A novel one-pot facile economic approach for the mass synthesis of exfoliated multilayered nitrogen-doped graphene-like nanosheets: new insights into the mechanistic study

Abstract

The present research focuses on providing a novel facile, cost-effective and eco-friendly method for the mass production of N-doped graphene-like nanosheets (NGLs), in order to industrially benefit the exploitation of N-doped graphene in electronics, which will lead to the remarkable prosperity of graphene-based nanoelectronics. NGLs have been synthesized through a one-pot single-step process involving hydrolysis/hydrothermal treatment of glucose under mild conditions, using cetyltrimethylammonium bromide (CTAB) and ammonia solution (NH₄OH) as the structure-directing agents. NGLs of high yield (65 wt%) and fascinating structural features, including low oxidation level, good crystalline structural order, and large laterally sized and well-exfoliated nanosheets, have been produced. The growth mechanism has been deeply investigated. The impressive chemical nature of CTAB has a synergistic effect in controlling the NGL structure. The cationic head of CTAB and anionic OH⁻ ions resulting from NH₄OH ionization have formed a passivating layer that played a profound role in hindering the NGL agglomeration and allowing the NGLs to grow into large lateral dimensions. Meanwhile, the polar (mainly H-bonding) and apolar (hydrophobic) interfacial interactions between the passivating layer and the graphitic network can be mainly considered responsible for the mild disturbed structural order inside the sp² crystals. On the other hand, the excessive decomposition of CTAB that is also accompanied by fair ammonia decomposition during the hydrothermal treatment resulted in plenty of hydrogen and nitrogen gases in the atmosphere. The nitrogen gas N-doped the graphitic structure and the hydrogen gas effectively deoxygenated it. Furthermore, the high evolution rate of gases throughout the synthesis system contributed to the obstruction of NGL agglomeration. These results emphasize the high yield and good quality of the synthesized NGLs, which makes such a strategy promising in trust acquisition for investors in industrial production of N-doped graphene.