研究目的
To compare the photoelectrochemical H2 evolution activity of two silicon photocathode nanostructuring strategies: direct nanostructuring of the silicon surface and incorporation of nanostructured zinc oxide to increase the electrocatalyst surface area on planar silicon, with the goal of promoting electrocatalysis while minimizing surface recombination.
研究成果
The ZnONW support strategy allows silicon photocathodes to achieve both high electrocatalytic activity from structured catalysts and retain the photoactivity of planar silicon homojunctions, outperforming direct silicon nanostructuring by approximately 50 mV at open circuit. This decoupling approach is a general strategy for integrating earth-abundant catalysts into solar fuels devices without compromising efficiency, with potential for further development using other transparent nanostructures.
研究不足
The durability of electrodes is limited by ZnO stability in strongly acidic electrolyte. There is a reduction in light-limited current density for nanostructured electrodes due to increased absorption in catalyst layers. Potential for optimization in catalyst placement and thickness to reduce parasitic light absorption.
1：Experimental Design and Method Selection:
The study compares two nanostructuring strategies for silicon photocathodes: direct nanostructuring of silicon and using nanostructured zinc oxide supports. Methods include atomic layer deposition (ALD), dry silicon etching, and solution-based deposition of ZnO nanowires.
2：Sample Selection and Data Sources:
Electrodes were fabricated using n+p-Si and n+-Si substrates, with various nanostructures (e.g., Si nanowires, ZnO nanowires) coated with MoS2 or Pt catalysts.
3：List of Experimental Equipment and Materials:
Equipment includes ALD systems, dry etching tools, SEM, STEM-EDS, LSV setups. Materials include silicon wafers, ZnO, TiO2, MoS2, Pt.
4：Experimental Procedures and Operational Workflow:
Fabrication involved ALD deposition of TiO2 and MoS2 on prepared surfaces, solution-based ZnONW deposition, and characterization via SEM, STEM-EDS, and photoelectrochemical measurements (LSV under 1 sun illumination in
5：5 M H2SO4). Data Analysis Methods:
Data were analyzed using LSV curves, modeling electrode behavior as a photovoltaic element in series with an electrocatalyst impedance element, and comparing potentials and current densities.
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