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Density Functional Theory study of Cu doped {0001} and {01${{\rm{\bar{1}}}}$2} surfaces of hematite for water splitting

Published online by Cambridge University Press:  01 March 2018

Joseph Simfukwe ,
Refilwe Edwin Mapasha ,
Artur Braun  and
Mmantsae Diale
Joseph Simfukwe*
Affiliation:
Department of Physics, University of Pretoria, Pretoria0002, South Africa Department of Physics, Copperbelt University, Riverside, Kitwe10101, Zambia
Refilwe Edwin Mapasha
Affiliation:
Department of Physics, University of Pretoria, Pretoria0002, South Africa
Artur Braun
Affiliation:
Laboratory for High Performance Ceramics. Empa. Swiss Federal Laboratories for Materials Science and Technology, CH -8600 Dübendorf, Switzerland
Mmantsae Diale
Affiliation:
Department of Physics, University of Pretoria, Pretoria0002, South Africa
*
*(Email: [email protected])

Abstract

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Density Functional Theory (DFT) calculations study of Cu doped {0001} and {01-12} surfaces of hematite for enhanced water splitting have been carried out. The doping was restricted to planes in the vicinity of the surface, specifically from the top most layers to the third inner layer of Fe atoms. Thermodynamic stabilities were evaluated based on surface energies and formation energies. The evaluation of thermodynamic stabilities (negative formation energy values) shows that the systems are thermodynamically stable which suggest that they can be synthesized in the laboratory under favorable conditions. Doping on the top most layer yields the energetically most favorable structure. The calculated charge density difference plots showed the concentration of charge mainly at the top of the surface (termination region), and this charge depleted from the Cu atom to the surrounding Fe and O atoms. This phenomenon (concentration of charge at the top of the surface) is likely to reduce the distance moved by the charge carriers, decrease in charge recombination leading to facile transfer of charge to the adsorbate and, suggesting improved photoelectrochemical water oxidation activity of hematite. The analysis of electron electronic structure reveals that Cu doped surface systems does not only decrease the band gap but also leads to the correct conduction band alignment for direct water splitting without external bias voltage.

Keywords

photovoltaicCudopant
Type
Articles
Information
MRS Advances , Volume 3 , Issue 13: Broader Impact , 2018 , pp. 669 - 678
Creative Commons
Creative Common License - CCCreative Common License - BY
This is an Open Access article, distributed under the terms of the Creative Commons Attribution licence (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted re-use, distribution, and reproduction in any medium, provided the original work is properly cited.
Copyright
Copyright © Materials Research Society 2018

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