The influence of electrochemical treatment on electrode reactions for vanadium redox-flow batteries

doi:10.1016/j.jechem.2018.03.021

能源化学(英文) ›› 2018, Vol. 27 ›› Issue (5): 1341-1352.DOI: 10.1016/j.jechem.2018.03.021

The influence of electrochemical treatment on electrode reactions for vanadium redox-flow batteries

Jens Noack^a,b, Nataliya Roznyatovskaya^a,b, Jessica Kunzendorf^b, Maria Skyllas-Kazacos^a,c, Chris Menictas^a,d, Jens Tübke^a,b

a German-Australian Alliance for Electrochemical Technologies for Storage of Renewable Energy(CENELEST), Mechanical and Manufacturing Engineering, University of New South Wales(UNSW), UNSW Sydney, NSW 2052, Australia;
b Fraunhofer-Institute for Chemical Technology, Applied Electrochemistry, Joseph-von-Fraunhofer-Str. 7, 76327 Pfinztal, Germany;
c hemical Engineering, University of New South Wales(UNSW), UNSW Sydney, NSW 2052, Australia;
d Mechanical and Manufacturing Engineering, University of New South Wales(UNSW), UNSW Sydney, NSW 2052, Australia

收稿日期:2017-12-18 修回日期:2018-03-08 出版日期:2018-09-15 发布日期:2018-09-15
通讯作者: Jens Noack,E-mail address:jens.noack@ict.fraunhofer.de
基金资助:
The authors would like to thank the German Federal Ministry of Education and Research (BMBF) for funding the project under the number 01DR17027,Hubert Weyrauch (Fraunhofer ICT) for carrying out the measurement of confocal microscopy,and Dr. Michael Haupt and Joachim Mayer (Fraunhofer IGB) for carrying out the XPS measurements and the peak fitting.

The influence of electrochemical treatment on electrode reactions for vanadium redox-flow batteries

Jens Noack^a,b, Nataliya Roznyatovskaya^a,b, Jessica Kunzendorf^b, Maria Skyllas-Kazacos^a,c, Chris Menictas^a,d, Jens Tübke^a,b

a German-Australian Alliance for Electrochemical Technologies for Storage of Renewable Energy(CENELEST), Mechanical and Manufacturing Engineering, University of New South Wales(UNSW), UNSW Sydney, NSW 2052, Australia;
b Fraunhofer-Institute for Chemical Technology, Applied Electrochemistry, Joseph-von-Fraunhofer-Str. 7, 76327 Pfinztal, Germany;
c hemical Engineering, University of New South Wales(UNSW), UNSW Sydney, NSW 2052, Australia;
d Mechanical and Manufacturing Engineering, University of New South Wales(UNSW), UNSW Sydney, NSW 2052, Australia

Received:2017-12-18 Revised:2018-03-08 Online:2018-09-15 Published:2018-09-15
Contact: Jens Noack,E-mail address:jens.noack@ict.fraunhofer.de
Supported by:
The authors would like to thank the German Federal Ministry of Education and Research (BMBF) for funding the project under the number 01DR17027,Hubert Weyrauch (Fraunhofer ICT) for carrying out the measurement of confocal microscopy,and Dr. Michael Haupt and Joachim Mayer (Fraunhofer IGB) for carrying out the XPS measurements and the peak fitting.

摘要/Abstract

摘要： Through targeted and reproducible electrochemical treatment of glassy carbon electrodes, investigations have been carried out on the electrochemical behaviour of the oxidation of V²⁺, VO²⁺ and the reductions of VO₂⁺, VO²⁺ and V³⁺ in order to pretreat electrodes specifically for use in vanadium redox flow batteries and, if possible, to treat them in situ. For this purpose, a glassy carbon electrode was treated potentiostatically for a period of 30 s at different potentials in the range of 500 mV-2000 mV vs. Hg/Hg₂SO₄ in 2 M H₂SO₄ and then linear sweep voltammograms were performed in the different vanadium-containing solutions. With this method, it could be shown that all reactions are extremely surface sensitive and the reaction speeds changed by several decades. The reaction rates increased significantly in all reactions compared to polished electrodes and had an optimum treatment potential of approx. 1600 mV vs. Hg/Hg₂SO₄, although the oxidation reaction of V²⁺ and the reduction reactions of V³⁺ and VO²⁺ had opposite tendencies to oxidation of VO²⁺ and the reduction of VO₂⁺ in the area of low treatment potentials. In the former, the kinetics increased and in the latter, they decreased. In addition, causes were investigated using confocal microscopy and XPS. No correlation was found to the roughness or size of the stretched surfaces, although these changed significantly as a result of the treatment. XPS measurements gave indications of a dependence on hydroxyl groups for the oxidation of VO²⁺ and the reduction of VO₂⁺, while for the reactions of oxygen-free cations and the reduction of VO²⁺ weak indications of a dependence on carboxyl groups were obtained.

关键词: Vanadium, Battery, Voltammetry, Treatment, Electrodes, Surface, Groups, Kinetics

Abstract: Through targeted and reproducible electrochemical treatment of glassy carbon electrodes, investigations have been carried out on the electrochemical behaviour of the oxidation of V²⁺, VO²⁺ and the reductions of VO₂⁺, VO²⁺ and V³⁺ in order to pretreat electrodes specifically for use in vanadium redox flow batteries and, if possible, to treat them in situ. For this purpose, a glassy carbon electrode was treated potentiostatically for a period of 30 s at different potentials in the range of 500 mV-2000 mV vs. Hg/Hg₂SO₄ in 2 M H₂SO₄ and then linear sweep voltammograms were performed in the different vanadium-containing solutions. With this method, it could be shown that all reactions are extremely surface sensitive and the reaction speeds changed by several decades. The reaction rates increased significantly in all reactions compared to polished electrodes and had an optimum treatment potential of approx. 1600 mV vs. Hg/Hg₂SO₄, although the oxidation reaction of V²⁺ and the reduction reactions of V³⁺ and VO²⁺ had opposite tendencies to oxidation of VO²⁺ and the reduction of VO₂⁺ in the area of low treatment potentials. In the former, the kinetics increased and in the latter, they decreased. In addition, causes were investigated using confocal microscopy and XPS. No correlation was found to the roughness or size of the stretched surfaces, although these changed significantly as a result of the treatment. XPS measurements gave indications of a dependence on hydroxyl groups for the oxidation of VO²⁺ and the reduction of VO₂⁺, while for the reactions of oxygen-free cations and the reduction of VO²⁺ weak indications of a dependence on carboxyl groups were obtained.

Key words: Vanadium, Battery, Voltammetry, Treatment, Electrodes, Surface, Groups, Kinetics

Jens Noack, Nataliya Roznyatovskaya, Jessica Kunzendorf, Maria Skyllas-Kazacos, Chris Menictas, Jens Tübke. The influence of electrochemical treatment on electrode reactions for vanadium redox-flow batteries[J]. 能源化学(英文), 2018, 27(5): 1341-1352.

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The influence of electrochemical treatment on electrode reactions for vanadium redox-flow batteries

The influence of electrochemical treatment on electrode reactions for vanadium redox-flow batteries

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