Automated assessment of redox potentials for dyes in dye-sensitized photoelectrochemical cells

Sustainable solutions for hydrogen production, such as dye-sensitized photoelectrochemical cells (DS-PEC), rely on the fundamental properties of its components whose modularity allows for their separate investigation. In this work, we design and execute a high-throughput scheme to tune the ground st...

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Bibliographic Details
Published in:Physical chemistry chemical physics : PCCP 2021-12, Vol.24 (1), p.197-21
Main Authors: Beli, Jelena, Förster, Arno, Menzel, Jan Paul, Buda, Francesco, Visscher, Lucas
Format: Article
Language:English
Subjects:
Chemistry
Dyes
Electrode potentials
Hydrogen production
Modularity
Photoelectrochemical devices
Solvent effect
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Summary:Sustainable solutions for hydrogen production, such as dye-sensitized photoelectrochemical cells (DS-PEC), rely on the fundamental properties of its components whose modularity allows for their separate investigation. In this work, we design and execute a high-throughput scheme to tune the ground state oxidation potential (GSOP) of perylene-type dyes by functionalizing them with different ligands. This allows us to identify promising candidates which can then be used to improve the cell's efficiency. First, we investigate the accuracy of different theoretical approaches by benchmarking them against experimentally determined GSOPs. We test different methods to calculate the vertical oxidation potential, including GW with different levels of self-consistency, Kohn-Sham (KS) orbital energies and total energy differences. We find that there is little difference in the performance of these methods. However, we show that it is crucial to take into account solvent effects as well as the structural relaxation of the dye after oxidation. Other thermodynamic contributions are negligible. Based on this benchmark, we decide on an optimal strategy, balancing computational cost and accuracy, to screen more than 1000 dyes and identify promising candidates which could be used to construct more robust DS-PECs. The alignment of the GSOP, calculated with the adiabatic approach for large number of dyes, with the limitations of a hypothetical system - the CB edge of TiO 2 semiconductor and highest oxidation potential of Ru-based WOC.
ISSN:1463-9076
1463-9084
1463-9084
DOI:10.1039/d1cp04218a