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Carbon dioxide capture from fuel gas streams under elevated pressures and temperatures using novel physical solvents.

机译:使用新型物理溶剂,可在高压和高温下从燃气流中捕获二氧化碳。

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摘要

he conventional processes for acid gas removal (AGR), including CO 2 in the Integrated Gasification Combined Cycle (IGCC) power generation facilities are: a chemical process, using methyl-diethanolamine (MDEA); a physical process, using chilled methanol (Rectisol) or a physical process, using mixtures of dimethylethers of polyetheleneglycol (Selexol). These conventional processes require cooling of the fuel gas streams for CO2 capture and subsequent reheating before sending to turbines, which decreases the plant thermal efficiency and increases the overall cost. Thus, there is a pressing need for developing an economical process which can capture CO2 from the hot fuel gas stream without significant cooling.;The overall objective of this study is to investigate the potential use of physical solvents for selective capture of CO2 from post water-gas-shift streams under relatively elevated pressures and temperatures. In order to achieve this objective, a comprehensive literature review was conducted to define an "ideal solvent" for CO2 capture and to identify six different physical solvents which should obey such a definition.;The first physical solvents identified were perfluorocarbons (PFCs), which are known to have low reactivity, high chemical stability and relatively low vapor pressures. Three different PFCs, known as PP10, PP11, and PP25, were selected as potential candidates for CO2 capture. The equilibrium solubilities of CO2 and N2 were measured in these PFCs under different operating conditions up to 30 bar and 500 K. These PFCs have relatively low viscosity at 500 K, very good thermal and chemical stabilities and showed high CO2 solubilities; hence they were considered as "ideal solvents." The CO2 solubilities in PP25 were found to be greater than in the other two PFCs. Due to its superior behavior, PP25 was selected for the development of a conceptual process for CO 2 capture form Pittsburgh No. 8 shifted fuel gas mixture using Aspen Plus simulator. Unfortunately, during the pressure-swing option for solvent regeneration, the solvent loss was significant due to the fact that the boiling point of PP25 is 533 K which is close to the absorber temperature (500 K). Also, other drawbacks of PFCs include, high cost, and absorption of other gases (light hydrocarbons) along with CO2.;It was then decided to seek different physical solvents, which have negligible vapor pressure, in addition to the other attractive properties of the "ideal solvent" in order to use in the Aspen Plus simulator. Extensive literature search led to Ionic Liquids (ILs), which are known to have unique properties in addition to extremely low vapor pressures, and therefore they were considered excellent candidates for the CO2 capture from fuel gas streams under elevated pressures and temperatures. Three ILs, namely TEGO IL K5, TEGO IL P9 and TEGO IL P51P, manufactured by Evonik Goldschmidt Chemical Corporation, were selected as potential solvents for CO2 capture. The solubilities of CO2, H2, H2S and N2 were measured in the TEGO IL K5 and the solubilities of CO2 and H2 were measured in the TEGO IL K5 at pressures up to 30 bar and temperatures from 300 to 500 K. Also, the density and viscosity of these three ILs were measured within the same pressure and temperature ranges, and the surface tension for TEGO IL K5 and TEGO IL P51P were measured from 296 to 369 K. Due to their superior performance for CO2 capture, the TEGO IL K5 and the TEGO IL P51P were selected to be used in the Aspen simulator for the conceptual process development. The density and surface tension data for the TEGO IL K5 and the TEGO IL P51P were used in Aspen Plus, employing the Peng-Robinson Equation of state (P-R EOS) to obtain the critical properties of the two ILs; and the measured solubility data were also used to obtain the binary interaction parameters between the shifted gas constituents and two ILs.;The Aspen Plus simulator was employed to develop a conceptual process for CO2 capture from a shifted fuel gas stream (102.52 kg/s) generated using Pittsburgh
机译:整体气化联合循环(IGCC)发电设施中的酸性气体去除(AGR)包括CO 2的常规工艺包括:化学工艺,使用甲基二乙醇胺(MDEA);使用冷却甲醇(Rectisol)的物理过程,或使用聚乙二醇(Selexol)的二甲醚混合物的物理过程。这些常规方法需要冷却燃料气体流以用于CO 2捕集并随后在送入涡轮之前进行重新加热,这降低了设备的热效率并增加了总成本。因此,迫切需要开发一种经济的方法,该方法可以在不显着冷却的情况下从热燃气流中捕集CO2。这项研究的总体目标是研究潜在地使用物理溶剂从后水中选择性捕集CO2的方法。 -在相对升高的压力和温度下的气体变换物流。为了实现此目标,进行了全面的文献综述,以定义用于捕集CO2的“理想溶剂”并确定应遵循此定义的六种不同的物理溶剂。;首先确定的物理溶剂是全氟化碳(PFC),已知具有低反应性,高化学稳定性和相对低的蒸气压。选择了三种不同的PFC(称为PP10,PP11和PP25)作为捕获CO2的潜在候选物。在高达30 bar和500 K的不同操作条件下,在这些PFC中测量了CO2和N2的平衡溶解度。这些PFC在500 K下具有相对较低的粘度,非常好的热稳定性和化学稳定性,并显示出较高的CO2溶解度;因此,它们被认为是“理想的溶剂”。发现PP25中的CO2溶解度高于其他两种PFC。由于其优异的性能,PP25被选中用于开发使用Aspen Plus模拟器从匹兹堡8号转换后的燃气混合物中捕获CO 2的概念性方法。不幸的是,在用于溶剂再生的变压方案中,由于PP25的沸点为533 K(接近吸收塔温度(500 K)),因此溶剂损失显着。此外,PFC的其他缺点包括成本高以及与CO2一起吸收其他气体(轻烃)的问题;然后决定寻求除蒸气压可忽略的不同物理溶剂之外,还要考虑PFC的其他诱人特性。 “理想溶剂”以便在Aspen Plus仿真器中使用。广泛的文献搜索导致了离子液体(ILs),该离子液体除了极低的蒸气压外还具有独特的性能,因此,它们被认为是在升高的压力和温度下从燃气流中捕集CO2的极佳候选者。选择了由赢创戈德施密特化学公司生产的三种IL,即TEGO IL K5,TEGO IL P9和TEGO IL P51P作为捕获二氧化碳的潜在溶剂。在TEGO IL K5中测量了CO2,H2,H2S和N2的溶解度,在最高30 bar的压力和300至500 K的温度下,在TEGO IL K5中测量了CO2和H2的溶解度。在相同的压力和温度范围内测量了这三种IL的粘度,TEGO IL K5和TEGO IL P51P的表面张力在296至369 K范围内测量。由于它们对二氧化碳的捕获性能优异,因此TEGO IL K5和选择TEGO IL P51P在Aspen仿真器中用于概念性过程开发。 TEGO IL K5和TEGO IL P51P的密度和表面张力数据已在Aspen Plus中使用,并使用了彭-罗宾逊状态方程(P-R EOS)来获得两个IL的临界特性。并使用测得的溶解度数据获得转换后的气体成分与两个IL之间的二元相互作用参数。;使用Aspen Plus模拟器开发了从转换后的燃气流(102.52 kg / s)捕集CO2的概念性过程使用匹兹堡生成

著录项

  • 作者

    Heintz, Yannick Jacques.;

  • 作者单位

    University of Pittsburgh.;

  • 授予单位 University of Pittsburgh.;
  • 学科 Engineering Chemical.
  • 学位 Ph.D.
  • 年度 2011
  • 页码 305 p.
  • 总页数 305
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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