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Borohydride-containing coordination polymers: synthesis, air stability and dehydrogenation
Kentaro Kadota1, Nghia Tuan Duong2, Yusuke Nishiyama2,3
1Department of Molecular Engineering , Graduate School of Engineering , Kyoto University , Katsura, Nishikyo-ku , Kyoto 615-8510 , Japan.
Chemical Science
|July 31, 2019
Summary
Researchers developed new metal-organic frameworks to control hydride reactivity. One material, [Zn(BH4)2(dipyridylpropane)], shows excellent dehydrogenation and air stability, crucial for hydrogen storage applications.
Area of Science:
- Materials Science
- Inorganic Chemistry
- Solid-State Chemistry
Background:
- Controlling hydride (H-) reactivity in crystal structures is challenging due to its strong electron-donating nature and reactivity with protic species.
- Metal borohydrides face a trade-off between dehydrogenation activity and air stability, necessitating control over borohydride (BH4-) reactivity.
Purpose of the Study:
- To synthesize and characterize BH4--based coordination polymers and metal-organic frameworks (MOFs).
- To regulate the reactivity of BH4- within these structures by manipulating coordination geometry and neighboring ligands.
- To identify materials exhibiting both high dehydrogenation performance and air stability for potential hydrogen storage applications.
Main Methods:
- Synthesis of a series of BH4--based coordination polymers/MOFs.
- Single crystal X-ray diffraction analysis to elucidate structural features.
- Temperature-programmed desorption, in situ synchrotron Powder X-ray Diffraction (PXRD), and solid-state Nuclear Magnetic Resonance (NMR) for mechanistic studies.
Main Results:
- The reactivity of BH4- was successfully regulated by coordination geometry and ligand environment within the synthesized frameworks.
- [Zn(BH4)2(dipyridylpropane)] demonstrated high dehydrogenation reactivity (1.4 wt% at 179 °C) and remarkable air stability (50% RH at 25 °C for 7 days).
- Single crystal X-ray diffraction identified H···H dihydrogen interactions and close packing of hydrophobic ligands as critical factors for achieving both reactivity and stability.
Conclusions:
- Coordination polymers and MOFs offer a viable platform for controlling hydride reactivity in materials.
- The identified structural features, including dihydrogen bonding and ligand packing, are key to designing stable and active metal borohydride materials.
- The developed material shows promise for applications requiring controlled hydrogen release and storage.
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