Neutron scattering for sustainable energy materials: investigations of proton dynamics in acceptor doped barium zirconates
Doctoral thesis, 2018
The results show a complex dynamics, arising from a distribution of different proton sites, a consequence of a disordered structure of the materials. Analysis of the short time scale dynamics discloses localized dynamics interpretable as proton jumps and reorientations of the hydroxyl groups. Faster local motions are observed in more distorted structures associated with higher doping levels, whereas no substantial differences are observed for different dopant ions. Analysis of the long time scale dynamics reveals long-range diffusion of protons, which can be described as a jump-diffusion process. Higher dopant concentrations lead to higher activation energies, still well below those for macroscopic proton conductivities, but larger fractions of mobile protons.
This new insight adds to the previous knowledge of proton dynamics in perovskite materials and can be useful to develop strategies for the design of improved proton conductors for technological applications
neutron scattering
fuel cells
QENS
Proton conductors
perovskites
proton dynamics
energy materials
Author
Daria Noferini
Chalmers, Physics, Condensed Matter Physics
Institut Laue-Langevin
Proton Dynamics in Hydrated BaZr0.9M0.1O2.95 (M = Y and Sc) Investigated with Neutron Spin-Echo
Journal of Physical Chemistry C,;Vol. 120(2016)p. 13963-13969
Journal article
Localized Proton Motions in Acceptor-Doped Barium Zirconates
Journal of Physical Chemistry C,;Vol. 121(2017)p. 7088-7093
Journal article
D. Noferini, M. M. Koza, G. J. Nilsen, and M. Karlsson, Study of the Hydration Level in Proton Conducting Oxides Using Neutron Diffraction with Polarization Analysis.
Role of the doping level in localized proton motions in acceptor-doped barium zirconate proton conductors
Physical Chemistry Chemical Physics,;Vol. 20(2018)p. 13697-13704
Journal article
Proton jump diffusion dynamics in hydrated barium zirconates studied by high-resolution neutron backscattering spectroscopy
Journal of Materials Chemistry A,;Vol. 6(2018)p. 7538-7546
Journal article
Hydrogen fuel cells are among the most important devices for energy conversion. However, to bring them into our everyday life, the challenge is to combine the advantages of a solid state conducting material with those of lowered operational temperatures (present ones are above 750 °C). A promising strategy to reach this goal is to use proton conducting oxides. Yet, a deep understanding of the proton conduction mechanism, that is how the protons move across the materials, is essential to design new conductors that meet the required properties for applications. To this aim, samples of barium zirconates, which are among the most promising proton conducting oxides, were experimentally characterized in this thesis using neutron scattering. With this technique it is possible to investigate both the structure (how the atoms are arranged) and dynamics (how the atoms move) of materials, by comparing the properties of a beam composed of neutrons before and after the collision with the sample. The obtained results provide important details to define a general mechanism of proton conduction and to understand how the fine tuning of the composition affects the performance of the proton conducting oxides. The new knowledge thus contribute to the further development of these materials and their applications.
Driving Forces
Sustainable development
Subject Categories
Ceramics
Materials Chemistry
Other Materials Engineering
Areas of Advance
Energy
Materials Science
Roots
Basic sciences
ISBN
978-91-7597-709-6
Doktorsavhandlingar vid Chalmers tekniska högskola. Ny serie: 4390
Publisher
Chalmers
Lecture Hall KA, House Chemistry, Kemigården 4
Opponent: Roberto Senesi, Dipartimento di Fisica, Università degli Studi di Roma Tor Vergata, Italy