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2. Stimuli-Modulated Metal Oxidation States in Photochromic MOFs

Author

Martin, Corey R., primary, Park, Kyoung Chul, additional, Leith, Gabrielle A., additional, Yu, Jierui, additional, Mathur, Abhijai, additional, Wilson, Gina R., additional, Gange, Gayathri B., additional, Barth, Emily L., additional, Ly, Richard T., additional, Manley, Olivia M., additional, Forrester, Kelly L., additional, Karakalos, Stavros G., additional, Smith, Mark D., additional, Makris, Thomas M., additional, Vannucci, Aaron K., additional, Peryshkov, Dmitry V., additional, and Shustova, Natalia B., additional

Published
2022
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4. J-dimer emission in interwoven metal-organic frameworks

Author

Newsome, Wesley J., Chakraborty, Arnab, Ly, Richard T., Pour, Gavin S., Fairchild, David C., Morris, Amanda J., Uribe-Romo, Fernando J., Newsome, Wesley J., Chakraborty, Arnab, Ly, Richard T., Pour, Gavin S., Fairchild, David C., Morris, Amanda J., and Uribe-Romo, Fernando J.

Abstract

J-dimer emission is an emergent property that occurs when pairs of ground state fluorophores associate, typically in a dilute solution medium. The resulting fluorescence is shifted with respect to the monomer. J-dimer emission, however, has never been observed in concentrated dispersions or in the solid state. We posited that multivariate (MTV) MOFs with double interwoven structures would help to isolate these dimers within their crystalline matrix. Using this strategy, J-aggregate density was controlled during crystallization by following a substitutional solid solution approach. Here, we identified the presence of J-dimers over the entire composition range for interwoven PIZOF-2/NNU-28 structures with variable amounts of a diethynyl-anthracene aggregate-forming link. We produced bulk crystals that systematically shifted their fluorescence from green to red with lifetimes (up to 13 ns) and quantum yields (up to 76%) characteristic of pi-pi stacked aggregates. Photophysical studies also revealed an equilibrium constant of dimerization, K-D = 1.5 +/- 0.3 M-1, enabling the first thermodynamic quantification of link-link interactions that occur during MOF assembly. Our findings elucidate the role that supramolecular effects play during crystallization of MTV MOFs, opening pathways for the preparation of solid-state materials with solution-like properties by design.

Published
2020
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5. J-dimer emission in interwoven metal-organic frameworks

Author

Chemistry, Newsome, Wesley J., Chakraborty, Arnab, Ly, Richard T., Pour, Gavin S., Fairchild, David C., Morris, Amanda J., Uribe-Romo, Fernando J., Chemistry, Newsome, Wesley J., Chakraborty, Arnab, Ly, Richard T., Pour, Gavin S., Fairchild, David C., Morris, Amanda J., and Uribe-Romo, Fernando J.

Abstract

J-dimer emission is an emergent property that occurs when pairs of ground state fluorophores associate, typically in a dilute solution medium. The resulting fluorescence is shifted with respect to the monomer. J-dimer emission, however, has never been observed in concentrated dispersions or in the solid state. We posited that multivariate (MTV) MOFs with double interwoven structures would help to isolate these dimers within their crystalline matrix. Using this strategy, J-aggregate density was controlled during crystallization by following a substitutional solid solution approach. Here, we identified the presence of J-dimers over the entire composition range for interwoven PIZOF-2/NNU-28 structures with variable amounts of a diethynyl-anthracene aggregate-forming link. We produced bulk crystals that systematically shifted their fluorescence from green to red with lifetimes (up to 13 ns) and quantum yields (up to 76%) characteristic of pi-pi stacked aggregates. Photophysical studies also revealed an equilibrium constant of dimerization, K-D = 1.5 +/- 0.3 M-1, enabling the first thermodynamic quantification of link-link interactions that occur during MOF assembly. Our findings elucidate the role that supramolecular effects play during crystallization of MTV MOFs, opening pathways for the preparation of solid-state materials with solution-like properties by design.

Published
2020

6. A Dual Threat: Redox‐Activity and Electronic Structures of Well‐Defined Donor–Acceptor Fulleretic Covalent‐Organic Materials

Author

Leith, Gabrielle A., primary, Rice, Allison M., additional, Yarbrough, Brandon J., additional, Berseneva, Anna A., additional, Ly, Richard T., additional, Buck, Charles N., additional, Chusov, Denis, additional, Brandt, Amy J., additional, Chen, Donna A., additional, Lamm, Benjamin W., additional, Stefik, Morgan, additional, Stephenson, Kenneth S., additional, Smith, Mark D., additional, Vannucci, Aaron K., additional, Pellechia, Perry J., additional, Garashchuk, Sophya, additional, and Shustova, Natalia B., additional

Published
2020
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8. “Boarding-Up”: Radiation Damage and Radionuclide Leaching Kinetics in Linker-Capped Metal–Organic Frameworks

Author

Berseneva, Anna A., primary, Martin, Corey R., additional, Galitskiy, Vladimir A., additional, Ejegbavwo, Otega A., additional, Leith, Gabrielle A., additional, Ly, Richard T., additional, Rice, Allison M., additional, Dolgopolova, Ekaterina A., additional, Smith, Mark D., additional, zur Loye, Hans-Conrad, additional, DiPrete, David P., additional, Amoroso, Jake W., additional, and Shustova, Natalia B., additional

Published
2019
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9. Thermodynamics and Electronic Properties of Heterometallic Multinuclear Actinide-Containing Metal–Organic Frameworks with “Structural Memory”

Author

Ejegbavwo, Otega A., primary, Martin, Corey R., additional, Olorunfemi, Oyindamola A., additional, Leith, Gabrielle A., additional, Ly, Richard T., additional, Rice, Allison M., additional, Dolgopolova, Ekaterina A., additional, Smith, Mark D., additional, Karakalos, Stavros G., additional, Birkner, Nancy, additional, Powell, Brian A., additional, Pandey, Shubham, additional, Koch, Robert J., additional, Misture, Scott T., additional, Loye, Hans-Conrad zur, additional, Phillpot, Simon R., additional, Brinkman, Kyle S., additional, and Shustova, Natalia B., additional

Published
2019
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11. “Boarding-Up”: Radiation Damage and Radionuclide Leaching Kinetics in Linker-Capped Metal–Organic Frameworks

Author

Berseneva, Anna A., Martin, Corey R., Galitskiy, Vladimir A., Ejegbavwo, Otega A., Leith, Gabrielle A., Ly, Richard T., Rice, Allison M., Dolgopolova, Ekaterina A., Smith, Mark D., zur Loye, Hans-Conrad, DiPrete, David P., Amoroso, Jake W., and Shustova, Natalia B.

Abstract

For the first time, we report the ability to control radionuclide species release kinetics in metal–organic frameworks (MOFs) as a function of postsynthetic capping linker installation, which is essential for understanding MOF potential as viable radionuclide wasteform materials or versatile platforms for sensing, leaching, and radionuclide sequestration. The radiation damage of prepared frameworks under γ radiation has also been studied. We envision that the presented studies are the first steps toward utilization of the reported scaffolds for more efficient nuclear waste administration.

Published
2020
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