Atomically Precise Strategy to a PtZn Alloy Nanocluster Catalyst for the Deep Dehydrogenation of n -Butane to 1,3-Butadiene

Jeffrey Camacho-Bunquin*, Magali S. Ferrandon, Hyuntae Sohn, A. Jeremy Kropf, Ce Yang, Jianguo Wen, Ryan A. Hackler, Cong Liu, Gokhan Celik, Christopher L. Marshall, Peter C. Stair, Massimiliano Delferro

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

72 Scopus citations

Abstract

The development of on-purpose 1,3-butadiene (BDE) technologies remains an active area in catalysis research, because of the importance of BDE in industrial polymer production. Here, we report on a nonoxidative dehydrogenation catalyst for the production of BDE prepared by atomically precise installation of platinum sites on a Zn-modified SiO2 support via atomic layer deposition (ALD). In situ reduction X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS), CO chemisorption, and high-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM) imaging of activated PtZn/SiO2, revealed the formation of a uniform, well-distributed subnanometer- to nanometer-sized PtZn (1.2 ± 0.3 nm) alloy as the active catalytic species.

Original languageEnglish (US)
Pages (from-to)10058-10063
Number of pages6
JournalACS Catalysis
Volume8
Issue number11
DOIs
StatePublished - Nov 2 2018

Funding

This work was supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC02-06CH11357. Use of the Advanced Photon Source is supported by the U.S. Department of Energy, Office of Science, and Office of the Basic Energy Sciences, under Contract No. DE-AC-02-06CH11357. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. Use of the TEM at the Center for Nanoscale Materials at Argonne National Laboratory is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The calculations were performed using the computational resources provided by the Laboratory Computing Resource Center (LCRC) at Argonne and National Energy Research Scientific Computing (NERSC) Center. We thank Dr. A. P. Sattelberger for helpful discussions and Dr. H. Kim for the UV-Raman spectrum of the spent catalyst. This work was supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC02-06CH11357. Use of the Advanced Photon Source is supported by the U.S. Department of Energy, Office of Science, and Office of the Basic Energy Sciences, under Contract No. DE-AC-02-06CH11357. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. Use of the TEM at the Center for Nanoscale Materials at Argonne National Laboratory is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The calculations were performed using the computational resources provided by the Laboratory Computing Resource Center (LCRC) at Argonne and National Energy Research Scientific Computing (NERSC) Center.

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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