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Understanding disorder and linker deficiency in porphyrinic zirconium-based metal-organic frameworks by resolving the ZrO cluster conundrum in PCN-221. | LitMetric

AI Article Synopsis

Article Abstract

Porphyrin-based metal-organic frameworks (MOFs), exemplified by MOF-525, PCN-221, and PCN-224, are promising systems for catalysis, optoelectronics, and solar energy conversion. However, subtle differences between synthetic protocols for these three MOFs give rise to vast discrepancies in purported product outcomes and description of framework topologies. Here, based on a comprehensive synthetic and structural analysis spanning local and long-range length scales, we show that PCN-221 consists of ZrO(OH) clusters in four distinct orientations within the unit cell, rather than ZrO clusters as originally published, and linker vacancies at levels of around 50%, which may form in a locally correlated manner. We propose disordered PCN-224 (dPCN-224) as a unified model to understand PCN-221, MOF-525, and PCN-224 by varying the degree of orientational cluster disorder, linker conformation and vacancies, and cluster-linker binding. Our work thus introduces a new perspective on network topology and disorder in Zr-MOFs and pinpoints the structural variables that direct their functional properties.

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Source
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8149457PMC
http://dx.doi.org/10.1038/s41467-021-23348-wDOI Listing

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