Complete H-D Exchange of Butene via D Absorbed in a Pd-Au Alloy

作者：Ogura Shohei^*; Okada Michio; Fukutani Katsuyuki

来源：Journal of Physical Chemistry C, 2015, 119(42): 23973-23977.

DOI：10.1021/acs.jpcc.5b07216

The H-D exchange reaction is one of the easiest ways to synthesize deuterium-labeled compounds. H-D exchange of olefins has been widely studied on metal surfaces such as Pd and Pt. However, H-D exchange of butene on these surfaces is hardly completed and always accompanied by hydrogenation or dehydrogenation, and its reaction mechanism is yet to be elucidated. In the present study, we investigated the reaction of cis-2- and 1-butenes with H and D atoms absorbed in the near-surface region of Pd70Au30(110) by using thermal desorption spectroscopy (TDS), reflection absorption infrared spectroscopy (RAIRS), and TDS simulation. We show complete H-D exchange of both butene isomers without hydrogenation and dehydrogenation. Similar product yield distributions for both butene isomers indicate a fast di-sigma bond migration on this surface, which is a key for the complete H-D exchange. Our results would lead to understanding and controlling the catalytic activity and selectivity of the Pd-Au alloy and Pd-related surfaces and would open up a new chemistry using absorbed hydrogen in combination with alloyed surfaces.

• 出版日期2015-10-22