Oxygen vacancy induced defect dipoles in BiVO4 for photoelectrocatalytic partial oxidation of methane

Xianlong Li, Zhiliang Wang (), Alireza Sasani, Ardeshir Baktash, Kai Wang, Haijiao Lu, Jiakang You, Peng Chen, Ping Chen, Yifan Bao, Shujun Zhang, Gang Liu and Lianzhou Wang ()
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Xianlong Li: The University of Queensland
Zhiliang Wang: The University of Queensland
Alireza Sasani: Université de Liège
Ardeshir Baktash: The University of Queensland
Kai Wang: The University of Queensland
Haijiao Lu: The University of Queensland
Jiakang You: The University of Queensland
Peng Chen: The University of Queensland
Ping Chen: The University of Queensland
Yifan Bao: The University of Queensland
Shujun Zhang: University of Wollongong
Gang Liu: Chinese Academy of Sciences
Lianzhou Wang: The University of Queensland

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41467-024-53426-8

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