Interconversions between Uranium Mono-metallofullerenes: Mechanistic Implications and Role of Asymmetric Cages

J Am Chem Soc. 2020 Jul 29;142(30):13112-13119. doi: 10.1021/jacs.0c04888. Epub 2020 Jul 16.

Abstract

The isolation and structural characterization of three new monometallic uranium metallofullerenes, U@D2(21)-C84, U@Cs(15)-C86, and U@C1(11)-C86, allowed us to complete an interconversion map for all the characterized uranium mono-metallofullerenes. The topological analysis reveals that asymmetric fullerene cages, which may be formed by roll and wrap processes directly from graphene, are the starting points for a series of highly symmetric fullerene structures via top-down and bottom-up growth mechanisms. Moreover, some asymmetric intermediates, such as C1(28324)-C80, can serve as precursors to form either larger cages in consecutive growing processes or smaller cages during cascade shrinking processes. This work provides evidence for both top-down and bottom-up processes happening simultaneously during the arcing processes. This study also sheds light on the prediction of possible cage structures for minor products produced in low yields in the soot.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, Non-P.H.S.