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Title: Evolution of Active Sites in Pt-Based Nanoalloy Catalysts for the Oxidation of Carbonaceous Species by Combined in Situ Infrared Spectroscopy and Total X-ray Scattering

Abstract

Here, we present results from combined in situ infrared spectroscopy and total X-ray scattering studies on the evolution of catalytically active sites in exemplary binary and ternary Pt-based nanoalloys during a sequence of CO oxidation–reactivation–CO oxidation reactions. We find that when within a particular compositional range, the fresh nanoalloys may exhibit high catalytic activity for low-temperature CO oxidation. Using surface-specific atomic pair distribution functions (PDFs) extracted from the in situ total X-ray scattering data, we find that, regardless of their chemical composition and initial catalytic activity, the fresh nanoalloys suffer a significant surface structural disorder during CO oxidation. Upon reactivation in oxygen atmosphere, the surface of used nanoalloy catalysts both partially oxidizes and orders. Remarkably, it largely retains its structural state when the nanoalloys are reused as CO oxidation catalysts. The seemingly inverse structural changes of studied nanoalloy catalysts occurring under CO oxidation and reactivation conditions affect the active sites on their surface significantly. In particular, through different mechanisms, both appear to reduce the CO binding strength to the nanoalloy’s surface and thus increase the catalytic stability of the nanoalloys. The findings provide clues for further optimization of nanoalloy catalysts for the oxidation of carbonaceous species through optimizing their composition,more » activation, and reactivation. Besides, the findings demonstrate the usefulness of combined in situ infrared spectroscopy and total X-ray scattering coupled to surface-specific atomic PDF analysis to the ongoing effort to produce advanced catalysts for environmentally and technologically important applications.« less

Authors:
ORCiD logo [1];  [1];  [2];  [2];  [2];  [2];  [2]; ORCiD logo [2];  [3]; ORCiD logo [3]
  1. Central Michigan Univ., Mount Pleasant, MI (United States). Dept. of Physics and Science of Advanced Materials Program
  2. State Univ. of New York (SUNY), Binghamton, NY (United States). Dept. of Chemistry
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS) and X-ray Science Division
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1462711
Grant/Contract Number:  
AC02-06CH11357; SC0006877; CHE 1566283
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 13; 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; 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; CO Oxidation; DRIAD-X; DRIFTS; in situ infrared spectroscopy; metallic nanoalloy catalysis; surface atomic structure; total X-ray scattering; thermochemical treatment

Citation Formats

Petkov, Valeri, Maswadeh, Yazan, Lu, Aolin, Shan, Shiyao, Kareem, Haval, Zhao, Yinguang, Luo, Jin, Zhong, Chuan-Jian, Beyer, Kevin, and Chapman, Karena. Evolution of Active Sites in Pt-Based Nanoalloy Catalysts for the Oxidation of Carbonaceous Species by Combined in Situ Infrared Spectroscopy and Total X-ray Scattering. United States: N. p., 2018. Web. doi:10.1021/acsami.7b19574.
Petkov, Valeri, Maswadeh, Yazan, Lu, Aolin, Shan, Shiyao, Kareem, Haval, Zhao, Yinguang, Luo, Jin, Zhong, Chuan-Jian, Beyer, Kevin, & Chapman, Karena. Evolution of Active Sites in Pt-Based Nanoalloy Catalysts for the Oxidation of Carbonaceous Species by Combined in Situ Infrared Spectroscopy and Total X-ray Scattering. United States. doi:10.1021/acsami.7b19574.
Petkov, Valeri, Maswadeh, Yazan, Lu, Aolin, Shan, Shiyao, Kareem, Haval, Zhao, Yinguang, Luo, Jin, Zhong, Chuan-Jian, Beyer, Kevin, and Chapman, Karena. Tue . "Evolution of Active Sites in Pt-Based Nanoalloy Catalysts for the Oxidation of Carbonaceous Species by Combined in Situ Infrared Spectroscopy and Total X-ray Scattering". United States. doi:10.1021/acsami.7b19574. https://www.osti.gov/servlets/purl/1462711.
@article{osti_1462711,
title = {Evolution of Active Sites in Pt-Based Nanoalloy Catalysts for the Oxidation of Carbonaceous Species by Combined in Situ Infrared Spectroscopy and Total X-ray Scattering},
author = {Petkov, Valeri and Maswadeh, Yazan and Lu, Aolin and Shan, Shiyao and Kareem, Haval and Zhao, Yinguang and Luo, Jin and Zhong, Chuan-Jian and Beyer, Kevin and Chapman, Karena},
abstractNote = {Here, we present results from combined in situ infrared spectroscopy and total X-ray scattering studies on the evolution of catalytically active sites in exemplary binary and ternary Pt-based nanoalloys during a sequence of CO oxidation–reactivation–CO oxidation reactions. We find that when within a particular compositional range, the fresh nanoalloys may exhibit high catalytic activity for low-temperature CO oxidation. Using surface-specific atomic pair distribution functions (PDFs) extracted from the in situ total X-ray scattering data, we find that, regardless of their chemical composition and initial catalytic activity, the fresh nanoalloys suffer a significant surface structural disorder during CO oxidation. Upon reactivation in oxygen atmosphere, the surface of used nanoalloy catalysts both partially oxidizes and orders. Remarkably, it largely retains its structural state when the nanoalloys are reused as CO oxidation catalysts. The seemingly inverse structural changes of studied nanoalloy catalysts occurring under CO oxidation and reactivation conditions affect the active sites on their surface significantly. In particular, through different mechanisms, both appear to reduce the CO binding strength to the nanoalloy’s surface and thus increase the catalytic stability of the nanoalloys. The findings provide clues for further optimization of nanoalloy catalysts for the oxidation of carbonaceous species through optimizing their composition, activation, and reactivation. Besides, the findings demonstrate the usefulness of combined in situ infrared spectroscopy and total X-ray scattering coupled to surface-specific atomic PDF analysis to the ongoing effort to produce advanced catalysts for environmentally and technologically important applications.},
doi = {10.1021/acsami.7b19574},
journal = {ACS Applied Materials and Interfaces},
issn = {1944-8244},
number = 13,
volume = 10,
place = {United States},
year = {2018},
month = {3}
}

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