ELECTROCHEMISTRY OF IMMOBILIZED MICROPARTICLES AND MICRODROPLETE: ACCESS TO FUNDAMENTAL DATA OF SOLID MATERIALS AND IONS
The idea to study the electrochemistry of immobilized microparticles has been published by this author for the first time in 1989. In the last 32 years, this approach has been shown to be very successful not only for analytical characterization of solid materials, but also applicable to extract ther...
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V.I.Vernadsky Institute of General and Inorganic Chemistry
2021
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Ukrainian Chemistry Journal| _version_ | 1871465755666546688 |
|---|---|
| author | Scholz, Fritz |
| author_facet | Scholz, Fritz |
| author_institution_txt_mv | [
{
"author": "Fritz Scholz",
"institution": "Universität Greifswald, Institut für Biochemie"
}
] |
| author_sort | Scholz, Fritz |
| baseUrl_str | https://ucj.org.ua/index.php/journal/oai |
| collection | OJS |
| datestamp_date | 2026-07-22T08:23:47Z |
| description | The idea to study the electrochemistry of immobilized microparticles has been published by this author for the first time in 1989. In the last 32 years, this approach has been shown to be very successful not only for analytical characterization of solid materials, but also applicable to extract thermodynamic and kinetic data, and even to determine the age of metal specimen. In 2000, it has been shown that the electrochemistry of immobilized microdroplets gives an elegant access to determine the Gibbs free energies of ion transfer between immiscible solvents. These measurements are performed with a standard 3-electrode potentiostate and can be used also for solvents, which cannot be used in experiments with the classical 4-electrode technique.
The electrochemistry of microparticles and microdroplets share several common features with respect to the electrode mechanisms: in both cases three-phase electrodes are realized and ion and electron transfer proceed simultaneously.
This talk reviews the activities of the speaker and his cooperation partners during the last 3 decades paying special attention to those results, which are of general interest. |
| doi_str_mv | 10.33609/2708-129X.87.09.2021.55-60 |
| first_indexed | 2025-09-24T17:43:41Z |
| format | Article |
| fulltext |
55
УДК 541.2+544.7 doi: 10.33609/2708-129X.87.09.2021.55-60
ELECTROCHEMISTRY OF IMMOBILIZED MICROPARTICLES
AND MICRODROPLETE: ACCESS TO FUNDAMENTAL DATA
OF SOLID MATERIALS AND IONS
F. Scholz1
1Universität Greifswald, Institut für Biochemie, Editor-in-Chief Journal of Solid State Electroche
mistry (http://link.springer.com/journal/10008) and Editor-in-Chief ChemTexts – The Textbook
Journal of Chemistry (http://link.springer.com/journal/40828)
Editor of “Monographs in Electrochemistry” (https://www.springer.com/series/7386)
Felix-Hausdorff-Straße 4, 17489 Greifswald, Germany
e-mail: fscholz@uni-greifswald.de
The idea to study the electrochemistry of immobilized microparticles has been published
by this author for the first time in 1989. In the last 32 years, this approach has been shown
to be very successful not only for analytical characterization of solid materials, but also ap-
plicable to extract thermodynamic and kinetic data, and even to determine the age of metal
specimen. In 2000, it has been shown that the electrochemistry of immobilized microdroplets
gives an elegant access to determine the Gibbs free energies of ion transfer between immis-
cible solvents. These measurements are performed with a standard 3-electrode potentiostate
and can be used also for solvents, which cannot be used in experiments with the classical
4-electrode technique.
The electrochemistry of microparticles and microdroplets share several common features
with respect to the electrode mechanisms: in both cases three-phase electrodes are realized
and ion and electron transfer proceed simultaneously.
This talk reviews the activities of the speaker and his cooperation partners during the last
3 decades paying special attention to those results, which are of general interest.
Key words: Electrochemistry of solids, three-phase electrodes, ion transfer between im-
miscible solvents.
ELECTROCHEMISTRY OF IMMOBILIZED MICROPARTICLES AND MICRODROPLETE:
ACCESS TO FUNDAMENTAL DATA OF SOLID MATERIALS AND IONS
56 ISSN 2708-129X. Укр. хім. журн., 2021
PHYSICAL CHEMISTRY
Electrochemistry of immobilized
micropartiles
The electrochemical analysis and charac-
terization of solid materials has always been a
great challenge; however, it remained confined
to electron conductors, mainly metals; it was
and still is the domain of corrosion science.
The last decades have also seen tremendous
advances in the insertion electrochemistry of
solid materials for batteries, almost exclusively
studied with compact macroscopic solid elect
rodes.
