학술논문

Facilitating hydrogen atom migration via a dense phase on palladium islands to a surrounding silver surface
Document Type
article
Source
Proceedings of the National Academy of Sciences of the United States of America. 117(37)
Subject
Inorganic Chemistry
Chemical Sciences
Physical Sciences
hydrogen spillover
palladium
silver
adsorbate migration
Language
Abstract
The migration of species across interfaces can crucially affect the performance of heterogeneous catalysts. A key concept in using bimetallic catalysts for hydrogenation is that the active metal supplies hydrogen atoms to the host metal, where selective hydrogenation can then occur. Herein, we demonstrate that, following dihydrogen dissociation on palladium islands, hydrogen atoms migrate from palladium to silver, to which they are generally less strongly bound. This migration is driven by the population of weakly bound states on the palladium at high hydrogen atom coverages which are nearly isoenergetic with binding sites on the silver. The rate of hydrogen atom migration depends on the palladium-silver interface length, with smaller palladium islands more efficiently supplying hydrogen atoms to the silver. This study demonstrates that hydrogen atoms can migrate from a more strongly binding metal to a more weakly binding surface under special conditions, such as high dihydrogen pressure.