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Combined Syngas and Hydrogen Production using Gas Switching Technology

合成气 甲烷 部分氧化 制氢 化学工程 氧气 氧化剂 化学 材料科学 蒸汽重整 有机化学 工程类
作者
Ambrose Ugwu,Abdelghafour Zaabout,Felix Donat,Geert van Diest,Knuth Albertsen,Christoph R. Müller,Shahriar Amini
出处
期刊:Industrial & Engineering Chemistry Research [American Chemical Society]
卷期号:60 (9): 3516-3531 被引量:19
标识
DOI:10.1021/acs.iecr.0c04335
摘要

This paper focuses on the experimental demonstration of a three-stage GST (gas switching technology) process (fuel, steam/CO2, and air stages) for syngas production from methane in the fuel stage and H2/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 °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 H2/CO molar ratio from 3.75 to 1 (at CO2/CH4 ratio of 1 at 950 °C and 1 bar). The reduced carbon deposition has maximized the purity of the H2 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 H2/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 H2/CO ratio beyond 3 without carbon deposition at H2O/CH4 ratio of 1 at 950 °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 °C.

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