Selective hydrogen production from formic acid decomposition on Pd-Au bimetallic surfaces

Wen Yueh Yu, Gregory M. Mullen, David W. Flaherty, C. Buddie Mullins

Research output: Contribution to journalArticlepeer-review

Abstract

Pd-Au catalysts have shown exceptional performance for selective hydrogen production via HCOOH decomposition, a promising alternative to solve issues associated with hydrogen storage and distribution. In this study, we utilized temperature-programmed desorption (TPD) and reactive molecular beam scattering (RMBS) in an attempt to unravel the factors governing the catalytic properties of Pd-Au bimetallic surfaces for HCOOH decomposition. Our results show that Pd atoms at the Pd-Au surface are responsible for activating HCOOH molecules; however, the selectivity of the reaction is dictated by the identity of the surface metal atoms adjacent to the Pd atoms. Pd atoms that reside at Pd-Au interface sites tend to favor dehydrogenation of HCOOH, whereas Pd atoms in Pd(111)-like sites, which lack neighboring Au atoms, favor dehydration of HCOOH. These observations suggest that the reactivity and selectivity of HCOOH decomposition on Pd-Au catalysts can be tailored by controlling the arrangement of surface Pd and Au atoms. The findings in this study may prove informative for rational design of Pd-Au catalysts for associated reactions including selective HCOOH decomposition for hydrogen production and electro-oxidation of HCOOH in the direct formic acid fuel cell.

Original languageEnglish (US)
Pages (from-to)11070-11078
Number of pages9
JournalJournal of the American Chemical Society
Volume136
Issue number31
DOIs
StatePublished - Aug 6 2014

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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