Interfacial Oxide Formation Limits the Photovoltage of α-SnWO4/NiOx Photoanodes Prepared by Pulsed Laser Deposition

Patrick Schnell, Moritz Kölbach, Markus Schleuning, Keisuke Obata, Rowshanak Irani, Ibbi Y. Ahmet, Moussab Harb, David E. Starr, Roel van de Krol, Fatwa F. Abdi

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19 Scopus citations


α-SnWO4 is a promising metal oxide photoanode material for direct photoelectrochemical water splitting. With a band gap of 1.9 eV, it ideally matches the requirements as a top absorber in a tandem device theoretically capable of achieving solar-to-hydrogen (STH) efficiencies above 20%. It suffers from photoelectrochemical instability, but NiOx protection layers have been shown to help overcome this limitation. At the same time, however, such protection layers seem to reduce the photovoltage that can be generated at the solid/electrolyte junction. In this study, an extensive analysis of the α-SnWO4/NiOx interface is performed by synchrotron-based hard X-ray photoelectron spectroscopy (HAXPES). NiOx deposition introduces a favorable upwards band bending, but also oxidizes Sn2+ to Sn4+ at the interface. By combining the HAXPES data with open circuit potential (OCP) analysis, density functional theory (DFT) calculations, and Monte Carlo-based photoemission spectra simulation, the presence of a thin oxide layer at the α-SnWO4/NiOx interface is suggested and shown to be responsible for the limited photovoltage. Based on this new-found understanding, suitable mitigation strategies can be proposed. Overall, this study demonstrates the complex nature of solid-state interfaces in multi-layer photoelectrodes, which needs to be unraveled to design efficient heterostructured photoelectrodes for solar water splitting.
Original languageEnglish (US)
Pages (from-to)2003183
JournalAdvanced Energy Materials
StatePublished - Jan 14 2021

Bibliographical note

KAUST Repository Item: Exported on 2021-02-02
Acknowledgements: The authors acknowledge financial support for this work from the Helmholtz International Research School “Hybrid Integrated Systems for Conversion of Solar Energy” (HI-SCORE), an initiative co-funded by the Initiative and Networking Fund of the Helmholtz Association. Part of the work was funded by the Volkswagen Foundation. They would also like to thank Roberto Felix Duarte and Regan Wilks for the access and technical assistance to the HiKE endstation, KMC-1 beamline at the BESSY-II synchrotron facility, as well as Karsten Harbauer and Ronen Gottesman for supporting the PLD experiments. M.H. thanks the KAUST Supercomputing Laboratory for the needed computational resources. The authors thank Ulrike Bloeck for recording the TEM images.
Open access funding enabled and organized by Projekt DEAL.


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