Xianlong Li^1*, Zhiliang Wang*^1*, Alireza Sasani^2*, Ardeshir Baktash^1*, Kai Wang^1*, haijiao Lu^1*, jiakang you^1*, Peng Chen^1*, Ping Chen^1*, Yifan Bao^1*, Shujun Zhang^3*, Gang Liu^4,5*, Lianzhou Wang*^1*

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.

* Corresponding authors emails: xianlong.li@uq.edu.au, zhiliang.wang@uq.edu.au, a.sasani@uliege.be, a.baktash@uq.edu.au, kai.wang@uq.edu.au, haijiao.lu@uq.edu.au, jiakang.you@uq.net.au, p.chen1@uq.edu.au, ping.chen1@uq.edu.au, y.bao@uq.edu.au, shujun@uow.edu.au, gangliu@imr.ac.cn, l.wang@uq.edu.au

DOI10.24435/materialscloud:gf-jd [version v1]

Publication date: Oct 01, 2024

How to cite this record

Xianlong Li, Zhiliang Wang*, Alireza Sasani, Ardeshir Baktash, Kai Wang, haijiao Lu, jiakang you, Peng Chen, Ping Chen, Yifan Bao, Shujun Zhang, Gang Liu, Lianzhou Wang*, Oxygen vacancy induced defect dipoles in BiVO4 for photoelectrocatalytic partial oxidation of methane, Materials Cloud Archive 2024.145 (2024), https://doi.org/10.24435/materialscloud:gf-jd

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.

Materials Cloud sections using this data

Files

File name	Size	Description
CONTCAR_BVO MD5md5:f3eecfc851e9e4d4e2d92771c9bb5d65	10.6 KiB	atomic coordination of BiVO4 in Figure 1a
CONTCAR_BVO-Vo MD5md5:fc26d7ebee4d35c63e68f0a564a5f50f	10.5 KiB	atomic coordination of BiVO4 with oxygen vacancies in Figure 1b
CONTCAR_BVO-1c MD5md5:5182bddf437405846834e5c979aa8d3e	2.9 KiB	atomic coordination of BiVO4 in Figure 1c
CONTCAR_BVO-Vo-1c MD5md5:6579003e6ba28efdb026a1b9eefc817f	2.8 KiB	atomic coordination of BiVO4 with oxygen vacancies in Figure 1c
NCOMMS-24-22524A.xlsx MD5md5:9b1ff5cbf976aa54ba34b7c0cc8c2923	4.4 MiB	original data for the plots in all figures

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External references

Keywords

Experimental electronic structure ARC