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Title: Aqueous phase hydrogenation of phenol catalyzed by Pd and PdAg on ZrO 2

Abstract

Hydrogenation of phenol in aqueous phase was studied over a series of ZrO2-supported Pd catalysts in order to explore the effects of particle size and of Ag addition on the activity of Pd. Kinetic assessments were performed in a batch reactor, on monometallic Pd/ZrO2 samples with different Pd loadings (0.5%, 1% and 2%), as well as on a 1% PdAg/ZrO2 sample. The turnover frequency (TOF) increases with the Pd particle size. The reaction orders in phenol and H2 indicate that the surface coverages by phenol, H2 and their derived intermediates are higher on 0.5% Pd/ZrO2 than on other samples. The activation energy was the lowest on the least active sample (0.5% Pd/ZrO2), while being identical on 1% and 2% Pd/ZrO2 catalysts. Thus, the significantly lower activity of the small Pd particles (1-2 nm on average) in 0.5%Pd/ZrO2 is explained by the unfavorable activation entropies for the strongly bound species. The presence of Ag increases considerably the TOF of the reaction by decreasing the Ea and increasing the coverages of phenol and H2.

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1422304
Report Number(s):
PNNL-SA-125711
Journal ID: ISSN 0926-860X; 48810; KC0302010
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Applied Catalysis. A, General; Journal Volume: 548; Journal Issue: C
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Resende, Karen A., Hori, Carla E., Noronha, Fabio B., Shi, Hui, Gutierrez, Oliver Y., Camaioni, Donald M., and Lercher, Johannes A. Aqueous phase hydrogenation of phenol catalyzed by Pd and PdAg on ZrO 2. United States: N. p., 2017. Web. doi:10.1016/j.apcata.2017.08.005.
Resende, Karen A., Hori, Carla E., Noronha, Fabio B., Shi, Hui, Gutierrez, Oliver Y., Camaioni, Donald M., & Lercher, Johannes A. Aqueous phase hydrogenation of phenol catalyzed by Pd and PdAg on ZrO 2. United States. doi:10.1016/j.apcata.2017.08.005.
Resende, Karen A., Hori, Carla E., Noronha, Fabio B., Shi, Hui, Gutierrez, Oliver Y., Camaioni, Donald M., and Lercher, Johannes A. Wed . "Aqueous phase hydrogenation of phenol catalyzed by Pd and PdAg on ZrO 2". United States. doi:10.1016/j.apcata.2017.08.005.
@article{osti_1422304,
title = {Aqueous phase hydrogenation of phenol catalyzed by Pd and PdAg on ZrO 2},
author = {Resende, Karen A. and Hori, Carla E. and Noronha, Fabio B. and Shi, Hui and Gutierrez, Oliver Y. and Camaioni, Donald M. and Lercher, Johannes A.},
abstractNote = {Hydrogenation of phenol in aqueous phase was studied over a series of ZrO2-supported Pd catalysts in order to explore the effects of particle size and of Ag addition on the activity of Pd. Kinetic assessments were performed in a batch reactor, on monometallic Pd/ZrO2 samples with different Pd loadings (0.5%, 1% and 2%), as well as on a 1% PdAg/ZrO2 sample. The turnover frequency (TOF) increases with the Pd particle size. The reaction orders in phenol and H2 indicate that the surface coverages by phenol, H2 and their derived intermediates are higher on 0.5% Pd/ZrO2 than on other samples. The activation energy was the lowest on the least active sample (0.5% Pd/ZrO2), while being identical on 1% and 2% Pd/ZrO2 catalysts. Thus, the significantly lower activity of the small Pd particles (1-2 nm on average) in 0.5%Pd/ZrO2 is explained by the unfavorable activation entropies for the strongly bound species. The presence of Ag increases considerably the TOF of the reaction by decreasing the Ea and increasing the coverages of phenol and H2.},
doi = {10.1016/j.apcata.2017.08.005},
journal = {Applied Catalysis. A, General},
number = C,
volume = 548,
place = {United States},
year = {Wed Nov 01 00:00:00 EDT 2017},
month = {Wed Nov 01 00:00:00 EDT 2017}
}