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

Abstract

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 Ih(7)-C80 fullerenes as nanocontainers, a diuranium carbide cluster, U=C=U, has been encapsulated and stabilized in the form of UCU@Ih(7)-C80. This endohedral fullerene was prepared utilizing the Krätschmer–Huffman arc discharge method, and was then co-crystallized with nickel(II) octaethylporphyrin (NiII-OEP) to produce UCU@Ih(7)-C80·[NiII-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@Ih(7)-C80 and the covalent nature of the U(f1)=C double bonds were further affirmed through various spectroscopic and theoretical analyses.

Authors:
 [1];  [2];  [1];  [2];  [3];  [3];  [4];  [5];  [5]; ORCiD logo [5];  [1];  [1];  [6]; ORCiD logo [6];  [1]; ORCiD logo [1];  [1];  [2];  [3]; ORCiD logo [7] more »;  [1] « less
  1. Soochow University, Suzhou, Jiangsu (China)
  2. Tsinghua Univ., Beijing (China)
  3. Universität Bonn (Germany)
  4. University of Texas, El Paso, TX (United States)
  5. State Univ. of New York, Buffalo, NY (United States)
  6. Leibniz Institute for Solid State and Materials Research, Dresden (Germany)
  7. Tsinghua Univ., Beijing (China); Universität Siegen (Germany)
Publication Date:
Research Org.:
State Univ. of New York, Buffalo, NY (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1511585
Alternate Identifier(s):
OSTI ID: 1631596
Grant/Contract Number:  
AC02-05CH11231; SC0001136
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

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, and Chen, Ning. A diuranium carbide cluster stabilized inside a C80 fullerene cage. United States: N. p., 2018. Web. doi:10.1038/s41467-018-05210-8.
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. A diuranium carbide cluster stabilized inside a C80 fullerene cage. United States. https://doi.org/10.1038/s41467-018-05210-8
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, and Chen, Ning. Mon . "A diuranium carbide cluster stabilized inside a C80 fullerene cage". United States. https://doi.org/10.1038/s41467-018-05210-8. https://www.osti.gov/servlets/purl/1511585.
@article{osti_1511585,
title = {A diuranium carbide cluster stabilized inside a C80 fullerene cage},
author = {Zhang, Xingxing and Li, Wanlu and Feng, Lai and Chen, Xin and Hansen, Andreas and Grimme, Stefan and Fortier, Skye and Sergentu, Dumitru-Claudiu and Duignan, Thomas J. and Autschbach, Jochen and Wang, Shuao and Wang, Yaofeng and Velkos, Giorgios and Popov, Alexey A. and Aghdassi, Nabi and Duhm, Steffen and Li, Xiaohong and Li, Jun and Echegoyen, Luis and Schwarz, W. H. Eugen and Chen, Ning},
abstractNote = {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 Ih(7)-C80 fullerenes as nanocontainers, a diuranium carbide cluster, U=C=U, has been encapsulated and stabilized in the form of UCU@Ih(7)-C80. This endohedral fullerene was prepared utilizing the Krätschmer–Huffman arc discharge method, and was then co-crystallized with nickel(II) octaethylporphyrin (NiII-OEP) to produce UCU@Ih(7)-C80·[NiII-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@Ih(7)-C80 and the covalent nature of the U(f1)=C double bonds were further affirmed through various spectroscopic and theoretical analyses.},
doi = {10.1038/s41467-018-05210-8},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {7}
}

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