Among the many attempts to expand the
applicability of electrochemical measurements
to solids, the early work of the Russian scien-
tist A. I. Glazunov [1] is noteworthy. He called
his technique electrography. A more detailed
review of the history of solid state electroana
lysis is available elsewhere [2]. Then, in 1989,
Scholz, Nitschke and Henrion [3] have shown
that metal particles can be transferred from a
piece of metal to the surface of a graphite elec-
trode by abrasion, i.e., by rubbing the graphite
electrode on the surface of the metal, and soon
after, the same authors have shown together
with Damaschun that also mineral particles
can be mechanically immobilized on an elec-
trode for electrochemical studies [4].
The purely analytical applications, i.e., the
quantitative analysis of alloys, minerals and
synthetic solid materials will not be discussed
here, as it is presented in detail in [2]. Instead,
attention is drawn on the possibility to deter-
mine the free energies of phase transition in
case of some minerals, when the two phases
can undergo reversible electrochemical reac-
tions to the same dissolved species [5, 6]. Stud-
ies of immobilized microparticles also allowed
to understand the dependencies of formal po-
tentials on structure parameters as ionic radii
and ion potentials, in case of polycyanomet-
alates [7, 8]. Another noteworthy topic is the
electrochemical study of solid solutions [9–12].
Whereas X-ray diffraction of solid solutions
requires a certain degree of crystallinity, the
electrochemical approach also works in case of
X-ray amorphous substances (see [10]).
A number of theoretical papers have been
published in which the mechanism of elec-
trode reactions of immobilized microparticles
is treated [13–17].
The electrochemical behavior of micropar-
ticles has also been studied by in-situ combi-
nation with X-ray diffraction [18], calorimetry
[19, 20], diffuse reflection spectroscopy [21],
and AFM [22–27]. These combinations al-
lowed distinguishing the different electrode
mechanisms. The studies of the electrochem-
istry of microparticles led to the development
of an approach for separating the Gibbs free
energies of ion and electron transfer in case of
reversible insertion electrochemical systems
[28, 29].
Finally, it is noteworthy to mention that the
electrochemistry of microparticles gives access
to the age of metal objects, be they of gold, cop-
per, bronze, or silver [30]. These electrochem-
ical age determinations are of very special va
lue because so far almost no direct methods of
age determinations of metals and alloys were
known.
Electrochemistry of immobilized
micro-droplets
When a droplet of an immiscible solvent
is immobilized on a suitable electrode, and
when that droplet contains a redox active com-
F. Scholz
57https://ucj.org.ua
UCJ № 9 / Vol. 87
pounds, but no salt, an electron transfer be-
tween the redox probe and the electrode ini
tiates an ion transfer between the bulk electro-
lyte solution and the droplet solvent. Similar
to the insertion electrochemistry of micropar-
ticles, the entire electrode is a three-phase
electrode. When the formal potential of the
redox probe in the droplet solvent is known,
simple voltammetric measurements with the
immobilized microdroplets allow determin-
ing the Gibbs free energies of transfer of the
ions, which are transferred between the sol-
vents [2, 31–43]. This approach allowed to de-
termine the Gibbs energies of ion transfer, i.e.,
the partition constants, of ions between water
and n-octanol [32, 39], which is not possible
when using the classical 4-electrode systems. It
was possible to quantify the chiral recognition
energies for ions using the solvent system wa-
ter / chiral organic solvent [33, 42]. Amino acid
anions, cations and also peptide ions have been
studied in order to quantify the lipophilicity of
these ions and their constituents [36, 38]. The
new technique of using immobilized droplet
electrodes considerably expanded the range of
ions and of solvents for which Gibbs free ener-
gies of ion transfer are accessible.
Acknowledgement
This research has been supported by
Deutsche Forschungsgemeinschaft
(DFG) for almost 30 years.
