Anal. Chem.
1997, 69, 558-562
Amperometric Sensor for Monitoring Ethylene
Larry R. Jordan† and Peter C. Hauser*,†
Department of Chemistry, The University of Auckland, Private Bag 92019, Auckland, New Zealand
George A. Dawson
Industrial Research Limited, P.O. Box 2225, Parnell, Auckland, New Zealand
Sensing electrodes were fabricated by chemical deposition
of gold onto a Nafion membrane. These electrodes, with
suitable choice of real surface area, applied potential,
supporting electrolyte, and gas flow rate, showed a detec-
tion limit of 40 ppb ethylene for a signal-to-noise ratio of
3. A linear response was observed up to at least 500
ppm. The choice of flow rate was especially influential
as it was found to affect the mechanism of the sensor
response, which is kinetically controlled even at relatively
low flow rates. No cross-sensitivity was found to ethanol
and acetaldehyde which might be present in certain
applications of the sensor, such as in horticulture.
A sensor for monitoring ethylene in produce stores is desired
because of the important role this gas plays in the postharvest
physiology of horticultural produce.1 Ethylene is given off by
produce and acts as a ripening hormone. The influence of
ethylene depends on the product, but concentrations as low as
several tens of parts per billion will cause a response in some
fruit.2 Hence, in storage facilities, the level of ethylene should
be kept low by either venting2 or using catalytic combustion
methods to scrub ethylene.3,4 However, since produce is stored
under refrigeration, this is energy consuming and therefore costly.
The situation is even more difficult when controlled atmospheres
with elevated carbon dioxide and humidity and reduced oxygen
levels are employed. Monitoring ethylene will allow a more
economical control of ethylene levels in produce storage facilities
and lead, one hopes, to better quality produce at the market.
Gas chromatography (GC) is still the most selective and
sensitive method used routinely for ethylene determination at
biologically active concentrations.1 An automated microprocessor
GC system has been developed using an alumina column and a
flame ionization detector for the monitoring of fruit and vegetables
in storage.5 Other GC detectors for ethylene, including tin oxide
semiconductor, photoionization, and photoacoustic devices, have
been described.1 Even though gas chromatography can be
automated, its use for the routine monitoring of ethylene in
† Present address: Department of Chemistry, The University of Basel,
Spitalstrasse 51, CH-4056 Basel, Switzerland.
(1) Abeles, F. B.; Morgan, P. W.; Salviet, M. E. Ethylene in Plant Biology, 2nd
ed.; Acadamic Press: San Diego, CA, 1992.
(2) McDonald, B.; Snowball, D. New Zealand Department of Scientific and
Industrial Research, Auckland Industrial Development Division, Publication
No. G.143, 1982.
(3) McDonald, B.; Harman, J. E. Sci. Hortic. 1982, 17, 113-23.
(4) Eastwell, K. C. Plant Physiol. 1978, 62, 723-6.
(5) Inaba, A.; Kubo, Y.; Nakamura, R. J. Jpn. Soc. Hortic. Sci. 1989, 58, 443-
8.
558 Analytical Chemistry, Vol. 69, No. 4, February 15, 1997
produce storage seems limited due to its complexity, high power
dissipation, and requirement for compressed gases, with resulting
low portability.
A chemiluminescence method for the monitoring of ethylene
has been described6 in which ethylene is reacted with ozone to
produce a chemiluminescent signal. Although the detection limit
of such a chemiluminescence device covers the low-ppb to ppm
ethylene range of interest, it is not suitable for all applications.
A sensor based on a platinum thin metal oxide semiconductor
field effect transistor (Pt TMOSFET) was found to have a detection
limit of ∼1 ppm ethylene.7 However, the sensor was almost twice
as sensitive to ammonia and ethanol compared to ethylene and
responded strongly to acetic acid, acetone, and ethyl acetate. The
response to alcohol would be a particular problem since ethanol
can be produced by fruit in storage.1
The oxidation of ethylene on Pt,8,9 Au,10,11 and Pd12 metal
electrodes in aqueous acid electrolyte has been reported in the
literature. The oxidation of ethylene on a Pt electrode in ethylene-
saturated 0.5 M H2SO4 produces CO2 as a reaction product. In
contrast to platinum, gold is inert to the chemisorption of ethylene,
resulting in partial oxidation to acetaldehyde.10 A residual current
due to corrosion is observed on Pd electrodes,13 making it not
ideal as a catalyst for a chemical sensor.
