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Main Authors: Komander, Kristina, Pálsson, Gunnar K., Droulias, Sotirios A., Tsakiris, Theofanis, Sörme, David, Wolff, Max, Primetzhofer, Daniel
Format: Preprint
Published: 2024
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Online Access:https://arxiv.org/abs/2411.07067
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author Komander, Kristina
Pálsson, Gunnar K.
Droulias, Sotirios A.
Tsakiris, Theofanis
Sörme, David
Wolff, Max
Primetzhofer, Daniel
author_facet Komander, Kristina
Pálsson, Gunnar K.
Droulias, Sotirios A.
Tsakiris, Theofanis
Sörme, David
Wolff, Max
Primetzhofer, Daniel
contents Nanoscaling interstitial metal hydrides offers opportunities for hydrogenation applications by enhancing kinetics, increasing surface area, and allowing for tunable properties. The introduction of interfaces impacts hydrogen absorption properties and distribution heterogeneously, making it however challenging to examine the multiple concurrent mechanisms, especially at the atomic level. Here we demonstrate the effect of proximity on interstitial hydrogen in ultrathin single crystalline vanadium films, by comparing hydride formation in identically strained Fe/V- and Cr/V-superlattices. Pressure concentration and excess resistivity isotherms show higher absolute solubility of hydrogen, higher critical temperature and concentration in the Cr/V-superlattice. Direct measurements of hydrogen site location and thermal vibrations show identical occupation of octahedral z sites at room temperature with a vibrational amplitude of 0.20-0.25 Å over a wide range of hydrogen concentrations. Our findings are consistent with a more extended region of hydrogen depletion in the vicinity of Fe compared to Cr, which showcases an inverse of the hydrogen spillover effect. Advancing the understanding of interface effects resolves previously puzzling differences in the hydrogen loading of Fe/V- and Cr/V-superlattices and is relevant for advancing both catalysis and storage.
format Preprint
id arxiv_https___arxiv_org_abs_2411_07067
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Inverse spillover and dimensionality effects on interstitial hydrogen
Komander, Kristina
Pálsson, Gunnar K.
Droulias, Sotirios A.
Tsakiris, Theofanis
Sörme, David
Wolff, Max
Primetzhofer, Daniel
Materials Science
Nanoscaling interstitial metal hydrides offers opportunities for hydrogenation applications by enhancing kinetics, increasing surface area, and allowing for tunable properties. The introduction of interfaces impacts hydrogen absorption properties and distribution heterogeneously, making it however challenging to examine the multiple concurrent mechanisms, especially at the atomic level. Here we demonstrate the effect of proximity on interstitial hydrogen in ultrathin single crystalline vanadium films, by comparing hydride formation in identically strained Fe/V- and Cr/V-superlattices. Pressure concentration and excess resistivity isotherms show higher absolute solubility of hydrogen, higher critical temperature and concentration in the Cr/V-superlattice. Direct measurements of hydrogen site location and thermal vibrations show identical occupation of octahedral z sites at room temperature with a vibrational amplitude of 0.20-0.25 Å over a wide range of hydrogen concentrations. Our findings are consistent with a more extended region of hydrogen depletion in the vicinity of Fe compared to Cr, which showcases an inverse of the hydrogen spillover effect. Advancing the understanding of interface effects resolves previously puzzling differences in the hydrogen loading of Fe/V- and Cr/V-superlattices and is relevant for advancing both catalysis and storage.
title Inverse spillover and dimensionality effects on interstitial hydrogen
topic Materials Science
url https://arxiv.org/abs/2411.07067