Gram-scale synthesis of MIL-125 nanoparticles and their solution processability

Fabrizio, Kevin; Gormley, Eoghan; Davenport, Audrey M.; Hendon, Christopher H.; Brozek, Carl K.

doi:10.1039/d3sc02257a

Cited by 4 publications

References 61 publications

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ChemFET Anion Sensor Based on MOF Nanoparticles

Banning,

Davenport,

Lakanen

et al. 2024

ChemPlusChem

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Nanoparticles of metal‐organic frameworks (nanoMOFs) possess the unusual combination of both internal and external surfaces. While internal surfaces have been the focus of fundamental and applications‐based MOF studies, the chemistry of the external surfaces remains scarcely understood. Herein we report that specific ion interactions with nanoparticles of Cu(1,2,3‐triazolate)2 (Cu(TA)2) resemble the Hofmeister behavior of proteins and the supramolecular chemistry of synthetic macromolecules. Inspired by these anion‐selective interactions, we tested the performance of Cu(TA)2 nanoparticles as chemical field effect transistor (ChemFET) anion sensors. Rather than size‐based selectivity, the detection limits of the devices exhibit a Hofmeister trend, with the greatest sensitivity towards anions perchlorate, iodide, and nitrate. These results highlight the importance of the pore‐based supramolecular interactions, rather than localized donor‐acceptor pairs, in designing MOF‐based technologies.

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ChemFET Anion Sensor Based on MOF Nanoparticles

Banning,

Davenport,

Lakanen

et al. 2024

ChemPlusChem

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Dynamic Quantum Sieving of a Hydrogen Isotope Mixture: Beyond the Limitations of Small Pore Sizes

Jung,

Park,

2024

ACS Appl. Energy Mater.

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Electrochemically Determined and Structurally Justified Thermochemistry of H atom Transfer on Ti-Oxo Nodes of the Colloidal Metal–Organic Framework Ti-MIL-125

Altınçekiç,

Lander,

Roslend

et al. 2024

J. Am. Chem. Soc.

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Titanium dioxide (TiO 2 ) has long been employed as a (photo)electrode for reactions relevant to energy storage and renewable energy synthesis. Proton-coupled electron transfer (PCET) reactions with equimolar amounts of protons and electrons at the TiO 2 surface or within the bulk structure lie at the center of these reactions. Because a proton and an electron are thermochemically equivalent to an H atom, these reactions are essentially H atom transfer reactions. Thermodynamics of H atom transfer has a complex dependence on the synthetic protocol and chemical history of the electrode, the reaction medium, and many others; together, these complications preclude the understanding of the H atom transfer thermochemistry with atomic-level structural knowledge. Herein, we report our success in employing open-circuit potential (E OCP ) measurements to quantitatively determine the H atom transfer thermochemistry at structurally well-defined Ti-oxo clusters within a colloidally stabilized metal− organic framework (MOF), Ti-MIL-125. The free energy to transfer H atom, Ti 3+ O−H bond dissociation free energy (BDFE), was measured to be 68(2) kcal mol −1 . To the best of our understanding, this is the first report on using E OCP measurements to quantify thermochemistry on any MOFs. The proton topology, the structural change upon the redox reaction, and BDFE values were further quantitatively corroborated using computational simulations. Furthermore, comparisons of the E OCP -derived BDFEs of Ti-MIL-125 to similar parameters in the literature suggest that E OCP should be the preferred method for quantitatively accurate BDFE calculations. The reported success in employing E OCP for nanosized Ti-MIL-125 should lay the ground for thermochemical measurements of other colloidal systems, which are otherwise challenging. Implications of these measurements on Ti-MIL-125 as an H atom acceptor in chemical reactions and comparisons with other MOFs/metal oxides are discussed.

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Gram-scale synthesis of MIL-125 nanoparticles and their solution processability

Abstract: Although metal–organic framework (MOF) photocatalysts have become ubiquitous, basic aspects of their photoredox mechanisms remain elusive.

Cited by 4 publications

References 61 publications

ChemFET Anion Sensor Based on MOF Nanoparticles

ChemFET Anion Sensor Based on MOF Nanoparticles

Dynamic Quantum Sieving of a Hydrogen Isotope Mixture: Beyond the Limitations of Small Pore Sizes

Electrochemically Determined and Structurally Justified Thermochemistry of H atom Transfer on Ti-Oxo Nodes of the Colloidal Metal–Organic Framework Ti-MIL-125

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