Abstract

The energy efficiency of heterogeneous catalytic processes may be improved by using mid-infrared light to excite gas-phase reactants during the reaction, since vibrational excitation of molecules has been shown to increase their reactivity at the gas-catalyst interface. A primary challenge for such light-enabled catalysis is the need to ensure close coupling between light-excited molecules and the catalyst throughout the reactor. Thus, it is imperative to understand how to couple infrared light efficiently to molecules near and inside catalytic material. Heterogenous catalysts are often nanoscale metal particles supported on high surface area, porous oxide materials and exhibit feature sizes across multiple scattering regimes with respect to the mid-infrared wavelength. These complex powders make a direct measurement of the scattering properties challenging. Here, we demonstrate that a combination of directional hemispherical measurements along with the in-line transmission measurement allow for a direct measurement of the scattered light signal. We implement this technique to study the scattering behavior of the catalytic support material γ-Al2O3 (with and without metal loading) between 1040 and 1220 cm−1. We first study how both the mean grain size affects the scattering behavior by comparing three different mean grain sizes spanning three orders of magnitude (2, 40, and 900 µm). Furthermore, we study how the addition of metal catalyst nanoparticles, Ru, or Cu, to the support material impacts the light scattering behavior of the powder. We find that the 40 µm grain size scatters the most (up to 97% at 1220 cm−1) and that the addition of metal nanoparticles narrows the scattering angle but does not decrease the scattering efficiency. The strong scattering of the 40 µm grains makes them the most ideal support material of those studied for the given spectrum because of their ability to distribute light within the reactor. Finally, we estimate that less than 100 mW of laser power is needed to cause significant excitation for testing mid-infrared catalysis in a Harrick Praying Mantis diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reactor, a magnitude easily available using commercial mid-infrared lasers. Our work also provides a mid-infrared foundation for a wide range of studies of light-enabled catalysis and can be extended to other wavelengths of light or to study the scattering behavior of other complex powders in other fields, including ceramics, biomaterials, and geology.

Original languageEnglish (US)
JournalApplied Spectroscopy
DOIs
StateAccepted/In press - 2021

All Science Journal Classification (ASJC) codes

  • Instrumentation
  • Spectroscopy

Keywords

  • Mid-infrared
  • catalysis
  • directional-hemispherical measurement
  • infrared extinction in powders
  • inhomogenous powders
  • scattering

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