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Electrochemical reduction of thin graphene-oxide films in aqueous solutions - Restoration of conductivity
Univ Belgrade, Fac Phys Chem, Studentski Trg 12-16, Belgrade 11000, Serbia..
Univ Sarajevo, Dept Chem, Fac Sci, Zmaja Bosne 33-35, Sarajevo, Bosnia & Herceg..
Univ Belgrade, Inst Phys Belgrade, Pregrev 118, Belgrade 11080, Serbia..
Brandenburg Tech Univ Cottbus Senftenberg, Inst Biotechnol, Dept Nanobiotechnol, D-01968 Senftenberg, Germany..
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2022 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 410, article id 140046Article in journal (Refereed) Published
Abstract [en]

Graphene oxide finds applications in different fields of science, including energy conversion. Electrochemical reduction of graphene oxide (GO) significantly improves its conductivity. However, the kinetics of this process depends on the solvent, supporting electrolyte, pH, and numerous other factors. Most studies report the macroscopic views and ex-situ properties of reduced GO. To expand the knowledge about GO reduction, in this study, we used cyclic voltammetry (CV), simultaneous 2 points and 4 points resistance measurement (s24), conductive atomic force microscopy (AFM), and theoretical calculations. Using CV, we demonstrated that the choice of supporting electrolyte (KCl or LiCl) influences the potential range in which electrochemical GO reduction occurs. The activation energy of this process was estimated to be below 30 kJ mol(-1) in both electrolytes, being significantly lower than that required for thermal reduction of GO. Simultaneous in situ s24 resistance measurements suggest that GO films reach a highly conductive state at deep negative potentials, with an abrupt, irreversible switch from non-conductive to the conductive state. However, conductive AFM presents a more exact picture of this process: the reduction of GO films starts locally while the formed conductive islands grow during the reduction. This mechanism was confirmed by theoretical calculations indicating that the reduction starts on isolated oxygen-functional groups over the GO basal plane, while clustered OH groups are more difficult to reduce. The presented results can help in tailoring reduced GO for a particular electrochemical application by precisely controlling the reduction degree and percentage of the conductive area of the reduced GO films.

Place, publisher, year, edition, pages
Elsevier BV , 2022. Vol. 410, article id 140046
Keywords [en]
Electrochemical reduction of graphene oxide, Supporting electrolyte effect, Simultaneous 2-point 4-point resistance mea-surements, Conductive atomic force microscopy, Theoretical calculations
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-311671DOI: 10.1016/j.electacta.2022.140046ISI: 000782653000005Scopus ID: 2-s2.0-85124489540OAI: oai:DiVA.org:kth-311671DiVA, id: diva2:1655285
Note

QC 20220502

Available from: 2022-05-02 Created: 2022-05-02 Last updated: 2022-06-25Bibliographically approved

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Skorodumova, Natalia N.Pašti, Igor

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