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Overcoming Synthetic Challenges: Solvent-Free Construction of a Cr-Phosphonate Framework with High Stability and Proton Conductivity.

Fan Yang,Zhiwen Shi,Lipeng Si,Zhengqing Zhang,Jing Ju,Junliang Sun,Xiaoge Wang,Chongli Zhong

Published 2025 in Journal of the American Chemical Society

ABSTRACT

The sustainable, green, solvent-free synthesis offers new pathways for constructing high-performance metal-organic frameworks (MOFs) that are challenging to access via conventional solution chemistry. Herein, using this approach, we synthesize a highly stable crystalline chromium-phosphonate MOF, TGU-20, while a different counterpart, TGU-30, was obtained in the solution with the same ligand and Cr3+ ion. Interestingly, the three-dimensional electron diffraction technique reveals that TGU-20 adopts a monodeprotonated bidentate phosphonate coordination mode, forming ultranarrow channels densely lined with proton-donating acid P-OH groups. In contrast, TGU-30 features a mixed mono/dideprotonated coordination, resulting in large channels with sparse P-OH sites. As a result, TGU-20 displays exceptional proton conductivity of over 10-2 S cm-1 at 100% RH with a very low activation energy of 0.10 eV, reaching record-high room-temperature proton conductivity among phosphonate MOFs and 2 orders of magnitude higher than that of TGU-30. Additionally, both MOFs exhibit high stability in harsh conditions, including highly concentrated strong acid. The solvent-free synthesis not only directly yields a chromium-phosphonate MOF for the first time but also opens a mild and green avenue for selectively tuning metal-ligand coordination in reticular chemistry.

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