Probing Active Sites in CuxPdy Cluster Catalysts by Machine-Learning-Assisted X-ray Absorption Spectroscopy
Abstract
Size selected clusters are important model catalysts due to their narrow size and compositional distributions, as well as enhanced activity and selectivity in many reactions. Still, their structureactivity relationships are, in general, elusive. The main reason is the difficulty to identify and quantitatively characterize 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.
- Authors:
-
[1];
[3];
[4]
- Stony Brook Univ., NY (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States); Czech Academy of Sciences, Prague (Czech Republic)
- Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1839972
- Alternate Identifier(s):
- OSTI ID: 1854091
- Report Number(s):
- BNL-222823-2022-JAAM
Journal ID: ISSN 1944-8244; 169678
- Grant/Contract Number:
- AC02-06CH11357; SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 45; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nanocatalysts; nanoclusters; size-selected clusters; machine learning; deep learning; XANES; palladium; X-ray absorption near edge spectroscopy; metal clusters; catalysts; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
Citation Formats
Liu, Yang, Halder, Avik, Seifert, Soenke, Marcella, Nicholas, Vajda, Stefan, and Frenkel, Anatoly I. Probing Active Sites in CuxPdy Cluster Catalysts by Machine-Learning-Assisted X-ray Absorption Spectroscopy. United States: N. p., 2021.
Web. doi:10.1021/acsami.1c06714.
Liu, Yang, Halder, Avik, Seifert, Soenke, Marcella, Nicholas, Vajda, Stefan, & Frenkel, Anatoly I. Probing Active Sites in CuxPdy Cluster Catalysts by Machine-Learning-Assisted X-ray Absorption Spectroscopy. United States. https://doi.org/10.1021/acsami.1c06714
Liu, Yang, Halder, Avik, Seifert, Soenke, Marcella, Nicholas, Vajda, Stefan, and Frenkel, Anatoly I. Tue .
"Probing Active Sites in CuxPdy Cluster Catalysts by Machine-Learning-Assisted X-ray Absorption Spectroscopy". United States. https://doi.org/10.1021/acsami.1c06714. https://www.osti.gov/servlets/purl/1839972.
@article{osti_1839972,
title = {Probing Active Sites in CuxPdy Cluster Catalysts by Machine-Learning-Assisted X-ray Absorption Spectroscopy},
author = {Liu, Yang and Halder, Avik and Seifert, Soenke and Marcella, Nicholas and Vajda, Stefan and Frenkel, Anatoly I.},
abstractNote = {Size selected clusters are important model catalysts due to their narrow size and compositional distributions, as well as enhanced activity and selectivity in many reactions. Still, their structureactivity relationships are, in general, elusive. The main reason is the difficulty to identify and quantitatively characterize 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.},
doi = {10.1021/acsami.1c06714},
journal = {ACS Applied Materials and Interfaces},
number = 45,
volume = 13,
place = {United States},
year = {Tue Jul 13 00:00:00 EDT 2021},
month = {Tue Jul 13 00:00:00 EDT 2021}
}
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