In Situ Construction of Hierarchical Diamond Supported on Carbon Nanowalls/Diamond for Enhanced Electron Field Emission

The integration of sp²-/sp³-bonded carbon has aroused increasing attention on attaining a great electron field emission (EFE) performance. Herein, a novel hierarchical diamond@carbon nanowalls/diamond (D@C/D) architecture is facilely prepared through the growth of the hybrid carbon nanowalls/diamond (C/D) film followed by the in situ hydrogen plasma treatment using microwave plasma chemical vapor deposition. The hierarchical D@C/D architecture is composed of thin diamond nanoplatelets sandwiched into carbon nanowalls (CNWs) as the bottom layer and the thickened nanoplatelets constituted by diamond nanograins as the upper layer. The hydrogen plasma plays an effective role in the transformation of sacrificial sp²-bonded CNWs to sp³-bonded diamond, eventually leading to the template thickening of diamond nanoplatelets in the upper layer. Impressively, the D@C/D-90 film demonstrates much better EFE behaviors of low turn-on potential (E_o = 4.3 V μm^-1), high current density (J_e@8 V μm^-1 = 20.81 mA cm^-1), and superior long-term stability, in comparison with the pristine C/D film (E_o = 6 V μm^-1, J_e@8 V μm^-1 = 0.33 mA cm^-1). The enhanced EFE performance of the hierarchical D@C/D film is ascribed to the well-established graphite pathway for electrons transported from the bottom to the top and the increased diamond emitting sites with negative electron-affinity and robust nature at the top. This work will promote the development of the high-performance cathode EFE material based on hybrid sp²/sp³-bonded carbon, and the method proposed here also provides an effective strategy to construct a diamond nanostructure for various applications.