Towards ALD thin film stabilized single-atom Pd 1 catalysts
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 »
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- Univ. of Alabama in Huntsville, Huntsville, AL (United States). Dept. of Chemical and Materials Engineering
- Univ. of Illinois, Chicago, IL (United States). Research Resources Center
- Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
- Argonne National Lab. (ANL), Argonne, IL (United States). Energy Systems Division
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
- Publication Date:
- Grant/Contract Number:
- AC05-00OR22725; CBET-1511820; AC02-06CH11357
- Type:
- Accepted Manuscript
- Journal Name:
- Nanoscale
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 33; Journal ID: ISSN 2040-3364
- Publisher:
- Royal Society of Chemistry
- 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)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY
- OSTI Identifier:
- 1319206
- Alternate Identifier(s):
- OSTI ID: 1337161
- Free Publicly Accessible Full Text
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Accepted Manuscript (DOE)
- Publisher's Version of Record
- https://doi.org/10.1039/c6nr04403d