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用于从环境空气中提取二氧化碳的蒸汽诱导聚乙烯亚胺浸渍γ-氧化铝吸附剂的结构变化。

Steam induced structural changes of a poly(ethylenimine) impregnated γ-alumina sorbent for CO2 extraction from ambient air.

作者信息

Sakwa-Novak Miles A, Jones Christopher W

机构信息

School of Chemical & Biomolecular Engineering, Georgia Institute of Technology , 311 Ferst Drive, Atlanta, Georgia 30332, United States.

出版信息

ACS Appl Mater Interfaces. 2014 Jun 25;6(12):9245-55. doi: 10.1021/am501500q. Epub 2014 Jun 4.

DOI:10.1021/am501500q
PMID:24896554
Abstract

Poly(ethylenimine) (PEI) impregnated mesoporous γ-alumina sorbents are utilized for CO2 adsorption from dry and humid simulated ambient air, and the sorbents are regenerated under an environment of flowing steam for times ranging from 5 min to 24 h of continuous exposure. The sorbents are compared on the basis of equilibrium CO2 capacities from simulated air at 400 ppm of CO2, 50% relative humidity, and 30 °C as well as their physiochemical characterization by means of X-ray diffraction (XRD), (27)Al NMR spectroscopy, IR spectroscopy, Raman spectroscopy, N2 physisorption, and elemental analysis. The sorbents retain better than 90% of the initial equilibrium capacity of ∼1.7 mmol/g at steam exposure times up to 12 h; however, PEI leaching reduced the capacity of the sorbent to 0.66 mmol/g after 24 h of continuous treatment. It is demonstrated that the γ-alumina support partially hydrates to form a boehmite crystal phase at steam times of 90 min and longer but that this phase transition occurs predominately between 90 min and 12 h of steam treatment, slowing at longer times of 12 and 24 h of treatment. Evidence is presented to suggest that the presence of boehmite on the sorbent surface does not significantly alter the amine efficiency of impregnated PEI. The collected results suggest that γ-alumina/PEI composite materials are promising sorbents for CO2 capture from ambient air with regeneration in flowing steam.

摘要

聚乙二胺(PEI)浸渍的介孔γ-氧化铝吸附剂用于从干燥和潮湿的模拟环境空气中吸附二氧化碳,并且吸附剂在流动蒸汽环境下连续暴露5分钟至24小时进行再生。基于在400 ppm二氧化碳、50%相对湿度和30°C的模拟空气中的平衡二氧化碳吸附量以及通过X射线衍射(XRD)、(27)Al核磁共振光谱、红外光谱、拉曼光谱、N2物理吸附和元素分析进行的物理化学表征,对吸附剂进行了比较。在蒸汽暴露时间长达12小时时,吸附剂保留了约1.7 mmol/g初始平衡容量的90%以上;然而,连续处理24小时后,PEI浸出使吸附剂的容量降至0.66 mmol/g。结果表明,γ-氧化铝载体在蒸汽处理90分钟及更长时间时会部分水合形成勃姆石晶相,但这种相变主要发生在蒸汽处理90分钟至12小时之间,在12小时和24小时的较长处理时间时减缓。有证据表明吸附剂表面勃姆石的存在不会显著改变浸渍PEI的胺效率。收集的结果表明,γ-氧化铝/PEI复合材料是从环境空气中捕获二氧化碳并在流动蒸汽中再生的有前景的吸附剂。

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