ЕЛЕКТРОХІМІЯ ІММОБІЛІЗОВАНИХ МІКРО
ЧАСТИНОК І МІКРОКРАПЕЛЬ: ПІДХІД ДО
ФУНДАМЕНТАЛЬНИХ ДАНИХ ТВЕРДИХ МА-
ТЕРІАЛІВ ТА ІОНІВ
Ф. Щольц1
Університет Грайфсвальда, Інститут біо
хімії, гол. редактор журналу «Електрохі-
мія твердого тіла» (http://link.springer.com/
journal/10008) та гол. редактор журналу
«Хрестоматійний підручник з хімії» (http://
link.springer.com/journal/40828),
редактор журналу «Монографії з електро-
хімії» (https://www.springer.com/series/7386)
Фелікс-Хаусдорф-штрасе 4, 17489 Грайфс
вальд, Німеччина
Ідею вивчення електрохімії іммобілізо-
ваних мікрочастинок було вперше опри-
люднено автором роботи в 1989 році. Отже,
за останні 32 роки цей підхід показав себе
дуже успішним не тільки для аналітичних
характеристик твердих матеріалів, а й для
застосування при отриманні термодина-
мічних і кінетичних даних і навіть визна-
чення віку металевих зразків. У 2000 році
було показано, що електрохімія іммобі-
лізованих мікрокрапель дає надійний до-
ступ для визначення вільних енергій Гіббса
– переносу іонів між незмішуваними роз-
чинниками. Ці виміри проводять із вико-
ристанням стандартного триелектродного
потенціостата і їх можна застосувати та-
кож для розчинників, які не можливо ви-
користовувати в експериментах із класич-
ною чотириелектродною технікою. Елек-
трохімія мікрочастинок і мікрокрапель має
кілька спільних рис відносно електродних
ELECTROCHEMISTRY OF IMMOBILIZED MICROPARTICLES AND MICRODROPLETE:
ACCESS TO FUNDAMENTAL DATA OF SOLID MATERIALS AND IONS
58 ISSN 2708-129X. Укр. хім. журн., 2021
PHYSICAL CHEMISTRY
механізмів: в обох випадках реалізуються
трифазні електроди і перенесення іонів та
електронів відбувається водночас. У пові-
домленні представлено результати діяль-
ності спікера і його партнерів зі співпраці
за останні 3 десятиліття, особливу увагу
приділено результатам, які становлять
спільний інтерес.
Ключові слова: електрохімія твердих тіл,
трифазні електроди, іонний перенос між
незмішуваними розчинниками.
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UCJ № 9 / Vol. 87
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trochem. Commun. 2004. 6: 409–412.
28. Cisternas R., Kahlert H., Wulff H., Scholz
F. The electrode responses of a tungsten
bronze electrode differ in potentiometry
and voltammetry and give access to the in-
dividual contributions of electron and pro-
ton transfer. Electrochem. Commun. 2015.
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29. Scholz F., Doménech-Carbó A. The thermo-
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trodes – a team play of electrons and ions
ELECTROCHEMISTRY OF IMMOBILIZED MICROPARTICLES AND MICRODROPLETE:
ACCESS TO FUNDAMENTAL DATA OF SOLID MATERIALS AND IONS
60 ISSN 2708-129X. Укр. хім. журн., 2021
PHYSICAL CHEMISTRY
across two separate interfaces (minireview).
Angew. Chem. Int. Ed. 2019. 19: 3279–3284.
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chemical age determinations of metallic
specimens — utilization of the corrosion
clock.Acc. Chem. Res. 2019. 52:400−406.
31. Scholz F., Komorsky-Lovrić Š., Lovrić M. A
new access to Gibbs free energies of transfer
of ions across liquid-liquid interfaces and a
new method to study electrochemical pro-
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Electrochem. Commun. 2000. 2: 112–118.
32. Gulaboski R., Mirčeski V., Scholz F. An
electrochemical method for the determina-
tion of the standard Gibbs energy of anion
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trochem. Commun. 2002. 4: 277–283.
33. Scholz F., Gulaboski R., Mirčeski V., Langer
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34. Mirčeski V., Gulaboski R., Scholz F. Deter-
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35. Komorsky-Lovrić Š., Riedl K., Gulaboski
R, Mirčeski V., Scholz F. Determination of
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interface. Langmuir. 2002. 18: 8000–8005;
Correction: 2003. 19: 3090.
36. Gulaboski R., Mirčeski V., Scholz F. Deter-
mination of the standard Gibbs energies
of transfer of cations and anions of amino
acids and small peptides across the water |
nitrobenzene interface. Amino Acids. 2003.
24: 149–154.
37. Gulaboski R., Riedl K., Scholz F. Standard
Gibbs energies of transfer of halogenate and
pseudohalogenate ions, halogen substituted
acetates, and cycloalkylcarboxylate anions
at the water| nitrobenzene interface. Phys.
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39. Bouchard G., Galland A., Carrupt P-A., Gu-
laboski R., Mirčeski V., Scholz F., Girault
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transfer of cations across the nitrobenzene
| water interface with the help of a three-
phase electrode. Electrochem. Commun.
2003. 5: 929–934.
41. Gulaboski R., Caban K., Stojek Z., Scholz
F.The determination of the standard Gibbs
energies of ion transfer between water and
heavy water by using the three-phase elec-
trode approach. Electrochem. Commun.
