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.
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