Highly Selective Oxidative Dehydrogenation of Ethane to Ethylene via Chemical Looping with Oxygen Uncoupling through Structural Engineering of the Oxygen Carrier
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Date
2022-06-16
Publication Type
Journal Article
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yes
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Abstract
The oxidative dehydrogenation of ethane (ODH) to produce ethylene offers advantages compared to the industry standard steam cracking, but its industrial application is hindered by costly air separation units needed to supply oxygen. A chemical-looping-based oxidative dehydrogenation (CL-ODH) scheme is presented, in which oxygen carriers supply gaseous oxygen in situ, which then reacts with ethane in the presence of a catalyst at a comparatively low temperature (500 °C). A common challenge of chemical looping processes beyond combustion is to suppress the overoxidation of hydrocarbons to COx to enable high product yields. It is demonstrated that the overoxidation of ethane can be eliminated completely through structural engineering of the perovskite oxygen carrier involving alkali-metal-based carbonate coatings, while maintaining the materials’ ability to generate oxygen. Through CL-ODH, higher ethylene selectivity (≈91%) and yields (≈39%) are achieved compared to the conventional ODH scheme without oxygen carrier and cofeeding air/ethane. 18O-labeling experiments demonstrate that the carbonate layer functions like a diffusion barrier for ethane while being permeable for oxygen. Both the CL-ODH scheme and the material design strategy can be extended to other catalytic oxidation or dehydrogenation reactions requiring oxygen at different temperatures, offering enormous potential to intensify such processes.
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published
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Journal / series
Volume
12 (13)
Pages / Article No.
2200405
Publisher
Wiley-VCH
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Date collected
Date created
Subject
chemical looping; ethylene production; material design; oxidative dehydrogenation; oxygen carrier
Organisational unit
03865 - Müller, Christoph R. / Müller, Christoph R.
Notes
Funding
180544 - NCCR Catalysis (phase I) (SNF)