Solar energy conversion using dye-sensitised liquid|liquid interfaces

Fermı́n, David J.; Duong, H. Dung; Ding, Zhifeng; Brevet, Pierre F.; Girault, Hubert H.

doi:10.1016/s1388-2481(98)00009-5

Cited by 34 publications

(31 citation statements)

References 9 publications

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“…Understanding electron transfer (ET) at the interface between two immiscible electrolyte solutions (IES) is of fundamental importance in electrochemistry, [1][2][3][4][5][6][7] solar energy conversion and "artificial photosynthesis," [8][9] and phase transfer catalysis, [10][11][12] and may also be relevant to understanding biological processes at membrane interfaces and in DNA environments. 13 The experimental study of ET at IES has a long history, 2 but up until recently, measurements of electron transfer rates have mainly utilized conventional electrochemical methods, where the interface was under potentiostatic control.…”

Section: Introductionmentioning

confidence: 99%

Photoinduced Excited State Electron Transfer at Liquid/Liquid Interfaces

Cooper

Benjamin

2014

J. Phys. Chem. B

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Abstract:Several aspects of the photoinduced electron transfer (ET) reaction between coumarin 314 (C314) and N,N-dimethylaniline (DMA) at the water/DMA interface are investigated by molecular dynamics simulations. New DMA and water/DMA potential energy surfaces are developed and used to characterize the neat water/DMA interface.The adsorption free energy, the rotational dynamics and the solvation dynamics of C314 at the liquid/liquid interface are investigated and are generally in reasonable agreement with available experimental data. The solvent free energy curves for the ET reaction between excited C314 and DMA molecules are calculated and compared with those calculated for a simple point charge model of the solute. It is found that the reorganization free energy is very small when the full molecular description of the solute is taken into account. An estimate of the ET rate constant is in reasonable agreement with experiment. Our calculations suggest that the polarity of the surface "reported" by the solute, as reflected by solvation dynamics and the reorganization free energy, is strongly solute-dependent.

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Section: Introductionmentioning

confidence: 99%

Photoinduced Excited State Electron Transfer at Liquid/Liquid Interfaces

Cooper

Benjamin

2014

J. Phys. Chem. B

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“…At this molecular junction, photocurrent responses originating from the heterogeneous quenching of photoexcited water-soluble dyes by hydrophobic redox species have been studied in detail [4][5][6][7][8][9][10][11]. It has been observed that the Galvani potential difference across the liquid|liquid interface can affect the surface coverage of the photoactive species as well as the dynamics of photoinduced electron transfer and back electron transfer.…”

Section: Introductionmentioning

confidence: 99%

Adsorption and photoreactivity of CdSe nanoparticles at liquid|liquid interfaces

Fermı́n

Abid

et al. 2005

Journal of Electroanalytical Chemistry

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The voltage induced assembly and photoreactivity of cadmium selenide (CdSe) nanoparticles protected by mercaptosuccinic acid are studied at the polarisable interface between water and 1,2-dichloroethane electrolyte solutions. Cyclic voltammograms and admittance measurements show an increase of the interface excess charge associated with the adsorption of CdSe nanoparticles as the Galvani potential difference is tuned to negative values with respect to the potential in the organic phase. Within the potential range where the nanoparticles are adsorbed, band-gap illumination leads to heterogeneous electron transfer from CdSe nanoparticles to electron acceptors located in the organic phase. The interfacial Galvani potential difference plays an important role in these phenomena, as it affects the interfacial density of the nanoparticles, as well as the driving force for the electron transfer. The photocurrent efficiency also strongly depends on the formal redox potential of the electron acceptor, indicating that the heterogeneous photoreaction is kinetically controlled. The interfacial electron transfer occurs via depopulation of the deep trap states in the band gap. Analysis of the photocurrent transient responses reveals that the magnitude of the instantaneous photocurrent upon illumination is determined by the kinetics of heterogeneous electron transfer, while photogenerated holes are swiftly captured by species present in the aqueous phase. The photocurrent decay upon constant illumination is associated with the diffusion of the acceptor to the interfacial region. From the phenomenological point of view, the photoelectrochemical behaviour of CdSe nanoparticles can be compared to a self-assembled ultrathin p-type semiconductor photoelectrode.

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“…During the last five years, efforts have been devoted to the exploration of fundamental aspects concerning the organisation and reactivity of photoactive species at the interface between two immiscible electrolyte solutions [15,19,20]. In these systems, the photoexcitation of dyes or semiconducting nanoparticles leads to heterogeneous charge transfer processes in the presence of redox couples located in the adjacent liquid phase [9,[12][13][14]18,[21][22][23][24][25][26][27]. These projects are relevant not only to theoretical aspects on electron transfer at molecular interfaces, but also to the development of new photoactive systems [9,22,28,29].…”

Section: Introductionmentioning

confidence: 99%

“…Recently, a series of papers based on photocurrent responses involving water soluble porphyrin species has addressed various aspects involved in the kinetics of photoinduced electron transfer across polarisable liquid| liquid junctions [12][13][14]18,[21][22][23][24][25][26][27]32]. A general description of the heterogeneous photoreaction is shown in Fig.…”

Section: Introductionmentioning

confidence: 99%

A generalised model for dynamic photocurrent responses at dye-sensitised liquid|liquid interfaces

Samec

Eugster

Fermı́n

2005

Journal of Electroanalytical Chemistry

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The heterogeneous photoinduced electron transfer involving dyes adsorbed at the interface between two immiscible electrolyte solutions and redox molecules located in the adjacent phase manifests itself as photocurrent responses under potentiostatic conditions. Photocurrent transients as functions of the light intensity and bias potential allow the extraction of insightful information on the kinetics of the various processes associated with the photoinduced reaction. Previous analyses of this type of responses were based on phenomenological models that did not consider mass transport. In the present paper, we develop a generalised model for photocurrent transients taking into account the diffusion of reacting species to the interface. Comparison with the experimental data confirms that the responses can be described adequately by applying stationary conditions to the surface concentration of the photoactive species. Mechanistic aspects associated with the nature of the photocurrent relaxation on the microsecond time scale are examined. In particular, the dependence of the transient response on the light intensity indicates that charge recombination proceeds mainly as a first order reaction from an interfacial geminate ion pair. Coupled ion transfer reactions involving the photoproducts can also contribute to the photocurrent, depending on the formal ion transfer potential of the corresponding species.

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Solar energy conversion using dye-sensitised liquid|liquid interfaces

Cited by 34 publications

References 9 publications

Photoinduced Excited State Electron Transfer at Liquid/Liquid Interfaces

Photoinduced Excited State Electron Transfer at Liquid/Liquid Interfaces

Adsorption and photoreactivity of CdSe nanoparticles at liquid|liquid interfaces

A generalised model for dynamic photocurrent responses at dye-sensitised liquid|liquid interfaces

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