Armatas Gerasimos S, Kanatzidis Mercouri G
Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, USA.
Nat Mater. 2009 Mar;8(3):217-22. doi: 10.1038/nmat2381. Epub 2009 Feb 15.
Mesoporous materials with tunable non-oxidic framework compositions can exhibit new kinds of functionality including internal surfaces with high polarizability. As the chemical and physical characteristics of the framework components can induce useful catalytic, absorption and optoelectronic features, the mesoporous structure can promote fast mass diffusion kinetics and size-selective transport of guest molecules. So far, synthetic efforts have resulted in mesoporous metal chalcogenides on using structure-directing moulds of soft or hard templates. These include ordered mesoporous II-VI semiconductors (such as CdS (refs 2,3), ZnS (ref. 4) and CdTe (ref. 5)). Recently, template-free synthetic routes for high-surface-area chalcogenide aerogels have been reported. Here, we describe a novel kind of porous materials based on germanium-rich chalcogenide networks and 'soft' highly polarizable surfaces. We demonstrate that these materials can exhibit excellent selectivity for separating hydrogen from carbon dioxide and methane. These highly polarizable mesoporous structures have important implications for membrane-based gas separation process technologies including hydrogen purification.
具有可调节非氧化物骨架组成的介孔材料可展现出新型功能，包括具有高极化率的内表面。由于骨架成分的化学和物理特性能够引发有用的催化、吸附及光电特性，介孔结构可促进客体分子的快速质量扩散动力学和尺寸选择性传输。到目前为止，通过使用软模板或硬模板的结构导向模具，合成工作已制备出介孔金属硫族化物。这些包括有序介孔II-VI族半导体（如CdS（参考文献2,3）、ZnS（参考文献4）和CdTe（参考文献5））。最近，已报道了用于高表面积硫族化物气凝胶的无模板合成路线。在此，我们描述了一种基于富锗硫族化物网络和“软”高极化率表面的新型多孔材料。我们证明这些材料在从二氧化碳和甲烷中分离氢气时可表现出优异的选择性。这些高极化率的介孔结构对包括氢气纯化在内的基于膜的气体分离工艺技术具有重要意义。
