Robust SrTiO3 Passivation of Silicon Photocathode by Reduced Graphene Oxide for Solar Water Splitting
Аутори
Ho, Hsin-ChiaSmiljanić, Milutin
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Jovanović, Zoran M.
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Čekada, Miha
Kovač, Janez
![](/themes/MirageVinar/images/orcid.png)
Koster, Gertjan
Hlinka, Jiří
Hodnik, Nejc
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Spreitzer, Matjaž
Чланак у часопису (Објављена верзија)
Метаподаци
Приказ свих података о документуАпстракт
Development of a robust photocathode using lowcost and high-performing materials, e.g., p-Si, to produce clean fuel hydrogen has remained challenging since the semiconductor substrate is easily susceptible to (photo)corrosion under photoelectrochemical (PEC) operational conditions. A protective layer over the substrate to simultaneously provide corrosion resistance and maintain efficient charge transfer across the device is therefore needed. To this end, in the present work, we utilized pulsed laser deposition (PLD) to prepare a high-quality SrTiO3 (STO) layer to passivate the p-Si substrate using a buffer layer of reduced graphene oxide (rGO). Specifically, a very thin (3.9 nm ∼10 unit cells) STO layer epitaxially overgrown on rGO-buffered Si showed the highest onset potential (0.326 V vs RHE) in comparison to the counterparts with thicker and/or nonepitaxial STO. The photovoltage, flat-band potential, and electrochemical impedance spectroscopy measurements revealed that the epitaxial... photocathode was more beneficial for charge separation, charge transfer, and targeted redox reaction than the nonepitaxial one. The STO/rGO/Si with a smooth and highly epitaxial STO layer outperforming the directly contacted STO/Si with a textured and polycrystalline STO layer showed the importance of having a well-defined passivation layer. In addition, the numerous pinholes formed in the directly contacted STO/Si led to the rapid degradation of the photocathode during the PEC measurements. The stability tests demonstrated the soundness of the epitaxial STO layer in passivating Si against corrosion. This study provided a facile approach for preparing a robust protection layer over a photoelectrode substrate in realizing an efficient and, at the same time, durable PEC device.
Кључне речи:
pulsed laser deposition, SrTiO3 / epitaxy / , reduced graphene oxide / protection layer / photoelectrochemical water splitting / onset potential / stabilityИзвор:
ACS Applied Materials & Interfaces, 2023, 15, 37, 44482-44492Финансирање / пројекти:
- Slovenian Research Agency [Project No. N2-0187]
- Czech Science Foundation 707 [Project No. 21-20110K]
- Slovenia - Serbia bilateral collaboration (Project “Photoelectrochemical Hydrogen Evolution from Epitaxial Silicon-Oxide Heterostructures (H2EPI)”)
DOI: 10.1021/acsami.3c07747
ISSN: 1944-8252
PubMed: 37695941
Scopus: 2-s2.0-85171900524
Колекције
Институција/група
VinčaTY - JOUR AU - Ho, Hsin-Chia AU - Smiljanić, Milutin AU - Jovanović, Zoran M. AU - Čekada, Miha AU - Kovač, Janez AU - Koster, Gertjan AU - Hlinka, Jiří AU - Hodnik, Nejc AU - Spreitzer, Matjaž PY - 2023 UR - https://vinar.vin.bg.ac.rs/handle/123456789/11587 AB - Development of a robust photocathode using lowcost and high-performing materials, e.g., p-Si, to produce clean fuel hydrogen has remained challenging since the semiconductor substrate is easily susceptible to (photo)corrosion under photoelectrochemical (PEC) operational conditions. A protective layer over the substrate to simultaneously provide corrosion resistance and maintain efficient charge transfer across the device is therefore needed. To this end, in the present work, we utilized pulsed laser deposition (PLD) to prepare a high-quality SrTiO3 (STO) layer to passivate the p-Si substrate using a buffer layer of reduced graphene oxide (rGO). Specifically, a very thin (3.9 nm ∼10 unit cells) STO layer epitaxially overgrown on rGO-buffered Si showed the highest onset potential (0.326 V vs RHE) in comparison to the counterparts with thicker and/or nonepitaxial STO. The photovoltage, flat-band potential, and electrochemical impedance spectroscopy measurements revealed that the epitaxial