ELSEVIER Journal of Electroanalytical Chemistry 444 (1998) 261-269
JOURNAL OF
A comparative kinetic investigation of ethylcinnamate
electrohydrodimerization on mercury and liquid gallium
Giovanni Pezzatini, Silvia Becagli, Massimo Innocenti, Rolando Guidelli *
Department of Chemistry, University o] Florence, Via Gino Capponi 9, 50121 Florence, haly
Received 21 October 1997
Abstract
Electrohydrodimerization (EHD) of ethylcinnamate (EC) on mercury takes place both from hydrotropic solutions of
tetraethylammonium-p-toluenesulphonate (TEA-PTS) and from dilute aqueous solutions of the strong surfactant Triton X-100.
In both cases the one-electron reduction wave due to hydrodimer formation satisfies the requirements for a rate-determining
homogeneous coupling of the electrochemically generated anion radicals. The kinetics of EC EHD on liquid gallium is identical
with that on mercury at the same temperature of 31°C in hydrotropic solutions of TEA-PTS; conversely, in aqueous Triton
X-100 it is faster than on mercury and satisfies the requirements for a rate-determining heterogeneous radical-radical coupling.
This behaviour is explained by a stronger adsorptivity of EC and its intermediate reduction products on gallium than on mercury,
so that Triton X-100 does not succeed in displacing these species completely from the electrode surface. The general trend
consisting in a higher adsorptivity of organic compounds with conjugated double bonds and/or aromatic rings on gallium than
on mercury is explained on the basis of the difference in hydrophilicity between these two metals. ,~) 1998 Elsevier Science S.A.
All rights reserved.
Keywords: Kinetic investigation; Ethylcinnamate; Electrohydrodimerization; Mercury; Gallium
I. Introduction
Electrocatalysis is mainly concerned with the influ-
ence of the nature of the metal upon the kinetics of
electrode processes. The electrode material does not
have a primary effect upon the kinetics of a given
electrode process if, in passing from reactant to
product, no chemical bonds are formed or broken, and
if all reacting species are nonspecifically adsorbed on
the electrode surface [1-3]. This situation is exemplified
by the Fe(II)/Fe(III) redox couple on several sp and
transition metals [2,3]. However, by far the majority of'
electrode processes involve breaking or making of
chemical bonds and a specific adsorption of the various
reacting species whose extent depends on the nature of
* Corresponding author. Tel.: +39 55 2757540; fax: + 39 55
244102; e-mail: guidelIi@CESIT1.UNIFL.IT
0022-0728/98/$19.00 © 1998 Elsevier Science S.A. All rights reserved.
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the metal. In this case, if the electrode process is
controlled by an electrochemical step, its rate may vary
by several orders of magnitude in passing from one
metal to another, and no general rule can be estab-
lished, since electrocatalytic effects depend drastically
upon the particular electrode process investigated. On
the other hand, if the electrode process is controlled by
a chemical step (e.g., a protonation or a coupling step),
then the changes in its rate with varying the electrode
material are less drastic and are amenable to a more
straightforward interpretation.
Small changes in the rate of an electrode process
require accurate measurements, which are more easily
achieved with liquid metals, since they allow a continu-
ous renewal of the electrode surface by the use of
dropping electrodes. In nature only two metals are
liquid in the proximity of room temperature, namely
mercury and gallium, the latter melting at 30°C. These