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1. Formation of Fully Stoichiometric, Oxidation-State Pure Neptunium and Plutonium Dioxides from Molecular Precursors.

Author

Peterson, Appie, Kelly, Sheridon, Arino, Trevor, Gunther, S, Ouellette, Erik, Wacker, Jennifer, Woods, Joshua, Teat, Simon, Lukens, Wayne, Arnold, John, Abergel, Rebecca, and Minasian, Stefan

Abstract

Amidate-based ligands (N-(tert-butyl)isobutyramide, ITA) bind κ2 to form homoleptic, 8-coordinate complexes with tetravalent 237Np (Np(ITA)4, 1-Np) and 242Pu (Pu(ITA)4, 1-Pu). These compounds complete an isostructural series from Th, U-Pu and allow for the direct comparison between many of the early actinides with stable tetravalent oxidation states by nuclear magnetic resonance (NMR) spectroscopy and single crystal X-ray diffraction (SCXRD). The molecular precursors are subjected to controlled thermolysis under mild conditions with the exclusion of exogenous air and moisture, facilitating the removal of the volatile organic ligands and ligand byproducts. The preformed metal-oxygen bond in the precursor, as well as the metal oxidation state, are maintained through the decomposition, forming fully stoichiometric, oxidation-state pure NpO2 and PuO2. Powder X-ray diffraction (PXRD), scanning transmission electron microscopy (STEM), and energy dispersive X-ray spectroscopy (EDS) elemental mapping supported the evaluation of these high-purity materials. This chemistry is applicable to a wide range of metals, including actinides, with accessible tetravalent oxidation states, and provides a consistent route to analytical standards of importance to the field of nuclear nonproliferation, forensics, and fundamental studies.

Published
2024

2. 4f-Orbital mixing increases the magnetic susceptibility of Cp′ 3 Eu

Author

Gunther, S Olivia, Qiao, Yusen, Smith, Patrick W, Ciccone, Sierra R, Ditter, Alexander S, Huh, Daniel N, Moreau, Liane M, Shuh, David K, Sun, Taoxiang, Arnold, Polly L, Booth, Corwin H, de Jong, Wibe A, Evans, William J, Lukens, Wayne W, and Minasian, Stefan G

Subjects
Inorganic Chemistry, Chemical Sciences, Chemical sciences
Abstract

Traditional models of lanthanide electronic structure suggest that bonding is predominantly ionic, and that covalent orbital mixing is not an important factor in determining magnetic properties. Here, 4f orbital mixing and its impact on the magnetic susceptibility of Cp'3Eu (Cp' = C5H4SiMe3) was analyzed experimentally using magnetometry and X-ray absorption spectroscopy (XAS) methods at the C K-, Eu M5,4-, and L3-edges. Pre-edge features in the experimental and TDDFT-calculated C K-edge XAS spectra provided unequivocal evidence of C 2p and Eu 4f orbital mixing in the π-antibonding orbital of a' symmetry. The charge-transfer configurations resulting from 4f orbital mixing were identified spectroscopically by using Eu M5,4-edge and L3-edge XAS. Modeling of variable-temperature magnetic susceptibility data showed excellent agreement with the XAS results and indicated that increased magnetic susceptibility of Cp'3Eu is due to removal of the degeneracy of the 7F1 excited state due to mixing between the ligand and Eu 4f orbitals.

Published
2024

3. The quest for safer nuclear fuels

Author

Gunther, S Olivia and Schacherl, Bianca

Subjects
Chemical Sciences, Chemical sciences
Abstract

As researchers explore innovative ways to make nuclear fuels more accident-tolerant, this report investigates the use of manganese ions as dopants for uranium oxide (UO2) fuels.

