Zhou Qiang, Liu Lan, Croiset Eric, Tan Zhongchao, Liu Qingcai, Yang Jian
College of Materials Science & Engineering, Chongqing University Chongqing China
Faculty of Engineering, University of Waterloo 200 University Avenue West Waterloo Ontario Canada N2L 3G1.
RSC Adv. 2019 Jun 27;9(35):20075-20086. doi: 10.1039/c9ra00164f. eCollection 2019 Jun 25.
The contribution of individual reactions to the overall heat of CO absorption, as well as conditions for solid NHHCO(s) formation in a chilled ammonia process (CAP) were studied using Aspen Plus at temperatures between 2 and 40 °C. The overall heat of absorption in the CAP first decreased and then increased with increasing CO loading. The increase in overall heat of absorption at high CO loading was found to be caused mostly by the prominent heat release from the formation of NHHCO(s). It was found that NHHCO(s) precipitation was promoted for conditions of CO loading above 0.7 mol CO/mol NH and temperatures less than 20 °C, which at the same time can dramatically increase the heat of CO absorption. As such, the CO loading is recommended to be around 0.6-0.7 mol CO/mol NH at temperatures below 20 °C, so that the overall absorption heat is at a low state (less than 60 kJ mol CO). It was also found that the overall heat of CO absorption did not change much with temperature when CO loading was less than 0.5 mol CO/mol NH, while, when the CO loading exceeded 0.7 mol CO/mol NH, the heat of absorption increased with decreasing temperature.
使用Aspen Plus在2至40°C的温度范围内,研究了各个反应对CO吸收总热量的贡献,以及在冷氨工艺(CAP)中形成固体NHHCO(s)的条件。CAP中的总吸收热量随着CO负载量的增加先降低后升高。发现在高CO负载量下总吸收热量的增加主要是由于NHHCO(s)形成时显著的热量释放。研究发现,当CO负载量高于0.7 mol CO/mol NH且温度低于20°C时,会促进NHHCO(s)沉淀,这同时会显著增加CO吸收的热量。因此,建议在温度低于20°C时,CO负载量为0.6 - 0.7 mol CO/mol NH左右,以使总吸收热量处于较低水平(小于60 kJ mol CO)。还发现,当CO负载量小于0.5 mol CO/mol NH时,CO吸收的总热量随温度变化不大,而当CO负载量超过0.7 mol CO/mol NH时,吸收热量随温度降低而增加。