Abstract
Catalytic dehydrogenation coupling of methane (DCM) represents an effective way to convert natural gas to more useful C2 products (C2H6, C2H4). In this work, BaCe0.85Tb0.05Co0.1O3−δ (BCTCo) perovskite hollow fiber membranes were fabricated by the combined phase inversion and sintering method. SrCe0.95Yb0.05O3−δ (SCYb) perovskite oxide was loaded as a catalyst onto the inner hollow fiber membrane surface, which promoted the CH4 conversion and the C2 hydrocarbon selectivity during the DCM reaction. The introduction of steam into the methane feed gas mixture elevated the C2 selectivity and yield due to the alleviation of coke deposition. Switching N2 to air as the sweep gas further increased the C2 selectivity and yield. However, the conversion of methane was limited by both the low permeability of the membrane and the insufficient catalytic activity of the catalyst, leading to low C2 yield.
Highlights
Methane coupling represents an economically promising route to directly convert natural gas feedstock into value-added C2 hydrocarbons such as ethane and ethylene [1].The two routes for methane coupling are oxidative coupling of methane (OCM) and nonoxidative dehydrogenation coupling of methane (DCM) [2]
BaCe0.85 Tb0.05 Co0.1 O3−δ (BCTCo) after the powders were fabricated into hollow fiber membranes by the spinning and sintering processes, which indicates that the perovskite structure was perfectly preserved during the spinning and sintering process
BaCe0.85 Tb0.05 Co0.1 O3−δ (BCTCo) hollow fiber membrane was prepared though a combined phase-inversion and sintering method with BCTCo perovskite powder as the raw ceramic materials
Summary
Methane coupling represents an economically promising route to directly convert natural gas feedstock into value-added C2 hydrocarbons such as ethane and ethylene [1]. The electrochemical attempts, a non-electrochemical approach was reported to catalyze CH4 pyrolysis to form C2 hydrocarbons and H2 on one side, while hydrogen was transported through a proton conducting membrane to the other side without the need of electrode or power supply [6].When the membrane is a mixed proton-electron conductor, the hydrogen can be extracted from the reaction system using the self-discharge phenomenon In this case, the external electric source, electrode materials and current collectors are unnecessary to transport protons across the solid electrolyte and the construction of the reactor is more simplified (permeation mode, Figure 1b). The SCYb oxide was reported to exhibit good DCM catalytic activity due to its high proton and electron-hole conductivities that favor the enhanced formation of C2 hydrocarbons while reducing that of COx
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