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Title: Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support

Abstract

Single atom catalysts have attracted attention because of improved atom efficiency, higher reactivity, and better selectivity. A major challenge is to achieve high surface concentrations while preventing these atoms from agglomeration at elevated temperatures. Here we investigate the formation of Pt single atoms on an industrial catalyst support. Using a combination of surface sensitive techniques such as XPS and LEIS, X-ray absorption spectroscopy, electron microscopy, as well as density functional theory, we demonstrate that cerium oxide can support Pt single atoms at high metal loading (3 wt% Pt), without forming any clusters or 3D aggregates when heated in air at 800 °C. The mechanism of trapping involves a reaction of the mobile PtO2 with under-coordinated cerium cations present at CeO2(111) step edges, allowing Pt to achieve a stable square planar configuration. The strong interaction of mobile single atom species with the support, present during catalyst sintering and regeneration, helps explain the sinter-resistance of ceria-supported metal catalysts.

Authors:
 [1];  [1];  [1];  [2];  [1];  [3];  [4];  [5];  [6];  [4];  [7];  [8];  [9];  [1];  [3];  [2]
  1. University of New Mexico
  2. UNIVERSITY OF NEW MEXICO
  3. WASHINGTON STATE UNIV
  4. Purdue University
  5. 1. Tascon GmbH
  6. Technische Universiteit Eindhoven
  7. JEOL LTD
  8. BATTELLE (PACIFIC NW LAB)
  9. Fuzhou University
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1530856
Report Number(s):
PNNL-SA-141231
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 9; Journal Issue: 5
Country of Publication:
United States
Language:
English

Citation Formats

Kunwar, Deepak, Zhou, Shulan, DelaRiva, Andrew, Peterson, Eric J., Xiong, Haifeng, Pereira Hernandez, Xavier I., Purdy, Stephen C., ter Veen, Rik, Brongersma, Hidde H., Miller, Jeffrey T., Hashiguchi, Hiroki, Kovarik, Libor, Lin, Sen, Guo, Hua, Wang, Yong, and Datye, Abhaya K. Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support. United States: N. p., 2019. Web. doi:10.1021/acscatal.8b04885.
Kunwar, Deepak, Zhou, Shulan, DelaRiva, Andrew, Peterson, Eric J., Xiong, Haifeng, Pereira Hernandez, Xavier I., Purdy, Stephen C., ter Veen, Rik, Brongersma, Hidde H., Miller, Jeffrey T., Hashiguchi, Hiroki, Kovarik, Libor, Lin, Sen, Guo, Hua, Wang, Yong, & Datye, Abhaya K. Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support. United States. doi:10.1021/acscatal.8b04885.
Kunwar, Deepak, Zhou, Shulan, DelaRiva, Andrew, Peterson, Eric J., Xiong, Haifeng, Pereira Hernandez, Xavier I., Purdy, Stephen C., ter Veen, Rik, Brongersma, Hidde H., Miller, Jeffrey T., Hashiguchi, Hiroki, Kovarik, Libor, Lin, Sen, Guo, Hua, Wang, Yong, and Datye, Abhaya K. Mon . "Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support". United States. doi:10.1021/acscatal.8b04885.
@article{osti_1530856,
title = {Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support},
author = {Kunwar, Deepak and Zhou, Shulan and DelaRiva, Andrew and Peterson, Eric J. and Xiong, Haifeng and Pereira Hernandez, Xavier I. and Purdy, Stephen C. and ter Veen, Rik and Brongersma, Hidde H. and Miller, Jeffrey T. and Hashiguchi, Hiroki and Kovarik, Libor and Lin, Sen and Guo, Hua and Wang, Yong and Datye, Abhaya K.},
abstractNote = {Single atom catalysts have attracted attention because of improved atom efficiency, higher reactivity, and better selectivity. A major challenge is to achieve high surface concentrations while preventing these atoms from agglomeration at elevated temperatures. Here we investigate the formation of Pt single atoms on an industrial catalyst support. Using a combination of surface sensitive techniques such as XPS and LEIS, X-ray absorption spectroscopy, electron microscopy, as well as density functional theory, we demonstrate that cerium oxide can support Pt single atoms at high metal loading (3 wt% Pt), without forming any clusters or 3D aggregates when heated in air at 800 °C. The mechanism of trapping involves a reaction of the mobile PtO2 with under-coordinated cerium cations present at CeO2(111) step edges, allowing Pt to achieve a stable square planar configuration. The strong interaction of mobile single atom species with the support, present during catalyst sintering and regeneration, helps explain the sinter-resistance of ceria-supported metal catalysts.},
doi = {10.1021/acscatal.8b04885},
journal = {ACS Catalysis},
number = 5,
volume = 9,
place = {United States},
year = {2019},
month = {5}
}