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polymers Article New Insights into Properties of Methanol Transport in Sulfonated Polysulfone Composite Membranes for Direct Methanol Fuel Cells Cataldo Simari 1,* , Isabella Nicotera 1 , Antonino Salvatore Aricò 2, Vincenzo Baglio 2 and Francesco Lufrano 2,* Citation: Simari,C.;Nicotera,I.; Aricò, A.S.; Baglio, V.; Lufrano, F. New Insights into Properties of Methanol Transport in Sulfonated Polysulfone Composite Membranes for Direct Methanol Fuel Cells. Polymers2021,13,1386. https:// doi.org/10.3390/polym13091386 Academic Editor: Dong Jin Yoo Received: 26 March 2021 Accepted: 22 April 2021 Published: 24 April 2021 1 2 * Correspondence: cataldo.simari@unical.it (C.S.); francesco.lufrano@itae.cnr.it (F.L.) Abstract: Methanol crossover through a polymer electrolyte membrane has numerous negative effects on direct methanol fuel cells (DMFCs) because it decreases the cell voltage due to a mixed potential (occurrence of both oxygen reduction and methanol oxidation reactions) at the cathode, lowers the overall fuel utilization and contributes to long-term membrane degradation. In this work, an investigation of methanol transport properties of composite membranes based on sulfonated polysulfone (sPSf) and modified silica filler is carried out using the PFG-NMR technique, mainly focusing on high methanol concentration (i.e., 5 M). The influence of methanol crossover on the performance of DMFCs equipped with low-cost sPSf-based membranes operating with 5 M methanol solution at the anode is studied, with particular emphasis on the composite membrane approach. Using a surface-modified-silica filler into composite membranes based on sPSf allows reducing methanol cross-over of 50% compared with the pristine membrane, making it a good candidate to be used as polymer electrolyte for high energy DMFCs. Keywords: direct methanol fuel cells; PFG-NMR; sulfonated polysulfone; methanol crossover; acidic silica 1. Introduction Direct methanol fuel cells (DMFCs) are envisaged as powerful systems for next gen- eration electronic devices, capable to sustain longer operation compared to Li-batteries without the drawbacks of the time-consuming charging process [1–5]. DMFCs utilize a polymer electrolyte membrane (PEM) as the electrolyte and separator between anode and cathode; the proton conductivity and methanol permeability of this latter are among the key factors limiting the DMFC performance, whereas the membrane cost and durability greatly influence the potential commercialization of complete devices [6–8]. State-of-the-art membranes for DMFCs are based on perfluorosulfonic acid membranes (PFSAs), such as Nafion® membranes, which are used successfully in DMFCs operating with a low methanol concentration (1 or 2 M) at the anode [9,10]. Operation with high methanol concentration produces high methanol permeation through the membrane, from the anode to the cathode, leading to a loss of fuel efficiency in the DMFC together with a mixed potential at the cathode with a consequent decrease of cell voltage, unless a cathodic catalyst tolerant to the alcohol is used [9,11,12]. Consequently, the research on new proton exchange membranes is mandatory not only to reduce the methanol permeation while maintaining a good proton conductivity, but also to reduce the cost compared to the expensive PFSA membranes. A series of different strategies are currently pursued to find polymer electrolytes able to replace PFSA membranes, maintaining or improving the performance of the DMFC, also Department of Chemistry and Chemical Technologies, University of Calabria, 87036 Arcavacata di Rende (CS), Italy; isabella.nicotera@unical.it CNR-ITAE, Istituto di Tecnologie Avanzate per l’Energia “Nicola Giordano”, Via Salita S. Lucia sopra Contesse n., 5-98126 S. Lucia-Messina, Italy; antonino.arico@itae.cnr.it (A.S.A.); vincenzo.baglio@itae.cnr.it (V.B.) Publisher’s Note: MDPI stays neutral with regard to jurisdictional claims in published maps and institutional affil- iations. Copyright: © 2021 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https:// creativecommons.org/licenses/by/ 4.0/). Polymers 2021, 13, 1386. https://doi.org/10.3390/polym13091386 https://www.mdpi.com/journal/polymersPDF Image | Properties of Methanol Transport for Direct Methanol Fuel Cells
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