School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA 30332, USA.
ChemSusChem. 2011 May 23;4(5):628-35. doi: 10.1002/cssc.201000355. Epub 2011 May 5.
Silica supported poly(ethyleneimine) (PEI) materials are prepared via impregnation and demonstrated to be promising adsorbents for CO(2) capture from ultra-dilute gas streams such as ambient air. A prototypical class 1 adsorbent, containing 45 wt% PEI (PEI/silica), and two new modified PEI-based aminosilica adsorbents, derived from PEI modified with 3-aminopropyltrimethoxysilane (A-PEI/silica) or tetraethyl orthotitanate (T-PEI/silica), are prepared and characterized by using thermogravimetric analysis and FTIR spectroscopy. The modifiers are shown to enhance the thermal stability of the polymer-oxide composites, leading to higher PEI decomposition temperatures. The modified adsorbents present extremely high CO(2) adsorption capacities under conditions simulating ambient air (400 ppm CO(2) in inert gas), exceeding 2 mol(CO (2)) kg(sorbent)(-1), as well as enhanced adsorption kinetics compared to conventional class 1 sorbents. The new adsorbents show excellent stability in cyclic adsorption-desorption operations, even under dry conditions in which aminosilica adsorbents are known to lose capacity due to urea formation. Thus, the adsorbents of this type can be considered promising materials for the direct capture of CO(2) from ultra-dilute gas streams such as ambient air.
采用浸渍法制备了负载在二氧化硅上的聚(亚乙基亚胺)(PEI)材料,它们被证明是从环境空气中等超低浓度气流中捕获 CO2 的有前途的吸附剂。一种典型的 1 类吸附剂,含有 45wt%的 PEI(PEI/二氧化硅),以及两种新的基于改性 PEI 的氨基硅基吸附剂,由用 3-氨丙基三甲氧基硅烷(A-PEI/二氧化硅)或原钛酸四乙酯(T-PEI/二氧化硅)改性的 PEI 制备,并通过热重分析和傅里叶变换红外光谱进行了表征。结果表明,改性剂提高了聚合物-氧化物复合材料的热稳定性,导致 PEI 分解温度升高。在模拟环境空气(惰性气体中 400ppm CO2)的条件下,改性吸附剂表现出极高的 CO2 吸附容量,超过 2mol(CO2)kg(吸附剂)-1,与传统的 1 类吸附剂相比,吸附动力学也得到了增强。即使在干燥条件下,即在氨基硅基吸附剂由于脲形成而失去容量的情况下,新型吸附剂在循环吸附-解吸操作中也表现出极好的稳定性。因此,这类吸附剂可被视为从环境空气等超低浓度气流中直接捕获 CO2 的有前途的材料。