTFE electrodes [5, 6]. No chemical or electrochemical regen-
eration of the electrodes was then necessary during the whole
working day.
The glassy carbon electrode was polished before each mea-
surement with alumina powder (particle size lower than 0.3 mm)
for 1 min; then it was sonicated in water and ®nally dried with a
clean tissue.
All measurements were carried out under ambient conditions.
For the voltammetric studies linear sweep voltammetric scans
were initiated from 0.00 V towards more positive values.
Amperometric measurements in ¯ow injection experiments were
performed by applying a potential of ‡1:0 V to the electrode.
Calibration plots for all the compounds under study were
obtained by injecting a 150 mL aliquot of the compound stock
solution into the carrier at a ¯ow rate of 3.0 mL minÿ1 .
Table 1. Electroanalytical data obtained by cyclic voltammetry at different graphite-EPD and graphite-Te¯on composite electrodes. See text for the
working medium used for each compound. GC: glassy carbon electrode.
ip : ib=Ep, [V]
Electrode Fe(CN)4ÿ
6 Ascorbic Penthachlorophenol
acid
Graphite-2% EPD 138=0.426 11.7=0.643 5.3=0.681
Graphite-4% EPD 144=0.426 8.2=0.662 2.6=0.691
Graphite-40% Te¯on 6.6=0.445 4.4=0.660 1.4=0.691
Graphite-60% Te¯on 2.9=0.558 1.5=0.596 2.1=0.747
GC 1.6=0.426 1.7=0.710 1.3=0.719
Electroanalysis 1999, 11, No. 3
L. Alonso et al.
3. Results and Discussion
As mentioned above, four different substances were selected
to test the behavior of graphite-EPD electrodes. From higher
to lower solubility in water, these substances were potassium
ferrocyanide, ascorbic acid, pentachlorophenol and thiram. Tak-
ing into account the electroanalytical data from the literature [5,
6], as well as some preliminary assays, different working media,
in which these compounds have been shown to exhibit good
electrochemical responses, were selected. Thus, aqueous solu-
tions of potassium ferrocyanide and ascorbic acid, using
0.1 mol Lÿ1 HCl and 0.1 mol Lÿ1 HClO4 as supporting electro-
lytes, respectively, a 2 : 98 methanol: 0.1 mol Lÿ1 phosphate
buffer solution of pH 7.0 for pentachlorophenol, and a 10 : 90
methanol : 0.1 mol Lÿ1 phosphate buffer solution of pH 7.4 for
thiram were employed.
Table 1 summarizes the data (Ep and the peak current to
background current ratio) obtained by cyclic voltammetry at the
three types of electrodes used. Two different percentages of EPD
and Te¯on were tested in the case of composite electrodes. As
can be observed, the oxidation response of each substance
appeared at similar potential values at the different electrodes.
However, the ip=ib ratio was always considerably higher at gra-
phite-EPD composite electrodes than at the other electrode
materials. This is specially true for the more hydrophilic analyte
checked and, in general, this trend becomes more evident as the
hydrophobicity of the compound decreased. As an example,
Figure 1 shows cyclic voltammograms recorded for Fe(CN)4ÿ 6
and ascorbic acid at a graphite-2% EPD composite electrode.
3.1. Voltammetric Behavior Under Hydrodynamic
Conditions
The graphite-to-insulator (EPD, Te¯on) ratio is an important
characteristic of the electrode material regarding properties such
as mechanical resistance, electrical conductivity, compatibility
with organic solvents and swelling phenomena in ¯owing sys-
tems. In this case, composite pellets with EPD contents lower
than 1% showed poor compactness which makes the electrode
construction dif®cult. The same drawback had been previously
observed for Te¯on composite electrodes with insulator percen-
tages lower than 40% [6]. Furthermore, EPD contents above 10%
(or 90% in the case of Te¯on) gave rise to a loss of conductivity
preventing the use of the pellets as electrode material. Therefore,
EPD contents of 1, 2 and 4%, as well as Te¯on percentages of 40,
60 and 80% were used for the fabrication of the composite
electrodes, which were tested under hydrodynamic conditions for
the above-mentioned four substances.
Thiram
4.1=0.738
1.9=0.719
1.5=0.738
1.5=0.747
1.5=0.738
Graphite-Ethylene=Propylene=Diene Terpolymer Composite Electrodes
Fig. 1. Cyclic voltammograms for Fe(CN)4ÿ
6 (a) and ascorbic acid (b) at a
graphite ± 2% EPD composite electrode. Dotted lines show background
voltammograms (0.1 mo Lÿ1 HCl and 0.1 mol Lÿ1 HClO4, respectively),
v ˆ 50 mVsÿ1 .
As an example, Figure 2 shows hydrodynamic voltammo-
grams for 1.0610ÿ4 mol Lÿ1 ascorbic acid and thiram obtained
at the graphite-EPD composite electrodes with a ¯ow rate of
3.0 mL minÿ1 . Obviously, the carrier solution consisted in each
case of the same working medium used for each particular
compound. As can be observed, well-de®ned current plateaus
were obtained in all cases, showing no signi®cant differences in
shape among them. Table 2 summarizes values for the half-wave
potential (E1=2 ) and the limiting current to background current
ratio (il=ib) obtained from this type of voltammograms at the
different electrode materials tested. As expected, both, the lim-
iting and the background currents decreased for the composite
electrodes as the insulator percentage increased, and, therefore,
the il=ib ratio constitutes a more appropriate parameter to check
the performance of the different electrode materials.
In general, it can be said that the half-wave potentials for the
more hydrophilic analytes (Fe(CN)4ÿ 6 and ascorbic acid)
appeared at less positive potentials at graphite-EPD electrodes
than at graphite-Te¯on electrodes. Furthermore, the E1=2 values
at the EPD composite electrodes are very similar to those
obtained at a conventional glassy carbon electrode. However, like
in cyclic coltammetry, the il=ib ratio for these compounds is
notably better at graphite-EPD composite electrodes, specially
for insulator percentages of 1±2%. Regarding pentachlorophenol
and thiram, the more hydrophobic compounds tested, their E1=2
values are similar and even lower at graphite-Te¯on electrodes
than at graphite-EPD electrodes and GC (0.71  0.01 V and
0.91  0.02 V, respectively), indicating a more hydrophobic nat-
ure of the Te¯on composite electrodes. The il=ib ratio for pen-
tachlorophenol is very similar at the different electrodes, whereas
it is considerably higher at graphite-EPD electrodes in the case of
thiram.
One of the most important practical features in the behavior of
composite electrodes under ¯owing conditions is their stability,
163
Fig. 2. Hydrodynamic voltammograms obtained at graphite ± 1% (1), 2%
(2) or 4% (3) EPD composite electrodes for 1.0610ÿ4 mol Lÿ1 ascorbic
acid (a) and thiram (b). Dotted voltammograms correspond to the
background voltammograms (0.1 mol Lÿ1 HClO4 and 10 : 90 methanol:
0.1 mol Lÿ1 phosphate buffer solution of pH 7.4 for ascorbic acid and
thiram, respectively); ¯ow rate, 3.0 mL minÿ1 .
that is, their resistance to fouling or their ability to yield repro-
ducible responses with no need of surface regeneration pre-
treatments. When consecutive hydrodynamic voltammograms
were registered with a conventional GC electrode, regeneration of
the electrode surface by polishing was necessary to obtain
reproducible voltammograms, specially for the more hydro-
phobic analytes. However, no polishing was needed between
consecutive scans both with graphite-EPD and graphite-Te¯on
electrodes, with RSD values for E1=2 and il=ib ranging between 1
and 5% (n ˆ 5). These results indicate good reproducibility of
the composite electrode responses with no need of pretreatment
of the electrode surface, which is specially advantageous under
¯owing working conditions.
3.2. Flow-Injection with Amperometric Detection.
Analytical Characteristics
The obtention of hydrodynamic voltammograms with well-
de®ned current plateaus at the composite electrodes allowed the
development of ¯ow-injection with amperometric detection
analytical methods for the four compounds tested. In order to be
able to compare results, the same constant applied potential was
Electroanalysis 1999, 11, No. 3
164 L. Alonso et al.

