Post-Synthetic Silver Ion and Sulfurization Treatment for Enhanced Performance in Sb2Se3 Water Splitting Photocathodes

Pardis Adams, Ramon Schnyder, Thomas Moehl, Jan Bühler, Angel Labordet Alvarez, Mirjana Dimitrievska, Keith McKenna, Wooseok Yang*, S. David Tilley*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

In the past decade, antimony selenide (Sb2Se3) has made significant progress as a solar energy conversion material. However, the photovoltage deficit continues to pose a challenge and is a major hurdle that must be overcome to reach its maximum solar conversion efficiency. In this study, various post-synthetic treatments are employed, of which the combination of a solution phase silver nitrate treatment and sulfurization has shown to be the most effective approach to mitigate the photovoltage deficit in this Sb2Se3-based device. A significant enhancement in the photovoltage is observed after the treatments, as evident by the increase in the onset potential from 0.18 to 0.40 V versus reversible hydrogen electrode. Multiwavelength Raman shows that combining these two treatments removes amorphous Se and metallic Sb from the surface and yields a high-quality surface layer of Sb2(S1−x, Sex)3 on the bulk Sb2Se3 photoabsorber layer. X-ray photoelectron spectroscopy with depth profiling reveals extensive incorporation of silver into the film. Density functional theory calculations suggest that silver ions can intercalate between the [Sb4Se6]n ribbons and remain in the Ag+ state. This effective treatment combination brings the practicality of the Sb2Se3 photocathode for water splitting one step closer to large-scale applications.

Original languageEnglish
Article number2310596
Number of pages9
JournalADVANCED FUNCTIONAL MATERIALS
Early online date29 Nov 2023
DOIs
Publication statusE-pub ahead of print - 29 Nov 2023

Bibliographical note

© 2023 Wiley-VCH GmbH. This is an author-produced version of the published paper. Uploaded in accordance with the University’s Research Publications and Open Access policy.

Funding Information:
This work was supported by the University of Zurich, URPP LightChEC, and SNF Project # 184737. W.Y. would like to thank the National R&D Program through the National Research Foundation of Korea (NRF), funded by the Ministry of Science and ICT RS‐2023‐0025177. K.P.M. would like to acknowledge membership in the UK's HEC Materials Chemistry Consortium, funded by EPSRC (EP/R029431 and EP/X035859). This work used the ARCHER2 UK National Supercomputing Service ( http://www.archer2.ac.uk ).

Keywords

  • photoelectrochemical water splitting
  • SbSe silver ion
  • solution treatments
  • sulfurization

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