Incorporating nitrogen (N) atom in graphene is considered a key technique for tuning its electrical properties. However, this is still a great challenge, and it is unclear how to build N-graphene with desired nitrogen configurations. There is a lack of experimental evidence to explain the influence and mechanism of structural defects for nitrogen incorporation into graphene compared to the derived DFT theories. Herein, this gap is bridged through a systematic study of different nitrogen-containing gaseous plasma post-treatments on graphene nanowalls (CNWs) to produce N-CNWs with incorporated and substituted nitrogen. The structural and morphological analyses describe a remarkable difference in the plasma–surface interaction, nitrogen concentration and nitrogen incorporation mechanism in CNWs by using different nitrogen-containing plasma. Electrical conductivity measurements revealed that the conductivity of the N-graphene is strongly influenced by the position and concentration of C–N bonding configurations. These findings open up a new pathway for the synthesis of N-graphene using plasma post-treatment to control the concentration and configuration of incorporated nitrogen for application-specific properties.

Carbon, one of the most abundant materials, is very attractive for many applications because it exists in a variety of forms based on dimensions, such as zero-dimensional (0D), one-dimensional (1D), two-dimensional (2D), and-three dimensional (3D). Carbon nanowall (CNW) is a vertically-oriented 2D form of a graphene-like structure with open boundaries, sharp edges, nonstacking morphology, large interlayer spacing, and a huge surface area. Plasma-enhanced chemical vapor deposition (PECVD) is widely used for the large-scale synthesis and functionalization of carbon nanowalls (CNWs) with different types of plasma activation. Plasma-enhanced techniques open up possibilities to improve the structure and morphology of CNWs by controlling the plasma discharge parameters. Plasma-assisted surface treatment on CNWs improves their stability against structural degradation and surface chemistry with enhanced electrical and chemical properties. These advantages broaden the applications of CNWs in electrochemical energy storage devices, catalysis, and electronic devices and sensing devices to extremely thin black body coatings. However, the controlled growth of CNWs for specific applications remains a challenge. In these aspects, this review discusses the growth of CNWs using different plasma activation, the influence of various plasma-discharge parameters, and plasma-assisted surface treatment techniques for tailoring the properties of CNWs. The challenges and possibilities of CNW-related research are also discussed.

The need for 2D vertical graphene nanosheets (VGNs) is driven by its great potential in diverse energy, electronics, and sensor applications, wherein many cases a low-temperature synthesis is preferred due to requirements of the manufacturing process. Unfortunately, most of today’s known methods, including plasma, require either relatively high temperatures or high plasma powers. Herein, we report on a controllable synthesis of VGNs at a pushed down low-temperature boundary for synthesis, the low temperatures (450 °C) and low plasma powers (30 W) using capacitively coupled plasma (CCP) driven by radio-frequency power at 13.56 MHz. The strategies implemented also include unrevealing the role of Nickel (Ni) catalyst thin film on the substrates (Si/Al). It was found that the Ni catalyst on Si/Al initiates the nucleation/growth of VGNs at 450 °C in comparison to the substrates without Ni catalyst. With increasing temperature, the graphene nanosheets become bigger in size, well-structured and well separated. The role of Ni catalysts is hence to boost the growth rate, density, and quality of the growing VGNs. Furthermore, this CCP method can be used to synthesize VGNs at the lowest temperatures possible so far on a variety of substrates and provide new opportunities in the practical application of VGNs.