Mixed uranyl and neptunyl cation–cation interaction-driven clusters: structures, energetic stability, and nuclear quadrupole interactions

文献情報

出版日 2020-05-02

DOI 10.1039/D0CP01068E

インパクトファクター 3.676

著者

Paweł Tecmer, Frank Schindler, Aleksandra Leszczyk, Katharina Boguslawski

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要旨

We present a state-of-the-art quantum chemical study of mixed cation–cation interaction (CCI) driven complexes composed of uranyl and neptunyl units. Specifically, we consider the stability of the D-shaped and T-shaped structural rearrangements in CCIs, various oxidation states of the uranium and neptunium atom (V and VI), as well as a different number of unpaired electrons. Furthermore, we scrutinize the nuclear quadrupole interactions of the bare actinyl subunits and the most stable mixed CCI clusters. The electric field gradients (and nuclear quadrupole coupling constants) of neptunyls are reported for the first time. The characteristic features of the nuclear quadrupole interactions for the bare neptunyl ions are very similar to those predicted for uranyls. When the CCI clusters are formed, a considerable asymmetry is introduced compared to the bare actinyl cations. Most importantly, we are able to distinguish different types of CCIs with respect to their structural arrangement and their total charge by analyzing the electric field gradients at the uranium and neptunium nuclei.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.