Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 115, Issue 31, Pages 7896-7900Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1800412115
Keywords
hydrogen; Pd-Au alloy; thermal desorption spectroscopy; nuclear reaction analysis; angle-resolved photoemission spectroscopy
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Funding
- Japan Society for the Promotion of Sciences (JSPS KAKENHI) [JP16K04957, JP17K19048, JP18H05518]
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Enhancement of hydrogen (H) absorption kinetics improves the performance of hydrogen-purifying membranes and hydrogenstorage materials, which is necessary for utilizing hydrogen as a carbon-free energy carrier. Pd-Au alloys are known to show higher hydrogen solubility than pure Pd. However, the effect of Au on the hydrogen penetration from the surface into the subsurface region has not been clarified so far. Here, we investigate the hydrogen absorption at Pd-Au surface alloys on Pd(110) by means of thermal desorption spectroscopy (TDS) and hydrogen depth profiling with nuclear reaction analysis (NRA). We demonstrate that alloying the Pd(110) surface with submonolayer amounts of Au dramatically accelerates the hydrogen absorption. The degree of acceleration shows a volcano-shaped form against Au coverage. This kinetic enhancement is explained by a reduced penetration barrier mainly caused by a destabilization of chemisorbed surface hydrogen, which is supported by density-functional-theory (DFT) calculations. The destabilization of chemisorbed surface hydrogen is attributed to the change of the surface electronic states as observed by angle-resolved photoemission spectroscopy (ARPES). If generalized, these discoveries may lead to improving and controlling the hydrogen transport across the surfaces of hydrogenabsorbing materials.
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