Metal-Organic Frameworks (MOFs) with open metal sites (OMS) interact strongly with a range of polar gases/vapors. However, under ambient conditions, their selective adsorption is generally impaired due to a high OMS affinity to water. This led previously to the privilege selection of hydrophobic MOFs for the selective capture/detection of volatile organic compounds (VOCs). Herein, we show that this paradigm is challenged by metal(III) polycarboxylates MOFs, bearing a high concentration of OMS, as MIL-100(Fe), enabling the selective capture of polar VOCs even in the presence of water. With experimental and computational tools, including single-component gravimetric and dynamic mixture adsorption measurements, in situ infrared (IR) spectroscopy and Density Functional Theory calculations we reveal that this adsorption mechanism involves a direct coordination of the VOC on the OMS, associated with an interaction energy that exceeds that of water. Hence, MOFs with OMS are demonstrated to be of interest for air purification purposes.
Download full-text PDF |
Source |
|---|---|
| http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10108120 | PMC |
| http://dx.doi.org/10.1002/anie.202211583 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Synergistic Binding Sites in a Robust and Scalable Metal-Organic Framework for Record CH Capture.
Small
January 2025
School of Materials and Chemical Engineering, Chuzhou University, Chuzhou, 239000, China.
Effectual CH reclamation from CH/N blends by existing physisorbents in industrialization confronts the adversity of frustrated separation performance, weak structural strength, and restricted scale-up preparation. To solve aforesaid bottlenecks, herein, a strategy is presented to fabricate synergistic strong recognition binding sites in a robust and scalable optimum Cu(pma) with ultramicroporous feature regarding superb CH separation versus N. By virtue of the synergistic contribution of multiple affinities accompanied by enormous potential field overlap of pore restriction, it imparts strong recognition binding toward CH molecules.
View Article and Find Full Text PDFLeveraging Cross-Diversity Machine Learning to Unveil Metal-Organic Frameworks with Open Copper Sites for Biogas Upgrading.
J Chem Theory Comput
January 2025
Department of Chemical and Bimolecular Engineering, National University of Singapore, 117576 Singapore.
Biogas, primarily composed of methane (CH) and carbon dioxide (CO), is considered an alternative renewable energy resource. Efficient CO/CH separation is essential for biogas upgrading to increase energy density, and in this context, metal-organic frameworks (MOFs) have demonstrated significant potential. Here, we integrate multiscale modeling with cross-diversity machine learning (ML) to unveil MOFs with open copper sites (OCS-MOFs) that exhibit exceptional CO/CH separation performance.
View Article and Find Full Text PDFMetal-organic frameworks as thermocatalysts for hydrogen peroxide generation and environmental antibacterial applications.
Sci Adv
January 2025
Department of Biomedical Engineering, National Taiwan University, Taipei 10617, Taiwan.
Reactive oxygen species (ROS) are highly reactive, making them useful for environmental and health applications. Traditionally, photocatalysts and piezocatalysts have been used to generate ROS, but their utilization is limited by various environmental and physical constraints. This study introduces metal-organic frameworks (MOFs) as modern thermocatalysts efficiently producing hydrogen peroxide (HO) from small temperature differences.
View Article and Find Full Text PDFGas-flow activation of MOFs: unlocking efficient catalysis through dynamic bonding.
Chem Sci
December 2024
Department of Physics & Chemistry, DGIST Daegu 42988 Korea
Article Synopsis
- Metal-organic frameworks (MOFs) are important materials used in various applications like catalysis and gas storage, but their open metal sites often get blocked by solvent molecules, requiring activation to use them effectively.
- Traditional activation methods use high temperatures, which can damage the MOFs, but a new 'gas-flow activation' technique employing inert gases at lower temperatures preserves their structure while effectively removing these solvent molecules.
- This study shows that this method not only works well with a specific MOF (HKUST-1) but is also applicable to other types, offering a safer, more efficient approach for activating MOFs without compromising their integrity.
Exploring the Fluorination and Hydroxylation of Pore-Space-Partitioned Metal-Organic Frameworks for CH/CH Separation.
Chem Asian J
January 2025
Institute of Clinical Pharmacy and Pharmaceutical Sciences, School of Pharmacy, College of Medicine, National Cheng Kung University, Tainan City, 70101, Taiwan.
We report three novel pore-space-partitioned metal-organic frameworks (MOFs) functionalized with fluorine and hydroxyl groups using 2,3,5,6-tetrafluorobenzene-1,4-dicarboxylic acid (F-BDC) and a new ligand 3,6-difluoro-2,5-dihydroxybenzene-1,4-dicarboxylic acid (F(OH)-BDC) as organic building blocks, with 1,3,5-tris(4-pyridyl)-2,4,6-triazine (TPT) as pore partition agent. With the polar fluorine and hydroxyl groups and the open metal sites being blocked by TPT, moderate molecule-framework interactions can be engineered. These three isoreticular microporous frameworks Mn-TPT-BDC-F (NCKU-21), Mn-TPT-BDC-F(OH) (NCKU-22), and Mg-TPT-BDC-F(OH) (NCKU-23) (NCKU=National Cheng Kung University) exhibit distinct single-component gas adsorption behaviors.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!