Continuous structure modification of metal-organic framework glasses via halide salts

Abstract Melting and glass formation of metal-organic frameworks (MOFs) allow them to be processed into bulk materials. However, two major challenges remain: only a small fraction of MOF crystals undergo melting and glass-formation, and no well-established strategies exist for tuning MOF glass struc...

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Main Authors: Fengming Cao, Søren S. Sørensen, Anders K. R. Christensen, Samraj Mollick, Xuan Ge, Daming Sun, Anders B. Nielsen, Niels Chr. Nielsen, Nina Lock, Ronghui Lu, Rebekka Klemmt, Peter K. Kristensen, Lars R. Jensen, Francesco Dallari, Jacopo Baglioni, Giulio Monaco, Martin A. Karlsen, Volodymyr Baran, Morten M. Smedskjaer
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-62143-9
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author Fengming Cao
Søren S. Sørensen
Anders K. R. Christensen
Samraj Mollick
Xuan Ge
Daming Sun
Anders B. Nielsen
Niels Chr. Nielsen
Nina Lock
Ronghui Lu
Rebekka Klemmt
Peter K. Kristensen
Lars R. Jensen
Francesco Dallari
Jacopo Baglioni
Giulio Monaco
Martin A. Karlsen
Volodymyr Baran
Morten M. Smedskjaer
author_facet Fengming Cao
Søren S. Sørensen
Anders K. R. Christensen
Samraj Mollick
Xuan Ge
Daming Sun
Anders B. Nielsen
Niels Chr. Nielsen
Nina Lock
Ronghui Lu
Rebekka Klemmt
Peter K. Kristensen
Lars R. Jensen
Francesco Dallari
Jacopo Baglioni
Giulio Monaco
Martin A. Karlsen
Volodymyr Baran
Morten M. Smedskjaer
author_sort Fengming Cao
collection DOAJ
description Abstract Melting and glass formation of metal-organic frameworks (MOFs) allow them to be processed into bulk materials. However, two major challenges remain: only a small fraction of MOF crystals undergo melting and glass-formation, and no well-established strategies exist for tuning MOF glass structures and properties. Here, we address both challenges through co-melting of zeolitic imidazole frameworks (ZIFs), a subset of MOFs, with heterocycle-based halide salts. The salt acts as a chemical “modifier”, akin to the role of alkali modifiers in traditional silicate glasses, e.g., allowing the melting of ZIF-8 that otherwise decomposes prior to melting. Through experimental and computational analyses, we show that the salts depolymerize the ZIFs, enabling continuous tuning of the fraction of bridging to non-bridging imidazolate linkers and, thereby, the thermal and mechanical properties. The proposed strategy enables diversification of MOF glass chemistry, tunable structures and properties, and ultimately an increased number of glass-forming MOFs with improved functionalities.
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spelling doaj-art-eb37eaf83e92482aafde0b018c1f49ec2025-08-20T03:43:00ZengNature PortfolioNature Communications2041-17232025-07-0116111210.1038/s41467-025-62143-9Continuous structure modification of metal-organic framework glasses via halide saltsFengming Cao0Søren S. Sørensen1Anders K. R. Christensen2Samraj Mollick3Xuan Ge4Daming Sun5Anders B. Nielsen6Niels Chr. Nielsen7Nina Lock8Ronghui Lu9Rebekka Klemmt10Peter K. Kristensen11Lars R. Jensen12Francesco Dallari13Jacopo Baglioni14Giulio Monaco15Martin A. Karlsen16Volodymyr Baran17Morten M. Smedskjaer18Department of Chemistry and Bioscience, Aalborg UniversityDepartment of Chemistry and Bioscience, Aalborg UniversityDepartment of Chemistry and Bioscience, Aalborg UniversityDepartment of Chemistry and Bioscience, Aalborg UniversityDepartment of Chemistry and Bioscience, Aalborg UniversityDepartment of Chemistry and Bioscience, Aalborg UniversityDepartment of Chemistry, Aarhus UniversityDepartment of Chemistry, Aarhus UniversityInterdisciplinary Nanoscience Center (iNANO), Aarhus UniversityInterdisciplinary Nanoscience Center (iNANO), Aarhus UniversityInterdisciplinary Nanoscience Center (iNANO), Aarhus UniversityDepartment of Materials and Production, Aalborg UniversityDepartment of Materials and Production, Aalborg UniversityDepartment of Physics and Astronomy ‘Galileo Galilei’, University of PadovaDepartment of Physics and Astronomy ‘Galileo Galilei’, University of PadovaDepartment of Physics and Astronomy ‘Galileo Galilei’, University of PadovaDeutsches-Elektronen Synchrotron (DESY)Deutsches-Elektronen Synchrotron (DESY)Department of Chemistry and Bioscience, Aalborg UniversityAbstract Melting and glass formation of metal-organic frameworks (MOFs) allow them to be processed into bulk materials. However, two major challenges remain: only a small fraction of MOF crystals undergo melting and glass-formation, and no well-established strategies exist for tuning MOF glass structures and properties. Here, we address both challenges through co-melting of zeolitic imidazole frameworks (ZIFs), a subset of MOFs, with heterocycle-based halide salts. The salt acts as a chemical “modifier”, akin to the role of alkali modifiers in traditional silicate glasses, e.g., allowing the melting of ZIF-8 that otherwise decomposes prior to melting. Through experimental and computational analyses, we show that the salts depolymerize the ZIFs, enabling continuous tuning of the fraction of bridging to non-bridging imidazolate linkers and, thereby, the thermal and mechanical properties. The proposed strategy enables diversification of MOF glass chemistry, tunable structures and properties, and ultimately an increased number of glass-forming MOFs with improved functionalities.https://doi.org/10.1038/s41467-025-62143-9
spellingShingle Fengming Cao
Søren S. Sørensen
Anders K. R. Christensen
Samraj Mollick
Xuan Ge
Daming Sun
Anders B. Nielsen
Niels Chr. Nielsen
Nina Lock
Ronghui Lu
Rebekka Klemmt
Peter K. Kristensen
Lars R. Jensen
Francesco Dallari
Jacopo Baglioni
Giulio Monaco
Martin A. Karlsen
Volodymyr Baran
Morten M. Smedskjaer
Continuous structure modification of metal-organic framework glasses via halide salts
Nature Communications
title Continuous structure modification of metal-organic framework glasses via halide salts
title_full Continuous structure modification of metal-organic framework glasses via halide salts
title_fullStr Continuous structure modification of metal-organic framework glasses via halide salts
title_full_unstemmed Continuous structure modification of metal-organic framework glasses via halide salts
title_short Continuous structure modification of metal-organic framework glasses via halide salts
title_sort continuous structure modification of metal organic framework glasses via halide salts
url https://doi.org/10.1038/s41467-025-62143-9
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