Journal
NATURE CHEMISTRY
Volume 5, Issue 10, Pages 880-885Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.1748
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Funding
- National Science Foundation [CHE-0938043, CHE-1011760]
- Hollings Marine Laboratory
- US Department of Energy [DE-AC02-05CH11231]
- Directorate For Engineering
- Emerging Frontiers & Multidisciplinary Activities [0938043] Funding Source: National Science Foundation
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Although fullerenes were discovered nearly three decades ago, the mechanism of their formation remains a mystery. Many versions of the classic 'bottom-up' formation mechanism have been advanced, starting with C 2 units that build up to form chains and rings of carbon atoms and ultimately form those well-known isolated fullerenes (for example, I h-C 60). In recent years, evidence from laboratory and interstellar observations has emerged to suggest a 'top-down' mechanism, whereby small isolated fullerenes are formed via shrinkage of giant fullerenes generated from graphene sheets. Here, we present molecular structural evidence for this top-down mechanism based on metal carbide metallofullerenes M2C2@C-1(51383)-C-84 (M=Y, Gd). We propose that the unique asymmetric C-1(51383)-C-84 cage with destabilizing fused pentagons is a preserved 'missing link' in the top-down mechanism, and in well-established rearrangement steps can form many well-known, high-symmetry fullerene structures that account for the majority of solvent-extractable metallofullerenes.
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