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1.
Nanoscale ; 10(25): 12123-12132, 2018 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-29915820

RESUMO

Recrystallization of bulk materials is a well-known phenomenon, which is widely used in commercial manufacturing. However, for low-dimensional materials like graphene, this process still remains an unresolved puzzle. Thus, the understanding of the underlying mechanisms and the required conditions for recrystallization in low dimensions is essential for the elaboration of routes towards the inexpensive and reliable production of high-quality nanomaterials. Here, we unveil the details of the efficient recrystallization of one-atom-thick pure and boron-doped polycrystalline graphene layers on a Co(0001) surface. By applying photoemission and electron diffraction, we show how more than 90% of the initially misoriented graphene grains can be reconstructed into a well-oriented and single-crystalline layer. The obtained recrystallized graphene/Co interface exhibits high structural quality with a pronounced sublattice asymmetry, which is important for achieving an unbalanced sublattice doping of graphene. By exploring the kinetics of recrystallization for native and B-doped graphene on Co, we were able to estimate the activation energy and propose a mechanism of this process.

2.
Nano Lett ; 16(7): 4535-43, 2016 07 13.
Artigo em Inglês | MEDLINE | ID: mdl-27248659

RESUMO

The implementation of future graphene-based electronics is essentially restricted by the absence of a band gap in the electronic structure of graphene. Options of how to create a band gap in a reproducible and processing compatible manner are very limited at the moment. A promising approach for the graphene band gap engineering is to introduce a large-scale sublattice asymmetry. Using photoelectron diffraction and spectroscopy we have demonstrated a selective incorporation of boron impurities into only one of the two graphene sublattices. We have shown that in the well-oriented graphene on the Co(0001) surface the carbon atoms occupy two nonequivalent positions with respect to the Co lattice, namely top and hollow sites. Boron impurities embedded into the graphene lattice preferably occupy the hollow sites due to a site-specific interaction with the Co pattern. Our theoretical calculations predict that such boron-doped graphene possesses a band gap that can be precisely controlled by the dopant concentration. B-graphene with doping asymmetry is, thus, a novel material, which is worth considering as a good candidate for electronic applications.

3.
ACS Nano ; 9(1): 320-6, 2015 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-25560087

RESUMO

Oxygen reduction reaction (ORR) plays a key role in lithium-air batteries (LABs) that attract great attention thanks to their high theoretical specific energy several times exceeding that of lithium-ion batteries. Because of their high surface area, high electric conductivity, and low specific weight, various carbons are often materials of choice for applications as the LAB cathode. Unfortunately, the possibility of practical application of such batteries is still under question as the sustainable operation of LABs with carbon cathodes is not demonstrated yet and the cyclability is quite poor, which is usually associated with oxygen reduced species side reactions. However, the mechanisms of carbon reactivity toward these species are still unclear. Here, we report a direct in situ X-ray photoelectron spectroscopy study of oxygen reduction by lithiated graphene and graphene-based materials. Although lithium peroxide (Li2O2) and lithium oxide (Li2O) reactions with carbon are thermodynamically favorable, neither of them was found to react even at elevated temperatures. As lithium superoxide is not stable at room temperature, potassium superoxide (KO2) prepared in situ was used instead to test the reactivity of graphene with superoxide species. In contrast to Li2O2 and Li2O, KO2 was demonstrated to be strongly reactive.

4.
Phys Chem Chem Phys ; 16(46): 25621-7, 2014 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-25352030

RESUMO

In this paper we propose a new and simple method to tune the carbon nanowall microstructure by sharp variation of CH4/H2 plasma conditions. Using theoretical calculations we demonstrated that the sharp variation of gas pressure and discharge current leads to significant variation of plasma radical composition. In some cases such perturbation creates the necessary conditions for the nucleation of smaller secondary nanowalls on the surface of primary ones.

5.
Nano Lett ; 13(10): 4697-701, 2013 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-24004050

RESUMO

Unfortunately, the practical applications of Li-O2 batteries are impeded by poor rechargeability. Here, for the first time we show that superoxide radicals generated at the cathode during discharge react with carbon that contains activated double bonds or aromatics to form epoxy groups and carbonates, which limits the rechargeability of Li-O2 cells. Carbon materials with a low amount of functional groups and defects demonstrate better stability thus keeping the carbon will-o'-the-wisp lit for lithium-air batteries.

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