Ferrocene compounds are promising redox shuttles for application in dye-sensitized solar cells (DSCs). Chemical modification of the cyclopentadienyl rings is easily achievable affording almost unlimited variation of the redox properties. This allows fine-tuning of the driving force for dye-regeneration and optimization of the energy conversion efficiency of DSCs. Herein, six ferrocene derivatives have been chosen for investigation which cover the large redox potential range of 0.85 V, by virtue of simple alkylation and halogenation of the cyclopentadienyl ring, and enable improved matching of the energy levels of the sensitizer and the electrolyte. Although the focus of this work was to examine the effect of the redox potential on charge transfer processes, DSCs were fabricated which achieved high energy conversion efficiencies of over 5%. Charge transfer reactions were studied to reveal the dependence of the dye regeneration rate, recombination losses and recombination pathways on the reaction driving force. An increase in redox potential led to a higher efficiency due to higher open circuit potentials until a threshold is reached. At this threshold, the driving force for dye regeneration (18 kJ mol−1, ΔE = 0.19 V) becomes too small for efficient device operation, leading to rapid recombination between the oxidized dye and electrons in the TiO2 conduction band. As a result of this work guidelines can be formulated to aid the selection of redox couples for a particular sensitizer in order to maximize the utilization of incident solar energy.

/pdf/dye-regeneration-and-charge-recombination-in-dye-sensitized-32f5fyvcqe.pdf

Dye regeneration and charge recombination in dye-sensitized solar cells with ferrocene derivatives as redox mediators

Publisher Summary The purpose of this chapter is to highlight a progress in the transition metal chemistry of some enzymes that catalyze oxidative and reductive reactions. These enzymes are referred to as oxidoreductases (1,2) and transition metals are usually found in their active sites. It is essential to understand basic principles of structural organization and mechanisms of action of the key enzymes used in amperometric biosensors. These are glucose oxidase from Aspergillus niger , horseradish peroxidase (HRP), and a group of pyrroloquinoline quinine (PQQ)-dependent enzymes such as alcohol and glucose dehydrogenases. Natural substrates of HRP are aromatic amines, phenols, indoles, sulfonates, which are usually oxidized into oligomers or polymers. Mediators as electron donors act instead of H 2 A in the peroxidase catalysis. Their role is to rapidly reduce Compounds I and II into the resting state. Glucose oxidase from A. niger and horseradish peroxidase are the enzymes that catalyze absolutely different reactions.

Transition metal chemistry of glucose oxidase, horseradish peroxidase, and related enzymes

Fabrication of bisferrocenyl derivative grafted HTPB with high iron content and its application in dopamine detection

Simple methods have been developed for the preparation of a series ofn-alkylferrocenes H(CH2)
 n
 Fc (n = 3, 5–8, or 12) based on Friedel-Crafts acylation of ferrocenes followed by reduction of the corresponding ketones with Zn amalgam. The properties of H(CH2)
 n
 Fc and the corresponding ferrocenium ions in micellar aqueous solutions and the behavior of water-soluble cations H(CH2)
 n
 Fc+ in the absence of micelles were studied by cyclic voltammetry. In all cases, the formal redox potentials of ferrocenes (E
o′) increase linearly asn increases up to 8. Whether micelles are present or not, the corresponding correlation equation has the following form:E
o′= α + βn, where β = 29 mV in all cases. The synthesis of (±)-1-ethyl-2-methylferrocene from racemic α-dimethylaminoethylferrocene is reported.

Synthesis and electrochemical properties of mono- and (±)-1,2-dialkylferrocenes and alkylferrocenium hexafluorophosphates in aqueous and micellar media

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Synthesis and electrochemical properties of mono- and (±)-1,2-dialkylferrocenes and alkylferrocenium hexafluorophosphates in aqueous and micellar media