Journal
MOLECULAR CATALYSIS
Volume 438, Issue -, Pages 93-102Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.mcat.2017.05.027
Keywords
Oxalate hydrogenation; Cu/ZrO2 catalyst; Acetic complex method; Dielectric constant; Synergistic effect
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Funding
- Inner Mongolia University of Science and Technology Innovation Fund [2016QDL-B33]
- National Natural Science Foundation of China [21466029, 21673272]
- Natural Science Foundation of Inner Mongolia [2014MS0210]
- PetroChina [PRIKY15042]
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Herein, the Cu species uniformly combining with highly crystalline ZrO2 nanosheets had been prepared by a one-pot acetic complex method. The selectivity to ethylene glycol of 98.9%, which corresponds to 99.8% conversion of diethyl oxalate was obtained over the one prepared by using acetic acid (AC) both as the complex agent and solvent. In addition, a stable performance was achieved (life span of >160 h). It also showed good performance in hydrogenation of dimethyl oxalate (95.7 h(-1) turnover frequency). Essentially, solvents with different dielectric constant employed in complexation process had a prominent influence on the structure and catalytic activity of Cu/ZrO2 catalyst via solvation. Besides, complexation process was also important since AC could be regarded as L-type ligands in a low dielectric constant solvent, forming of ion-clusters which resulted in exclusive formation of the Cu-O-Zr interface after calcination. Evidently, the surface synergistic effect held the key to the continuous hydrogenation reaction related to the activation of the carbonyl groups and the hydrogen dissociation, thus creating a synergetic nanoenvironment for the successful completion of the multi step turning into one-step in the series reaction. (C) 2017 Elsevier B.V. All rights reserved.
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