Published
2024

4. Isolable fluorinated triphenylmethyl cation salts of [HCB 11 Cl 11 ] − : demonstration of remarkable hydride affinity

Author

Gunther, S Olivia, Lee, Chun-I, Song, Ellen, Bhuvanesh, Nattamai, and Ozerov, Oleg V

Subjects
Chemical Sciences
Abstract

Significantly fluorinated triarylmethyl cations have long attracted attention as potentially accessible highly reactive carbocations, but their isolation in a convenient form has proved elusive. We show that abstraction of chloride with a cationic silylium reagent leads to the facile formation of di-, tetra-, and hexafluorinated trityl cations, which could be isolated as analytically pure salts with the [HCB11Cl11]- counterion and are compatible with (halo)arene solvents. The F6Tr+ cation carrying six meta-F substituents was computationally predicted to possess up to 20% higher hydride affinity than the parent triphenylmethyl cation Tr+. We report that indeed F6Tr+ displays reactivity unmatched by Tr+. F6Tr+ at ambient temperature abstracts hydrides from the C-H bonds in tetraethylsilane, mesitylene, methylcyclohexane, and catalyzes Friedel-Crafts alkylation of arenes with ethylene, while Tr+ does none of these.

Published
2022

7. Annual (2023) taxonomic update of RNA-directed RNA polymerase-encoding negative-sense RNA viruses (realm Riboviria: kingdom Orthornavirae: phylum Negarnaviricota)

