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Mesoporous germanium-rich chalcogenido frameworks with highly polarizable surfaces and relevance to gas separation

Nature Materials volume 8, pages 217–222 (2009)Cite this article

Abstract

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 molecules1. 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 reported6,7. 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.

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Figure 1: XRD and optical absorption spectra of mesostructured and mesoporous NU–GeQ-N.
Figure 2: TEM images of mesoporous NU–GeQ-N.
Figure 3: Nitrogen adsorption–desorption isotherms of mesoporous NU–GeQ-1 and NU–GeQ-2 materials.
Figure 4: Adsorption isotherms, heat of adsorption and gas mixture separation curves of mesoporous NU–GeQ-N.

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Acknowledgements

These studies were supported primarily by the Nanoscale Science and Engineering Initiative of the National Science Foundation under NSF Award Number EEC-0647560. We thank Peter C. Stair for the use of a mass-spectrometer gas analyser. This work made use of the J.B. Cohen X-ray Diffraction facility and the Electron Probe Instrumentation Center (EPIC) and Keck Interdisciplinary Surface Science (Keck-II) facility of NUANCE Center at Northwestern University.

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  1. Gerasimos S. Armatas

    Present address: Present address: Department of Materials Science and Technology, University of Crete, 71003 Heraklion, Greece,

Authors and Affiliations

  1. Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, USA

    Gerasimos S. Armatas & Mercouri G. Kanatzidis

  2. Materials Science Division, Argonne National Laboratory, Chicago, Illinois 60439, USA

    Mercouri G. Kanatzidis

Authors
  1. Gerasimos S. Armatas
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  2. Mercouri G. Kanatzidis
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Correspondence to Gerasimos S. Armatas or Mercouri G. Kanatzidis.

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Armatas, G., Kanatzidis, M. Mesoporous germanium-rich chalcogenido frameworks with highly polarizable surfaces and relevance to gas separation. Nature Mater 8, 217–222 (2009). https://doi.org/10.1038/nmat2381

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