2004. 6: 215–218.
42. Scholz F., Gulaboski R. Gibbs energies of
transfer of chiral anions across the interface
water|chiral organic solvent determined
with the help of three-phase electrodes. Fa
raday Discussions. 2005. 129: 169–177.
43. Scholz F., Gulaboski R. Determination of
Gibbs energies of ion transfer across water/
organic liquid interfaces with three-phase
electrodes. Chem. Phys. Chem. 2005. 6: 16–
28.
Стаття надійшла 20. 09. 2021.
|
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| last_indexed | 2026-07-23T01:07:05Z |
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| spelling | oai:ojs2.1444248.nisspano.web.hosting-test.net:article-3542026-07-22T08:23:47Z ELECTROCHEMISTRY OF IMMOBILIZED MICROPARTICLES AND MICRODROPLETE: ACCESS TO FUNDAMENTAL DATA OF SOLID MATERIALS AND IONS Scholz, Fritz Electrochemistry of solids, three-phase electrodes, ion transfer between immiscible solvents. The idea to study the electrochemistry of immobilized microparticles has been published by this author for the first time in 1989. In the last 32 years, this approach has been shown to be very successful not only for analytical characterization of solid materials, but also applicable to extract thermodynamic and kinetic data, and even to determine the age of metal specimen. In 2000, it has been shown that the electrochemistry of immobilized microdroplets gives an elegant access to determine the Gibbs free energies of ion transfer between immiscible solvents. These measurements are performed with a standard 3-electrode potentiostate and can be used also for solvents, which cannot be used in experiments with the classical 4-electrode technique. The electrochemistry of microparticles and microdroplets share several common features with respect to the electrode mechanisms: in both cases three-phase electrodes are realized and ion and electron transfer proceed simultaneously. This talk reviews the activities of the speaker and his cooperation partners during the last 3 decades paying special attention to those results, which are of general interest. V.I.Vernadsky Institute of General and Inorganic Chemistry 2021-10-25 Article Article Physical chemistry Физическая xимия Фізична xімія application/pdf https://ucj.org.ua/index.php/journal/article/view/354 10.33609/2708-129X.87.09.2021.55-60 Ukrainian Chemistry Journal; Vol. 87 No. 9 (2021): Ukrainian Chemistry Journal; 55-60 Украинский химический журнал; ##issue.vol## 87 ##issue.no## 9 (2021): Ukrainian Chemistry Journal; 55-60 Український хімічний журнал; Том 87 № 9 (2021): Український хімічний журнал; 55-60 2708-129X 2708-1281 en https://ucj.org.ua/index.php/journal/article/view/354/189 Copyright (c) 2021 Fritz Scholz https://creativecommons.org/licenses/by-nc/4.0 |
| spellingShingle | Scholz, Fritz ELECTROCHEMISTRY OF IMMOBILIZED MICROPARTICLES AND MICRODROPLETE: ACCESS TO FUNDAMENTAL DATA OF SOLID MATERIALS AND IONS |
| title | ELECTROCHEMISTRY OF IMMOBILIZED MICROPARTICLES AND MICRODROPLETE: ACCESS TO FUNDAMENTAL DATA OF SOLID MATERIALS AND IONS |
| title_full | ELECTROCHEMISTRY OF IMMOBILIZED MICROPARTICLES AND MICRODROPLETE: ACCESS TO FUNDAMENTAL DATA OF SOLID MATERIALS AND IONS |
| title_fullStr | ELECTROCHEMISTRY OF IMMOBILIZED MICROPARTICLES AND MICRODROPLETE: ACCESS TO FUNDAMENTAL DATA OF SOLID MATERIALS AND IONS |
| title_full_unstemmed | ELECTROCHEMISTRY OF IMMOBILIZED MICROPARTICLES AND MICRODROPLETE: ACCESS TO FUNDAMENTAL DATA OF SOLID MATERIALS AND IONS |
| title_short | ELECTROCHEMISTRY OF IMMOBILIZED MICROPARTICLES AND MICRODROPLETE: ACCESS TO FUNDAMENTAL DATA OF SOLID MATERIALS AND IONS |
| title_sort | electrochemistry of immobilized microparticles and microdroplete: access to fundamental data of solid materials and ions |
| topic_facet | Electrochemistry of solids three-phase electrodes ion transfer between immiscible solvents. |
| url | https://ucj.org.ua/index.php/journal/article/view/354 |
| work_keys_str_mv | AT scholzfritz electrochemistryofimmobilizedmicroparticlesandmicrodropleteaccesstofundamentaldataofsolidmaterialsandions |