Origin of extended visible light absorption in nitrogen-doped CuTa2O6 perovskites: the role of copper defects

Morten Weiss; Anja Hofmann; Roland Marschall

doi:10.1515/znb-2023-0094

Published by De Gruyter April 5, 2024

Origin of extended visible light absorption in nitrogen-doped CuTa₂O₆ perovskites: the role of copper defects

Morten Weiss , Anja Hofmann and Roland Marschall

From the journal Zeitschrift für Naturforschung B

https://doi.org/10.1515/znb-2023-0094

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Abstract

The optical band gap of the semiconductor CuTa₂O₆, synthesised via solid-state reaction, can be greatly reduced by annealing in ammonia, which leads to a significant red-shift of the visible light absorption. Using X-ray photoelectron spectroscopy (XPS), we have shown that this absorption extension does not result from the incorporation of nitrogen, but can be attributed to copper defects formed under the reducing conditions of ammonia treatment. Photocatalytic hydrogen evolution experiments were used to investigate the influence of these defects on the photocatalytic performance. We have further shown that CuTa₂O₆ with similar increased visible light absorption can be prepared by annealing with an organic reducing agent – sodium citrate – in inert gas atmosphere.

Keywords: copper tantalate; perovskite; visible light absorption; photocatalysis

Dedicated to Professor Thomas Bredow of the University of Bonn on the occasion of his 60th birthday.

Corresponding author: Roland Marschall, Department of Chemistry, University of Bayreuth, Universitätsstraße 30, 95440 Bayreuth, Germany, E-mail: roland.marschall@uni-bayreuth.de

Acknowledgments

The authors would like to thank Julia Schulze (Justus-Liebig University Giessen, Germany) for mercury intrusion measurement, and Dr. Jana Timm for physisorption measurements (University of Bayreuth). The authors also thank the Bavarian Polymer Institute (BPI) Keylab “Device Engineering” for use of XPS and the Keylab “Electron and Optical Microscopy” for use of the SEM. M.W. and R.M. gratefully acknowledge funding by the BMBF (German Ministry of Education and Research), research project CO₂SimO (033RC029B).

Research ethics: Not applicable.
Author contributions: R.M. planed the study, M.W. and A.H. performed the experiments. The authors have accepted responsibility for the entire content of this manuscript and approved its submission.
Competing interests: The authors state no conflict of interest.
Research funding: This work was funded by the BMBF (German Ministry of Education and Research), research project CO₂SimO (033RC029B).
Data availability: The raw data can be obtained on request from the corresponding author.

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Supplementary Material

This article contains supplementary material (https://doi.org/10.1515/znb-2023-0094).

Received: 2023-10-30

Accepted: 2023-11-30

Published Online: 2024-04-05

Published in Print: 2024-04-25