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Early stage structural development of prototypical zeolitic imidazolate framework (ZIF) in solution

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Abstract

Given the wide-ranging potential applications of metal organic frameworks (MOFs), an emerging imperative is to understand their formation with atomic scale precision. This will aid in designing syntheses for next-generation MOFs with enhanced properties and functionalities. Major challenges are to characterize the early-stage seeds, and the pathways to framework growth, which require synthesis coupled with in situ structural characterization sensitive to nanoscale structures in solution. Here we report measurements of an in situ synthesis of a prototypical MOF, ZIF-8, utilizing synchrotron X-ray atomic pair distribution function (PDF) analysis optimized for sensitivity to dilute species, complemented by mass spectrometry, electron microscopy, and density functional theory calculations. We observe that despite rapid formation of the crystalline product, a high concentration of Zn(2-MeIm)4 (2-MeIm = 2-methylimidazolate) initially forms and persists as stable clusters over long times. A secondary, amorphous phase also pervades during the synthesis, which has a structural similarity to the final ZIF-8 and may act as an intermediate to the final product.

Graphical abstract: Early stage structural development of prototypical zeolitic imidazolate framework (ZIF) in solution

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Publication details

The article was received on 25 Oct 2017, accepted on 03 Feb 2018 and first published on 05 Feb 2018


Article type: Paper
DOI: 10.1039/C7NR07949D
Citation: Nanoscale, 2018, Advance Article
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    Early stage structural development of prototypical zeolitic imidazolate framework (ZIF) in solution

    M. W. Terban, D. Banerjee, S. Ghose, B. Medasani, A. Shukla, B. A. Legg, Y. Zhou, Z. Zhu, M. L. Sushko, J. J. De Yoreo, J. Liu, P. K. Thallapally and S. J. L. Billinge, Nanoscale, 2018, Advance Article , DOI: 10.1039/C7NR07949D

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