Author

Kuhn, J, Abe, J, Adkins, S, Alkhovsky, S, Avsic-Zupanc, T, Ayllon, M, Bahl, J, Balkema-Buschmann, A, Ballinger, M, Baranwal, V, Beer, M, Bejerman, N, Bergeron, E, Biedenkopf, N, Blair, C, Blasdell, K, Blouin, A, Bradfute, S, Briese, T, Brown, P, Buchholz, U, Buchmeier, M, Bukreyev, A, Burt, F, Buttner, C, Calisher, C, Cao, M, Casas, I, Chandran, K, Charrel, R, Chaturvedi, K, Chooi, K, Crane, A, Bo, E, de la Torre, J, de Souza, W, de Swart, R, Debat, H, Dheilly, N, Di Paola, N, Di Serio, F, Dietzgen, R, Digiaro, M, Drexler, J, Duprex, W, Durrwald, R, Easton, A, Elbeaino, T, Ergunay, K, Feng, G, Firth, A, Fooks, A, Formenty, P, Freitas-Astua, J, Gago-Zachert, S, Garcia, M, Garcia-Sastre, A, Garrison, A, Gaskin, T, Gong, W, Gonzalez, J, de Bellocq, J, Griffiths, A, Groschup, M, Gunther, I, Gunther, S, Hammond, J, Hasegawa, Y, Hayashi, K, Hepojoki, J, Higgins, C, Hongo, S, Horie, M, Hughes, H, Hume, A, Hyndman, T, Ikeda, K, Jiang, D, Jonson, G, Junglen, S, Klempa, B, Klingstrom, J, Kondo, H, Koonin, E, Krupovic, M, Kubota, K, Kurath, G, Laenen, L, Lambert, A, Li, J, Liu, R, Lukashevich, I, Macdiarmid, R, Maes, P, Marklewitz, M, Marshall, S, Marzano, S, Mccauley, J, Mirazimi, A, Muhlberger, E, Nabeshima, T, Naidu, R, Natsuaki, T, Navarro, B, Navarro, J, Neriya, Y, Netesov, S, Neumann, G, Nowotny, N, Nunes, M, Ochoa-Corona, F, Okada, T, Palacios, G, Pallas, V, Papa, A, Paraskevopoulou, S, Parrish, C, Pauvolid-Correa, A, Paweska, J, Perez, D, Pfaff, F, Plemper, R, Postler, T, Rabbidge, L, Radoshitzky, S, Ramos-Gonzalez, P, Rehanek, M, Resende, R, Reyes, C, Rodrigues, T, Romanowski, V, Rubbenstroth, D, Rubino, L, Runstadler, J, Sabanadzovic, S, Sadiq, S, Salvato, M, Sasaya, T, Schwemmle, M, Sharpe, S, Shi, M, Shimomoto, Y, Sidharthan, V, Sironi, M, Smither, S, Song, J, Spann, K, Spengler, J, Stenglein, M, Takada, A, Takeyama, S, Tatara, A, Tesh, R, Thornburg, N, Tian, X, Tischler, N, Tomitaka, Y, Tomonaga, K, Tordo, N, Tu, C, Turina, M, Tzanetakis, I, Vaira, A, van den Hoogen, B, Vanmechelen, B, Vasilakis, N, Verbeek, M, von Bargen, S, Wada, J, Wahl, V, Walker, P, Waltzek, T, Whitfield, A, Wolf, Y, Xia, H, Xylogianni, E, Yanagisawa, H, Yano, K, Ye, G, Yuan, Z, Zerbini, F, Zhang, G, Zhang, S, Zhang, Y, Zhao, L, Okland, A, Kuhn J. H., Abe J., Adkins S., Alkhovsky S. V., Avsic-Zupanc T., Ayllon M. A., Bahl J., Balkema-Buschmann A., Ballinger M. J., Baranwal V. K., Beer M., Bejerman N., Bergeron E., Biedenkopf N., Blair C. D., Blasdell K. R., Blouin A. G., Bradfute S. B., Briese T., Brown P. A., Buchholz U. J., Buchmeier M. J., Bukreyev A., Burt F., Buttner C., Calisher C. H., Cao M., Casas I., Chandran K., Charrel R. N., Chaturvedi K. K., Chooi K. M., Crane A., Bo E. D., de la Torre J. C., de Souza W. M., de Swart R. L., Debat H., Dheilly N. M., Di Paola N., Di Serio F., Dietzgen R. G., Digiaro M., Drexler J. F., Duprex W. P., Durrwald R., Easton A. J., Elbeaino T., Ergunay K., Feng G., Firth A. E., Fooks A. R., Formenty P. B. H., Freitas-Astua J., Gago-Zachert S., Garcia M. L., Garcia-Sastre A., Garrison A. R., Gaskin T. R., Gong W., Gonzalez J. -P. J., de Bellocq J., Griffiths A., Groschup M. H., Gunther I., Gunther S., Hammond J., Hasegawa Y., Hayashi K., Hepojoki J., Higgins C. M., Hongo S., Horie M., Hughes H. R., Hume A. J., Hyndman T. H., Ikeda K., Jiang D., Jonson G. B., Junglen S., Klempa