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Hematite nanostructures are strong candidates for the development of sustainable water splitting technologies. However, major challenges exist in improving charge density and minimizing charge recombination rates for a competitive photoelectrochemical performance based on hematite without compromising sustainability aspects. Here we develop a synthetic strategy to leverage earth-abundant Al3+ and Zr4+ in a dual-chemical modification to synergistically minimize small polaron effects and interfacial charge recombination. The solution-based method simultaneously induces Al3+ doping of the hematite crystal lattice while Zr4+ forms interfacial excess, creating a single-phased homogeneous nanostructured thin film. The engineered photoanode increased photocurrent from 0.7 mA cm-2 for pristine hematite up to 4.5 mA cm-2 at 1.23 V and beyond 6.0 mA cm-2 when applying an overpotential of 300 mV under simulated sunlight illumination (100 mW cm-2). The results demonstrate the potential of dual-modification design using solution-based processes to enable sustainable energy technologies.
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Hafnium boosts charge carrier dynamics in hematite for improved solar water splitting
The work demonstrates a three-fold increase in photoelectrochemical efficiency of hematite nanorods as a result of the combination of Hafnium surface doping and the incorporation of a ZrO2 underlayer on FTO. While the ZrO2 layer reduced the electron loss from the back-injection into the FTO contact support, Hafnium surface doping did not significantly alter the hematite lattice structure. But rather, Hafnium induced nanorod diameter reduction from 32 ± 2 and 26 ± 2 nm, with a consequent increase in the active surface area. The linear sweep voltammetry measurements with 100 mW cm−2 illumination in a 500 nm photoanode thickness showed a photocurrent density of 2.07 mA cm−2 at 1.23 V in a reversible hydrogen electrode (RHE). The value contrasts with the bare hematite rods (0.75 mA cm−2), highlighting the photoanode design's role in improving solar power hydrogen production.
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- PAR ID:
- 10407994
- Publisher / Repository:
- Elsevier
- Date Published:
- Journal Name:
- Materials Letters
- Volume:
- 340
- Issue:
- C
- ISSN:
- 0167-577X
- Page Range / eLocation ID:
- 134176
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1016/j.matlet.2023.134176
