Proton
chemistry is a fascinating field with both fundamental and
applied aspects. The development of solid-state proton conductors
relying on abundant elements could help bring these two aspects. In
this scope, we synthesized a disordered structure which, as revealed
by the real-space refinement of the pair distribution function, has
been identified to be the trititanate arrangement. The layered structure
is stabilized by the presence of hydronium ions and water molecules
located in the interlayer space. This compound displays a high ionic
conductivity of 4·10–2 S/m with an activation
energy of 0.24 eV, assigned to H+ mobility as shown by
broadband dielectric spectroscopy. Proton mobility was further evidenced
by solid-state proton nuclear magnetic resonance. Density functional
theory calculations revealed that proton transfer occurs both within
the interlayer space and with terminal oxide of the titanate framework
through a Grotthuss-based mechanism rationalizing the high conductivity
measured experimentally. Finally, we investigated the electrochemical
properties with respect to the proton as a charge carrier using proton-free
(KCl) and proton-donor (buffer acetic acid) electrolytes. The results
showed that the structure can reversibly intercalate protons at a
very high rate opening existing perspectives in the development of
negative electrode materials for aqueous proton batteries. Overall,
this study helps better understand the proton transfer mechanism occurring
in a confined layered-type structure.
Heteroepitaxial Y2O3 films were grown on Si(100) substrates by the technique of reactive ionized cluster beam deposition. The crystallinity of the films was investigated with reflection high energy electron diffraction (RHEED), glancing angle x-ray diffraction (GXRD), and the interface was examined by high resolution transmission electron microscopy (HRTEM). Under the condition of 5 kV acceleration voltage at the substrate temperature of 800 °C, the Y2O3 film grows epitaxially on the Si(100) substrate. RHEED and GXRD results revealed that the epitaxial relationship between Y2O3 and Si(100) is Y2O3(110)//Si(100), and HRTEM observation showed a sharp interface without an amorphous layer.
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