H–D Exchange Mechanism of Butene on a D‑Absorbed Pd–Au Alloy Surface

Complete H–D exchange of butene was reported on a D-absorbed Pd–Au alloy surface. However, its reaction mechanism has not been clarified yet. Here we investigate the reaction of cis-2- and 1-butene on Pd70Au30(110) by means of high-resolution electron energy loss spectroscopy. We demonstrate that bo...

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Veröffentlicht in:Journal of physical chemistry. C 2019-04, Vol.123 (13), p.7854-7860
Hauptverfasser: Ogura, Shohei, Ohno, Satoshi, Mukai, Kozo, Yoshinobu, Jun, Fukutani, Katsuyuki
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Sprache:eng
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Zusammenfassung:Complete H–D exchange of butene was reported on a D-absorbed Pd–Au alloy surface. However, its reaction mechanism has not been clarified yet. Here we investigate the reaction of cis-2- and 1-butene on Pd70Au30(110) by means of high-resolution electron energy loss spectroscopy. We demonstrate that both butene isomers are in the π-bonded state and that 1-butene irreversibly converts to cis-2-butene around 250 K. This isomerization accounts for previously observed similar product distributions in the H–D exchange reaction of cis-2- and 1-butene on the D-absorbed Pd70Au30(110) surface. Since the reverse change from cis-2- to 1-butene is not observed at any temperature, we conclude that the H–D exchange proceeds by the dissociative mechanism via vinylic and π-allylic intermediates rather than the Horiuti–Polanyi mechanism.
ISSN:1932-7447
1932-7455
DOI:10.1021/acs.jpcc.8b06964