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Ionic Liquid Electrolytes for Photoelectrochemical Solar Cells
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Inorganic Chemistry.
2005 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

Potential electrolytes for dye-sensitized photoelectrochemical solar cells have been synthesized and their applicability has been investigated. Different experimental techniques were used in order to characterize the synthesized electrolytes, such as elemental analysis, electrospray ionisation/mass spectrometry, cyclic voltammetry, dynamic viscosity measurements, as well as impedance, Raman and NMR spectroscopy. Some crystal structures were characterized by using single crystal X-ray diffraction.

In order to verify the eligibility of the ionic compounds as electrolytes for photoelectrochemical solar cells, photocurrent density/photovoltage and incident photon-to-current conversion efficiency measurements were performed, using different kinds of light sources as solar simulators. In electron kinetic studies, the electron transport times in the solar cells were investigated by using intensitymodulated photocurrent and photovoltage spectroscopy. The accumulated charge present in the semiconductor was studied in photocurrent transient measurements.

The ionic liquids were successfully used as solar cell electrolytes, especially those originating from the diethyl and dibutyl-alkylsulphonium iodides. The highest overall conversion efficiency of almost 4 % was achieved by a dye-sensitized, nanocrystalline solar cell using (Bu2MeS)I:I2 (100:1) as electrolyte (Air Mass 1.5 spectrum at 100 W m-2), quite compatible with the standard efficiencies provided by organic solvent-containing cells. Several solar cells with iodine-doped metal-iodidebased electrolytes reached stable efficiencies over 2 %. The (Bu2MeS)I:I2-containing cells showed better long-term stabilities than the organic solvent-based cells, and provided the fastest electron transports as well as the highest charge accumulation.

Several polypyridyl-ruthenium complexes were tested as solar cell sensitizers. No general improvements could be observed according to the addition of amphiphilic co-adsorbents to the dyes or nanopartices of titanium dioxide to the electrolytes. For ionic liquid-containing solar cells, a saturation phenomena in the short-circuit current densities emerged at increased light intensities, probably due to inherent material transport limitation within the systems.

Some iodoargentates and -cuprates were structurally characterized, consisting of monomeric or polymeric entities with anionic networks or layers. A system of metal iodide crownether complexes were employed and tested as electrolytes in photoelectrochemical solar cells, though with poorer results. Also, the crystal structure of a copper-iodide-(12-crown-4) complex has been characterized

Place, publisher, year, edition, pages
Stockholm: KTH , 2005. , xii, 121 p.
Series
Trita-OOK, ISSN 0348-825X ; 1081
Keyword [en]
Ionic liquid electrolytes, Photoelectrochemical solar cells
National Category
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-426ISBN: 91-7178-122-6 (print)OAI: oai:DiVA.org:kth-426DiVA: diva2:11504
Public defence
2005-09-30, D2, KTH, Lindstedtsvägen 5, Stockholm, 13:00
Opponent
Supervisors
Note
QC 20101013Available from: 2005-09-22 Created: 2005-09-22 Last updated: 2010-10-13Bibliographically approved
List of papers
1. Molten and solid trialkylsulfonium iodides and their polyiodides as electrolytes in dye-sensitized nanocrystalline solar cells
Open this publication in new window or tab >>Molten and solid trialkylsulfonium iodides and their polyiodides as electrolytes in dye-sensitized nanocrystalline solar cells
2003 (English)In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 107, no 49, 13665-13670 p.Article in journal (Refereed) Published
Abstract [en]

Potential new electrolytes for dye-sensitized nanocrystalline solar cells (DNSCs) of Gratzel type based on trialkylsulfonium iodides have been investigated. Room temperature molten salts of (Et2MeS)I, (Bu2MeS)I, and (Bu2EtS)I, with iodine in low concentrations, revealed good conducting abilities. DNSCs using iodine-doped (Bu2MeS)l as electrolyte achieved an overall light-to-electricity conversion efficiency of 3.7% in simulated AM 1.5 solar light at a light intensity of 0.1 Sun. The effects from varying the temperature during the IN measurements were studied, as well as the effects of 4-tert-butylpyridine treatment of the electrodes.

Keyword
Electric conductivity, Electrochemical electrodes, Iodine, Solar cells, Temperature, Dye sensitized nanocrystalline solar cells, Light-to-electricity conversion efficiency, Polyiodides, Room temperature molten salts, Trialkylsulfonium iodides
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:kth:diva-6709 (URN)10.1021/jp036859v (DOI)000187009700020 ()
Note
QC 20101013Available from: 2005-09-22 Created: 2005-09-22 Last updated: 2017-12-14Bibliographically approved
2. Molten and Solid Metal-Iodide-Doped Trialkylsulphonium Iodides and Polyiodides as Electrolytes in Dye-Sensitized Nanocrystalline Solar Cells
Open this publication in new window or tab >>Molten and Solid Metal-Iodide-Doped Trialkylsulphonium Iodides and Polyiodides as Electrolytes in Dye-Sensitized Nanocrystalline Solar Cells
Show others...
2004 (English)In: Solar Energy Materials and Solar Cells, ISSN 0927-0248, E-ISSN 1879-3398, Vol. 82, no 3, 345-360 p.Article in journal (Refereed) Published
Abstract [en]

