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Interfacial charge separation and photovoltaic efficiency in Fe(ii)–carbene sensitized solar cells
- Source :
- Physical Chemistry Chemical Physics, Physical Chemistry Chemical Physics, Royal Society of Chemistry, 2016, 18 (40), pp.28069-28081. 〈10.1039/C6CP05535D〉, Physical Chemistry Chemical Physics, Royal Society of Chemistry, 2016, 18 (40), pp.28069-28081. ⟨10.1039/C6CP05535D⟩, Physical Chemistry Chemical Physics, 2016, 18 (40), pp.28069-28081. ⟨10.1039/C6CP05535D⟩, ResearcherID
- Publication Year :
- 2016
- Publisher :
- HAL CCSD, 2016.
-
Abstract
- International audience; The first combined theoretical and photovoltaic characterization of both homoleptic and heteroleptic Fe(II)–carbene sensitized photoanodes in working dye sensitized solar cells (DSSCs) has been performed. Three new heteroleptic Fe(II)–NHC dye sensitizers have been synthesized, characterized and tested. Despite an improved interfacial charge separation in comparison to the homoleptic compounds, the heteroleptic complexes did not show boosted photovoltaic performances. The ab initio quantitative analysis of the interfacial electron and hole transfers and the measured photovoltaic data clearly evidenced fast recombination reactions for heteroleptics, even associated with un unfavorable directional electron flow, and hence slower injection rates, in the case of homoleptics. Notably, quantum mechanics calculations revealed that deprotonation of the not anchored carboxylic function in the homoleptic complex can effectively accelerate the electron injection rate and completely suppress the electron recombination to the oxidized dye. This result suggests that introduction of strong electron-donating substituents on the not-anchored carbene ligand in heteroleptic complexes, in such a way of mimicking the electronic effects of the carboxylate functionality, should yield markedly improved interfacial charge generation properties. The present results, providing for the first time a detailed understanding of the interfacial electron transfers and photovoltaic characterization in Fe(II)–carbene sensitized solar cells, open the way to a rational molecular engineering of efficient iron-based dyes for photoelectrochemical applications.
- Subjects :
- Ab initio
General Physics and Astronomy
02 engineering and technology
010402 general chemistry
Photochemistry
Iron(II) complexes
01 natural sciences
7. Clean energy
DFT
Molecular engineering
chemistry.chemical_compound
Deprotonation
[ CHIM.ORGA ] Chemical Sciences/Organic chemistry
Electronic effect
[CHIM.COOR]Chemical Sciences/Coordination chemistry
Carboxylate
Physical and Theoretical Chemistry
Homoleptic
electron recombination
ComputingMilieux_MISCELLANEOUS
[CHIM.ORGA]Chemical Sciences/Organic chemistry
[ CHIM.COOR ] Chemical Sciences/Coordination chemistry
[CHIM.COOR] Chemical Sciences/Coordination chemistry
021001 nanoscience & nanotechnology
[CHIM.ORGA] Chemical Sciences/Organic chemistry
0104 chemical sciences
dye-sensitized TiO2
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry
Dye-sensitized solar cell
[CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
chemistry
[ CHIM.THEO ] Chemical Sciences/Theoretical and/or physical chemistry
electron injection
0210 nano-technology
Carbene
Subjects
Details
- Language :
- English
- ISSN :
- 14639076 and 14639084
- Database :
- OpenAIRE
- Journal :
- Physical Chemistry Chemical Physics, Physical Chemistry Chemical Physics, Royal Society of Chemistry, 2016, 18 (40), pp.28069-28081. 〈10.1039/C6CP05535D〉, Physical Chemistry Chemical Physics, Royal Society of Chemistry, 2016, 18 (40), pp.28069-28081. ⟨10.1039/C6CP05535D⟩, Physical Chemistry Chemical Physics, 2016, 18 (40), pp.28069-28081. ⟨10.1039/C6CP05535D⟩, ResearcherID
- Accession number :
- edsair.doi.dedup.....989be427498f93bd72a9bfdc35c564bb