Study of Anion Exchange Membrane Properties Incorporating N-spirocyclic Quaternary Ammonium Cations and Aqueous Organic Redox Flow Battery Performance

Tsehaye, Misgina Tilahun; Yang, Xian; Janoschka, Tobias; Hager, Martin D.; Schubert, Ulrich S.; Alloin, Fannie; Iojoiu, Cristina

doi:10.3390/membranes11050367

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Study of Anion Exchange Membrane Properties Incorporating N-spirocyclic Quaternary Ammonium Cations and Aqueous Organic Redox Flow Battery Performance

Misgina Tilahun Tsehaye

^1,†

^2,3,4,†

^4,*,

^2,3

^2,3,

^1,5,*

and

Cristina Iojoiu

^1,5,*

Univ. Grenoble Alpes, Univ. Savoie Mont Blanc, CNRS, Grenoble INP, LEPMI, 38 000 Grenoble, France

Laboratory of Organic and Macromolecular Chemistry (IOMC), Friedrich Schiller University Jena, Humboldtstrasse 10, 07743 Jena, Germany

Center for Energy and Environmental Chemistry Jena (CEEC Jena), Friedrich Schiller University Jena, Philosophenweg 7a, 07743 Jena, Germany

⁴

JenaBatteries GmbH, Otto-Schott-Strasse 15, 07745 Jena, Germany

⁵

Réseau sur le Stockage Electrochimique de l’Energie (RS2E), CNRS, FR3459, CEDEX, 80 039 Amiens, France

Authors to whom correspondence should be addressed.

^†

Authors contributed equally.

Academic Editor: Patric Jannasch

Membranes 2021, 11(5), 367; https://doi.org/10.3390/membranes11050367

Received: 5 May 2021 / Revised: 13 May 2021 / Accepted: 14 May 2021 / Published: 18 May 2021

(This article belongs to the Section Membrane Analysis and Characterization)

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Abstract

Flexible cross-linked anion exchange membranes (AEMs) based on poly (p-phenylene oxide) grafted with N-spirocyclic quaternary ammonium cations were synthesized via UV-induced free-radical polymerization by using diallylpiperidinium chloride as an ionic monomer. Five membranes with ion exchange capacity (IEC) varying between 1.5 to 2.8 mmol Cl⁻·g⁻¹ polymer were obtained and the correlation between IEC, water uptake, state of water in the membrane and ionic conductivity was studied. In the second part of this study, the influence of properties of four of these membranes on cell cycling stability and performance was investigated in an aqueous organic redox flow battery (AORFB) employing dimethyl viologen (MV) and N,N,N-2,2,6,6-heptamethylpiperidinyl oxy-4-ammonium chloride (TMA-TEMPO). The influence of membrane properties on cell cycling stability and performance was studied. At low-current density (20 mA·cm⁻²), the best capacity retention was obtained with lower IEC membranes for which the water uptake, freezable water and TMA-TEMPO and MV crossover are low. However, at a high current density (80 mA·cm⁻²), membrane resistance plays an important role and a membrane with moderate IEC, more precisely, moderate ion conductivity and water uptake was found to maintain the best overall cell performance. The results in this work contribute to the basic understanding of the relationship between membrane properties and cell performance, providing insights guiding the development of advanced membranes to improve the efficiency and power capability for AORFB systems. View Full-Text

Keywords: anion exchange membrane; poly (diallylpiperidinium chloride); TMA-TEMPO/MV; aqueous organic redox flow battery; cyclability

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MDPI and ACS Style

Tsehaye, M.T.; Yang, X.; Janoschka, T.; Hager, M.D.; Schubert, U.S.; Alloin, F.; Iojoiu, C. Study of Anion Exchange Membrane Properties Incorporating N-spirocyclic Quaternary Ammonium Cations and Aqueous Organic Redox Flow Battery Performance. Membranes 2021, 11, 367. https://doi.org/10.3390/membranes11050367

