Published October 1, 2024 | Version v1
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Oxygen vacancy induced defect dipoles in BiVO4 for photoelectrocatalytic partial oxidation of methane

  • 1. Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, Queensland, 4072, Australia.
  • 2. CESAM QMAT Physique Théorique des Matériaux, Université de Liège, Liège, Belgium
  • 3. Institute for Superconducting and Electronic Materials, Faculty of Engineering and Information Sciences, University of Wollongong, New South Wales 2500, Australia.
  • 4. Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, Shenyang, 110016, China.
  • 5. School of Materials Science and Engineering, University of Science and Technology of China, 72 Wenhua Road, Shenyang, 110016, China.

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Description

A strong driving force for charge separation and transfer in semiconductors is essential for designing effective photoelectrodes for solar energy conversion. While defect engineering and polarization alignment can enhance this process, their potential interference within a photoelectrode remains unclear. Here we show that oxygen vacancies in bismuth vanadate (BiVO4) can create defect dipoles due to a disruption of symmetry. The modified photoelectrodes exhibit a strong correlation between charge separation and transfer capability and external electrical poling, which is not seen in unmodified samples. Applying poling at -150 Volt boosts charge separation and transfer efficiency to over 90 %. A photocurrent density of 6.3 mA cm-2 is achieved on the photoelectrode after loading with a nickel-iron oxide-based cocatalyst. Furthermore, using generated holes for methane partial oxidation can produce methanol with a Faradaic efficiency of approximately 6 %. These findings provide valuable insights into the photoelectrocatalytic conversion of greenhouse gases into valuable chemical products.

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References

Journal reference
X. Li, Z. Wang, A. Sasani, A. Baktash, K. Wang, H. Lu, J. You, P. Chen, P. Chen, Y. Bao, S. Zhang, G. Liu, L. Wang, Nat. Commun., 2024, accepted, doi: DOI:10.1038/s41467-024-53426-8