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Post-Synthetic Silver Ion and Sulfurization Treatment for Enhanced Performance in Sb$_2$Se$_3$ Water Splitting Photocathodes


Adams, Pardis; Schnyder, Ramon; Moehl, Thomas; Bühler, Jan; Alvarez, Angel Labordet; Dimitrievska, Mirjana; McKenna, Keith; Yang, Wooseok; Tilley, S David (2024). Post-Synthetic Silver Ion and Sulfurization Treatment for Enhanced Performance in Sb$_2$Se$_3$ Water Splitting Photocathodes. Advanced Functional Materials, 34(10):2310596.

Abstract

In the past decade, antimony selenide (Sb$_2$Se$_3$) 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 Sb$_2$Se$_3$-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 Sb$_2$(S$_{1−x}$, Se$_x$)$_3$ on the bulk Sb$_2$Se$_3$ 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 [Sb$_4$Se$_6$]$_n$ ribbons and remain in the Ag$^+$ state. This effective treatment combination brings the practicality of the Sb$_2$Se$_3$ photocathode for water splitting one step closer to large-scale applications.

Abstract

In the past decade, antimony selenide (Sb$_2$Se$_3$) 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 Sb$_2$Se$_3$-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 Sb$_2$(S$_{1−x}$, Se$_x$)$_3$ on the bulk Sb$_2$Se$_3$ 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 [Sb$_4$Se$_6$]$_n$ ribbons and remain in the Ag$^+$ state. This effective treatment combination brings the practicality of the Sb$_2$Se$_3$ photocathode for water splitting one step closer to large-scale applications.

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Additional indexing

Other titles:Post-Synthetic Silver Ion and Sulfurization Treatment for Enhanced Performance in Sb2Se3 Water Splitting Photocathodes
Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
08 Research Priority Programs > Solar Light to Chemical Energy Conversion
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > Electronic, Optical and Magnetic Materials
Physical Sciences > General Chemistry
Physical Sciences > Biomaterials
Physical Sciences > General Materials Science
Physical Sciences > Condensed Matter Physics
Physical Sciences > Electrochemistry
Uncontrolled Keywords:Electrochemistry, Condensed Matter Physics, Biomaterials, Electronic, Optical and Magnetic Materials
Language:English
Date:4 March 2024
Deposited On:20 Feb 2024 08:47
Last Modified:30 Apr 2024 01:47
Publisher:Wiley-Blackwell Publishing, Inc.
ISSN:1616-301X
Additional Information:This is the peer reviewed version of the following article: P. Adams, R. Schnyder, T. Moehl, J. Bühler, A. L. Alvarez, M. Dimitrievska, K. McKenna, W. Yang, S. D. Tilley, Post-Synthetic Silver Ion and Sulfurization Treatment for Enhanced Performance in Sb2Se3 Water Splitting Photocathodes. Adv. Funct. Mater. 2023, 2310596, which has been published in final form at https://doi.org/10.1002/adfm.202310596. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. (http://www.wileyauthors.com/self-archiving)
OA Status:Closed
Publisher DOI:https://doi.org/10.1002/adfm.202310596
Project Information:
  • : FunderSNSF
  • : Grant ID184737
  • : Project TitlePhotoelectrochemical Synthesis of Hydrogen and Value-Added Chemicals for a Sustainable Chemical Industry