Abstract
Although fullerenes can be efficiently generated from graphite in high yield, the route to the formation of these symmetrical and aesthetically pleasing carbon cages from a flat graphene sheet remains a mystery. The most widely accepted mechanisms postulate that the graphene structure dissociates to very small clusters of carbon atoms such as C2, which subsequently coalesce to form fullerene cages through a series of intermediates. In this Article, aberration-corrected transmission electron microscopy directly visualizes, in real time, a process of fullerene formation from a graphene sheet. Quantum chemical modelling explains four critical steps in a top-down mechanism of fullerene formation: (i) loss of carbon atoms at the edge of graphene, leading to (ii) the formation of pentagons, which (iii) triggers the curving of graphene into a bowl-shaped structure and which (iv) subsequently zips up its open edges to form a closed fullerene structure.
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Acknowledgements
This work was supported by the Engineering and Physical Sciences Research Council (Career Acceleration Fellowship to E.B., grant no. EP/C545273/1 to A.N.K.), the European Science Foundation, the Royal Society, the DFG (German Research Foundation) and the State Baden-Württemberg within the SALVE (Sub Angström Low Voltage Electron Microscopy) project and by the DFG within Collaborative Research Centre (SFB) 569.
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A.C. conceived, designed and carried out experiments. U.K. contributed to the development of the experimental methodology and the discussion of the results. E.B. and N.A.B. performed theoretical modelling and contributed equally to this work. A.N.K. proposed the mechanism and wrote the original manuscript. All authors discussed the results and commented on the manuscript.
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Chuvilin, A., Kaiser, U., Bichoutskaia, E. et al. Direct transformation of graphene to fullerene. Nature Chem 2, 450–453 (2010). https://doi.org/10.1038/nchem.644
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DOI: https://doi.org/10.1038/nchem.644
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