Towards ALD thin film stabilized single-atom Pd 1 catalysts

Piernavieja-Hermida, Mar; Lu, Zheng; White, Anderson; Low, Ke-Bin; Wu, Tianpin; Elam, Jeffrey W.; Wu, Zili; Lei, Yu

doi:10.1039/c6nr04403d

Towards ALD thin film stabilized single-atom Pd ₁ catalysts

Journal Article · Wed Jul 27 00:00:00 EDT 2016 · Nanoscale

DOI:https://doi.org/10.1039/c6nr04403d· OSTI ID:1319206

Piernavieja-Hermida, Mar ^[1]; Lu, Zheng ^[1]; White, Anderson ^[1]; Low, Ke-Bin ^[2]; Wu, Tianpin ^[3]; Elam, Jeffrey W. ^[4]; Wu, Zili ^[5]; Lei, Yu ^[1]

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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: National Science Foundation (NSF); ORAU; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22) - National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725

OSTI ID:: 1319206

Alternate ID(s):: OSTI ID: 1337161

Journal Information:: Nanoscale, Journal Name: Nanoscale Journal Issue: 33 Vol. 8; ISSN NANOHL; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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