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@ARTICLE{berrck:859820,
author = {Überrück, Till and Neudert, Oliver and Kreuer,
Klaus-Dieter and Blümich, Bernhard and Granwehr, Josef and
Stapf, Siegfried and Han, Songi},
title = {{E}ffect of nitroxide spin probes on the transport
properties of {N}afion membranes},
journal = {Physical chemistry, chemical physics},
volume = {20},
number = {41},
issn = {1463-9084},
address = {Cambridge},
publisher = {RSC Publ.66479},
reportid = {FZJ-2019-00651},
pages = {26660 - 26674},
year = {2018},
abstract = {Nafion is the most common material used as a proton
exchange membrane in fuel cells. Yet, details of the
transport pathways for protons and water in the inner
membrane are still under debate. Overhauser Dynamic Nuclear
Polarization (ODNP) has proven to be a useful tool for
probing hydration dynamics and interactions within 5–8 Å
of protein and soft material surfaces. Recently it was
suggested that ODNP can also be applied to analyze surface
water dynamics along Nafion's inner membrane. Here we
interrogate the viability of this method for Nafion by
carrying out a series of measurements relying on 1H nuclear
magnetic resonance (NMR) relaxometry and diffusometry
experiments with and without ODNP hyperpolarization,
accompanied by other complementary characterization methods
including small angle X-ray scattering (SAXS), thermal
gravimetric analysis (TGA) of hydration, and proton
conductivity by AC impedance spectroscopy. Our comprehensive
study shows that commonly used paramagnetic spin
probes—here, stable nitroxide radicals—for ODNP, as well
as their diamagnetic analogues, reduce the inner membrane
surface hydrophilicity, depending on the location and
concentration of the spin probe. This heavily reduces the
hydration of Nafion, hence increases the tortuosity of the
inner membrane morphology and/or increases the activiation
barrier for water transport, and consequently impedes water
diffusion, transport, and proton conductivity.},
cin = {IEK-9},
ddc = {540},
cid = {I:(DE-Juel1)IEK-9-20110218},
pnm = {135 - Fuel Cells (POF3-135)},
pid = {G:(DE-HGF)POF3-135},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:30320331},
UT = {WOS:000448665900063},
doi = {10.1039/C8CP04607G},
url = {https://juser.fz-juelich.de/record/859820},
}