Extending the Row of Lanthanide Tetrafluorides: A Combined Matrix-Isolation and Quantum-Chemical Study

Chemistry : a European Journal
Thomas Vent-SchmidtSebastian Riedel

Abstract

Only the neutral tetrafluorides of Ce, Pr, and Tb as well as the [LnF7 ](3-) anions of Dy and Nd, with the metal in the +IV oxidation state, have been previously reported. We report our attempts to extend the row of neutral lanthanide tetrafluorides through the reaction of laser-ablated metal atoms with fluorine and their stabilization and characterization by matrix-isolation IR spectroscopy. In addition to the above three tetrafluorides, we found two new tetrafluorides, (3) NdF4 and (7) DyF4 , both of which are in the +IV oxidation state, which extends this lanthanide oxidation state to two new metals. Our experimental results are supported by quantum-chemical calculations and the role of the lanthanide oxidation state is discussed for both the LnF4 and [LnF4 ](-) species. Most of the LnF4 species are predicted to be in the +IV oxidation state and all of the [LnF4 ](-) anions are predicted to be in the +III oxidation state. The LnF4 species are predicted to be strong oxidizing agents and the LnF3 species are predicted to be moderate to strong Lewis acids.

References

Jan 24, 2009·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Giuseppe Lanza, Camilla Minichino
Jul 3, 2010·Inorganic Chemistry·Sebastian RiedelLester Andrews
Sep 17, 2011·Journal of the American Chemical Society·Matthew R MacDonaldWilliam J Evans
May 16, 2012·Journal of the American Chemical Society·Matthew R MacDonaldWilliam J Evans
Mar 14, 2013·Journal of Computational Chemistry·Eric D GlendeningFrank Weinhold
May 24, 2013·Journal of the American Chemical Society·Matthew R MacDonaldWilliam J Evans
Dec 19, 2013·Inorganic Chemistry·Tanya MikulasLester Andrews
May 6, 2015·The Journal of Physical Chemistry. a·K Sahan ThanthiriwatteDavid A Dixon
Jun 4, 2015·Angewandte Chemie·Thomas Vent-SchmidtSebastian Riedel
Oct 3, 2015·Chemistry : a European Journal·Felix BrosiSebastian Riedel
Nov 7, 2015·Inorganic Chemistry·Thomas Vent-Schmidt, Sebastian Riedel

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Citations

May 10, 2017·Journal of Chemical Theory and Computation·Lucas E AebersoldAngela K Wilson
Jun 11, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Thaige P GompaHenry S La Pierre
Aug 24, 2019·The Journal of Physical Chemistry. a·Zongtang FangDavid A Dixon

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