Table 2. E1=2 and limiting-to-background current ratio (il=ib) obtained by hydrodynamic voltammetry at graphite-EPD and graphite-Te¯on composite
electrodes. Flow rate: 3.0 mL minÿ1 ; concentration for each compound: 1.0610ÿ4 mol Lÿ1 .
E1=2 [V]=il : ib

Electrode Fe(CN)4ÿ
6 Ascorbic acid Pentachlorophenol Thiram
Graphite-1% EPD 0.43 0.02=20.47 0.07 0.66  0.01=9.2  0.7 0.69  0.02=1.6  0.2 0.802  0.006=10.1  0.8
Graphite-2% EPD 0.41 0.01=13.17 0.05 0.73  0.7=8.8  0.2 0.71  0.01=3.0  0.1 0.802 0.006=3.81  0.04
Graphite-4% EPD 0.40 0.01=9.51  0.09 0.73  0.2=5.4  0.2 0.68  0.02=1.80  0.05 0.738 0.006=4.61  0.03
Graphite-40% Te¯on 0.41 0.02=3.86  0.05 0.88  0.2=5.2  0.2 0.79  0.01=1.82  0.09 0.78 0.01=1.10  0.09
Graphite-60% Te¯on 0.42 0.02=2.92  0.02 0.88  0.1=5.6  0.1 0.71  0.01=2.18  0.06 0.79 0.01=1.9  0.1
Graphite-80% Te¯on 0.41 0.01=2.763 0.009 0.98  0.02=4.43 0.09 0.68  0.02=2.37  0.02 0.64 0.02=2.43  0.04

