Ugwu Ambrose, Zaabout Abdelghafour, Donat Felix, van Diest Geert, Albertsen Knuth, Müller Christoph, Amini Shahriar
Department of Energy and Process Engineering, Norwegian University of Science and Technology, Trondheim, 7491, Norway.
Process Technology Department, SINTEF Industry, Trondheim, 7465, Norway.
Ind Eng Chem Res. 2021 Mar 10;60(9):3516-3531. doi: 10.1021/acs.iecr.0c04335. Epub 2021 Feb 28.
This paper focuses on the experimental demonstration of a three-stage GST (gas switching technology) process (fuel, steam/CO, and air stages) for syngas production from methane in the fuel stage and H/CO production in the steam/CO stage using a lanthanum-based oxygen carrier (LaSrFeAlO). 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 CO with CH at the fuel stage reduced carbon deposition significantly, thus reducing the syngas H/CO molar ratio from 3.75 to 1 (at CO/CH ratio of 1 at 950 °C and 1 bar). The reduced carbon deposition has maximized the purity of the H produced in the consecutive steam stage thus increasing the process attractiveness for the combined production of syngas and pure hydrogen. Interestingly, the cofeeding of CO with CH at the fuel stage showed a stable syngas production over 12 hours continuously and maintained the H/CO ratio at almost unity, suggesting that the oxygen carrier was exposed to simultaneous partial oxidation of CH with the lattice oxygen which was restored instantly by the incoming CO. Furthermore, the addition of steam to the fuel stage could tune up the H/CO ratio beyond 3 without carbon deposition at HO/CH 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.
本文重点介绍了一种三段式GST(气体切换技术)工艺(燃料、蒸汽/CO和空气段)的实验演示,该工艺用于在燃料段由甲烷生产合成气,并在蒸汽/CO段使用镧基氧载体(LaSrFeAlO)生产H/CO。实验在750 - 950℃的温度和高达5巴的压力下进行。结果表明,氧载体在燃料段对将甲烷氧化为合成气具有高选择性,随着温度升高工艺性能有所改善,尽管无法避免积碳。在燃料段将CO与CH共进料可显著减少积碳,从而使合成气的H/CO摩尔比从3.75降至1(在950℃和1巴下CO/CH比为1时)。积碳的减少使后续蒸汽段产生的H的纯度最大化,从而提高了该工艺对合成气和纯氢联合生产的吸引力。有趣的是,在燃料段将CO与CH共进料在连续12小时内显示出稳定的合成气生产,并将H/CO比维持在几乎为1,这表明氧载体同时经历了CH与晶格氧的部分氧化,而晶格氧会被进入的CO立即恢复。此外,在燃料段添加蒸汽可将H/CO比调节至3以上,在950℃和1巴下H₂O/CH比为1时无积碳;使得气体切换部分氧化产生的合成气适用于不同的下游工艺,例如气制液工艺。该工艺在更高压力下也得到了演示,在5巴和950℃下实现了超过70%的燃料转化率。