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Mechanism of carbon nanotubes unzipping into graphene ribbons
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Figures

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FIG. 1.

Optimized geometries [(a)–(e)] of the structures obtained when approaching the opener anion to the CNT connecting initially two of the oxygen atoms from the permanganate to the B1–B5 bonds, respectively, (vide infra).

Image of FIG. 2.

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FIG. 2.

(a) (3,3) armchair CNT with , , and , and two edge bonds, (all labeled bonds but are orthogonal to the plane of the page). Conformations (b) after an oxygen-pair attack to bond ; (c) after a couple of oxygen pairs attack and ; (d) when an oxygen pair attacks conformation (b) on , and (e) when an attacking oxygen pair breaks on conformation (b).

Image of FIG. 3.

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FIG. 3.

[(a)–(f)] Optimized structures obtained through the gradual unzipping of a (5,5) CNT. Pairs of oxygen atoms are added sequentially. A new geometry optimization is performed after each pair addition of oxygen atoms.

Image of FIG. 4.

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FIG. 4.

The edges of the unopened (5,5) CNT [Fig. 3(f)] are passivated with hydrogen atoms (a) and the optimized structure (b) opens on the internal bond B1 but not on the edge bond B5. Hydrogen passivation of the (6,0) zigzag CNT (c) followed by oxidation of the path of internal bonds slanted by 30° relative to the CNT rims leads to the unzipping of the tube (d).

Image of FIG. 5.

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FIG. 5.

Chemical reaction of an armchair (3,3) CNT with on an acidic environment. (a) Bare armchair (3,3) CNT. (b) CNT attacked on an internal bond by on . (c) CNT is attacked on a second bond parallel to the first one with the forward pointing attacking O-atom parallel to the CNT axis on acidic medium . (d) Final structure from the initial one in (c); the attacked bond does not break and the anion goes to the edge of the CNT. (e) An alternative second attacking , with the attacking O-atom pointing downward to the hole left by the first attack; the attacked bond and acidic medium are as in (c). (f) Final structure from the initial one in (e); the attacked bond breaks leading to an unzipped CNT; flattening of the ribbon is impeded by the moieties product of the reaction.

Tables

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Table I.

Energies and binding energies for the CNT, the permanganate, and the optimized structures of CNT when is bonded, unbounded, on B1–B5, as shown in Fig. 1. The C–C distance corresponds to the carbons bonded to the oxygen atoms.

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Table II.

Total and binding energies for the (3,3) CNT and attacking oxygen pair structures. Second-pair binding energy yields the binding energy of an oxygen-pair after a successful attack of bond by a first oxygen pair. Multiplicities of the structures are included in parenthesis.

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Table III.

Total energies of each step in the studied unzipping process shown in Figs. 3 and 4(b) along with the lengths of the carbon-carbon distance in each oxidized bond.

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/content/aip/journal/jcp/131/3/10.1063/1.3170926
2009-07-21
2014-04-16

Abstract

The fabrication of graphenenanoribbons from carbon nanotubes(CNTs) treated with potassium permanganate in a concentrated sulfuric acid solution has been reported by Kosynkin et al. [Nature (London)458, 872 (2009)]. Here we report ab initio density functional theory calculations of such unzipping process. We find that the unzipping starts with the potassium permanganate attacking one of the internal C–C bonds of the CNT, stretching and breaking it. The created defect weakens neighboring bonds along the length of the CNT, making them energetically prone to be attacked too.

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Scitation: Mechanism of carbon nanotubes unzipping into graphene ribbons
http://aip.metastore.ingenta.com/content/aip/journal/jcp/131/3/10.1063/1.3170926
10.1063/1.3170926
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