Theoretical and experimental study of charge transfer processes in photocatalysis on anatase-TiO2

• Applicants: Professor Dr. Peter Deák; Professor Dr. Michael Reichling
• Subject Area: Theoretical Chemistry: Molecules, Materials, Surfaces
• Term: from 2017 to 2022
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 320293423

• Final Report Year: 2023

Final Report Abstract

Theoretical modelling of solids and solid surfaces are mostly based on the periodic repetition of a large unit of the crystal. If charged systems have to be treated, as e.g. in photocatalysis and in the theoretical description of tunneling microscopy, or for dopants in semiconductors and nearsurface solid state qubits, a counter charge has to be introduced, in order to avoid a divergent Coulomb energy. The interaction of the repeated charges creates a spurious electrostatic potential, affecting both the total and the one-electron energies, as well as the wave function. Earlier, methods existed only for the a posteriori correction of the total energy. We have developed a general self-consistent potential correction (SCPC) method, which can be applied both in 3D- and 2D-periodic systems, and used it to investigate solid state qubits in diamond and problems of photocatalysis on TiO2. Delays in the development of SCPC, but also in building the necessary experimental equipment and conditions, have prevented the effective interaction of the theoretical and experimental part of the project. The theoretical results on photocatalytic denitrification on TiO2 have been published after the end of the project, and the ones on the true photocatalytic oxidation of CO will be submitted for publication soon.

Publications

• SLABCC: Total energy correction code for charged periodic slab models. Computer Physics Communications, 240, 101-105.
  Farzalipour, Tabriz Meisam; Aradi, Bálint; Frauenheim, Thomas & Deák, Peter
  
• Activity and Mechanism Mapping of Photocatalytic NO2 Conversion on the Anatase TiO2(101) Surface. American Geophysical Union (AGU).
  P. Guo; X. Fu; P. Deák; T. Frauenheim & J. Xiao
  
• Self-Consistent Potential Correction for Charged Periodic Systems. Physical Review Letters, 126(7).
  Chagas, da Silva Mauricio; Lorke, Michael; Aradi, Bálint; Farzalipour, Tabriz Meisam; Frauenheim, Thomas; Rubio, Angel; Rocca, Dario & Deák, Peter
  
• Fundamental Limit of Selectivity in Photocatalytic Denitrification over Titania. American Geophysical Union (AGU).
  P.Guo; P. Deák; X. Fu; T. Frauenheim & J. Xiao
  
• Predictive Theoretical Model for the Selective Electroreduction of Nitrate to Ammonia. American Geophysical Union (AGU).
  T. Mou; Y. Wang; P. Deák; H. Li; J. Long; X. Fu; B. Zhang; T. Frauenheim & J. Xiao