selected for all electrode materials and analytes. So, this potential
should be high enough to allow the oxidation of these com-
pounds and to be placed in the limiting current zone for each of
them. A potential value of ‡1:00 V accomplished these condi-
tions and, therefore, it was chosen to carry out the amperometric
detection under ¯ow-injection conditions.
Figure 3 shows calibration plots for Fe(CN)4ÿ 6 (a) and penta-
chlorophenol (b) obtained at different electrode materials. As can
be observed, a considerable increase in the slope of the calibra-
tion plots was produced when the graphite-EPD composite
electrode was used as working electrode, which implies a higher
sensitivity assuming that the active area approaches the geometric
Fig. 3. Calibration plots for Fe(CN)4ÿ
6 and pentachlorophenol obtained at
a graphite-2% EPD (m), a graphite - 60 % Te¯on (j), and glassy carbon
(d) electrode by ¯ow-injection with amperometric detection; ¯ow rate:
3.0 mL minÿ1 , Vi ˆ 150 mL; Eapp ˆ ‡ 1.00 V.
area of the electrode. The analytical characteristics of the corre-
sponding calibration plots at the graphite-EPD composite elec-
trode are summarized in Table 3. Relative standard deviation
values were calculated from ten different solutions at a con-
centration level of 1.0610ÿ6 mol Lÿ1 of each analyte. Moreover,
the RSD values obtained for the ip measurements from 50
repetitive injections of each analyte at the same concentration
level are also shown in Table 3, these indicate good resistance to
fouling of the graphite-EPD composite electrode under ¯owing
conditions. Limits of determination and detection were calculated
according to the 10 s [16] and 3 sb=m criteria [17], respectively,
where m is the slope of the calibration plot and sb is the standard
deviation (n ˆ 10) of the signals from 1.0610ÿ6 mol Lÿ1 ana-
lyte. As can be deduced, similar ranges of linearity and detection
limits were obtained for all the compounds tested independently
of their hydrophobicity. These analytical characteristics are
slightly better than those achieved with a conventional GC
electrode provided that a regeneration of the electrode surface
was accomplished after each set of measurements when this latter
electrode material was used.
These results show fairly well that the developed graphite-EPD
composite electrodes can be advantageously used as working
electrodes for the amperometric detection of different types of
analytes (hydrophilic or hydrophobic) under ¯owing conditions.
Finally, the changes in the amperometric responses of the
composite electrodes with the decrease in the polarity of the
carrier solution, due to the presence of increasing percentages of
organic solvents such as methanol or acetonitrile, were also
checked. As an example, Figure 4 shows the dependence of ip for
ascorbic acid and pentachlorophenol on the amount of these
organic solvents in the carrier solution. As can be observed, the
peak current decreased when the percentage of organic solvent in
the carrier solution increased, which agrees with the behavior
previously reported for graphite-Te¯on composite electrodes
[15]. This trend was much more pronounced in the case of the
presence of acetonitrile. Actually, methanol contents higher than
30% for ascorbic acid or 40% for pentachlorophenol, or acet-
onitrile contents higher than 20% for both compounds gave rise
to such a big decrease in the ip=ib ratio that no useful amperometric
responses at the graphite-EPD composite electrode could be
obtained. However, low but still useful signals could be measured
at a glassy carbon electrode even for methanol or acetonitrile
contents of 50±60%. This behavior can be extended, in general,
also for Fe (CN)4ÿ 6 and thiram. In conclusion, the developed
graphite-EPD composite electrode exhibited an advantageous
behavior with respect to conventional glassy carbon electrodes
when the carrier solution (or mobile phase) was constituted by
methanol:water mixtures with a low organic solvent content.

