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Borohydride-containing coordination polymers: synthesis, air stability and dehydrogenation

Abstract

Control of the reactivity of hydride (H) in crystal structures has been a challenge because of its strong electron-donating ability and reactivity with protic species. For metal borohydrides, the dehydrogenation activity and air stability are in a trade-off, and control of the reactivity of BH4− has been demanded. For the purpose, we synthesize a series of BH4-based coordination polymers/metal–organic frameworks. The reactivity of BH4 in the structures is regulated by coordination geometry and neighboring ligands, and one of the compounds [Zn(BH4)2(dipyridylpropane)] exhibits both high dehydrogenation reactivity (1.4 wt% at 179 °C) and high air stability (50 RH% at 25 °C, 7 days). Single crystal X-ray diffraction analysis reveals that Hδ+···Hδ− dihydrogen interactions and close packing of hydrophobic ligands are the key for the reactivity and stability. The dehydrogenation mechanism is investigated by temperature-programmed desorption, in situ synchrotron PXRD and solid-state NMR.

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Publication details

The article was received on 12 Feb 2019, accepted on 11 May 2019 and first published on 13 May 2019


Article type: Edge Article
DOI: 10.1039/C9SC00731H
Chem. Sci., 2019, Accepted Manuscript
  • Open access: Creative Commons BY-NC license
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    Borohydride-containing coordination polymers: synthesis, air stability and dehydrogenation

    K. Kadota, N. T. Duong, Y. Nishiyama, E. Sivaniah, S. Kitagawa and S. Horike, Chem. Sci., 2019, Accepted Manuscript , DOI: 10.1039/C9SC00731H

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