Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
Publication date: 11th July 2022
Hydrogen production through photoelectrochemical (PEC) water splitting has attracted the attention of researchers as a promising and sustainable approach to converting sunlight into a high-energy fuel. The development of c-Si based photoelectrodes has grown in recent years and has shown excellent results as a p-type light-absorbing semiconductor, achieving high PEC conversion efficiency and long-term stability. Although the TiO2 layer provides chemical stability to the device over a wide pH range, the photopotential generated at the c-Si/TiO2 heterojunction is insufficient due to its unfavorable band alignment between the c-Si absorber and the Electron Transport Layer based on TiO2. One of the strategies used to improve the alignment of the energy levels consists of the intercalation of a very thin layer with a dipole moment. The electrical transport is carried out by the tunnel effect, while the dipole moment modifies the vacuum levels, improving the alignment of the Fermi levels and reducing the energy barriers. In our case we used polyethyleneimine (PEI)-based dipole molecules between the c-Si and the TiO2 layer, resulting in the the final structure of the device as Al/V2Ox/c-Si/PEI/TiO2/Pt.
The devices were submitted to PEC's measurements in 0.5 mol L−1 H2S04 (pH 1.0) as support electrolyte and 1 sun of illumination, using Ag/AgCl(KCl sat.) and Pt plate as reference and counter electrode, respectively. Pt cocatalyst was galvanostatically deposited in three steps of 50, 100 and 200 μA cm−2 with 10 min of each deposition from 1 mmol L−1 H2PtCl6 in PBS supporting electrolyte at pH 6.5. From the linear sweep voltammetry, the best device exhibited an Eonset = 0.23 VRHE and a jph = 31.7 mA cm−2 at 0 VRHE. As a result, ABPE achieved ~2% PEC conversion at 0.11 VRHE. In summary, we can conclude that the use of dipole interlayers to improve the alignment of Fermi levels is a promising approach to improving water splitting in PEC.
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