期刊
JOURNAL OF MEMBRANE SCIENCE
卷 661, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.memsci.2022.120915
关键词
Membrane reactor; Flue gas; Methane; Ethane; Ethylene
资金
- US Department of Energy, Office of Fossil Energy, National Energy Technology Laboratory [DE -FE-0031634]
- National Science Foundation [CBET-1924095]
Researchers have developed a new membrane reactor that captures CO2 and O-2 from flue gas and uses them to convert methane into ethane and ethylene. The reactor achieves higher selectivity of the C-2 products by reducing the oxidizing power of the oxidant and lowering the local oxygen partial pressure. Experimental results using a button-type membrane reactor with a diluted methane and argon mixture as the feedstock show a 12% C-2 yield and approximately 57% C-2 selectivity.
Oxidative coupling of methane (OCM), which transforms CH4 into C-2 products (C2H6 and C2H4) with molecular O-2 as the oxidant, is one of the most studied direct methane conversions (DMCs). However, a major technical hurdle to the OCM process is to achieve high CH4 conversion at high C-2 (C2H6 and C2H4) selectivity. One rudimentary cause for this tradeoff' behavior is the high chemical reactivity of the products (C2H6 or C2H4), which can be re-oxidized by O-2. To overcome this thermodynamic challenge, minimizing the oxidizing power of the oxidant and lowering the local oxygen partial pressure are keys. In this work, we demonstrate a new membrane reactor that capture CO2/O-2 from a flue gas and uses it for OCM conversion. The results show that the co-captured CO2/O-2 mixture converts CH4 into C2H6 in the presence of a 2%Mn-5%Na2WO4/SiO2 catalyst, followed by thermal cracking of C2H6 into C2H4 and H-2. The presence of CO2 decreases the local partial pressure of O-2, thus reducing the propensity of C- (2)-products re-oxidation and leading to a higher C-2 selectivity. We show that a small button-type membrane reactor can achieve 12% C-2 yield with similar to 57% C-2-selectivity using a diluted CH4-Ar mixture as the feedstock. We expect higher C-2 yield with tubular plug-flow membrane reactors in the future. We also highlight the unique advantage of the membrane reactor in intensifying CO2 capture from both flue gas and OCM purification process into one single step.
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