Labreche Ying, Fan Yanfang, Rezaei Fateme, Lively Ryan P, Jones Christopher W, Koros William J
School of Chemical & Biomolecular Engineering, Georgia Institute of Technology , 311 Ferst Drive NW, Atlanta, Georgia 30332-0100, United States.
ACS Appl Mater Interfaces. 2014 Nov 12;6(21):19336-46. doi: 10.1021/am505419w. Epub 2014 Oct 14.
Amine-loaded poly(amide-imide) (PAI)/silica hollow fiber sorbents are created and used in a rapid temperature swing adsorption (RTSA) system for CO2 capture under simulated postcombustion flue gas conditions. Poly(ethylenimine) (PEI) is infused into the PAI/mesoporous silica hollow fiber sorbents during fiber solvent exchange steps after fiber spinning. A lumen-side barrier layer is also successfully formed on the bore side of PAI/silica hollow fiber sorbents by using a mixture of Neoprene with cross-linking agents in a post-treatment process. The amine loaded fibers are tested in shell-and-tube modules by exposure on the shell side at 1 atm and 35 °C to simulated flue gas with an inert tracer (14 mol % CO2, 72 mol % N2, and 14 mol % He, at 100% relative humidity (RH)). The fibers show a breakthrough CO2 capacity of 0.85 mmol/g-fiber and a pseudoequilibrium CO2 uptake of 1.19 mmol/g-fiber. When tested in the temperature range of 35-75 °C, the PAI/silica/PEI fiber sorbents show a maximum CO2 capacity at 65 °C, owing to a trade-off between thermodynamic and kinetic factors. To overcome mass transfer limitations in rigidified PEI infused in the silica, an alternate PEI infusion method using a glycerol/PEI/methanol mixture is developed, and the CO2 sorption performance is improved significantly, effectively doubling the functional sorption capacity. Specifically, the glycerol-plasticized sorbents are found to have a breakthrough and equilibrium CO2 capacity of 1.3 and 2.0 mmol/g of dry fiber sorbent at 35 °C, respectively. Thus, this work demonstrates two PAI-based sorbents that are optimized for different sorption conditions with the PAI/silica/PEI sorbents operating effectively at 65 °C and the PAI/silica/PEI-glycerol sorbents operating well at 35 °C with significantly improved sorption capacity.
制备了负载胺的聚(酰胺 - 酰亚胺)(PAI)/二氧化硅中空纤维吸附剂,并将其用于快速变温吸附(RTSA)系统中,以在模拟燃烧后烟道气条件下捕集二氧化碳。在纤维纺丝后的纤维溶剂交换步骤中,将聚乙二胺(PEI)注入到PAI /介孔二氧化硅中空纤维吸附剂中。通过在处理后过程中使用氯丁橡胶与交联剂的混合物,还成功地在PAI /二氧化硅中空纤维吸附剂的孔道侧形成了内腔侧阻挡层。将负载胺的纤维在壳管式模块中进行测试,在1个大气压和35°C下,使壳侧暴露于含有惰性示踪剂(14摩尔%CO₂、72摩尔%N₂和14摩尔%He,相对湿度(RH)为100%)的模拟烟道气中。这些纤维的二氧化碳穿透容量为0.85 mmol / g - 纤维,假平衡二氧化碳吸收量为1.19 mmol / g - 纤维。当在35 - 75°C的温度范围内进行测试时,由于热力学和动力学因素之间的权衡,PAI /二氧化硅/ PEI纤维吸附剂在65°C时显示出最大的二氧化碳容量。为了克服注入二氧化硅中的刚性化PEI中的传质限制,开发了一种使用甘油/ PEI /甲醇混合物的替代PEI注入方法,并且二氧化碳吸附性能得到了显著改善,有效地使功能吸附容量增加了一倍。具体而言,发现甘油增塑的吸附剂在35°C下的二氧化碳穿透容量和平衡容量分别为1.3和2.0 mmol / g干纤维吸附剂。因此,这项工作展示了两种针对不同吸附条件进行优化的基于PAI的吸附剂,其中PAI /二氧化硅/ PEI吸附剂在65°C下有效运行,而PAI /二氧化硅/ PEI - 甘油吸附剂在35°C下运行良好,吸附容量显著提高。