Influence of dioxygen on the promotional effect of Bi during Pt-catalyzed oxidation of 1,6-hexanediol

Xie, Jiahan; Huang, Benjamin; Yin, Kehua; Pham, Hien N.; Unocic, Raymond R.; Datye, Abhaya K.; Davis, Robert J.

doi:10.1021/acscatal.6b00972

Influence of dioxygen on the promotional effect of Bi during Pt-catalyzed oxidation of 1,6-hexanediol

Journal Article · Tue May 24 00:00:00 EDT 2016 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.6b00972· OSTI ID:1261533

Xie, Jiahan ^[1]; Huang, Benjamin ^[1]; Yin, Kehua ^[1]; Pham, Hien N. ^[2]; Unocic, Raymond R. ^[3]; Datye, Abhaya K. ^[2]; Davis, Robert J. ^[1]

Univ. of Virginia, Charlottesville, VA (United States)
Univ. of New Mexico, Albuquerque, NM (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

In this study, a series of carbon-supported, Bi-promoted Pt catalysts with various Bi/Pt atomic ratios was prepared by selectively depositing Bi on Pt nanoparticles. The catalysts were evaluated for 1,6-hexanediol oxidation activity in aqueous solvent under different dioxygen pressures. The rate of diol oxidation on the basis of Pt loading over a Bi-promoted catalyst was 3 times faster than that of an unpromoted Pt catalyst under 0.02 MPa of O₂, whereas the unpromoted catalyst was more active than the promoted catalyst under 1 MPa of O₂. After liquid-phase catalyst pretreatment and 1,6-hexanediol oxidation, migration of Bi on the carbon support was observed. The reaction order in O₂ was 0 over Bi-promoted Pt/C in comparison to 0.75 over unpromoted Pt/C in the range of 0.02–0.2 MPa of O₂. Under low O₂ pressure, rate measurements in D₂O instead of H₂O solvent revealed a moderate kinetic isotope effect (rate_H₂O/rate_D₂O) on 1,6-hexanediol oxidation over Pt/C (KIE = 1.4), whereas a negligible effect was observed on Bi-Pt/C (KIE = 0.9), indicating that the promotional effect of Bi could be related to the formation of surface hydroxyl groups from the reaction of dioxygen and water. No significant change in product distribution or catalyst stability was observed with Bi promotion, regardless of the dioxygen pressure.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1261533

Alternate ID(s):: OSTI ID: 1354400

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 7 Vol. 6; ISSN 2155-5435

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Bi
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alcohol oxidation
catalyst restructuring
dioxygen pressure
heterogeneous catalysts
isotope effect
promotional effect

Influence of dioxygen on the promotional effect of Bi during Pt-catalyzed oxidation of 1,6-hexanediol

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