The deposition of precious metals on solid polymer electrolytes
(SPE) by chemical deposition allows the construction of efficient
electrodes for the oxidation or reduction of gases directly in the
vapor phase. Such electrochemical cells have for example been
demonstrated for the reduction or oxidation of alcohol vapors,14,15
carbon dioxide,16,17 and carbon monoxide.18
The use of SPE bonded electrodes for amperometric sensors
has resulted in a number of catalyst and membrane config-
(6) Quickert, N.; Findlay, W. J.; Monkman, J. L. Sci. Total Environ. 1975, 3,
323-8.
(7) Winquist, F.; Lundström, I. Anal. Chim. Acta 1990, 231, 93-100.
(8) Triaca, W. E.; Rabockai, T.; Arvia, A. J. J. Electroanal. Chem. 1979, 126,
218-26.
(9) Piovano, S. M.; Chialvo, A. C.; Triaca, W. E.; Arvia, A. J. J. Appl. Electrochem.
1987, 17, 147-55.
(10) Pastor, E.; Schmidt, V. M. J. Electroanal. Chem. 1995, 383, 175-80.
(11) Schmidt, V. M.; Pastor, E. J. Electroanal. Chem. 1994, 376, 65-72.
(12) Otsuka, K.; Shimizu, Y.; Yamanaka, I. J. Electrochem. Soc. 1990, 137, 2076-
81.
(13) Dahms, H.; Bockris, J. O. M. J. Electrochem. Soc. 1964, 111, 728-36.
(14) Enea, O. J. Electroanal. Chem. 1987, 235, 393-401.
(15) Liu, R.; Fedkiw, P. S. J. Electrochem. Soc. 1992, 139, 3514-23.
(16) Cook, R. L.; MacDuff, R. C.; Sammells, A. F. J. Electrochem. Soc. 1990,
137, 187-9.
(17) Komatsu, S.; Tanaka, M.; Okumura, A.; Kungi, A. Electrochim. Acta 1995,
40, 745-53.
(18) Kita, H.; Nakajima, H. Electrochim. Acta 1986, 31, 193-200.
S0003-2700(96)01011-6 CCC: $14.00 © 1997 American Chemical Society
urations.19-24 To maximize the current and hence the sensitivity
of an amperometric sensor, particular consideration must be given
to the real surface area of the electrode (the surface roughness)
and the diffusion rate of analyte to the electrode. Sensors for
ozone23 and hydrogen sulfide24 with the noble metal catalyst vapor
deposited directly onto the surface of the Nafion membrane have
been described. The remarkable sensitivities achieved have been
attributed to the direct access of analyte gas to the reaction
interface due to the avoidance of any membrane permeation
step.23,24
The fabrication of gold-Nafion electrodes is not as common
as platinum-Nafion electrodes, which are well documented in the
literature due to the importance of platinum-catalyzed electro-
chemical reactions for applications such as fuel cells25 and water
electrolyzers.26 Previous gold-Nafion sensor electrodes have
utilized vapor deposition techniques.23 The efficiencies of these
electrodes, however, is expected to be low compared to electrodes
formed by chemical deposition as the gold is in less intimate
contact with the Nafion.
A noble metal-Nafion configuration is described in this paper
which is suitable for the amperometric monitoring of ethylene in
produce storage atmospheres with regard to the high sensitivity
and selectivity required.
EXPERIMENTAL SECTION
Platinum Electrode. For the fabrication of platinum-Nafion
electrodes, the impregnation-reduction procedure described in
the literature27,28 was used. The first step utilizes the cation
exchange properties of the Nafion membrane to impregnate the
membrane with a cationic platinum salt [tetraammineplatinum-
(II) chloride]. Next, the platinum salt is reduced to platinum metal
using sodium borohydride as the reducing agent. Being an
anionic compound, BH4- has limited penetration of the Nafion
and therefore the platinum salt is reduced close to the Nafion-
reducing solution interface, producing a thin, porous catalyst layer
which is in intimate contact with the Nafion but also exposed to
the surface allowing contact to a current collector.
