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Tuning reactivity layer-by-layer: formic acid activation on Ag/Pd(111).

Mustafa Karatok1, Kaining Duanmu2, Christopher R O'Connor1

  • 1Department of Chemistry and Chemical Biology, Harvard University Cambridge MA 02138 USA friend@fas.harvard.edu.

Chemical Science
|June 7, 2021
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Summary

A single atomic layer of silver on palladium exhibits unique reactivity for formic acid decomposition, crucial for hydrogen fuel production. This enhanced catalytic activity is layer-specific, highlighting the importance of precise material control.

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Area of Science:

  • Materials Science
  • Surface Science
  • Catalysis

Background:

  • Ultrathin metal films offer tunable electronic structures for heterogeneous catalysis.
  • Controlling material properties is key to enhancing reactivity and selectivity.
  • Formic acid decomposition is vital for hydrogen (H2) generation in fuel cells.

Purpose of the Study:

  • To investigate the reactivity of a 1-atomic layer silver (Ag) film on palladium (Pd(111)) towards formic acid.
  • To compare the catalytic behavior of ultrathin Ag films with bulk Ag.
  • To understand the role of electronic structure modification in catalytic performance.

Main Methods:

  • Infrared reflection absorption spectroscopy (IRRAS) for surface analysis.
  • X-ray photoelectron spectroscopy (XPS) for electronic structure determination.
  • Density functional theory (DFT) calculations to model the system.

Main Results:

  • A 1-atomic layer Ag/Pd(111) film shows significant reactivity towards formic acid below room temperature, unlike bulk Ag.
  • Two-monolayer Ag films exhibit unreactive behavior, reverting to bulk Ag properties.
  • The Ag monolayer is continuous and electronically modified compared to bulk Ag, confirmed by spectroscopy and DFT.

Conclusions:

  • The electronic structure of Ag monolayers on Pd(111) is altered, leading to distinct catalytic reactivity.
  • Enhanced reactivity is observed only for the first atomic layer, emphasizing the need for precise material engineering.
  • This study demonstrates the potential of ultrathin films for tailored catalytic applications.