期刊
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
卷 60, 期 9, 页码 3516-3531出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.iecr.0c04335
关键词
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资金
- ACT GaSTech project [271511]
- Research Council of Norway
- Swiss Office of Energy
- European Commission under the Horizon 2020 programme, ACT Grant [691712]
This paper presents experimental demonstration of a three-stage GST process for syngas and H-2/CO production from methane using a lanthanum-based oxygen carrier. The results show high selectivity in oxidizing methane to syngas, reduced carbon deposition by co-feeding CO2 with CH4, and the potential to tune up the H-2/CO ratio with the addition of steam, making the process suitable for various downstream applications. At higher pressures, the process achieves over 70% fuel conversion at 5 bar and 950 degrees C.
This paper focuses on the experimental demonstration of a threestage GST (gas switching technology) process (fuel, steam/CO2, and air stages) for syngas production from methane in the fuel stage and H-2/CO production in the steam/ CO2 stage using a lanthanum- based oxygen carrier (La0.85Sr0.15Fe0.95Al0.05O3). Experiments were performed at temperatures between 750-950 degrees C and pressures up to 5 bar. The results show that the oxygen carrier exhibits high selectivity to oxidizing methane to syngas at the fuel stage with improved process performance with increasing temperature although carbon deposition could not be avoided. Co-feeding CO2 with CH4 at the fuel stage reduced carbon deposition significantly, thus reducing the syngas H-2/CO molar ratio from 3.75 to 1 (at CO2/CH4 ratio of 1 at 950 degrees C and 1 bar). The reduced carbon deposition has maximized the purity of the H-2 produced in the consecutive steam stage thus increasing the process attractiveness for the combined production of syngas and pure hydrogen. Interestingly, the cofeeding of CO2 with CH4 at the fuel stage showed a stable syngas production over 12 hours continuously and maintained the H-2/CO ratio at almost unity, suggesting that the oxygen carrier was exposed to simultaneous partial oxidation of CH4 with the lattice oxygen which was restored instantly by the incoming CO2. Furthermore, the addition of steam to the fuel stage could tune up the H-2/CO ratio beyond 3 without carbon deposition at H2O/ CH4 ratio of 1 at 950 degrees C and 1 bar; making the syngas from gas switching partial oxidation suitable for different downstream processes, for example, gas-to-liquid processes. The process was also demonstrated at higher pressures with over 70% fuel conversion achieved at 5 bar and 950 degrees C.
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