Gold Electrode. Two chemical deposition methods were
investigated. The first procedure was an impregnation-reduction
method analogous to the one used for platinum deposition using
a cationic gold salt [tetraamminegold(III) nitrate], which was
synthesized29 from tetrachloroauric acid. The second method has
been described previously.16 In this procedure, tetrachloroauric
acid, which is in contact with only one side of the membrane, is
reduced to gold metal using a reducing agent that diffuses through
from the opposite face.
The impregnation-reduction method produced gold deposits
which were unfortunately not localized near the Nafion surface
(19) Tierney, M. J.; Kim, H.-O. L. Anal. Chem. 1993, 65, 3435-40.
(20) Yan, H.; Lu, J. Sens. Actuators B 1989, 19, 33-40.
(21) Yan, H.; Liu, C.-C. Sens. Actuators B 1994, 17, 165-8.
(22) Otagawa, T.; Madou, M.; Wing, S.; Rich-Alexander, J.; Kusanagi, S.; Fujioka,
T.; Yasuda, A. Sens. Actuators B 1990, 1, 319-25.
(23) Schiavon, G.; Zotti, G.; Bontempelli, G.; Farnia, G.; Sandona, G. Anal. Chem.
1990, 62, 293-8.
(24) Schiavon, G.; Zotti, G.; Toniolo, R.; Bontempelli, G. Anal. Chem. 1995,
67, 318-23.
(25) Paik, W.-K.; Springer, T. E.; Srinivason, S. J. Electrochem. Soc. 1989, 136,
644-9.
(26) Millet, P.; Alleau, T.; Durand, R. J. Appl. Electrochem. 1993, 23, 322-31.
(27) Millet, P.; Durand, R.; Dartyge, E.; Tourillon, G.; Fontaine, A. J. Electrochem.
Soc. 1993, 140, 1373-80.
(28) Liu, R.; Her, W.-H.; Fredkiw, P. S. J. Electrochem. Soc. 1992, 139, 15-23.
(29) Skibsted, L. H.; Bjerrum, J. Acta Chem. Scand. 1974, 28, 740-6.
Figure 1. Schematic diagram of the electrochemical cell and gas
flow fitting; (WE) working or sensing electrode; (RE) reference
electrode; (CE) counter electrode.
as revealed in transmission electron micrographs of cross sections.
This is possibly due to the kinetics of the gold(III) reduction by
borohydride being too slow. Such an effect was reported to be
the case for Ir-Nafion electrodes prepared by the reduction of
[Ir(H2O)6]3+ incorporated into a Nafion membrane.26 The gold-
Nafion electrodes prepared by the impregnation-reduction pro-
cedure did not produce high currents in cyclic voltammetry
experiments when exposed to ethylene gas and so were not
suitable as sensing electrodes. The second method in which
HAuCl4 was reduced resulted in gold deposits on the surface of
the Nafion. The real surface areas of the Au-Nafion electrodes
were determined from the charge due to the reduction of the oxide
monolayer in the cathodic sweep of the cyclic voltammogram
based on a reported charge density18 of 420 µC/cm2. Electrode
areas of up to 460 cm2 were obtained. The geometric surface
area of the electrode was 0.79 cm2, giving a roughness factor of
up to 580, indicating high real surface area gold electrodes
comparable to those reported for platinum electrodes which have
been chemically deposited in Nafion membranes.28
Electrode Assembly. The electrode arrangement is shown
schematically in Figure 1. The electrochemical cell consists of a
Plexiglas cell which contains the 0.5 M H2SO4 electrolyte and the
electrodes. The cell enables contact of the metal-deposited side
of the sensing electrode (the metal-Nafion electrode) with a
flowing gas stream and the back side with the electrolyte. The
exposed geometric working electrode area to the gas stream was
0.79 cm2. The sensing electrode and a gold or platinum foil
current collector with a 1 cm diameter hole cut to expose the
Nafion electrode to the gas stream were fixed in place between
the cell and a gas manifold and the assembly secured in place
with M3 stainless steel screws.
The reference electrode used was a mercury/mercurous
sulfate electrode (MSE; REF-601, Radiometer Analytical, Lyon,
France) with a 0.5 M H2SO4 filling solution. All potentials reported
here have been converted to the standard hydrogen scale (SHE)
by adding 640 mV. Wire of the same metal as the sensing
electrode was used as the counter electrode, 99.99% purity (Advent
Research Materials Ltd., Suffolk, U.K.).
