Hong Tao, Niu Zhenbin, Hu Xunxiang, Gmernicki Kevin, Cheng Shiwang, Fan Fei, Johnson J Casey, Hong Eunice, Mahurin Shannon, Jiang De-en, Long Brian, Mays Jimmy, Sokolov Alexei, Saito Tomonori
Department of Chemistry, University of Tennessee, Knoxville, TN, 37996, USA.
Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
ChemSusChem. 2015 Nov;8(21):3595-604. doi: 10.1002/cssc.201500903. Epub 2015 Oct 20.
The development of high-performance materials for carbon dioxide separation and capture will significantly contribute to a solution for climate change. Herein, (bicycloheptenyl)ethyl-terminated polydimethylsiloxane (PDMSPNB) membranes with varied cross-link densities were synthesized via ring-opening metathesis polymerization. The developed polymer membranes show higher permeability and better selectivity than those of conventional cross-linked PDMS membrane. The achieved performance (CO2 permeability≈6800 Barrer; CO2 /N2 selectivity≈14) is very promising for practical applications. The key to achieving this high performance is the use of an in situ cross-linking method for difunctional PDMS macromonomers, which provides lightly cross-linked membranes. By combining positron annihilation lifetime spectroscopy, broadband dielectric spectroscopy, and gas solubility measurements, key parameters necessary for achieving excellent performance have been elucidated.
用于二氧化碳分离和捕获的高性能材料的开发将极大地有助于解决气候变化问题。在此,通过开环易位聚合合成了具有不同交联密度的(双环庚烯基)乙基封端的聚二甲基硅氧烷(PDMSPNB)膜。所开发的聚合物膜比传统的交联PDMS膜具有更高的渗透率和更好的选择性。所实现的性能(CO₂渗透率≈6800巴雷;CO₂/N₂选择性≈14)对于实际应用非常有前景。实现这种高性能的关键是对双官能PDMS大分子单体使用原位交联方法,该方法可提供轻度交联的膜。通过结合正电子湮没寿命谱、宽带介电谱和气体溶解度测量,阐明了实现优异性能所需的关键参数。