Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 136, Issue 31, Pages 11070-11078Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja505192v
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Funding
- Department of Energy [DE-FG02-04ER15587]
- Welch Foundation [F-1436]
- National Science Foundation
- U.S. Department of Energy (DOE) [DE-FG02-04ER15587] Funding Source: U.S. Department of Energy (DOE)
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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.
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