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Structure Sensitivity of Acetylene Semi-Hydrogenation on Pt Single Atoms and Subnanometer Clusters

Publication ,  Journal Article
Kuo, CT; Lu, Y; Kovarik, L; Engelhard, M; Karim, AM
Published in: ACS Catalysis
January 1, 2019

Oxide-supported Pt-group single atoms and clusters in the subnanometer size regime maximize the metal utilization and have shown extraordinary catalytic properties for many reactions including selective hydrogenation. Establishing relations between the metal nuclearity and electronic and catalytic properties is crucial for catalyst design. Here, we varied the nuclearity of Pt supported on TiO2 from single atoms to subnanometer clusters to larger nanoparticles to develop such relations for acetylene hydrogenation. We show that, in contrast to the low selectivity on large Pt nanoparticles, in the subnanometer size regime, Pt exhibits remarkably high selectivity to ethylene. Through a combination of X-ray photoelectron spectroscopy and calorimetry, we demonstrate that the origin of high selectivity is the decreased electron density on Pt and destabilization of C2H4 as the Pt nuclearity decreases. However, as the Pt nuclearity decreased, the activity for H2 activation and acetylene hydrogenation decreased, indicating a trade-off between activity and selectivity. The results show that, while different properties emerge in the subnanometer regime, Pt supported on TiO2 appears to be bound by similar scaling and Brønsted-Evans-Polanyi relationships as on metal surfaces.

Duke Scholars

Published In

ACS Catalysis

DOI

EISSN

2155-5435

Publication Date

January 1, 2019

Start / End Page

11030 / 11041

Related Subject Headings

  • 3406 Physical chemistry
  • 3405 Organic chemistry
  • 3106 Industrial biotechnology
  • 0904 Chemical Engineering
  • 0305 Organic Chemistry
  • 0302 Inorganic Chemistry
 

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Kuo, C. T., Lu, Y., Kovarik, L., Engelhard, M., & Karim, A. M. (2019). Structure Sensitivity of Acetylene Semi-Hydrogenation on Pt Single Atoms and Subnanometer Clusters. ACS Catalysis, 11030–11041. https://doi.org/10.1021/acscatal.9b02840
Kuo, C. T., Y. Lu, L. Kovarik, M. Engelhard, and A. M. Karim. “Structure Sensitivity of Acetylene Semi-Hydrogenation on Pt Single Atoms and Subnanometer Clusters.” ACS Catalysis, January 1, 2019, 11030–41. https://doi.org/10.1021/acscatal.9b02840.
Kuo CT, Lu Y, Kovarik L, Engelhard M, Karim AM. Structure Sensitivity of Acetylene Semi-Hydrogenation on Pt Single Atoms and Subnanometer Clusters. ACS Catalysis. 2019 Jan 1;11030–41.
Kuo, C. T., et al. “Structure Sensitivity of Acetylene Semi-Hydrogenation on Pt Single Atoms and Subnanometer Clusters.” ACS Catalysis, Jan. 2019, pp. 11030–41. Scopus, doi:10.1021/acscatal.9b02840.
Kuo CT, Lu Y, Kovarik L, Engelhard M, Karim AM. Structure Sensitivity of Acetylene Semi-Hydrogenation on Pt Single Atoms and Subnanometer Clusters. ACS Catalysis. 2019 Jan 1;11030–11041.
Journal cover image

Published In

ACS Catalysis

DOI

EISSN

2155-5435

Publication Date

January 1, 2019

Start / End Page

11030 / 11041

Related Subject Headings

  • 3406 Physical chemistry
  • 3405 Organic chemistry
  • 3106 Industrial biotechnology
  • 0904 Chemical Engineering
  • 0305 Organic Chemistry
  • 0302 Inorganic Chemistry