A diuranium carbide cluster stabilized inside a C80 fullerene cage

Zhang, Xingxing; Li, Wanlu; Feng, Lai; Chen, Xin; Hansen, Andreas; Grimme, Stefan; Fortier, Skye; Sergentu, Dumitru-Claudiu; Duignan, Thomas J.; Autschbach, Jochen; Wang, Shuao; Wang, Yaofeng; Velkos, Giorgios; Popov, Alexey A.; Aghdassi, Nabi; Duhm, Steffen; Li, Xiaohong; Li, Jun; Echegoyen, Luis; Schwarz, W. H.  Eugen; Chen, Ning

doi:10.1038/s41467-018-05210-8

Title: A diuranium carbide cluster stabilized inside a C₈₀ fullerene cage

Journal Article · 15 July 2018 · Nature Communications

DOI: https://doi.org/10.1038/s41467-018-05210-8 · OSTI ID:1511585

Zhang, Xingxing ^[1]; Li, Wanlu ^[2]; Feng, Lai ^[3]; Chen, Xin ^[2]; Hansen, Andreas ^[4]; Grimme, Stefan ^[4]; Fortier, Skye ^[5]; Sergentu, Dumitru-Claudiu ^[6]; Duignan, Thomas J. ^[6];

^[6]; Wang, Shuao ^[3]; Wang, Yaofeng ^[3]; Velkos, Giorgios ^[7];

^[7]; Aghdassi, Nabi ^[3];

^[3]; Li, Xiaohong ^[3]; Li, Jun ^[2]; Echegoyen, Luis ^[4];

^[8] more »

Soochow University, Suzhou, Jiangsu (China); None
Tsinghua Univ., Beijing (China)
Soochow University, Suzhou, Jiangsu (China)
Universität Bonn (Germany)
University of Texas, El Paso, TX (United States)
State Univ. of New York, Buffalo, NY (United States)
Leibniz Institute for Solid State and Materials Research, Dresden (Germany)
Tsinghua Univ., Beijing (China); Universität Siegen (Germany)

Unsupported non-bridged uranium–carbon double bonds have long been sought after in actinide chemistry as fundamental synthetic targets in the study of actinide-ligand multiple bonding. Here we report that, utilizing I_h(7)-C₈₀ fullerenes as nanocontainers, a diuranium carbide cluster, U=C=U, has been encapsulated and stabilized in the form of UCU@I_h(7)-C₈₀. This endohedral fullerene was prepared utilizing the Krätschmer–Huffman arc discharge method, and was then co-crystallized with nickel(II) octaethylporphyrin (Ni^II-OEP) to produce UCU@I_h(7)-C₈₀·[Ni^II-OEP] as single crystals. X-ray diffraction analysis reveals a cage-stabilized, carbide-bridged, bent UCU cluster with unexpectedly short uranium–carbon distances (2.03 Å) indicative of covalent U=C double-bond character. The quantum-chemical results suggest that both U atoms in the UCU unit have formal oxidation state of +5. The structural features of UCU@I_h(7)-C₈₀ and the covalent nature of the U(f¹)=C double bonds were further affirmed through various spectroscopic and theoretical analyses.

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Research Organization:: State Univ. of New York, Buffalo, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-05CH11231; SC0001136

OSTI ID:: 1511585

Alternate ID(s):: OSTI ID: 1631596

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 9; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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