Virtual High Throughput Screening Confirmed Experimentally: Porous Coordination Polymer Hydration
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- 7 October 2009
- journal article
- research article
- Published by American Chemical Society (ACS) in Journal of the American Chemical Society
- Vol. 131 (43), 15834-15842
- https://doi.org/10.1021/ja9061344
Abstract
Hydrothermal stability is a pertinent issue to address for many industrial applications where percent levels of water can be present at temperatures ranging from subambient to several hundred degrees. Our objective is to understand relative stabilities of MOF materials through experimental testing combined with molecular modeling. This will enable the ultimate design of materials with improved hydrothermal stability, while maintaining the properties of interest. The tools that we have employed for these studies include quantum mechanical calculations based upon cluster models and combinatorial steaming methods whereby a steam stability map was formulated according to the relative stability of different materials. The experimental steaming method allows for high throughput screening of materials stability over a broad range of steam levels as well as in-depth investigation of structural transformations under more highly resolved conditions, while the cluster model presented here yields the correct trends in hydrothermal stability. Good agreement was observed between predicted relative stabilities of materials by molecular modeling and experimental results. Fundamental information from these studies has provided insight into how metal composition and coordination, chemical functionality of organic linker, framework dimensionality, and interpenetration affect the relative stabilities of PCP materials. This work suggests that the strength of the bond between the metal oxide cluster and the bridging linker is important in determining the hydrothermal stability of the PCP. Although the flexibility of the framework plays a role, it is not as important as the metal−linker bond strength. This demonstration of alignment between experimental and calculated observations has proven the validity of the method, and the insight derived herein insight facilitates direction in designing ideal MOF materials with improved hydrothermal stability for desired applications.Keywords
This publication has 52 references indexed in Scilit:
- Selective gas adsorption and separation in metal–organic frameworksChemical Society Reviews, 2009
- A microdiffraction set-up for nanoporous metal–organic-framework-type solidsNature Materials, 2007
- The Interaction of Water with MOF-5 Simulated by Molecular DynamicsJournal of the American Chemical Society, 2006
- Exceptional chemical and thermal stability of zeolitic imidazolate frameworksProceedings of the National Academy of Sciences, 2006
- A Microporous Metal–Organic Framework for Gas‐Chromatographic Separation of AlkanesAngewandte Chemie-International Edition, 2006
- Metal–organic frameworks: a new class of porous materialsMicroporous and Mesoporous Materials, 2004
- Very Large Breathing Effect in the First Nanoporous Chromium(III)-Based Solids: MIL-53 or CrIII(OH)·{O2C−C6H4−CO2}·{HO2C−C6H4−CO2H}x·H2OyJournal of the American Chemical Society, 2002
- Classification of metal ions according to their complexing properties: a data-driven approachAnalytica Chimica Acta, 2002
- A Chemically Functionalizable Nanoporous Material [Cu 3 (TMA) 2 (H 2 O) 3 ]
n
Science, 1999
- Crystal-Molecular Structure and Magnetic Properties of Cr3 (CH3.COO)6 O Cl.5H2ONature, 1965