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Lee, Jae Sung
Eco-friendly Catalysis and Energy Lab
Research Interests
  • Photocatalytic water splitting, artificial photosynthesis, fuel cells, heterogeneous catalysis

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Nature and role of active states of Pd and Cu in the oxidative carbonylation of phenols with Pd/C and cuprous oxide

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Title
Nature and role of active states of Pd and Cu in the oxidative carbonylation of phenols with Pd/C and cuprous oxide
Other Titles
Nature and role of active states of Pd and Cu in the oxidative carbonylation of phenols with Pd/C and cuprous oxide
Author
Kim, Won BaePark, Eun DuckLee, Chul WooLee, Jae Sung
Keywords
active states; Pd metal; linear cuprous dibromide complex; role of Bu4NBr; oxidative carbonylation of phenols; XANES; EXAFS; Pd and CuK-edges
Issue Date
2003-09
Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
Citation
JOURNAL OF CATALYSIS, v.218, no.2, pp.334 - 347
Abstract
Active states of palladium and copper for the oxidative carbonylation of phenol and bisphenol-A were investigated using X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) for Pd and Cu K-edges. The initial states of Pd and Cu were carbon-supported metallic Pd and cuprous oxide, respectively. During oxidative carbonylation, however, the metallic character of palladium was enhanced, as indicated by Pd K-edge XANES spectra taken before and after the reaction. Furthermore, Pd-Pd coordination number increased from ca. 6.0 to 11.0, as determined by the quantitative EXAFS analyses of Pd K-edge. The initial crystalline cuprous oxide was converted by reaction with Bu4NBr into an unusual linear cuprous dibromide complex stabilized by tetrabutylammonium cation. Qualitative XANES and EXAFS analyses of Cu K-edge identified the structural and electronic configuration of the cuprous complex that was found to be the active main catalyst. There was a direct correlation between the formation of the cuprous complex and the catalytic activity and selectivity. Based on these results, a possible catalytic reaction scheme was proposed for the oxidative carbonylation of phenols with the catalytic system of Pd/C, an inorganic cuprous compound and Bu4NBr. (C) 2003 Elsevier Inc. All rights reserved
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DOI
10.1016/S0021-9517(03)00089-7
ISSN
0021-9517
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ECHE_Journal Papers
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