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| Naji, M. |
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| Motta, Antonella |
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| Aletan, Dirar |
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| Mohamed, Tarek |
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| Ertürk, Emre |
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| Taccardi, Nicola |
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| Kononenko, Denys |
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| Petrov, R. H. | Madrid |
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| Alshaaer, Mazen | Brussels |
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| Bih, L. |
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| Casati, R. |
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| Muller, Hermance |
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| Kočí, Jan | Prague |
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| Šuljagić, Marija |
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| Kalteremidou, Kalliopi-Artemi | Brussels |
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| Azam, Siraj |
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| Ospanova, Alyiya |
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| Blanpain, Bart |
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| Ali, M. A. |
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| Popa, V. |
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| Rančić, M. |
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| Ollier, Nadège |
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| Azevedo, Nuno Monteiro |
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| Landes, Michael |
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| Rignanese, Gian-Marco |
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Spiccia, Leone
in Cooperation with on an Cooperation-Score of 37%
Topics
Publications (15/15 displayed)
- 2017Polypyridyl Iron Complex as a Hole-Transporting Material for Formamidinium Lead Bromide Perovskite Solar Cellscitations
- 2017Dipole-field-assisted charge extraction in metal-perovskite-metal back-contact solar cellscitations
- 2017Vertically Aligned Interlayer Expanded MoS2 Nanosheets on a Carbon Support for Hydrogen Evolution Electrocatalysiscitations
- 2017A facile deposition method for CuSCN: Exploring the influence of CuSCN on J-V hysteresis in planar perovskite solar cellscitations
- 2016Solar water oxidation by multicomponent TaON photoanodes functionalized with nickel oxidecitations
- 2016Enhancing the Optoelectronic Performance of Perovskite Solar Cells via a Textured CH3NH3PbI3 Morphologycitations
- 2016Parameters responsible for the degradation of CH3NH3PbI3-based solar cells on polymer substratescitations
- 2016Enhancing the optoelectronic performance of perovskite solar cells via a textured CH3NH3PbI3 morphologycitations
- 2016Highly dispersed cobalt oxide on TaON as efficient photoanodes for long-term solar water splittingcitations
- 2014Gas-assisted preparation of lead iodide perovskite films consisting of a monolayer of single crystalline grains for high efficiency planar solar cellscitations
- 2012Electrodeposited MnOx films from ionic liquid for electrocatalytic water oxidationcitations
- 2007Recognition of thymine and related nucleosides by a ZnII-cyclen complex bearing a ferrocenyl pendant
- 2007Modification of mesoporous TiO2 electrodes by surface treatment with titanium(IV), indium(III) and zirconium(IV) oxide precursors: preparation, characterization and photovoltaic performance in dye-sensitized nanocrystalline solar cells
- 2005BaTiO3-coated TiO2 working electrodes for use in dye-sensitised solar cells
- 2000Experimental and theoretical investigations of the effect of deprotonation on electronic spectra and reversible potentials of photovoltaic sensitizerscitations
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article
Experimental and theoretical investigations of the effect of deprotonation on electronic spectra and reversible potentials of photovoltaic sensitizers
Abstract
<p>Deprotonation of the photovoltaic dye sensitizers cis-(H<sub>2</sub>-dcbpy)<sub>2</sub>RuX<sub>2</sub> (L<sub>2</sub>RuX<sub>2</sub>) (X= -CN<sup>-</sup>, -NCS<sup>-</sup>; H<sub>2</sub>-dcbpy = L = 2,2'-bipyridine-4,4'- dicarboxylic acid) can be achieved in dimethylformamide by reductive electrolysis at platinum electrodes at 20 °C, which allows the thermodynamic and spectral changes associated with deprotonation to be established. The overall reaction that occurs when a potential of -2.0 V vs Fc/Fc<sup>+</sup> (Fc = ferrocene) is applied to a platinum electrode can be summarized as (H<sub>2</sub>- dcbpy)<sub>2</sub>Ru(NCS)<sub>2</sub> + xe<sup>-</sup> → [(H<sub>2-</sub>(x)/<sub>2</sub>-dcbpy(x)/<sup>2-</sup>)<sub>2</sub>Ru(NCS)<sub>2</sub>](x)<sup>-</sup> + (x)/<sub>2</sub>H<sub>2</sub>, where x is always slightly less than 4. Thus, under certain experimental conditions, [(H-dcbpy<sup>-</sup>)<sub>2</sub>RuX<sub>2</sub>]<sup>2-</sup> is believed to be the major product formed by bulk electrolysis, where H-dcbpy<sup>-</sup> is the singly deprotonated H<sub>2</sub>-dcbpy ligand. The hydrogen gas formed in this electrochemically induced deprotonation can be generated heterogeneously at the electrode surface or via homogeneous redox reactions between ligand- reduced forms of L<sub>2</sub>RuX<sub>2</sub> and protons or water. Short time domains, reduced temperatures, and glassy carbon electrodes lead to detection of transiently stable ligand-reduced forms of L<sub>2</sub>RuX<sub>2</sub>. The reversible half-wave potentials for the ligand-based reduction of electrochemically generated deprotonated L<sub>2</sub>RuX<sub>2</sub> are 0.65 V more negative than their protonated counterparts. In contrast, deprotonation leads to the metal-based oxidation process being shifted by only about 0.3 V. Interestingly, protonated and deprotonated forms of L<sub>2</sub>RuX<sub>2</sub> do not coexist in a facile acid-base equilibrium state on the voltammetric time scale. Data obtained from electrogenerated deprotonated forms of the sensitizers are compared to those found for 'salts' used in photovoltaic cells which are prepared by reaction of L<sub>2</sub>RuX<sub>2</sub> with tetrabutylammonium hydroxide. Molecular orbital calculations were employed to provide theoretical insights into the effect of deprotonation on reversible potentials and electronic spectra, and results are in good agreement with experimentally obtained data. Electronic spectra, measured in situ during the course of reduction in a spectroelectrochemical cell, reveal that all bands shift to higher energies and that the absorbance decreases as deprotonation occurs. Implications of the importance of the findings related to reduction potentials and electronic spectra to the operation of photovoltaic cells that utilize deprotonated forms of sensitizers are considered.</p>