A magnetic resonance and electrochemical study of the role of polymer mobility in supporting hydrogen transport in perfluorosulfonic acid membranes

Literature Information

Publication Date 2018-06-25
DOI 10.1039/C8CP02676A
Impact Factor 3.676
Authors

Z. Blossom Yan, Alan P. Young, Gillian R. Goward


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Abstract

Perfluorosulfonic acid (PFSA) materials have been used in polymer electrolyte membrane fuel cells (PEMFCs) as electrolyte materials due to their mechanical durability and high proton conductivity. To understand the fundamental chemistry at a molecular level in material performance properties, we have developed and validated method for evaluating local dynamics using 19F double-quantum solid-state nuclear magnetic resonance (ssNMR) spectroscopy. The local dynamics information can be separated and analyzed in terms of fluorine interactions with respect to the different temperatures and hydration levels. The polymer side chain is proven to be more locally mobile which is reflected by the lower apparent dipolar coupling constant (Dapp) compared to the backbone. This observation agrees with the micro-phase separation morphology evolution. In the current study, different types of PFSA materials were explored and compared. The dynamics investigation of the PFSA materials has been conducted at various conditions. In operando membrane performance analyses were performed in parallel at Ballard Power Systems. PFSA membranes were prepared into membrane electrode assemblies (MEAs), with catalyst layers and gas diffusion layers. From the cyclic voltammetry measurements, the H2 crossover values were extracted. These data reveal a strong correlation between the proton conductivity and the site-specific PFSA side chain local dynamics. Moreover, a correlation was drawn between increasing side chain mobility (lower Dapp), and increased H2 permeability. The link between the fundamental dynamics study and this key PFSA performance analysis provides insight into proton transport mechanisms.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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