The conductivity and solar cell performance of metal-iodide-doped trialkylsulphonium iodides and polyiodides have been investigated as electrolytes in dye-sensitized nanocrystalline solar cells (DNSCs). Nine different metal-iodide-containing (R2R′S)I with additional iodine provided overall solar-to-electric energy conversion efficiencies of over 2%, while used as electrolytes in DNSCs in simulated AM 1.5 solar light at the light intensity of 100Wm-2. The highest overall conversion efficiency, 3.1%, was achieved by using the electrolyte (Bu2MeS)I: AgI:I2 in the proportions (1:0.03:0.05). The effects from 4-tert-butylpyridine treatment of the electrodes were studied. The effects of metal-iodide doping were also investigated with respect to speciation in the electrolytes and potential influence on electrochemical conductivity.

Keyword
Dye-sensitized nanocrystalline solar cell, Electrolyte, Metal iodide, Room-temperature molten salt, Trialkylsulphonium iodide
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-6710 (URN)10.1016/j.solmat.2003.12.005 (DOI)000221289200002 ()2-s2.0-2142642337 (Scopus ID)
Note
QC 20100923Available from: 2005-09-22 Created: 2005-09-22 Last updated: 2017-12-14Bibliographically approved
3. Iodoargentates and Cuprates Stabilized by Sulphonium Cations with Long Alkyl Chains
Open this publication in new window or tab >>Iodoargentates and Cuprates Stabilized by Sulphonium Cations with Long Alkyl Chains
2003 (English)In: European Journal of Inorganic Chemistry, ISSN 1434-1948, E-ISSN 1099-1948, no 12, 2352-2355 p.Article in journal (Refereed) Published
Abstract [en]

[DodMe2S]22AgI3 and [DodMe2S] Ag2I3 were obtained from mixtures of dodecyldimethylsulfonium iodide and silver iodide in acetonitrile solution. [DodMe2S]2AgI3 crystallizes in the orthorhombic crystal system, space group Pbca and contains trigonal planar anions AgI32-, while [DodMe2S] Ag2I3 crystallizes in the triclinic crystal system, space group P1, and consists of polymeric anions 1(Ag2I3)-. In both structures, the sulfonium cations form a layer of parallel and interpenetrating dodecyl chains with the sulfoniumdimethyl groups on both sides of the layer. [DodMe2S]2CuI3 was obtained from dodecyldimethylsulfonium iodide and copper iodide mixtures and is isostructural with the corresponding silver compound.

Keyword
Cations, Copper, Crystal structure, Iodide, Silver
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:kth:diva-6711 (URN)10.1002/ejic.200200667 (DOI)000184022400019 ()
Note
QC 20100920Available from: 2005-09-22 Created: 2005-09-22 Last updated: 2017-12-14Bibliographically approved
4. Novel Layered Structures Formed by Iodocuprate Clusters Stabilized by Dialkylsulphide Ligands
Open this publication in new window or tab >>Novel Layered Structures Formed by Iodocuprate Clusters Stabilized by Dialkylsulphide Ligands
2004 (English)In: Zeitschrift für Anorganische und Allgemeines Chemie, ISSN 0044-2313, E-ISSN 1521-3749, Vol. 630, no 3, 413-416 p.Article in journal (Refereed) Published
Abstract [en]

From solutions of copper iodide and dodecyldimethyl-sulphonium iodide in acetonitrile, single crystals of [Cu4I4-(DodecylMeS) 4] (1) and [Cu3I4(DodecylMeS) 3](DodecylMe2S) (2) could be obtained. Both compounds crystallize in the triclinic crystal system, space group P1 (1: a = 957.23(1), b = 967.25(2), c = 3818.38(6) pm, α = 90.3837(6)°, β = 86.4687(7)°, γ = 75.0996(7)°; 2: a = 874.23(1), b = 979.29(1), c = 4388.75(4) pm, α = 90.4472(3)°, β = 94.7088(3)°, γ = 116.1162(3)°). 1 consists of tetrahedral Cu4 clusters, which are capped by four iodide ions over the tetrahedral faces. 2 contains trigonal Cu3 clusters, which are coordinated by four iodide ions, one centered over the plane, three bridging over the edges of the Cu3 triangle. In both compounds, the S atoms of (DodecylMeS) ligands coordinate to the Cu atoms. In 2, a (DodecylMe2S) cation is also present.

