School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive, Atlanta, Georgia 30332, USA.
J Am Chem Soc. 2012 Jul 4;134(26):10757-60. doi: 10.1021/ja303136e. Epub 2012 Jun 20.
The CO(2) adsorption characteristics of prototypical poly(ethyleneimine)/silica composite adsorbents can be drastically enhanced by altering the acid/base properties of the oxide support via incorporation of Zr into the silica support. Introduction of an optimal amount of Zr resulted in a significant improvement in the CO(2) capacity and amine efficiency under dilute (simulated flue gas) and ultradilute (simulated ambient air) conditions. Adsorption experiments combined with detailed characterization by thermogravimetric analysis, temperature-programmed desorption, and in situ FT-IR spectroscopy clearly demonstrate a stabilizing effect of amphoteric Zr sites that enhances the adsorbent capacity, regenerability, and stability over continued recycling. It is suggested that the important role of the surface properties of the oxide support in these polymer/oxide composite adsorbents has been largely overlooked and that the properties may be even further enhanced in the future by tuning the acid/base properties of the support.
通过在氧化硅载体中引入锆,可以显著改变氧化物载体的酸碱性质,从而极大地增强典型的聚乙烯亚胺/氧化硅复合吸附剂的 CO2 吸附特性。引入适量的锆可显著提高在稀(模拟烟道气)和超稀(模拟环境空气)条件下的 CO2 容量和胺效率。吸附实验结合热重分析、程序升温脱附以及原位傅里叶变换红外光谱的详细表征清楚地表明,两性 Zr 位的稳定作用增强了吸附剂的容量、可再生性和在持续循环中的稳定性。有人认为,在这些聚合物/氧化硅复合吸附剂中,氧化物载体的表面性质起着重要作用,但目前在很大程度上被忽视了,通过调整载体的酸碱性质,未来这些性质可能会进一步增强。