Cargando…

Experimentally Validated Ab Initio Crystal Structure Prediction of Novel Metal–Organic Framework Materials

[Image: see text] First-principles crystal structure prediction (CSP) is the most powerful approach for materials discovery, enabling the prediction and evaluation of properties of new solid phases based only on a diagram of their underlying components. Here, we present the first CSP-based discovery...

Descripción completa

Detalles Bibliográficos
Autores principales: Xu, Yizhi, Marrett, Joseph M., Titi, Hatem M., Darby, James P., Morris, Andrew J., Friščić, Tomislav, Arhangelskis, Mihails
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9936577/
https://www.ncbi.nlm.nih.gov/pubmed/36719794
http://dx.doi.org/10.1021/jacs.2c12095
_version_ 1784890260041236480
author Xu, Yizhi
Marrett, Joseph M.
Titi, Hatem M.
Darby, James P.
Morris, Andrew J.
Friščić, Tomislav
Arhangelskis, Mihails
author_facet Xu, Yizhi
Marrett, Joseph M.
Titi, Hatem M.
Darby, James P.
Morris, Andrew J.
Friščić, Tomislav
Arhangelskis, Mihails
author_sort Xu, Yizhi
collection PubMed
description [Image: see text] First-principles crystal structure prediction (CSP) is the most powerful approach for materials discovery, enabling the prediction and evaluation of properties of new solid phases based only on a diagram of their underlying components. Here, we present the first CSP-based discovery of metal–organic frameworks (MOFs), offering a broader alternative to conventional techniques, which rely on geometry, intuition, and experimental screening. Phase landscapes were calculated for three systems involving flexible Cu(II) nodes, which could adopt a potentially limitless number of network topologies and are not amenable to conventional MOF design. The CSP procedure was validated experimentally through the synthesis of materials whose structures perfectly matched those found among the lowest-energy calculated structures and whose relevant properties, such as combustion energies, could immediately be evaluated from CSP-derived structures.
format Online
Article
Text
id pubmed-9936577
institution National Center for Biotechnology Information
language English
publishDate 2023
publisher American Chemical Society
record_format MEDLINE/PubMed
spelling pubmed-99365772023-02-18 Experimentally Validated Ab Initio Crystal Structure Prediction of Novel Metal–Organic Framework Materials Xu, Yizhi Marrett, Joseph M. Titi, Hatem M. Darby, James P. Morris, Andrew J. Friščić, Tomislav Arhangelskis, Mihails J Am Chem Soc [Image: see text] First-principles crystal structure prediction (CSP) is the most powerful approach for materials discovery, enabling the prediction and evaluation of properties of new solid phases based only on a diagram of their underlying components. Here, we present the first CSP-based discovery of metal–organic frameworks (MOFs), offering a broader alternative to conventional techniques, which rely on geometry, intuition, and experimental screening. Phase landscapes were calculated for three systems involving flexible Cu(II) nodes, which could adopt a potentially limitless number of network topologies and are not amenable to conventional MOF design. The CSP procedure was validated experimentally through the synthesis of materials whose structures perfectly matched those found among the lowest-energy calculated structures and whose relevant properties, such as combustion energies, could immediately be evaluated from CSP-derived structures. American Chemical Society 2023-01-31 /pmc/articles/PMC9936577/ /pubmed/36719794 http://dx.doi.org/10.1021/jacs.2c12095 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Xu, Yizhi
Marrett, Joseph M.
Titi, Hatem M.
Darby, James P.
Morris, Andrew J.
Friščić, Tomislav
Arhangelskis, Mihails
Experimentally Validated Ab Initio Crystal Structure Prediction of Novel Metal–Organic Framework Materials
title Experimentally Validated Ab Initio Crystal Structure Prediction of Novel Metal–Organic Framework Materials
title_full Experimentally Validated Ab Initio Crystal Structure Prediction of Novel Metal–Organic Framework Materials
title_fullStr Experimentally Validated Ab Initio Crystal Structure Prediction of Novel Metal–Organic Framework Materials
title_full_unstemmed Experimentally Validated Ab Initio Crystal Structure Prediction of Novel Metal–Organic Framework Materials
title_short Experimentally Validated Ab Initio Crystal Structure Prediction of Novel Metal–Organic Framework Materials
title_sort experimentally validated ab initio crystal structure prediction of novel metal–organic framework materials
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9936577/
https://www.ncbi.nlm.nih.gov/pubmed/36719794
http://dx.doi.org/10.1021/jacs.2c12095
work_keys_str_mv AT xuyizhi experimentallyvalidatedabinitiocrystalstructurepredictionofnovelmetalorganicframeworkmaterials
AT marrettjosephm experimentallyvalidatedabinitiocrystalstructurepredictionofnovelmetalorganicframeworkmaterials
AT titihatemm experimentallyvalidatedabinitiocrystalstructurepredictionofnovelmetalorganicframeworkmaterials
AT darbyjamesp experimentallyvalidatedabinitiocrystalstructurepredictionofnovelmetalorganicframeworkmaterials
AT morrisandrewj experimentallyvalidatedabinitiocrystalstructurepredictionofnovelmetalorganicframeworkmaterials
AT friscictomislav experimentallyvalidatedabinitiocrystalstructurepredictionofnovelmetalorganicframeworkmaterials
AT arhangelskismihails experimentallyvalidatedabinitiocrystalstructurepredictionofnovelmetalorganicframeworkmaterials