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

Terban, Maxwell W.; Banerjee, Debasis; Ghose, Sanjit; Medasani, Bharat; Shukla, Anil; Legg, Benjamin A.; Zhou, Yufan; Zhu, Zihua; Sushko, Maria L.; De Yoreo, James J.; Liu, Jun; Thallapally, Praveen K.; Billinge, Simon J.  L.

doi:10.1039/C7NR07949D

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

Journal Article · Mon Feb 05 00:00:00 EST 2018 · Nanoscale

DOI:https://doi.org/10.1039/C7NR07949D· OSTI ID:1426463

^[1]; Banerjee, Debasis ^[2];

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^[2]; Shukla, Anil ^[4]; Legg, Benjamin A. ^[5]; Zhou, Yufan ^[4];

^[4];

^[2]; De Yoreo, James J. ^[5]; Liu, Jun ^[6];

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^[7]

Columbia Univ., New York, NY (United States). Dept. of Applied Physics and Applied Mathematics
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical and Computational Science Directorate
Brookhaven National Laboratory (BNL), Upton, NY (United States)National Synchrotron Light Source II (NSLS-II)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). W. R. Wiley Environmental Molecular Sciences Lab.
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical and Computational Science Directorate; Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy & Environment Directorate
Columbia Univ., New York, NY (United States). Dept. of Applied Physics and Applied Mathematics; Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)National Synchrotron Light Source II (NSLS-II)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Biological and Environmental Research (BER); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; AC05-76RL01830

OSTI ID:: 1426463

Report Number(s):: BNL-203353-2018-JAAM; NANOHL; TRN: US1802290

Journal Information:: Nanoscale, Vol. 10, Issue 9; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 43 works

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