Mechanochemical Solid Form Screening of Zeolitic Imidazolate Frameworks Using Structure-Directing Liquid Additives Article Swipe

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Ivana Brekalo , Katarina Lisac , Joseph R. Ramirez , Petra Pongrac , Andreas Puškarić , Srećko Valić , Yizhi Xu , M.J. Ferguson , Joseph M. Marrett , Mihails Arhangelskis , Tomislav Friščić , K.T. Holman ·

YOU? · · 2025 · Open Access · · DOI: https://doi.org/10.1021/jacs.5c04043

We demonstrate a systematic application of the mechanochemical liquid-assisted grinding (LAG) methodology to screen for forms of zinc imidazolate (ZnIm₂), of fundamental importance as the simplest member of the zeolitic imidazolate framework materials family. The exploration of 45 different liquid additives, selected based on their molecular structure and physicochemical properties has resulted in eight different ZnIm₂ topological forms, appearing in 13 crystallographically distinct solid forms (including two previously unknown forms of the crb (BCT) topology), amorphous phases, and the interrupted moc-Zn₄Im₈HIm. All prepared topological forms were also explored computationally, using dispersion-corrected periodic density functional theory (DFT) calculations, enabling the rationalization of screening outcomes, and setting the stage for future prediction of additive-directed metal-organic framework (MOF) synthesis. This first systematic exploration of LAG in screening for three-dimensional MOFs demonstrates the potential of the liquid additive to not only accelerate materials synthesis, but also to direct it toward topologically different MOFs. The discovery of novel forms of a material that already exhibits at least 21 crystallographically and functionally different forms provides a strong testimony on the power of mechanochemistry in metal-organic materials discovery.

Related Topics

Metal–Organic Framework

Adsorption

Polymer

Engineering

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Chemistry Zeolitic imidazolate framework Imidazolate Liquid crystalline Chemical engineering Organic chemistry Metal-organic framework Adsorption Polymer Engineering

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Type: article
Language: en
Landing Page: https://doi.org/10.1021/jacs.5c04043
OA Status: hybrid
Cited By: 1
References: 130
Related Works: 10
OpenAlex ID: https://openalex.org/W4412643206

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DOI: https://doi.org/10.1021/jacs.5c04043

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Title: Mechanochemical Solid Form Screening of Zeolitic Imidazolate Frameworks Using Structure-Directing Liquid Additives

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Language: en

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Publication year: 2025

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Publication date: 2025-07-24

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Authors: Ivana Brekalo, Katarina Lisac, Joseph R. Ramirez, Petra Pongrac, Andreas Puškarić, Srećko Valić, Yizhi Xu, M.J. Ferguson, Joseph M. Marrett, Mihails Arhangelskis, Tomislav Friščić, K.T. Holman

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Landing page: https://doi.org/10.1021/jacs.5c04043

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Concepts: Chemistry, Zeolitic imidazolate framework, Imidazolate, Liquid crystalline, Chemical engineering, Organic chemistry, Metal-organic framework, Adsorption, Polymer, Engineering

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Cited by: 1

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