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Title: Single-site Pt/La-Al 2O 3 stabilized by barium as an active and stable catalyst in purifying CO and C 3H 6 emissions

Abstract

High-temperature operations present a substantial challenge for developing industrial-capable precious metal catalysts (e.g. Pt/alumina), where the scarce metal atoms easily become wasted as sintered nanoparticles. Using fully dispersed precious metal atoms to deliver the catalysis remains an elusive goal. On a widely used La-stabilized alumina support, we find that the atomically dispersed Pt 1(II)-O x- species, rather than the much more visible large metal particles, are the actual catalytic sites for the CO and C 3H 6 oxidation reactions. Unfortunately, the La dopants in alumina support will not hinder the sintering of the active Pt1(II)-Ox- species. As a natural next step, the Ba-Ox- species were introduced to specifically stabilize the single-atom Pt on the La-stabilized alumina support. By implementing this improved formulation, the atomically dispersed Pt on alumina retains the original full dispersion even after 650 °C hydrothermal aging. Intriguingly, with or without the barium additives and/or sintered platinum particles in the catalysts, the intrinsic activity per Pt atom stays intact. Along with other experimental evidence, this leads to the finding that the single-atom Pt is the true catalytic site for the oxidation of CO and C 3H 6 in the widely-used Pt/La-Al 2O 3 material system. This work providesmore » a new perspective for efficient precious metal utilization under demanding catalytic conditions.« less

Authors:
 [1];  [1];  [2];  [3];  [4];  [1];  [4];  [1];  [4]
  1. Tianjin Univ., Tianjin (China). School of Chemical Engineering & Technology
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  3. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  4. General Motors Global Research and Development, Warren, MI (United States). Chemical and Materials Systems Lab.
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); General Motors, R&D, Warren, MI (United States); National Key Research and Development Program of China
OSTI Identifier:
1492696
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Applied Catalysis B: Environmental
Additional Journal Information:
Journal Volume: 244; Journal Issue: C; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Alumina; Emissions purification; High-temperature stability; Platinum; Single-atom catalyst

Citation Formats

Wang, Hui, Dong, Jinshi, Allard, Lawrence F., Lee, Sungsik, Oh, Se, Wang, Jun, Li, Wei, Shen, Meiqing, and Yang, Ming. Single-site Pt/La-Al2O3 stabilized by barium as an active and stable catalyst in purifying CO and C3H6 emissions. United States: N. p., 2018. Web. doi:10.1016/j.apcatb.2018.11.034.
Wang, Hui, Dong, Jinshi, Allard, Lawrence F., Lee, Sungsik, Oh, Se, Wang, Jun, Li, Wei, Shen, Meiqing, & Yang, Ming. Single-site Pt/La-Al2O3 stabilized by barium as an active and stable catalyst in purifying CO and C3H6 emissions. United States. doi:10.1016/j.apcatb.2018.11.034.
Wang, Hui, Dong, Jinshi, Allard, Lawrence F., Lee, Sungsik, Oh, Se, Wang, Jun, Li, Wei, Shen, Meiqing, and Yang, Ming. Mon . "Single-site Pt/La-Al2O3 stabilized by barium as an active and stable catalyst in purifying CO and C3H6 emissions". United States. doi:10.1016/j.apcatb.2018.11.034. https://www.osti.gov/servlets/purl/1492696.
@article{osti_1492696,
title = {Single-site Pt/La-Al2O3 stabilized by barium as an active and stable catalyst in purifying CO and C3H6 emissions},
author = {Wang, Hui and Dong, Jinshi and Allard, Lawrence F. and Lee, Sungsik and Oh, Se and Wang, Jun and Li, Wei and Shen, Meiqing and Yang, Ming},
abstractNote = {High-temperature operations present a substantial challenge for developing industrial-capable precious metal catalysts (e.g. Pt/alumina), where the scarce metal atoms easily become wasted as sintered nanoparticles. Using fully dispersed precious metal atoms to deliver the catalysis remains an elusive goal. On a widely used La-stabilized alumina support, we find that the atomically dispersed Pt1(II)-Ox- species, rather than the much more visible large metal particles, are the actual catalytic sites for the CO and C3H6 oxidation reactions. Unfortunately, the La dopants in alumina support will not hinder the sintering of the active Pt1(II)-Ox- species. As a natural next step, the Ba-Ox- species were introduced to specifically stabilize the single-atom Pt on the La-stabilized alumina support. By implementing this improved formulation, the atomically dispersed Pt on alumina retains the original full dispersion even after 650 °C hydrothermal aging. Intriguingly, with or without the barium additives and/or sintered platinum particles in the catalysts, the intrinsic activity per Pt atom stays intact. Along with other experimental evidence, this leads to the finding that the single-atom Pt is the true catalytic site for the oxidation of CO and C3H6 in the widely-used Pt/La-Al2O3 material system. This work provides a new perspective for efficient precious metal utilization under demanding catalytic conditions.},
doi = {10.1016/j.apcatb.2018.11.034},
journal = {Applied Catalysis B: Environmental},
number = C,
volume = 244,
place = {United States},
year = {2018},
month = {11}
}

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