Analytical Chemistry, Vol. 69, No. 4, February 15, 1997 559
 Chemicals and Instrumentation. A BAS-100B/W poten-
tiostat (Bioanalytical Systems, West Lafayette, IN) was used for
applying fixed potentials and performing voltammetric experi-
ments. The sampled current voltammetry technique was used
for some initial experiments instead of cyclic voltammetry as, with
suitably long step times, it discriminates against the oxidation of
ethylene adsorbed at a lower potential on the electrode surface.
This was found to be especially important in the case of ethylene
reactions on platinum where ethylene can be adsorbed, but not
oxidized, in the “double-layer only” region. The resulting volta-
mmogram therefore shows only the ethylene reactions expected
for fixed potential amperometry.
Mass flow controllers type 1159B (MKS Instruments Inc.,
Andover, MA) were used to provide gas mixtures of known
concentration by blending of a calibration gas mixture and pure
nitrogen or air (BOC, Auckland, New Zealand). The mass flow
controllers were connected to the gas cylinders via 1/4 in. outer
diameter Nylon tubing using 1/4 in. Swagelok fittings. Swagelok
T piece was used. to mix the gases from the mass flow controllers.
An adapter from 1/4 in. Swagelok to 1/4 in. × 28 fittings (built
in-house) was used for connection to the sensor via Teflon tubing
with a 1 mm internal diameter (Alltech, Auckland, New Zealand).

RESULTS AND DISCUSSION

Reaction of Ethylene at SPE Electrodes. (1) Platinum.
In Figure 2 sampled current voltammograms for ethylene on Pt-
SPE and Au-SPE electrodes are shown. As evidenced in Figure
2a, oxidation of ethylene could not be observed on platinum. It is
thought that the adsorption of ethylene on platinum is hindered
by the formation of an oxide layer in the potential region where
its oxidation would occur at room temperature. Therefore it was
not possible to use oxidation on platinum in an amperometric
method.
The electrochemical reduction process seen at low potentials
in Figure 2a can also not be exploited for amperometric sensing
in real atmospheres since oxygen reduction occurs in the same
potential range.
(2) Gold. As opposed to platinum, the oxidation of ethylene
on gold occurs prior to oxide layer formation since the potential
for gold oxide monolayer formation is ∼400 mV more anodic than
for the corresponding platinum oxides.30,31 This makes ampero-
metric detection possible as evidenced by the anodic current in
the presence of ethylene in the sampled current voltammogram
displayed in Figure 2b. It is also shown in Figure 2b that the
high overpotential required for the oxygen reduction reaction on
gold23 enables the detection of ethylene in the presence of oxygen
over a wide potential range. The decrease in the ethylene
oxidation current seen in Figure 2b above ∼+1.35 V coincides
with the gold oxide formation which is seen in the anodic sweep
of the cyclic voltammogram of Figure 3. The potential just below
gold oxide monolayer formation is therefore the highest potential
suitable for monitoring ethylene.
When the 0.5 M H2SO4 electrolyte was replaced with 0.5 M
K2SO4 at pH 5 the oxidation of ethylene was inhibited. This is
consistent with the findings of Dahms and Bockris,13 who reported
that the potential at which ethylene oxidation on gold commences
is not dependent on pH. Due to the negative shift in potential for
(30) Bard, A. J. Encyclopedia of Electrochemistry of the Elements; Marcel Dekker
Inc.: New York, 1975; Vol. IV.
(31) Bard, A. J. Encyclopedia of Electrochemistry of the Elements; Marcel Dekker
Inc.: New York, 1976; Vol. VI.
Figure 2. Sampled current voltammogram of (a) platinum-Nafion
electrode and (b) gold-Nafion electrode: sweep rate 5 mV/s; hold
time 8 s; sample time 50 ms; electrolyte 0.5 M H2SO4; gas flow rate
100 cm3/min. Nitrogen, ]; air, +; ethylene (100%), 0
the gold oxide layer formation by ∼300 mV (60 mV per pH unit)30
but no corresponding cathodic shift in the potential at which
ethylene is oxidized, the available overpotential at pH 5 is expected
to be very small, resulting in low observed currents. Lowering
the pH by using more concentrated sulfuric acid would move the
formation of the gold oxide layer in the anodic direction by 60
mV per unit pH,30 thereby increasing the available overpotential
that can be applied to the sensing electrode before gold oxide
formation commences. However, increasing the H2SO4 concen-
tration from 0.5 to 5 M would shift the oxide formation by only
60 mV. Use of concentrated acid was therefore not investigated
in this work.
