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Title: Towards ALD thin film stabilized single-atom Pd 1 catalysts

Abstract

Supported precious metal single-atom catalysts have shown interesting activity and selectivity in recent studies. However, agglomeration of these highly mobile mononuclear surface species can eliminate their unique catalytic properties. In this paper, we study a strategy for synthesizing thin film stabilized single-atom Pd 1 catalysts using atomic layer deposition (ALD). The thermal stability of the Pd 1 catalysts is significantly enhanced by creating a nanocavity thin film structure. In situ infrared spectroscopy and Pd K-edge X-ray absorption spectroscopy (XAS) revealed that the Pd 1 was anchored on the surface through chlorine sites. The thin film stabilized Pd 1 catalysts were thermally stable under both oxidation and reduction conditions. The catalytic performance in the methanol decomposition reaction is found to depend on the thickness of protecting layers. While Pd 1 catalysts showed promising activity at low temperature in a methanol decomposition reaction, 14 cycle TiO 2 protected Pd 1 was less active at high temperature. Pd L 3 edge XAS indicated that the low reactivity compared with Pd nanoparticles is due to the strong adsorption of carbon monoxide even at 250 °C. Lastly, these results clearly show that the ALD nanocavities provide a basis for future design of single-atom catalysts thatmore » are highly efficient and stable.« less

Authors:
 [1];  [1];  [1];  [2];  [3];  [4];  [5];  [1]
  1. Univ. of Alabama in Huntsville, Huntsville, AL (United States). Dept. of Chemical and Materials Engineering
  2. Univ. of Illinois, Chicago, IL (United States). Research Resources Center
  3. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Energy Systems Division
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); 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); ORAU; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22) - National Science Foundation (NSF)
OSTI Identifier:
1319206
Alternate Identifier(s):
OSTI ID: 1337161
Grant/Contract Number:  
AC05-00OR22725; CBET-1511820; AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 8; Journal Issue: 33; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Piernavieja-Hermida, Mar, Lu, Zheng, White, Anderson, Low, Ke-Bin, Wu, Tianpin, Elam, Jeffrey W., Wu, Zili, and Lei, Yu. Towards ALD thin film stabilized single-atom Pd 1 catalysts. United States: N. p., 2016. Web. doi:10.1039/c6nr04403d.
Piernavieja-Hermida, Mar, Lu, Zheng, White, Anderson, Low, Ke-Bin, Wu, Tianpin, Elam, Jeffrey W., Wu, Zili, & Lei, Yu. Towards ALD thin film stabilized single-atom Pd 1 catalysts. United States. doi:10.1039/c6nr04403d.
Piernavieja-Hermida, Mar, Lu, Zheng, White, Anderson, Low, Ke-Bin, Wu, Tianpin, Elam, Jeffrey W., Wu, Zili, and Lei, Yu. Wed . "Towards ALD thin film stabilized single-atom Pd 1 catalysts". United States. doi:10.1039/c6nr04403d. https://www.osti.gov/servlets/purl/1319206.
@article{osti_1319206,
title = {Towards ALD thin film stabilized single-atom Pd 1 catalysts},
author = {Piernavieja-Hermida, Mar and Lu, Zheng and White, Anderson and Low, Ke-Bin and Wu, Tianpin and Elam, Jeffrey W. and Wu, Zili and Lei, Yu},
abstractNote = {Supported precious metal single-atom catalysts have shown interesting activity and selectivity in recent studies. However, agglomeration of these highly mobile mononuclear surface species can eliminate their unique catalytic properties. In this paper, we study a strategy for synthesizing thin film stabilized single-atom Pd1 catalysts using atomic layer deposition (ALD). The thermal stability of the Pd1 catalysts is significantly enhanced by creating a nanocavity thin film structure. In situ infrared spectroscopy and Pd K-edge X-ray absorption spectroscopy (XAS) revealed that the Pd1 was anchored on the surface through chlorine sites. The thin film stabilized Pd1 catalysts were thermally stable under both oxidation and reduction conditions. The catalytic performance in the methanol decomposition reaction is found to depend on the thickness of protecting layers. While Pd1 catalysts showed promising activity at low temperature in a methanol decomposition reaction, 14 cycle TiO2 protected Pd1 was less active at high temperature. Pd L3 edge XAS indicated that the low reactivity compared with Pd nanoparticles is due to the strong adsorption of carbon monoxide even at 250 °C. Lastly, these results clearly show that the ALD nanocavities provide a basis for future design of single-atom catalysts that are highly efficient and stable.},
doi = {10.1039/c6nr04403d},
journal = {Nanoscale},
number = 33,
volume = 8,
place = {United States},
year = {Wed Jul 27 00:00:00 EDT 2016},
month = {Wed Jul 27 00:00:00 EDT 2016}
}

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Works referenced in this record:

Increased Silver Activity for Direct Propylene Epoxidation via Subnanometer Size Effects
journal, April 2010


Atomic Layer Deposition: An Overview
journal, January 2010

  • George, Steven M.
  • Chemical Reviews, Vol. 110, Issue 1, p. 111-131
  • DOI: 10.1021/cr900056b