Hydrodeoxygenation of phenol over zirconia supported Pd bimetallic catalysts. The effect of second metal on catalyst performance

Resende, Karen A.; Teles, Camila A.; Jacobs, Gary; Davis, Burtron H.; Cronauer, Donald C.; Jeremy Kropf, A.; Marshall, Christopher L.; Hori, Carla E.; Noronha, Fabio B.

doi:10.1016/j.apcatb.2018.03.041

Hydrodeoxygenation of phenol over zirconia supported Pd bimetallic catalysts. The effect of second metal on catalyst performance

Journal Article · Wed Mar 21 00:00:00 EDT 2018 · Applied Catalysis B: Environmental

DOI:https://doi.org/10.1016/j.apcatb.2018.03.041· OSTI ID:1429389

Resende, Karen A. ^[1]; Teles, Camila A. ^[2]; Jacobs, Gary ^[3]; Davis, Burtron H. ^[4]; Cronauer, Donald C. ^[5]; Jeremy Kropf, A. ^[5]; Marshall, Christopher L. ^[5]; Hori, Carla E. ^[1]; Noronha, Fabio B. ^[6]

Federal Univ. of Uberlandia, Uberlandia (Brazil). School of Chemical Engineering
National Inst. of Technology, Rio de Janeiro (Brazil). Catalysis Division; Military Institute of Engineering, Rio de Janeiro (Brazil). Chemical Engineering Dept.
Univ. of Kentucky, Lexington, KY (United States). Center for Applied Energy Research; Univ. of Texas, San Antonio, TX (United States). Dept. of Biomedical Engineering, Dept. of Mechanical Engineering, and Chemical Engineering Program
Univ. of Kentucky, Lexington, KY (United States). Center for Applied Energy Research
Argonne National Lab. (ANL), Argonne, IL (United States)
National Inst. of Technology, Rio de Janeiro (Brazil). Catalysis Division; Military Institute of Engineering, Rio de Janeiro (Brazil). Chemical Engineering Dept.

Here, this work investigated the effect of the addition of a second metal (Cu, Ag, Zn, Sn) on the performance of Pd/ZrO₂ catalyst for HDO of phenol at 573 K in the gas phase. The incorporation of dopants resulted in the formation of Pd–X (Cu, Ag, Zn) alloys, which reduced the reaction rate for HDO and increased the selectivity to hydrogenation products (cyclohexanone and cyclohexanol). The lower activity of the bimetallic catalysts was due to the segregation of the second metal on the surface of the Pd particle. For PdSn/ZrO₂, alloying was also observed but tin oxide was still present on the surface after reduction at 773 K. For Pd and PdSn/ZrO₂, the oxophilic sites represented by Zr and Sn cations promotes the hydrogenation of the carbonyl group of the keto-tautomer intermediate formed, producing benzene as the main product. All catalysts significantly deactivated during the reaction but the deactivation degree depended on the type of the metal. Pd/ZrO₂ and PdZn/ZrO₂ and PdAg/ZrO₂ exhibited approximately the same deactivation degree. However, the loss of activity was less pronounced for PdSn/ZrO2 catalyst. Finally, Pd dispersion significantly decreased during the reaction, indicating that the sintering of Pd particles is one of the causes for catalyst deactivation.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq); Coordenação de Aperfeiçoamento de Pessoal de Ensino Superio (CAPES); USDOE Office of Fossil Energy (FE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1429389

Journal Information:: Applied Catalysis B: Environmental, Journal Name: Applied Catalysis B: Environmental Journal Issue: C Vol. 232; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Hydrodeoxygenation of phenol over zirconia supported Pd bimetallic catalysts. The effect of second metal on catalyst performance

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