Aqueous stability is a critical property for the application of metal-organic framework (MOF) materials in humid conditions. The sampling of the free energy surface for a water reaction is challenging due to a lack of a reactive force field. Here, we developed a ReaxFF force field for simulating the reaction of zeolitic imidazole frameworks (ZIFs) with water. We carried out metadynamics simulations based on ReaxFF to study the reaction of water with a few different types of MOFs. We also conducted an experimental water immersion test and characterized the XRD, TG, and gas adsorption properties of the MOFs before and after the immersion test. By considering the energy barrier for a hydrolysis reaction, the simulation results are in good agreement with the experiments. MOFs with open structures and large pores are found to be unstable in metadynamics simulations, where the water molecule can attack or bond with the metallic node relatively easily. In contrast, it is more difficult for water to attack the Zn atom in the ZnN tetrahedral structure of ZIFs. We also found that ZIFs with the -NO functional groups have higher water stability. Discrepancies between the metadynamics simulation and gas adsorption experiments have been accounted for from the phase/crystallinity change of the structure reflected in the X-ray diffraction and thermogravimetry analysis of the MOF samples.
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http://dx.doi.org/10.1021/acs.jpcb.3c00563 | DOI Listing |
Chem Sci
January 2025
State Key Laboratory of Physical Chemistry of Solid Surfaces and Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry College of Chemistry and Chemical Engineering, Xiamen University Xiamen 361005 China
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View Article and Find Full Text PDFComput Biol Chem
January 2025
Drug Discovery and Development Laboratory (DDD Lab), Department of Pharmaceutical Technology, Jadavpur University, Kolkata 700032, India. Electronic address:
Multiple myeloma (MM) is the second most frequently diagnosed hematological malignancy, presenting limited treatment options with no curative potential and significant drug resistance. Recent studies involving genetic knockdown established the crucial role of GRK6 in upholding the viability of MM cells, emphasizing the need to identify potential inhibitors. Computational exploration of GRK6 inhibitors has not been attempted previously.
View Article and Find Full Text PDFJ Phys Chem A
January 2025
Department of Chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education, Tsinghua University, Beijing 100084, China.
The fundamental hydrolysis behavior of tetravalent actinide cations (An) with a high charge is crucial for understanding their solution chemistry, particularly in nuclear fuel reprocessing and environmental behavior. Using Th as a reference of the An series, this work employed both the periodic model and the cluster model to calculate the first hydrolysis reaction constant (p) of the Th aqua ion and conducted a detailed evaluation of these approaches. In the periodic model, molecular dynamics (AIMD) simulations of Th in the explicit solvation environment are conducted, using metadynamics and constrained molecular dynamics to calculate p values.
View Article and Find Full Text PDFJ Chem Inf Model
January 2025
Medicinal Chemistry and Drug Design Technologies Department, Chiesi Farmaceutici S.p.A., Largo F. Belloli 11/A, 43122 Parma, Italy.
Janus kinase type 3 (JAK3), an emerging target for treating autoimmune diseases, possesses a front pocket cysteine that is targeted by covalent modifiers, best represented by the marketed drug ritlecitinib (). Recently, 2,3-dihydro-1-inden-1-ylcyanamides have been developed as novel JAK3 inhibitors. Among them, the -(6-(7-pyrrolo[2,3-]pyrimidin-4-yl)-2,3-dihydro-1-inden-1-yl)cyanamide inhibitor () and its methylated analogue (), while being potent inhibitors, displayed different mechanisms of action (covalent vs noncovalent) and binding modes (Casimiro-Garcia et al.
View Article and Find Full Text PDFACS Chem Neurosci
January 2025
National Center for Natural Products Research, University of Mississippi, University, Mississippi 38677, United States.
Cannabinoid receptor 1 (CB1R) has been extensively studied as a potential therapeutic target for various conditions, including pain management, obesity, emesis, and metabolic syndrome. Unlike orthosteric agonists such as Δ-tetrahydrocannabinol (THC), cannabidiol (CBD) has been identified as a negative allosteric modulator (NAM) of CB1R, among its other pharmacological targets. Previous computational and structural studies have proposed various binding sites for CB1R NAMs.
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