Journal
NANO RESEARCH
Volume 14, Issue 7, Pages 2285-2293Publisher
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-020-3223-9
Keywords
silicon; local atomic structure; water splitting; photocathodes; hydrogen generation
Categories
Funding
- National Key Research and Development Program of China [2018YFB1502003, 2017YFE0193900]
- National Natural Science Foundation of China [51961165103, 21875183]
- National Program for Support of Top-notch Young Professionals
- Youth Innovation Team of Shaanxi Universities
- [MoST 107-2112-M-032-004-MY3]
- [108-2218-E-032-003-MY3]
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The deposition of a WO3 thin layer on a p-Si substrate significantly improves the PEC performance of the photoelectrode, leading to increased cathodic photocurrent density and anodic shift in onset potential for water reduction. Variations in oxygen pressures during deposition can modulate the W-O bond covalency and WO6 octahedral structure symmetry, enhancing charge carrier transport and separation. Additionally, manipulation of W-O local atomic structures in the deposited WO3 layer contributes to a significant improvement in PEC performance for solar hydrogen generation.
Self-passivation in aqueous solution and sluggish surface reaction kinetics significantly limit the photoelectrochemical (PEC) performances of silicon-based photoelectrodes. Herein, a WO3 thin layer is deposited on the p-Si substrate by pulsed laser deposition (PLD), acting as a photocathode for PEC hydrogen generation. Compared to bare p-Si, the single-junctional p-Si/WO3 photoelectrodes exhibit excellent and stable PEC performances with significantly increased cathodic photocurrent density and exceptional anodic shift in onset potential for water reduction. It is revealed that the WO3 layer could reduce the charge transfer resistance across the electrode/electrolyte interface by eliminating the effect of Fermi level pinning on the surface of p-Si. More importantly, by varying the oxygen pressures during PLD, the collaborative modulation of W-O bond covalency and WO6 octahedral structure symmetry contributes to the promoted charge carrier transport and separation. Meanwhile, a large band bending at the p-Si/WO3 junction, induced by the optimized O vacancy contents in WO3, could provide a photovoltage as high as similar to 500 mV to efficiently drive charge transfer to overcome the water reduction overpotential. Synergistically, by manipulating W-O local atomic structures in the deposited WO3 layer, a great improvement in PEC performance could be achieved over the single-junctional p-Si/WO3 photocathodes for solar hydrogen generation.
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