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March 14, 2018Journal of the American Chemical Society268 citationsOpen Access

Fine Tuning and Specific Binding Sites with a Porous Hydrogen-Bonded Metal-Complex Framework for Gas Selective Separations

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ZBZongbi BaoDXDanyan XieGCGanggang Chang

Key Points

  • Develop a stable, permanently porous hydrogen-bonded metal-complex framework to achieve efficient and selective separation of acetylene from ethylene at room temperature.
  • Synthesized a microporous hydrogen-bonded metal-complex framework (HOF-21) combining coordination bonding with hydrogen-bonding networks.
  • Assessed gas separation performance for C2H2/C2H4 mixtures and tested framework regeneration via immersion in water and salt solutions.
  • Characterized gas-framework binding interactions and structural mechanisms using computational modeling and neutron powder diffraction experiments.
  • Achieved high C2H2/C2H4 separation selectivity at room temperature via pore-size sieving and specific hydrogen-bonding interactions between C2H2 and terminal SiF6(2-) sites.
  • Demonstrated complete restoration of the collapsed framework structure upon simple immersion in water or salt solution, establishing exceptional water stability for hydrogen-bonded frameworks.

Abstract

Research on hydrogen-bonded organic frameworks (HOFs) has been developed for quite a long time; however, those with both established permanent porosities and functional properties are extremely rare due to weak hydrogen-bonding interactions among molecular organic linkers, which are much more fragile and difficult to stabilize. Herein, through judiciously combining the superiority of both the moderately stable coordination bonds in metal-organic frameworks and hydrogen bonds, we have realized a microporous hydrogen-bonded metal-complex or metallotecton framework HOF-21, which not only shows permanent porosity, but also exhibits highly selective separation performance of C2H2/C2H4 at room temperature. The outstanding separation performance can be ascribed to sieving effect confined by the fine-tuning pores and the superimposed hydrogen-bonding interaction between C2H2 and SiF62- on both ends as validated by both modeling and neutron powder diffraction experiments. More importantly, the collapsed HOF-21 can be restored by simply immersing it into water or salt solution. To the best of our knowledge, such extraordinary water stability and restorability of HOF-21 were observed for the first time in HOFs, underlying the bright perspective of such new HOF materials for their industrial usage.

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Cite This Study

Bao et al. (2018) studied this question.

synapsesocial.com/papers/69df270fd9e0feb21c591ca3https://doi.org/10.1021/jacs.7b13706
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