Pang Simon H, Lively Ryan P, Jones Christopher W
School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive, Atlanta, GA, 30332, USA.
ChemSusChem. 2018 Aug 9;11(15):2628-2637. doi: 10.1002/cssc.201800438. Epub 2018 Jul 9.
Aminopolymer-based solid sorbents have been widely investigated for the capture of CO from dilute streams such as flue gas or ambient air. However, the oxidative stability of the widely studied aminopolymer, poly(ethylenimine) (PEI), is limited, causing it to lose its CO capture capacity after exposure to oxygen at elevated temperatures. Here, we demonstrate the use of linear poly(propylenimine) (PPI), synthesized through a simple cationic ring-opening polymerization, as a more oxidatively stable alternative to PEI with high CO capacity and amine efficiency. The performance of linear PPI/SBA-15 composites was investigated over a range of CO capture conditions (CO partial pressure, adsorption temperature) to examine the tradeoff between adsorption capacity and sorption-site accessibility, which was expected to be more limited in linear polymers relative to the prototypical hyperbranched PEI. Linear PPI/SBA-15 composites were more efficient at CO capture and retained 65-83 % of their CO capacity after exposure to a harsh oxidative treatment, compared to 20-40 % retention for linear PEI. Additionally, we demonstrated long-term stability of linear PPI sorbents over 50 adsorption/desorption cycles with no loss in performance. Combined with other strategies for improving the oxidative stability and adsorption kinetics, linear PPI may play a role as a component of stable solid adsorbents in commercial applications for CO capture.
基于氨基聚合物的固体吸附剂已被广泛研究用于从烟道气或环境空气等稀气流中捕获一氧化碳。然而,广泛研究的氨基聚合物聚乙烯亚胺(PEI)的氧化稳定性有限,导致其在高温下暴露于氧气后失去一氧化碳捕获能力。在此,我们展示了通过简单的阳离子开环聚合合成的线性聚丙撑亚胺(PPI)作为PEI的一种氧化稳定性更高的替代品,具有高一氧化碳捕获能力和胺效率。研究了线性PPI/SBA - 15复合材料在一系列一氧化碳捕获条件(一氧化碳分压、吸附温度)下的性能,以考察吸附容量和吸附位点可及性之间的权衡,预计相对于典型的超支化PEI,线性聚合物中的这种权衡更为有限。线性PPI/SBA - 15复合材料在一氧化碳捕获方面更高效,在经过苛刻的氧化处理后保留了其65 - 83%的一氧化碳捕获能力,而线性PEI的保留率为20 - 40%。此外,我们证明了线性PPI吸附剂在50次吸附/解吸循环中的长期稳定性,性能无损失。结合其他提高氧化稳定性和吸附动力学的策略,线性PPI可能在一氧化碳捕获的商业应用中作为稳定固体吸附剂的一个组成部分发挥作用。