Inhibiting Charge Recombination in -Ru(NCS) Diimine Sensitizers with Aromatic Substituents.

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ID: 67430
2019
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Abstract
A series of -[Ru(LL)(dcbH)(NCS)] compounds, where dcbH = 2,2'-bipyridine-4,4'-dicarboxylic acid and LL = 1,10-phenanthroline (Ru(phen)), 4,7-dipyrrole-1,10-phenanthroline (Ru(pyr)), 4,7-diindole-1,10-phenanthroline (Ru(ind)), or 4,7-dicarbazole-1,10-phenanthroline (Ru(cbz)), was investigated for application as sensitizers in mesoporous TiO dye-sensitized solar cells (DSSCs). A systematic increase in the number of rings of the aromatic substituents at the 4,7-positions of the 1,10-phenanthroline allowed tuning of the molecular size of the sensitizers and the energy stored in the excited state while maintaining the same ground-state Ru reduction potentials. These small structural changes had a significant influence on the rates and/or efficiencies of electron injection, back-electron transfer, recombination to oxidized mediators, lateral self-exchange electron transfer, and regeneration through iodide oxidation that were reflected in distinct photoelectrochemical performance of full operating DSSCs. The global efficiencies, open-circuit voltages, and short-circuit current densities of the DSSCs consistently followed the trend Ru(pyr) < Ru(ind) < Ru(phen) < Ru(cbz), and the most optimal performance of Ru(cbz) was ascribed to dramatically slower recombination to the oxidized redox mediators. Transient photovoltage and transient absorption experiments both revealed significantly slower recombination as the size of the aromatic substituents increased with Ru(cbz) providing the most promising behavior for application in dye sensitization.
Reference Key
muller2019inhibitingacs Use this key to autocite in the manuscript while using SciMatic Manuscript Manager or Thesis Manager
Authors Müller, Andressa V;de Oliveira, Kleber T;Meyer, Gerald J;Polo, André S;
Journal ACS applied materials & interfaces
Year 2019
DOI
10.1021/acsami.9b15448
URL
Keywords
electron transfer regeneration recombination dssc hole-hopping steric effects

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