Estimating Bulk-Composition-Dependent H₂ Adsorption Energies on Cu_xPd_1–x Alloy (111) Surfaces

Abstract

The bulk-composition-dependent dissociative adsorption energy of hydrogen on CuPd alloys has been measured experimentally and modeled using density functional theory. The hydrogen adsorption energy cannot be simply defined by a single reactive site or as a composition weighted average of the pure metal components. We developed a modeling approach that uses a basis of active sites weighted by a model site probability distribution to estimate a bulk-composition-dependent adsorption energy. The approach includes segregation under reaction conditions. With this method, we can explain the composition-dependent adsorption energy of hydrogen on Cu-rich alloy surfaces. In Pd-rich alloys, a Pd-hydride phase may form, which results in deviations from trends on the metallic alloy surface.

High‐throughput methods using composition and structure spread libraries

“…The microreactor was used in two recent studies that examined the reactivity of a Cu x Pd 1– x CSAF for H 2 ‐D 2 exchange . In that work, the conversion of H 2 to HD was measured at 100 locations on the CSAF as a function of temperature (300–600 K).…”

“…Above x Pd = 0.40, however, this trend ceased, with adsorption barriers becoming independent of Pd composition. To investigate this phenomenon, we developed a novel approach to modeling composition spread alloy surfaces using density functional theory . We found that the region of near linear decrease in adsorption barriers with lower values than suggested by linear interpolation of the pure component values, x Pd < 0.40 were readily explained by hydrogen‐induced segregation of Pd to the surface.…”

Examples of Effective Data Sharing in Scientific Publishing

“…We will provide an example of this for a paper we recently published in ACS Catalysis on "Estimating Bulk-Composition-Dependent H 2 Adsorption Energies on Cu x Pd 1−x Alloy (111) Surfaces". 11 The Supporting Information file for that article is available for free. 12 When opened in a PDF reader that supports attachments, one can see that there are attachments (see Figure 1 a).…”

“…11 The Supporting Information file for that article is available for free. 12 When opened in a PDF reader that supports attachments, one can see that there are attachments (see Figure 1 a). Alternatively, while reading the PDF file, the reader is alerted that there is an attachment by the presence of a thumbtack icon (Figure 1 b), which can be double clicked to open the file.…”

Data sharing in Surface Science

“…Through scripting, one could recreate the actual The key point here is that the data was read by a computer from the 146 supporting information file, and then reused to create a new figure. We 147 have used this approach to embed both computational and experimen-148 tal temperature programmed desorption data in supporting informa-149 tion [25], and experimental reactivity and segregation data [30,31].…”