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Title: Oxidative Dehydrogenation of Ethane: A Chemical Looping Approach

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [1]
  1. Department of Chemical & Biological Engineering, N.C. State University, 911 Partners Way Raleigh NC 27695-7905 USA
  2. EcoCatalytic Technologies LLC, 9 Deer Park Drive, Suite J-1. Monmouth Junction NJ 08852 USA
Publication Date:
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
OSTI Identifier:
1400563
Grant/Contract Number:
AR0000327
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Energy Technology
Additional Journal Information:
Journal Volume: 4; Journal Issue: 10; Related Information: CHORUS Timestamp: 2017-10-20 15:08:35; Journal ID: ISSN 2194-4288
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Neal, Luke M., Yusuf, Seif, Sofranko, John A., and Li, Fanxing. Oxidative Dehydrogenation of Ethane: A Chemical Looping Approach. Germany: N. p., 2016. Web. doi:10.1002/ente.201600074.
Neal, Luke M., Yusuf, Seif, Sofranko, John A., & Li, Fanxing. Oxidative Dehydrogenation of Ethane: A Chemical Looping Approach. Germany. doi:10.1002/ente.201600074.
Neal, Luke M., Yusuf, Seif, Sofranko, John A., and Li, Fanxing. 2016. "Oxidative Dehydrogenation of Ethane: A Chemical Looping Approach". Germany. doi:10.1002/ente.201600074.
@article{osti_1400563,
title = {Oxidative Dehydrogenation of Ethane: A Chemical Looping Approach},
author = {Neal, Luke M. and Yusuf, Seif and Sofranko, John A. and Li, Fanxing},
abstractNote = {},
doi = {10.1002/ente.201600074},
journal = {Energy Technology},
number = 10,
volume = 4,
place = {Germany},
year = 2016,
month = 6
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1002/ente.201600074

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  • The addition of chloride ions to a Li{sup +}-MgO catalyst at a ratio of Cl/Li {>=} 0.9 significantly improves the yields of ethylene that can be achieved during the oxidative dehydrogenation (OXD) of ethane. At 620{degrees}C, C{sub 2}H{sub 4} yields of 58% (75% conversion, 77% selectivity) have been maintained for up to 50 h on stream. These ethylene yields are consistent with the large C{sub 2}H{sub 4}/{sub 2}H{sub 6} ratios that are attained over these catalysts during the oxidative coupling of CH{sub 4}. The activity of the catalysts with Cl/Li {>=} 0.9 is partly a result of the fact CO{submore » 2} formed during the reaction does not poison the catalyst. In addition, the surface areas of the chlorided catalysts are greater than those which contain a comparable amount of Li, but no chloride ions. Based upon the activity results, CO{sub 2} temperature-programmed desorption data, and X-ray photoelectron spectra, a model has been proposed in which lithium is mainly present as LiCl on the MgO support, provided a nearly stoichiometric amount of chloride is available. The active centers are believed to be associated with a thin (atomic) layer of Li{sub 2}O that partially covers the LiCl crystallites. This Li{sub 2}O is capable of activating {sub 2}H{sub 6}, but its basic strength has been modified so that it does not form carbonate ions at 620{degrees}C. When the amount of chloride is limited, or is not present at all, multilayers of more strongly basic Li{sub 2}O form on the surface of LiCl and/or on the MgO. In the presence of CO{sub 2}, this Li{sub 2}O is extensively converted to Li{sub 2}CO{sub 3}, which is inactive for the OXD reaction. 20 refs., 9 figs., 6 tabs.« less
  • An inert-membrane catalytic reactor has been tested for the oxidative dehydrogenation of ethane. This reactor consists of a fixed bed of Li/MgO catalyst encompassed by a porous ceramic membrane. Oxygen was permeated through the membrane while ethane was fed axially. Two different configurations of the membrane reactor were tested: a homogeneous wall membrane reactor and a mixed system which was equivalent to a membrane reactor followed by a conventional fixed bed reactor. Using this system, high conversions of ethane were obtained, while maintaining a good selectivity. This gave yields to ethylene and higher hydrocarbons of up to 57%. In addition,more » the membrane reactor allowed a safe and stable operation, even when a relatively high proportion of oxygen was used in the overall feed.« less
  • Vanadium pentoxide catalysts have been studied in the partial oxidation reaction of ethane in the 723-843 K temperature range. The relationship between the acid-base properties and the catalytic behavior was investigated. The number and character of acidic sites of V{sub 2}O{sub 5} catalysts were determined by studying the adsorption of a basic molecule using microcalorimetry. The reducibility level and the evolution of the surface state, as well as the heat evolved, were studied by using a pulse method with pure ethane only. The reaction of ethane oxidative dehydrogenation was studied by a continuous flow method and the activation energies formore » the formation of C{sub 2}H{sub 4} and CO were calculated. The selectivity of the catalyst was interpreted in connection with the acid-base properties. The strong sites were observed to decrease rapidly with time on stream, although the catalysts were still active. Temperature-programmed reduction of V{sub 2}O{sub 5} using a TG-DSC coupling was also investigated with hydrogen, ethylene, or ethane as reducers. The different heats of reduction are given. It was observed that C{sub 2}H{sub 4} is a much more efficient reducing agent than H{sub 2} and C{sub 2}H{sub 6}. Following each reduction, reoxidation studies by oxygen were performed in the same equipment showing clearly different step in the reoxidation process. 20 refs., 8 figs., 1 tab.« less
  • The selective conversion of ethane into ethylene is currently being studied because of the economic impact of using natural gas and LPG`s raw materials to produce chemicals and polymers. The available technology for the production of ethylene is the steam cracking of ethane, although it is a highly energy-intensive process. Several approaches to this problem have been considered, although oxidative dehydrogenation (ODH) remains prominent. The principal reason for this lies in the fact that dehydrogenation in the presence of oxygen is thermodynamically favored and coking side reactions are minimized. The present note reports preliminary results in the performance for themore » ODH reaction of ethane of a new family of vanadium-loaded {alpha}-Ti phosphate catalyst. Moreover, although these catalysts show modest activity with negligible production of CO{sub 2}, a second objective was to report data on the genesis of surface sites during on-stream operation.« less
  • The oxidative dehydrogenation of ethane to ethylene over Pt-coated foam monoliths in oxygen with varying levels of nitrogen dilution has been simulated using a 24-step model of adsorption, desorption and surface reactions. Reaction parameters for these elementary steps were obtained from surface science and catalysis literature or fit to previously reported experimental data. The model agrees with the experimental data remarkably well, mimicking the selectivity and conversion trends observed experimentally with changing operating conditions. The model shows that a purely heterogeneous mechanism can be used to simulate the experimental results collected near atmospheric pressure accurately, suggesting that the mechanism themore » authors propose is sufficiently accurate to capture the main features of this reaction system. This model can also be used to examine this reaction system under conditions experimentally inaccessible. Application of this predictive ability to operation of this type of reactor under probable industrial conditions suggests that excellent ethylene yields are possible.« less