Selective Hydrogen Production from Formic Acid Decomposition on Pd鈥揂u Bimetallic Surfaces
详细信息 查看全文
- 作者：Wen-Yueh Yu ; Gregory M. Mullen ; David W. Flaherty ; C. Buddie Mullins
- 刊名：Journal of the American Chemical Society
- 出版年：2014
- 出版时间：August 6, 2014
- 年：2014
- 卷：136
- 期：31
- 页码：11070-11078
- 全文大小：443K
- ISSN：1520-5126
文摘
Pd鈥揂u 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鈥揂u bimetallic surfaces for HCOOH decomposition. Our results show that Pd atoms at the Pd鈥揂u 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鈥揂u 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鈥揂u 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鈥揂u catalysts for associated reactions including selective HCOOH decomposition for hydrogen production and electro-oxidation of HCOOH in the direct formic acid fuel cell.