Sensor Performance. The dynamic response of the gold-
Nafion amperometric sensor to ppm levels of ethylene is shown
in Figure 4. A potential of +1.25 V, which is close to the highest
potential at which ethylene is oxidized, was applied to the sensing
electrode. The gas side of the sensing electrode was exposed to
a gas stream with a constant flow of 100 cm3/min, and on the
reverse side a 0.5 M H2SO4 electrolyte was used to contact the
membrane. A detection limit of 40 ppb is obtainable based on a
signal-to-noise ratio of 3. The relative standard deviation between
measurements was found to be 0.5% as determined by taking five

560 Analytical Chemistry, Vol. 69, No. 4, February 15, 1997

Figure 3. Cyclic voltammogram of gold-Nafion electrode with
nitrogen flow on gas side: sweep rate 50 mV/s; electrolyte 0.5 M
H2SO4.
Figure 4. Dynamic response of sensor to ethylene (0-10 ppm):
gas flow 100 cm3/min-1; real electrode surface area 245 cm2; applied
potential +1.25 V vs SHE.
consecutive measurements of a 10 ppm ethylene standard over a
0.5 h period. The response was found to be linear up to at least
500 ppmsalthough at this concentration the signal was found to
decay rapidly but to recover when the cell was flushed with
nitrogen or air. A similar phenomenon has been reported for
electrochemical fuel cell sensors,32 where the probable cause has
been reported to be the slow removal of the polar reaction
products, acetaldehyde and acetic acid, which can hydrogen bond
to the electrode surface. It is most likely, since the partial
oxidation of ethylene on gold produces acetaldehyde, that the slow
removal of this reaction product is the cause of the signal decay.
In the application of produce storage the ethylene concentration
of interest is normally below several ppm. However, if high
concentrations of ethylene were being measured, it may be
possible to avoid loss of sensitivity, due to buildup of the reaction
(32) Bahari, S. M.; Criddle, W. J.; Thomas, J. D. R. Analyst 1992, 117, 701-6.
Figure 5. Response of sensor to 10 ppm ethylene as a function of
flow rate (0-100 cm3/min) and applied potential. Real electrode
surface area 245 cm2.
product, by simply reducing the overpotential at which ethylene
is measured to a value where product accumulation does not
become rate limiting.
The sensor response to 10 ppm ethylene showed no short-
term loss of sensitivity. After several days of continuous operation
a decrease in sensitivity was noted which could, however, be
reversed by applying a brief anodic cleaning potential to the
sensing electrode. Room temperature fluctuations appeared to
affect the sensitivity of the sensor but by not worse than a 2%
change in signal per degree C.
Effect of Real Electrode Surface Area. The Faradaic signal
due to oxidation of ethylene was found to increase with the real
surface area of the electrode. However, at higher surface areas
the increase in current was limitedsprobably due to mass
transport of gas through the pores of the gold deposit limiting
the current. The background noise also increased with increasing
electrode surface area but at a rate less than that of the signal.
The best detection limit was found for a surface area of ∼200 cm2.
It is expected that high surface area electrodes are not necessarily
ideal for all gas sensing applications since, if the kinetic reaction
rate is fast enough, the sensitivity should be diffusion limited and
dependent only on the geometric area of the electrode. High
surface area electrodes are therefore most useful when the kinetic
reaction rate is slow, such as in the oxidation of hydrocarbons.33
In the case of ethylene oxidation on gold, the reaction kinetics
are relatively slow according to thermodynamic calculations13 and
also the overpotential that can be applied is limited by the gold
oxide monolayer formation.
Influence of Flow Rate. The flow rate dependence of the
sensor response to 10 ppm ethylene is shown in Figure 5. In
this experiment, fixed potentials between +0.95 and +1.25 V were
applied and for each potential, after a stable residual current had
been attained, the flow rate of the ethylene standard was
systematically varied. The sensor response was found to be highly
flow rate dependent at low flow but to be relatively constant at
higher flow rates. The effect is most noticeable at lower applied
(33) Chang, S. C.; Stetter, J. R.; Cha, C. S. Talanta 1993, 40, 461-77.
