American Chemical Society
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Probing Active Sites in CuxPdy Cluster Catalysts by Machine-Learning-Assisted X‑ray Absorption Spectroscopy

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journal contribution
posted on 2021-07-13, 16:15 authored by Yang Liu, Avik Halder, Soenke Seifert, Nicholas Marcella, Stefan Vajda, Anatoly I. Frenkel
Size-selected clusters are important model catalysts because of their narrow size and compositional distributions, as well as enhanced activity and selectivity in many reactions. Still, their structure–activity relationships are, in general, elusive. The main reason is the difficulty in identifying and quantitatively characterizing the catalytic active site in the clusters when it is confined within subnanometric dimensions and under the continuous structural changes the clusters can undergo in reaction conditions. Using machine learning approaches for analysis of the operando X-ray absorption near-edge structure spectra, we obtained accurate speciation of the CuxPdy cluster types during the propane oxidation reaction and the structural information about each type. As a result, we elucidated the information about active species and relative roles of Cu and Pd in the clusters.