Abstract
γ-Al2O3 nanoparticles promote pyrolytic carbon deposition of CH4 at temperatures higher than 800 °C to give single-walled nanoporous graphene (NPG) materials without the need for transition metals as reaction centers. To accelerate the development of efficient reactions for NPG synthesis, we have investigated early-stage CH4 activation for NPG formation on γ-Al2O3 nanoparticles via reaction kinetics and surface analysis. The formation of NPG was promoted at oxygen vacancies on (100) surfaces of γ-Al2O3 nanoparticles following surface activation by CH4. The kinetic analysis was well corroborated by a computational study using density functional theory. Surface defects generated as a result of surface activation by CH4 make it kinetically feasible to obtain single-layered NPG, demonstrating the importance of precise control of oxygen vacancies for carbon growth.
Highlights
Graphene is a two-dimentional (2D) allotrope of carbon arranged in a planarly hexagonal lattice, that displays high elasticity and electronic/thermal conductivity.[1]
We found that the dissociative adsorption of CH4 on the oxygen vacancy is the rate-limiting step, which is in agreement with our experiments, and that the dissociative addition undergoes in terms of the Lewis acid-base mechanism.[25,72,73,74]
Carbon growth was promoted at the oxygen vacancies without the introduction of transition metal reaction centers
Summary
Graphene is a two-dimentional (2D) allotrope of carbon arranged in a planarly hexagonal lattice, that displays high elasticity and electronic/thermal conductivity.[1]. We found that the formation of NPG is promoted at oxygen vacancies on (100) surfaces of -Al2O3, which are generated at temperatures higher than 800°C in the presence of CH4.
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