Facile synthesis and optimization of graphene oxide reduction by annealing in hydrazine vapour in ambient air for potential application in perovskite solar cells

Abstract

Graphene oxide (GO) was synthesized from graphite via a modified Hummer's method, followed by thermal and chemical reductions to produce reduced graphene oxide (RGO) samples at various temperatures. A suite of characterization techniques including Fourier Transform Infrared Spectroscopy (FTIR), Scanning Electron Microscopy (SEM), Energy-Dispersive X-ray Spectroscopy (EDS), UV-Visible Spectroscopy, thermogravimetric analysis (TGA), X-ray diffraction (XRD), and Hall effect measurements were employed to assess the structural, morphological, optical, and electrical properties of the samples. FTIR analysis confirmed the successful functionalization of graphite to GO and subsequent reduction to reduced graphene oxide, with peak intensities decreasing as the reduction temperature increased. UV-visible spectroscopy of GO showed a maximum absorption at 235 nm which confirmed the synthesis of GO while the reduction revealed a notable red shift in absorption peaks with increasing annealing temperature, and that signified a reduction in bandgap. XRD analyses demonstrated the removal of oxygen functional groups. The X-ray diffraction (XRD) analysis of GO showed diffraction at 2θ = 10.74° which revealed a fully oxidized graphene oxide with oxygen-containing functional groups, and hence an increase in interlayer spacing (d₀₀₂) from 3.341 Å (graphite) to 8.228 Å (GO). Upon reduction, there is a gradual decrease in d₀₀₂ from 8.228 Å (GO) to 3.387 Å (HRGO300), suggesting the gradual removal of intercalated oxygen molecules, and hence the gradual restoration of sp² hybridisation in graphene. The EDS analysis revealed an increase in the carbon-to-oxygen (C/O) ratio from 1.78 in GO to 2.75 in HRGO300 as the annealing temperature for the reduction process increased which further confirmed the removal of oxygen functional groups. The Hall effect data showed hole mobility of 4.634 x10¹ (GO), 4.831 x10¹ (HRGO200), and 5.462 x10⁰ (HRGO300) with conductivities of 8.985 x10^-5 (GO), 1.087 x10⁰ (HRGO200) and 1.791 x10¹ 1/Ω cm, suggesting an increase in conductivity as the annealing temperature increased as revealed in the EDS. Out of the three samples identified as hole transport materials, the sample HRGO300 with the highest C/O ratio of 2.75 has the highest conductivity, and hence most suitable for application as hole transport material in perovskite solar cell.