skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Highly selective and stable Cu/SiO 2 catalysts prepared with a green method for hydrogenation of diethyl oxalate into ethylene glycol

Authors:
; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1416769
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Applied Catalysis. B, Environmental
Additional Journal Information:
Journal Volume: 209; Journal Issue: C; Related Information: CHORUS Timestamp: 2018-01-11 21:35:50; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Country of Publication:
Netherlands
Language:
English

Citation Formats

Ding, Jie, Popa, Tiberiu, Tang, Jinke, Gasem, Khaled A. M., Fan, Maohong, and Zhong, Qin. Highly selective and stable Cu/SiO 2 catalysts prepared with a green method for hydrogenation of diethyl oxalate into ethylene glycol. Netherlands: N. p., 2017. Web. doi:10.1016/j.apcatb.2017.02.072.
Ding, Jie, Popa, Tiberiu, Tang, Jinke, Gasem, Khaled A. M., Fan, Maohong, & Zhong, Qin. Highly selective and stable Cu/SiO 2 catalysts prepared with a green method for hydrogenation of diethyl oxalate into ethylene glycol. Netherlands. doi:10.1016/j.apcatb.2017.02.072.
Ding, Jie, Popa, Tiberiu, Tang, Jinke, Gasem, Khaled A. M., Fan, Maohong, and Zhong, Qin. 2017. "Highly selective and stable Cu/SiO 2 catalysts prepared with a green method for hydrogenation of diethyl oxalate into ethylene glycol". Netherlands. doi:10.1016/j.apcatb.2017.02.072.
@article{osti_1416769,
title = {Highly selective and stable Cu/SiO 2 catalysts prepared with a green method for hydrogenation of diethyl oxalate into ethylene glycol},
author = {Ding, Jie and Popa, Tiberiu and Tang, Jinke and Gasem, Khaled A. M. and Fan, Maohong and Zhong, Qin},
abstractNote = {},
doi = {10.1016/j.apcatb.2017.02.072},
journal = {Applied Catalysis. B, Environmental},
number = C,
volume = 209,
place = {Netherlands},
year = 2017,
month = 7
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on March 17, 2018
Publisher's Accepted Manuscript

Citation Metrics:
Cited by: 1work
Citation information provided by
Web of Science

Save / Share:
  • The reaction kinetics of the catalytic hydrogenation of diethyl oxalate to ethylene glycol in the vapor phase over a copper-base catalyst were studied. The experiments were carried out in a continuous flow microreactor. The experimental work was based on the following consecutive reaction scheme: C{sub 2}H{sub 5}COOCOOC{sub 2}H{sub 5} + 4H{sub 2} {leftrightarrow} HOCH{sub 2}CH{sub 2}OH + 2C{sub 2}H{sub 5}OH; HOCH{sub 2}CH{sub 2}OH + H{sub 2} {yields} C{sub 2}H{sub 5}OH + H{sub 2}O. Fourteen competing kinetic models obtained from the possible mechanisms have been proposed for the above scheme. By fitting the experimental data to each model, rate equations weremore » found to best fit the data. In the model from the above rate equations were obtained the hydrogenation reaction of diethyl oxalate follows the Langmuir-Hinshelwood mechanism in which hydrogen adsorbs dissociatively. The surface reaction step was rate-limiting for both the main and side reaction.« less
  • Hydrogenation studies of carbon monoxide to methanol and ethylene glycol by homogeneous ruthenium catalysts in several types of solvents are reported. In contrast to previous reports of catalysis under extreme pressures, these studies were conducted at pressures of 340 atm and below. Overall rates of carbon monoxide hydrogenation in these catalytic reactions (in several types of solvents) are nearly equal to those recently reported for a similar ruthenium system operated at much higher pressure - for example, a rate of 8.3 x 10/sup -3/ turnovers s/sup -1/ was observed, as compared with a reported rate (to methanol and methyl formate)more » of 1.05 x 10/sup -2/ s/sup -1/ at 270/sup 0/C under 1300 atm in THF solvent. This comparison exhibits the importance of solvent effects in homogeneous catalysis, even when the catalyst is presumably uncharged and mononuclear; rate improvements obtainable by large increases in pressure may also be achieved by appropriate choice of solvents. An even more important role of reactive, carboxylic acid solvents in this system is demonstrated by the discovery that they cause formation of a two-carbon product by a catalyst which otherwise produces only methanol. The function of this unique solvent/promoter is apparently to intercept a catalytic intermediate and change the course of its reaction. Further research based on these results is in progress.« less
  • In the production of ethylene from the steam cracking of natural gas, small amounts of acetylene and butadiene are produced. Downstream, acetylene can present a hazard in a cryogenic separation process while nonselective hydrogenation removes acetylene as well as valuable ethylene and butadiene. With the aid of adsorption measurements, a selective hydrogenation catalyst has been designed. Small-pore zeolites, which serve as catalytic supports and provide reactant selective control, were ion-exchanged with Ni{sup 2+} and subsequently reduced. Compared to a commercial catalyst in which 60% of butadiene and all of the acetylene are hydrogenated, these new catalysts totally hydrogenate acetylene withmore » only 10-20% hydrogenation of the butadiene and almost no hydrogenation of ethylene. To achieve selective hydrogenation, poisoning of the metal sites on the external zeolite surface is essential in order to obtain a product spectrum dominated by catalytic sites within the zeolite framework.« less
  • The selective hydrogenation of acetylene in the presence of ethylene has been studied on K+ exchanged {beta}-zeolite supported Pd and PdAg catalysts. Results from batch reactor studies with Fourier transform infrared spectroscopy (FTIR) have shown that the K+-{beta}-zeolite support is more selective than the Al2O3 or Na+-{beta}-zeolite supports toward the hydrogenation of acetylene. The rate and equilibrium constants for Pd/K+-{beta}-zeolite and PdAg/K+-{beta}-zeolite were determined using a Langmuir-Hinshelwood model. The selectivity of the PdAg bimetallic catalyst is twice of that of the Pd catalyst. Results from flow reactor studies show that the PdAg/K+-{beta}-zeolite catalyst has higher selectivity but lower activity towardmore » acetylene hydrogenation than the Pd/K+-{beta}-zeolite catalyst. The selectivity to the undesirable ethane by-product is inhibited on the bimetallic catalyst. Extended X-ray absorption fine structure (EXAFS) studies and transmission electron microscope (TEM) analysis confirm the formation of Pd-Ag bimetallic bonds in the PdAg/K+-{beta}-zeolite catalyst.« less