Electroanalysis 1999, 11, No. 3

Graphite-Ethylene=Propylene=Diene Terpolymer Composite Electrodes 165

Table 3. Analytical characteristics of the calibration plots obtained by ¯ow-injection with amperometric detection at graphite-2% EPD composite
electrodes. Carrier solution: 0.1 mol Lÿ1 HCl (Fe(CN)4ÿ6 ), 0.1 mol L
ÿ1
HClO4 (ascorbic acid), 2 : 98 methanol: 0.1 mol Lÿ1 phosphate buffer pH 7.0
(pentachlorophenol), and 10 : 90 methanol: 0.1 mol Lÿ1 phosphate buffer of pH 7.4 (thiram); ¯ow rate: 3.0 mL minÿ1 , Vi ˆ 150 mL; Eapp ˆ ‡ 1.00 V.
Fe(CN)4ÿ
6 Ascorbic acid Pentachlorophenol Thiram
Linear range [mM] 0.7±10 0.5±10 1±10 0.5±8
r 0.998 0.999 0.998 0.994
Slope [mA L m molÿ1 ] 0.037  0.001 0.033  0.001 0.033  0.001 0.10 0.04
Intercept [mA] 7 0.018  0.006 7 0.005  0.002 7 0.008  0.007 0.0  0.2
Limit of determination [mM] 1.6 1.9 1.5 1.0
Limit of detection [mM] 0.5 0.5 0.5 0.3
RSD [%] [a]=[b] 8.3=5.6 8.6=5.9 7.5=7.4 4.3=6.9
[a] calculated from 10 different 1.0610ÿ6 mol Lÿ1 solutions of each analyte; [b] calculated from 50 repetitive
injections of each analyte at a 1.0610ÿ6 mol Lÿ1 concentration level.

Fig. 4. Dependence of peak current for ascorbic acid (a), and pentachlorophenol (b), on the acetonitrile and methanol content in the carrier solution,
obtained at graphite-2% EPD (m) and glassy carbon (d) electrodes by ¯ow-injection with amperometric detection. Other conditions as in Figure 3.

4. Conclusions cially advantageous when comparing with a conventional elec-

All the above results demonstrate that the composite material
constituted by a mixture of graphite and the ethylene=
propylene=diene terpolymer can be used as voltammetric elec-
trode material as well as indicator electrode under ¯owing con-
ditions. EPD contents around 2% ensure a good compactness of
the material, which facilitates the electrode fabrication, and also
an adequate conductivity. These electrodes exhibit very good
signal-to-background ratios for analytes of different hydro-
phobicity, although this advantage is specially remarkable as the
solubility in water of the target compound is higher. Furthermore,
the composite EPD electrodes yielded reproducible results with
no need of pretreatment of the electrode surface, which is spe-
trode material such as glassy carbon. However, the presence of a
high content of organic solvent in the working solution gives rise
to a dramatic decrease in the amperometric response under
¯owing conditions, which limits the advantageous use of these
electrodes to predominantly aqueous media.
5. Acknowledgements
The ®nancial support of the SubdireccioÂn General de Forma-
cioÂn y PromocioÂn del Conocimiento, Project PD96-0640 is
gratefuly acknowledged.

Electroanalysis 1999, 11, No. 3

166
6. References
[1] D.E. Tallman, S.L. Petersen, Electroanalysis 1990, 2, 499.
[2] K. Kalcher, J.M. Kauffmann, J. Wang, I. Svancara, K. Vytras, C.
Neuhold, Z. Yang, Electroanalysis, 1995, 7, 5.
[3] J. Wang, Electrochim. Acta 1981, 26, 1721.
[4] M. Khayyami, G. Johansson, D. Kriz, B. Xie, P.O. Larsson, B.
Danielsson, Talanta 1996, 43, 957.
[5] C. FernaÂndez, A.J. Reviejo, J.M. PingarroÂn, Anal. Chim. Acta 1995,
314, 13.
[6] C. FernaÂndez, A.J. Reviejo, J.M. PingarroÂn, Anal. Chim. Acta 1995,
305, 192.
[7] D.E. Tallman, Weisshaar, J. Liquid Chromatog. 1983, 6, 2157.
[8] K. Stulik, V. Pacakova, B. StarkovaÂ, J. Chromatogr. 1981, 213,
41.
Electroanalysis 1999, 11, No. 3
L. Alonso et al.
[9] F. AlbertuÂs, A. Llereva, J. Alpizar, V. CerdaÂ, M. Luque. A. RõÂos, M.
ValcaÂrcel, Anal. Chim. Acta 1997, 355, 23.
[10] K.E. Creasy, Diss. Abstr. Int. B, 1990, 51, 2852; Chem. Abstr. 114:
110658a.
[11] J. Wang, P.V.A. Pamidi, C. Parrado, D.S. Park, J.M. PingarroÂn,
Electroanalysis 1997, 9, 908.
[12] J. Wang, N. Naser, Anal. Chim. Acta 1995, 316, 253.
[13] E. Diego, L. AguÈÂõ, A. GonzaÂlez-CorteÂs, P. YaÂnÄez-SedenÄo, J.M.
PingarroÂn, J.M. Kauffmann, Electroanalysis 1998, 10, 33.
[14] D. Guyomard, Y. Piffard, F. Leroux, M. Tournoux, Fr. Demande FR
2,730,988, Chem. Abstr. 126: 77446c, 1997.
[15] C. FernaÂndez, A.J. Reviejo, L.M. Polo, J.M. PingarroÂn, Talanta
1996, 43, 1341.
[16] ACS Committee on Environmental Improvement, Anal. Chem.
1983, 55, 2210.
[17] K. Hasebe, J. Osteryoung, Anal. Chem. 1975, 47, 2412.