Chemistry (all); Biochemistry, Genetics and Molecular Biology (all); Physics and Astronomy (all)
Abstract :
[en] 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.
Disciplines :
Chemistry
Author, co-author :
Li, Xianlong; Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, QLD, 4072, Australia
Wang, Zhiliang ; Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, QLD, 4072, Australia. zhiliang.wang@uq.edu.au
Sasani, Alireza ; Université de Liège - ULiège > Département de physique > Physique théorique des matériaux
Baktash, Ardeshir ; Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, QLD, 4072, Australia
Wang, Kai ; Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, QLD, 4072, Australia
Lu, Haijiao ; Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, QLD, 4072, Australia
You, Jiakang; Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, QLD, 4072, Australia
Chen, Peng; Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, QLD, 4072, Australia
Chen, Ping; Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, QLD, 4072, Australia
Bao, Yifan; Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, QLD, 4072, Australia
Zhang, Shujun ; Institute for Superconducting and Electronic Materials, Faculty of Engineering and Information Sciences, University of Wollongong, New South Wales, 2500, Australia
Liu, Gang ; Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, Shenyang, 110016, China ; School of Materials Science and Engineering, University of Science and Technology of China, 72 Wenhua Road, Shenyang, 110016, China
Wang, Lianzhou ; Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, QLD, 4072, Australia. l.wang@uq.edu.au
The authors would like to acknowledge the support by Australian Research Council through its DECRA (DE210100930, DE230101712), Discovery (DP200101900, DP230100462), Future Fellowship (FT230100251) and Laureate Fellowship (FL190100139) schemes. This work was performed in part at the Queensland node of the Australian National Fabrication Facility. This research was undertaken on the X-ray Absorption Spectroscopy and Soft X-ray Absorption Spectroscopy beamlines at the Australian Synchrotron, part of ANSTO. A company established under the National Collaborative Research Infrastructure Strategy to provide nano and microfabrication facilities for Australia\u2019s researchers. The authors acknowledge the facilities, and the scientific and technical assistance, of the Australian Microscopy and Microanalysis Research Facility at the Centre for Microscopy and Microanalysis, The University of Queensland. X. L., J. Y. and Y. B. acknowledge scholarship support from UQ Graduate School.
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