Reduction of Propionic Acid over a Pd-Promoted ReOx/SiO2 Catalyst Probed by X-ray Absorption Spectroscopy and Transient Kinetic Analysis

Kammert, James D.; Xie, Jiahan; Godfrey, Ian J.; Unocic, Raymond R.; Stavitski, Eli; Attenkofer, Klaus; Sankar, Gopinathan; Davis, Robert J.

doi:10.1021/acssuschemeng.8b02820

Title: Reduction of Propionic Acid over a Pd-Promoted ReO_x/SiO₂ Catalyst Probed by X-ray Absorption Spectroscopy and Transient Kinetic Analysis

Journal Article · 11 July 2018 · ACS Sustainable Chemistry & Engineering

DOI: https://doi.org/10.1021/acssuschemeng.8b02820 · OSTI ID:1477954

Kammert, James D. ^[1];

^[1];

^[2];

^[3]; Stavitski, Eli ^[4]; Attenkofer, Klaus ^[4];

^[2];

^[1]

Univ. of Virginia, Charlottesville, VA (United States)
Univ. College London, London (United Kingdom)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)

A Pd-promoted Re/SiO₂ catalyst was prepared by sequential impregnation and compared to monometallic Pd/SiO₂ and Re/SiO₂. All samples were characterized by electron microscopy, H₂ and CO chemisorption, H₂ temperature-programmed reduction, and in situ X-ray absorption spectroscopy at the Re L_III and Pd K-edges. The samples were also tested in the reduction of propionic acid to 1-propanol and propionaldehyde at 433 K in 0.1–0.2 MPa H₂. Whereas monometallic Pd was inactive for carboxylic acid reduction, monometallic Re catalyzed aldehyde formation but only after high-temperature prereduction that produced metallic Re. When Pd was present with Re in a bimetallic catalyst, Pd facilitated the reduction of Re in H₂ to ~+4 oxidation state at modest temperatures, producing an active catalyst for the conversion of propionic acid to 1-propanol. Under the conditions of this study, the orders of reaction in propionic acid and H₂ were approximately zero and one, respectively. Transient kinetic analysis of the carboxylic acid reduction to alcohols revealed that at least 50% of the Re in the bimetallic catalyst participated in the catalytic reaction. In conclusion, the Pd is proposed to enhance the catalytic activity of the bimetallic catalyst by spilling over hydrogen that can partially reduce Re and react with surface intermediates.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704

OSTI ID:: 1477954

Alternate ID(s):: OSTI ID: 1495984

Report Number(s):: BNL--209173-2018-JAAM

Journal Information:: ACS Sustainable Chemistry & Engineering, Journal Name: ACS Sustainable Chemistry & Engineering Journal Issue: 9 Vol. 6; ISSN 2168-0485

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Reduction of Propionic Acid over a Pd-Promoted ReOx/SiO2 Catalyst Probed by X-ray Absorption Spectroscopy and Transient Kinetic Analysis

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Title: Reduction of Propionic Acid over a Pd-Promoted ReO_x/SiO₂ Catalyst Probed by X-ray Absorption Spectroscopy and Transient Kinetic Analysis