photocathode was more beneficial for charge separation, charge transfer, and targeted redox reaction than the nonepitaxial one. The STO/rGO/Si with a smooth and highly epitaxial STO layer outperforming the directly contacted STO/Si with a textured and polycrystalline STO layer showed the importance of having a well-defined passivation layer. In addition, the numerous pinholes formed in the directly contacted STO/Si led to the rapid degradation of the photocathode during the PEC measurements. The stability tests demonstrated the soundness of the epitaxial STO layer in passivating Si against corrosion. This study provided a facile approach for preparing a robust protection layer over a photoelectrode substrate in realizing an efficient and, at the same time, durable PEC device. T2 - ACS Applied Materials & Interfaces T1 - Robust SrTiO3 Passivation of Silicon Photocathode by Reduced Graphene Oxide for Solar Water Splitting VL - 15 IS - 37 SP - 44482 EP - 44492 DO - 10.1021/acsami.3c07747 ER -
@article{ author = "Ho, Hsin-Chia and Smiljanić, Milutin and Jovanović, Zoran M. and Čekada, Miha and Kovač, Janez and Koster, Gertjan and Hlinka, Jiří and Hodnik, Nejc and Spreitzer, Matjaž", year = "2023", abstract = "Development of a robust photocathode using lowcost and high-performing materials, e.g., p-Si, to produce clean fuel hydrogen has remained challenging since the semiconductor substrate is easily susceptible to (photo)corrosion under photoelectrochemical (PEC) operational conditions. A protective layer over the substrate to simultaneously provide corrosion resistance and maintain efficient charge transfer across the device is therefore needed. To this end, in the present work, we utilized pulsed laser deposition (PLD) to prepare a high-quality SrTiO3 (STO) layer to passivate the p-Si substrate using a buffer layer of reduced graphene oxide (rGO). Specifically, a very thin (3.9 nm ∼10 unit cells) STO layer epitaxially overgrown on rGO-buffered Si showed the highest onset potential (0.326 V vs RHE) in comparison to the counterparts with thicker and/or nonepitaxial STO. The photovoltage, flat-band potential, and electrochemical impedance spectroscopy measurements revealed that the epitaxial photocathode was more beneficial for charge separation, charge transfer, and targeted redox reaction than the nonepitaxial one. The STO/rGO/Si with a smooth and highly epitaxial STO layer outperforming the directly contacted STO/Si with a textured and polycrystalline STO layer showed the importance of having a well-defined passivation layer. In addition, the numerous pinholes formed in the directly contacted STO/Si led to the rapid degradation of the photocathode during the PEC measurements. The stability tests demonstrated the soundness of the epitaxial STO layer in passivating Si against corrosion. This study provided a facile approach for preparing a robust protection layer over a photoelectrode substrate in realizing an efficient and, at the same time, durable PEC device.", journal = "ACS Applied Materials & Interfaces", title = "Robust SrTiO3 Passivation of Silicon Photocathode by Reduced Graphene Oxide for Solar Water Splitting", volume = "15", number = "37", pages = "44482-44492", doi = "10.1021/acsami.3c07747" }
Ho, H., Smiljanić, M., Jovanović, Z. M., Čekada, M., Kovač, J., Koster, G., Hlinka, J., Hodnik, N.,& Spreitzer, M.. (2023). Robust SrTiO3 Passivation of Silicon Photocathode by Reduced Graphene Oxide for Solar Water Splitting. in ACS Applied Materials & Interfaces, 15(37), 44482-44492. https://doi.org/10.1021/acsami.3c07747
Ho H, Smiljanić M, Jovanović ZM, Čekada M, Kovač J, Koster G, Hlinka J, Hodnik N, Spreitzer M. Robust SrTiO3 Passivation of Silicon Photocathode by Reduced Graphene Oxide for Solar Water Splitting. in ACS Applied Materials & Interfaces. 2023;15(37):44482-44492. doi:10.1021/acsami.3c07747 .
Ho, Hsin-Chia, Smiljanić, Milutin, Jovanović, Zoran M., Čekada, Miha, Kovač, Janez, Koster, Gertjan, Hlinka, Jiří, Hodnik, Nejc, Spreitzer, Matjaž, "Robust SrTiO3 Passivation of Silicon Photocathode by Reduced Graphene Oxide for Solar Water Splitting" in ACS Applied Materials & Interfaces, 15, no. 37 (2023):44482-44492, https://doi.org/10.1021/acsami.3c07747 . .