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

Kuo, Chun-Te; Lu, Yubing; Kovarik, Libor; Engelhard, Mark H.; Karim, Ayman M.

doi:10.1021/acscatal.9b02840

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

Journal Article · 22 October 2019 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.9b02840 · OSTI ID:1615019

Kuo, Chun-Te ^[1];

^[1];

^[2];

^[1]

Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

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. Lastly, 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.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1615019

Report Number(s):: PNNL-SA-144951

Journal Information:: ACS Catalysis, Vol. 9, Issue 12; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
single-atom catalysts
subnanometer clusters
H₂ activation
selective hydrogenation
X-ray photoelectron spectroscopy infrared spectroscopy
calorimetry
scanning transmission electron microscopy