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

Here, this work investigated the effect of the addition of a second metal (Cu, Ag, Zn, Sn) on the performance of Pd/ZrO 2 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/ZrO 2, alloying was also observed but tin oxide was still present on the surface after reduction at 773 K. For Pd and PdSn/ZrO 2, 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/ZrO 2 and PdZn/ZrO 2 and PdAg/ZrO 2 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 particlesmore » is one of the causes for catalyst deactivation.« less
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [5] ;  [5] ;  [1] ;  [6]
  1. Federal Univ. of Uberlandia, Uberlandia (Brazil). School of Chemical Engineering
  2. National Inst. of Technology, Rio de Janeiro (Brazil). Catalysis Division; Military Institute of Engineering, Rio de Janeiro (Brazil). Chemical Engineering Dept.
  3. 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
  4. Univ. of Kentucky, Lexington, KY (United States). Center for Applied Energy Research
  5. Argonne National Lab. (ANL), Argonne, IL (United States)
  6. National Inst. of Technology, Rio de Janeiro (Brazil). Catalysis Division; Military Institute of Engineering, Rio de Janeiro (Brazil). Chemical Engineering Dept.
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Applied Catalysis. B, Environmental
Additional Journal Information:
Journal Volume: 232; Journal Issue: C; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); USDOE Office of Fossil Energy (FE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Coordenação de Aperfeiçoamento de Pessoal de Ensino Superio (CAPES); Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; hydrodeoxygenation; bimetallic catalysts; bio-oil; oxophilic sites; phenol; stability
OSTI Identifier:
1429389