Targeted Synthesis of a Highly Stable Aluminium Phosphonate Metal–Organic Framework Showing Reversible HCl Adsorption

A concept for obtaining isoreticular compounds with tri‐ instead of tetravalent metal cations using highly acidic reaction conditions was developed and successfully applied in a high throughput study using N,N′‐piperazinebis(methylenephosphonic acid) (H4PMP), that resulted in the discovery of a new...

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Veröffentlicht in:Angewandte Chemie International Edition Jg. 62; H. 26; S. e202303561 - n/a
Hauptverfasser: Reichenau, Timm M., Steinke, Felix, Wharmby, Michael T., Näther, Christian, Engesser, Tobias A., Stock, Norbert
Format: Journal Article
Sprache:Englisch
Veröffentlicht: Germany Wiley Subscription Services, Inc 26.06.2023
Ausgabe:International ed. in English
Schlagworte:
Adsorption
Aluminium Phosphonate
Aluminum
Aqueous solutions
Cations
Desorption
Framework Stability
HCl Adsorption
High-Throughput
Infrared spectroscopy
Metal ions
Metal-organic frameworks
Metal–Organic Framework
Phosphonates
Vapor phases
HCl Adsorption
High-Throughput
Metal-Organic Framework
Aluminium Phosphonate
Framework Stability
ISSN:1433-7851, 1521-3773, 1521-3773
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Zusammenfassung:A concept for obtaining isoreticular compounds with tri‐ instead of tetravalent metal cations using highly acidic reaction conditions was developed and successfully applied in a high throughput study using N,N′‐piperazinebis(methylenephosphonic acid) (H4PMP), that resulted in the discovery of a new porous aluminium phosphonate denoted CAU‐60⋅6 HCl. The high‐throughput study was subsequently extended to other trivalent metal ions. Al‐CAU‐60⋅6 HCl demonstrates reversible desorption of HCl (18.3 wt % loading) with three distinct compositions observed with zero, four or six HCl molecules per formula unit. Structural changes were followed in detail by powder X‐ray diffraction, EDX analysis as well as IR spectroscopy. Rapid desorption of HCl in water within minutes and subsequent adsorption from the gas phase and from aqueous solution are shown. Furthermore, it is possible to adsorb HBr into the guest free Al‐CAU‐60 framework, demonstrating the high stability of this compound. Protons make the difference. Highly acidic synthesis conditions were employed to synthesize porous MIII‐phosphonates with different degrees of framework protonation. Rapid release of HCl in solution and re‐adsorption from aqueous solution and from the gas phase is demonstrated and structural changes that accompany these processes are elucidated.
Bibliographie:These authors contributed equally to this work
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ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.202303561