Analytical Chemistry, Vol. 69, No. 4, February 15, 1997 561
Table 1. Response of Sensor to Other Gases Relative
to That of Ethylene
gas rel sensor gas rel sensor
measured response measured response
acetylene 7.4 NO 1.8
ethanol 0 NO2 0.3
acetaldehyde 0 SO2 2.5
CO 0 ethylene 1.0
potentials. At high overpotential and low flow rates, the current
becomes independent of potential. These findings are thought
to be due to a change in response mechanism: At high flow rate,
the stagnant air boundary layer at the gas-electrode interface is
reduced to an extent that the reaction is limited by the kinetic
reaction rate even for the highest overpotential possible. When
the flow is reduced, the stagnant boundary layer is increased and
a diffusion-limited contribution to the response is seen at higher
overpotentials. A principle advantage of a diffusion-limited re-
sponse is that the signal is relatively independent of the applied
potential so that accurate control of the potential is not required.33
However, careful control of the flow rate is required and the
sensitivity of the sensor may be compromised. The kinetically
limited response achieved at higher flow rates is independent of
flow although in this case accurate control of the applied potential
is necessary. Kinetic control of the electrode process is not
expected at such low flow rates in gas diffusion electrodes
employing Teflon-bound noble metal catalysts where the Teflon
membrane acts as a barrier to mass transport.34 The lower rate
of diffusion observed for such gas electrodes would limit the
obtainable sensitivity, and therefore, they may not be suitable for
the monitoring of low levels of ethylene.
Selectivity. The sensor response to some other electroactive
compounds relative to the response of ethylene is shown in Table
1. The cross-sensitivity to acetaldehyde (100 ppm) and ethanol
(100 ppm) was tested because these species are potential inter-
ferants as they can occur in fruit storage facilities at relatively
high concentrations1 and are electroactive compounds.33 Both of
these compounds showed no response, which is consistent with
the reported selectivity of gold catalysts to only unsaturated
organic compounds.11 Acetylene (10 ppm) was investigated due
to its reported reactivity on gold in the same potential region
(34) Bay, H. W.; Blurton, K. F.; Sedlak, J. M.; Valentine, A. M. Anal. Chem.
1974, 46, 1837-9.
562 Analytical Chemistry, Vol. 69, No. 4, February 15, 1997
where ethylene oxidizes.11 The oxidation current for acetylene
was found to be ∼7 times that for ethylene, which is consistent
with its complete oxidation to CO2. However, this species is not
expected to be present in fruit stores. The reducing combustion
products SO2, NO2, and NO showed a significant response
although they too are not expected to be present in a storage
atmosphere. Unlike ethylene SO2, NO2 and NO were found to
be reactive above the gold oxide monolayer formation potential,
indicating the possibility of determining these interferants and
ethylene by difference. Oxidising gases such as ozone and
chlorine are not expected to interfere due to the positive potential
applied to the electrode. No cross-sensitivity was seen to CO (100
ppm).
CONCLUSION
Gold has been shown to be a suitable noble metal catalyst for
the sensing electrode of an amperometric ethylene sensor. This
is in a way unexpected as gold is a relatively poor catalyst
compared with platinum and only 2 electrons are produced per
ethylene molecule on gold compared with 12 produced during
complete oxidation on platinum. However, because gold is a poor
catalyst for organic compounds in general and only reacts with
unsaturated organic compounds, which can weakly (in the case
of ethylene) and strongly (in the case of acetylene) interact with
the gold surface via double and triple bonds, good selectivity is
obtained. Even if platinum could oxidize ethylene at room
temperature, compounds such as ethanol, which are well-known
to react on platinum,15,33 would be potential interferants in a
platinum amperometric sensor.
High real surface electrodes produced by chemical deposition
make up for the limitations of the relatively slow reaction kinetics
of ethylene oxidation on gold and together with fast diffusion due
to the absence of any membrane permeation result in a highly
sensitive amperometric sensor for ethylene monitoring.
ACKNOWLEDGMENT
The authors thank the Foundation for Research Science and
Technology (New Zealand) for funding this work and G. A. Wright
of the University of Auckland for his friendly participation in part
of it.
Received for review October 2, 1996. Accepted December
11, 1996.X
AC9610117
X
Abstract published in Advance ACS Abstracts, January 15, 1997.