Keyword
copper, iodide, cluster, crystal structure
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:kth:diva-6712 (URN)10.1002/zaac.200300379 (DOI)000220405300015 ()2-s2.0-4644265939 (Scopus ID)
Note
QC 20100924Available from: 2005-09-22 Created: 2005-09-22 Last updated: 2017-12-14Bibliographically approved
5. Bis[bis(12-crown-4)potassium] hexaiodotetracuprate(I)
Open this publication in new window or tab >>Bis[bis(12-crown-4)potassium] hexaiodotetracuprate(I)
2004 (English)In: Acta Crystallographica Section E: Structure Reports Online, ISSN 1600-5368, E-ISSN 1600-5368, Vol. 60, no 5, M548-M550 p.Article in journal (Refereed) Published
Abstract [en]

From 12-crown-4, KI, and CuI in an acetone solution, the title compound, [K(C16H32O8)(2)](2)[Cu4I6], was obtained. It consists of sandwich-type [(12-crown-4)(2)K](+) complex cations and polymeric [Cu4I6](2-) anions. The latter consist of CuI4 tetrahedra, which share edges and faces to form infinite chains.

Keyword
Acetone, Complexation, Crystal structure, Crystallization, Hydrogen bonds, Ions, Iridium compounds, Single crystals, Bond angles, Bond distances, Coordination geometry, Probability displacement ellipsoids
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:kth:diva-6713 (URN)10.1107/S1600536804007780 (DOI)000221174800016 ()2-s2.0-18444411664 (Scopus ID)
Note
QC 20101013Available from: 2005-09-22 Created: 2005-09-22 Last updated: 2017-12-14Bibliographically approved
6. Long-Term Stability Studies under Indoor Light Conditions of Dye-Sensitized Nanocrystalline Solar Cells Containing Room-Temperature Ionic Liquid Electrolytes
Open this publication in new window or tab >>Long-Term Stability Studies under Indoor Light Conditions of Dye-Sensitized Nanocrystalline Solar Cells Containing Room-Temperature Ionic Liquid Electrolytes
2005 (English)Article in journal (Other academic) Submitted
Keyword
Long-term stability, Dye-sensitized solar cell, Electrolyte, Ionic liquid, Sulphonium iodide
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:kth:diva-6714 (URN)
Note
QS 2010 QS 20120319Available from: 2005-09-22 Created: 2005-09-22 Last updated: 2012-03-19Bibliographically approved
7. Electron transport and recombination in dye-sensitized solar cells with ionic liquid electrolytes
Open this publication in new window or tab >>Electron transport and recombination in dye-sensitized solar cells with ionic liquid electrolytes
2006 (English)In: Journal of Electroanalytical Chemistry, ISSN 0022-0728, E-ISSN 1873-2569, Vol. 586, no 1, 56-61 p.Article in journal (Refereed) Published
Abstract [en]

The electron transport and recombination in dye-sensitized TiO2 solar cells with different electrolytes have been investigated. The electrolytes were based on iodine-doped ionic liquids (diethylmethylsulphonium, dibutylmethylsulphonium or 3-hexyl-1-methylimidazolium iodide) or an organic solvent (3-methoxypropionitrile with LiI, I-2 and 1-methylbenzimidazole). The most viscous electrolytes showed a clear limitation in photocurrent, which can be attributed to a low diffusion coefficient for the triiodide that transports positive charge to the counter electrode. No essential difference was found in the electron transport properties of the solar cells, which appear to be dominated by the properties of the nanostructured TiO2 film. The intensity-modulated photocurrent response was strongly affected by current saturation. This is proposed being caused by recombination processes. The electron lifetime is depending on the type of cation used in the ionic liquid, where bulky, less absorptive cations seem to give longer lifetimes.

Keyword
dye sensitization, solar cell, TiO2, electrolyte, ionic liquid, electron transport, nanoporous tio2, efficiency, diffusion, molten, salts
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:kth:diva-15346 (URN)10.1016/j.jelechem.2005.09.011 (DOI)000233521000008 ()2-s2.0-27744482655 (Scopus ID)
Note
QC 20100525Available from: 2010-08-05 Created: 2010-08-05 Last updated: 2017-12-12Bibliographically approved
8. Photoelectrochemical Studies of Nanocrystalline Solar Cells Sensitized with Polypyridyl-Ruthenium Complexes and Containing Room-Temperature Ionic Liquids or an Organic Liquid-Based Electrolyte
Open this publication in new window or tab >>Photoelectrochemical Studies of Nanocrystalline Solar Cells Sensitized with Polypyridyl-Ruthenium Complexes and Containing Room-Temperature Ionic Liquids or an Organic Liquid-Based Electrolyte
2005 (English)Article in journal (Other academic) Submitted
Keyword
Dye-sensitized, Nanocrystalline solar cell, Electrolyte, Ionic liquid, Sulphonium iodide
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:kth:diva-6716 (URN)
Note
QS 2010 QS 20120319Available from: 2005-09-22 Created: 2005-09-22 Last updated: 2012-03-19Bibliographically approved

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