B., Klingstrom J., Kondo H., Koonin E. V., Krupovic M., Kubota K., Kurath G., Laenen L., Lambert A. J., Li J., Li J. -M., Liu R., Lukashevich I. S., MacDiarmid R. M., Maes P., Marklewitz M., Marshall S. H., Marzano S. -Y. L., McCauley J. W., Mirazimi A., Muhlberger E., Nabeshima T., Naidu R., Natsuaki T., Navarro B., Navarro J. A., Neriya Y., Netesov S. V., Neumann G., Nowotny N., Nunes M. R. T., Ochoa-Corona F. M., Okada T., Palacios G., Pallas V., Papa A., Paraskevopoulou S., Parrish C. R., Pauvolid-Correa A., Paweska J. T., Perez D. R., Pfaff F., Plemper R. K., Postler T. S., Rabbidge L. O., Radoshitzky S. R., Ramos-Gonzalez P. L., Rehanek M., Resende R. O., Reyes C. A., Rodrigues T. C. S., Romanowski V., Rubbenstroth D., Rubino L., Runstadler J. A., Sabanadzovic S., Sadiq S., Salvato M. S., Sasaya T., Schwemmle M., Sharpe S. R., Shi M., Shimomoto Y., Sidharthan V. K., Sironi M., Smither S., Song J. -W., Spann K. M., Spengler J. R., Stenglein M. D., Takada A., Takeyama S., Tatara A., Tesh R. B., Thornburg N. J., Tian X., Tischler N. D., Tomitaka Y., Tomonaga K., Tordo N., Tu C., Turina M., Tzanetakis I. E., Vaira A. M., van den Hoogen B., Vanmechelen B., Vasilakis N., Verbeek M., von Bargen S., Wada J., Wahl V., Walker P. J., Waltzek T. B., Whitfield A. E., Wolf Y. I., Xia H., Xylogianni E., Yanagisawa H., Yano K., Ye G., Yuan Z., Zerbini F. M., Zhang G., Zhang S., Zhang Y. -Z., Zhao L., Okland A. L., Kuhn, J, Abe, J, Adkins, S, Alkhovsky, S, Avsic-Zupanc, T, Ayllon, M, Bahl, J, Balkema-Buschmann, A, Ballinger, M, Baranwal, V, Beer, M, Bejerman, N, Bergeron, E, Biedenkopf, N, Blair, C, Blasdell, K, Blouin, A, Bradfute, S, Briese, T, Brown, P, Buchholz, U, Buchmeier, M, Bukreyev, A, Burt, F, Buttner, C, Calisher, C, Cao, M, Casas, I, Chandran, K, Charrel, R, Chaturvedi, K, Chooi, K, Crane, A, Bo, E, de la Torre, J, de Souza, W, de Swart, R, Debat, H, Dheilly, N, Di Paola, N, Di Serio, F, Dietzgen, R, Digiaro, M, Drexler, J, Duprex, W, Durrwald, R, Easton, A, Elbeaino, T, Ergunay, K, Feng, G, Firth, A, Fooks, A, Formenty, P, Freitas-Astua, J, Gago-Zachert, S, Garcia, M, Garcia-Sastre, A, Garrison, A, Gaskin, T, Gong, W, Gonzalez, J, de Bellocq, J, Griffiths, A, Groschup, M, Gunther, I, Gunther, S, Hammond, J, Hasegawa, Y, Hayashi, K, Hepojoki, J, Higgins, C, Hongo, S, Horie, M, Hughes, H, Hume, A, Hyndman, T, Ikeda, K, Jiang, D, Jonson, G, Junglen, S, Klempa, B, Klingstrom, J, Kondo, H, Koonin, E, Krupovic, M, Kubota, K, Kurath, G, Laenen, L, Lambert, A, Li, J, Liu, R, Lukashevich, I, Macdiarmid, R, Maes, P, Marklewitz, M, Marshall, S, Marzano, S, Mccauley, J, Mirazimi, A, Muhlberger, E, Nabeshima, T, Naidu, R, Natsuaki, T, Navarro, B, Navarro, J, Neriya, Y, Netesov, S, Neumann, G, Nowotny, N, Nunes, M, Ochoa-Corona, F, Okada, T, Palacios, G, Pallas, V, Papa, A, Paraskevopoulou, S, Parrish, C, Pauvolid-Correa, A, Paweska, J, Perez, D, Pfaff, F, Plemper, R, Postler, T, Rabbidge, L, Radoshitzky, S, Ramos-Gonzalez, P, Rehanek, M, Resende, R, Reyes, C, Rodrigues, T, Romanowski, V, Rubbenstroth, D, Rubino, L, Runstadler, J, Sabanadzovic, S, Sadiq, S, Salvato, M, Sasaya, T, Schwemmle, M, Sharpe, S, Shi, M, Shimomoto, Y, Sidharthan, V, Sironi, M, Smither, S, Song, J, Spann, K, Spengler, J, Stenglein, M, Takada, A, Takeyama, S, Tatara, A, Tesh, R, Thornburg, N, Tian, X, Tischler, N, Tomitaka, Y, Tomonaga, K, Tordo, N, Tu, C, Turina, M, Tzanetakis, I, Vaira, A, van