AMA Style

Tsehaye MT, Yang X, Janoschka T, Hager MD, Schubert US, Alloin F, Iojoiu C. Study of Anion Exchange Membrane Properties Incorporating N-spirocyclic Quaternary Ammonium Cations and Aqueous Organic Redox Flow Battery Performance. Membranes. 2021; 11(5):367. https://doi.org/10.3390/membranes11050367

Chicago/Turabian Style

Tsehaye, Misgina T., Xian Yang, Tobias Janoschka, Martin D. Hager, Ulrich S. Schubert, Fannie Alloin, and Cristina Iojoiu. 2021. "Study of Anion Exchange Membrane Properties Incorporating N-spirocyclic Quaternary Ammonium Cations and Aqueous Organic Redox Flow Battery Performance" Membranes 11, no. 5: 367. https://doi.org/10.3390/membranes11050367

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Author Biographies

Misgina Tilahun Tsehaye

Dr. Misgina Tilahun Tsehaye studied Erasmus Mundus master in membrane engineering at the Université Toulouse III - Paul Sabatier (Toulouse, France), University of Chemistry and Technology (Prague, Czech Republic), Universidade NOVA de Lisboa (Lisbon, Portugal) and KU Leuven (Leuven, Belgium). He received his Ph.D. degree from the University of Grenoble Alpes in 2021, and is currently a postdoctoral researcher at the Flemish Institute for Technological Research (VITO, Belgium). His research focuses on membrane development for redox flow batteries and fuel cells.

Xian Yang

Xian Yang is an early stage researcher at JenaBatteries GmbH within the FlowCamp project under the European’s Horizon 2020 and a PhD candidate at Friedrich-Schiller-University Jena. She received her Bachelor’s degree in Applied Chemistry and went on study in Chemistry and Physics of Polymers. Her research interests are redox flow batteries (RFBs) and energy storage solutions. She is now focusing on developing compatible materials for organic redox flow batteries and RFB systems.

Tobias Janoschka

Tobias Janoschka studied chemistry (Dipl.) and economics (M. Sc.) at Friedrich Schiller University Jena. During his PhD studies in the research group of Prof. U. S. Schubert, he specialized in organic chemistry and polymer batteries. In 2013, Tobias co-founded JenaBatteries GmbH; a company that develops metal-free redox flow batteries for stationary applications. Today, he leads JenaBatteries’ corporate development activities. In recognition of his contributions towards the field of organic energy storage, including thirty scientific papers as well as several patents, he was awarded the IQ Innovation Award (2015) and the Thuringian Research Prize (2017).

Ulrich S. Schubert

Dr. Fannie Alloin is a CNRS scientist since 1995, DR since 2011. She has worked in the synthesis and characterization of electrolytes and electrolyte/electrode interfaces for electrochemical devices. Her research activities involve the development of innovative electrolytes as well as their physico-chemical, and electrochemical characterizations with the view to understanding their mechanisms and thus propose innovative solutions for future electrochemical generators. More recently, she has broadened her skills in organic positive electrodes. The research is mainly focused on Li-ion battery technology, Li-metal polymer, Li-sulfur, Redox flow battery and Mg battery. Dr. Alloin is the LEPMI Lab director (65 permanent staff members and more than 80 non-permanent) which is one of the leading labs in France on material for energy devices and electrochemistry. She has published 120 peer-reviewed papers and is co-inventor of 21 patents dealing with electrochemical energy sources.

Cristina Iojoiu

Cristina Iojoiu is Senior Research Scientist at National Center for Scientific Research (CNRS) in the Laboratory of Electrochemistry and Physical-chemistry of Materials and Interfaces (LEPMI), Grenoble, France. Her activity is focused on the designing and physicochemical and electrochemical characterization of ionomers, salts, ionic liquids and polymer electrolytes dedicated to energy sources such as: batteries (lithium-polymer, lithium-ion, Ca, Na, redox flow) and fuel cells (protonic and alkaline conducting membranes). She is co-author of >80 peer-reviewed papers and 6 book chapters and co-inventor of 16 patents.

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Study of Anion Exchange Membrane Properties Incorporating N-spirocyclic Quaternary Ammonium Cations and Aqueous Organic Redox Flow Battery Performance

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