den Hoogen, B, Vanmechelen, B, Vasilakis, N, Verbeek, M, von Bargen, S, Wada, J, Wahl, V, Walker, P, Waltzek, T, Whitfield, A, Wolf, Y, Xia, H, Xylogianni, E, Yanagisawa, H, Yano, K, Ye, G, Yuan, Z, Zerbini, F, Zhang, G, Zhang, S, Zhang, Y, Zhao, L, Okland, A, Kuhn J. H., Abe J., Adkins S., Alkhovsky S. V., Avsic-Zupanc T., Ayllon M. A., Bahl J., Balkema-Buschmann A., Ballinger M. J., Baranwal V. K., Beer M., Bejerman N., Bergeron E., Biedenkopf N., Blair C. D., Blasdell K. R., Blouin A. G., Bradfute S. B., Briese T., Brown P. A., Buchholz U. J., Buchmeier M. J., Bukreyev A., Burt F., Buttner C., Calisher C. H., Cao M., Casas I., Chandran K., Charrel R. N., Chaturvedi K. K., Chooi K. M., Crane A., Bo E. D., de la Torre J. C., de Souza W. M., de Swart R. L., Debat H., Dheilly N. M., Di Paola N., Di Serio F., Dietzgen R. G., Digiaro M., Drexler J. F., Duprex W. P., Durrwald R., Easton A. J., Elbeaino T., Ergunay K., Feng G., Firth A. E., Fooks A. R., Formenty P. B. H., Freitas-Astua J., Gago-Zachert S., Garcia M. L., Garcia-Sastre A., Garrison A. R., Gaskin T. R., Gong W., Gonzalez J. -P. J., de Bellocq J., Griffiths A., Groschup M. H., Gunther I., Gunther S., Hammond J., Hasegawa Y., Hayashi K., Hepojoki J., Higgins C. M., Hongo S., Horie M., Hughes H. R., Hume A. J., Hyndman T. H., Ikeda K., Jiang D., Jonson G. B., Junglen S., Klempa B., Klingstrom J., Kondo H., Koonin E. V., Krupovic M., Kubota K., Kurath G., Laenen L., Lambert A. J., Li J., Li J. -M., Liu R., Lukashevich I. S., MacDiarmid R. M., Maes P., Marklewitz M., Marshall S. H., Marzano S. -Y. L., McCauley J. W., Mirazimi A., Muhlberger E., Nabeshima T., Naidu R., Natsuaki T., Navarro B., Navarro J. A., Neriya Y., Netesov S. V., Neumann G., Nowotny N., Nunes M. R. T., Ochoa-Corona F. M., Okada T., Palacios G., Pallas V., Papa A., Paraskevopoulou S., Parrish C. R., Pauvolid-Correa A., Paweska J. T., Perez D. R., Pfaff F., Plemper R. K., Postler T. S., Rabbidge L. O., Radoshitzky S. R., Ramos-Gonzalez P. L., Rehanek M., Resende R. O., Reyes C. A., Rodrigues T. C. S., Romanowski V., Rubbenstroth D., Rubino L., Runstadler J. A., Sabanadzovic S., Sadiq S., Salvato M. S., Sasaya T., Schwemmle M., Sharpe S. R., Shi M., Shimomoto Y., Sidharthan V. K., Sironi M., Smither S., Song J. -W., Spann K. M., Spengler J. R., Stenglein M. D., Takada A., Takeyama S., Tatara A., Tesh R. B., Thornburg N. J., Tian X., Tischler N. D., Tomitaka Y., Tomonaga K., Tordo N., Tu C., Turina M., Tzanetakis I. E., Vaira A. M., van den Hoogen B., Vanmechelen B., Vasilakis N., Verbeek M., von Bargen S., Wada J., Wahl V., Walker P. J., Waltzek T. B., Whitfield A. E., Wolf Y. I., Xia H., Xylogianni E., Yanagisawa H., Yano K., Ye G., Yuan Z., Zerbini F. M., Zhang G., Zhang S., Zhang Y. -Z., Zhao L., and Okland A. L.

Abstract

In April 2023, following the annual International Committee on Taxonomy of Viruses (ICTV) ratification vote on newly proposed taxa, the phylum Negarnaviricota was amended and emended. The phylum was expanded by one new family, 14 new genera, and 140 new species. Two genera and 538 species were renamed. One species was moved, and four were abolished. This article presents the updated taxonomy of Negarnaviricota as now accepted by the ICTV

Published
2023

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