CN1320663C - Solar cell based on polymer doped quasi-solid state electrolyte material and its prepn. method - Google Patents
Solar cell based on polymer doped quasi-solid state electrolyte material and its prepn. method Download PDFInfo
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- CN1320663C CN1320663C CNB2004100178301A CN200410017830A CN1320663C CN 1320663 C CN1320663 C CN 1320663C CN B2004100178301 A CNB2004100178301 A CN B2004100178301A CN 200410017830 A CN200410017830 A CN 200410017830A CN 1320663 C CN1320663 C CN 1320663C
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Abstract
The present invention relates to a dye sensitization nanometer crystal solar battery using a polymer doping quasi solid electrolyte and a preparing method thereof, which belong to the technical field of a dye sensitization nanometer crystal solar battery. In the dye sensitization nanometer crystal solar battery, the polymer doping quasi solid electrolyte assembled on the surface of a wide-gap semiconductor nanometer crystal film of an absorbing photosensitizer is used for replacing a liquid electrolyte, and thus, the leakage problem of an electrolyte is efficiently solved. In the condition that the photoelectric conversion efficiency of the dye sensitization nanometer crystal solar battery is obscurely reduced, the service life of the dye sensitization nanometer crystal solar battery can be greatly extended.
Description
Technical field
This invention belongs to solar cell electrolyte material field, is specifically related to a kind of dye sensitized nano crystal salar battery that adopts polymer-doped quasi-solid electrolyte material and preparation method thereof.Compare with the solar cell that adopts traditional liquid electrolyte, this quasi-solid electrolyte has solved the leakage problem of solvent effectively, and under the prerequisite of the electricity conversion of not obvious reduction battery, can prolong the useful life of dye sensitized nano crystal salar battery significantly.
Background technology
Along with development of human society, demand to the energy is increasing, also more and more higher to environment requirement, and be that the conventional energy resource resource is exhausted day by day with the fossil fuel, the environmental pollution that causes is also serious day by day, therefore develops the strategic decision that solar energy has become countries in the world government sustainable development new and renewable sources of energy.At present, although account for the solar cell of main flow is monocrystalline silicon and non-crystal silicon solar cell, but owing to expensive price limits its extensive use, this makes people begin to explore cheap novel solar battery, under such environment, the dye sensitized nano crystal salar battery that works out by Michael Gr professor tzel of Lausanne, SUI university just arise at the historic moment (referring to international patent application book WO91/16719).
It is work electrode that the dye sensitized nano crystal semiconductor solar cell adopts the nanometer crystal film of the wide bandgap semiconductor of surface adsorption sensitising agent, because nanometer crystal film has very large specific area, a large amount of sensitising agents can be adsorbed, thereby sunlight can be absorbed effectively.At present, the electrolyte of dye sensitized nano crystal salar battery mainly adopts and contains I
3 -/ I
2Organic solvents such as the acetonitrile of oxidation-reduction pair, but liquid electrolyte exists the problem of solvent evaporates and leakage.All solid state electrolyte mainly is P-type inorganic semiconductor, organic hole transferring material at present, but the electronics of all solid state electrolyte and ionic conductivity sharply descend, and therefore adopt the photoelectricity changing effect of all solid state dye sensitized nano crystal salar battery unsatisfactory.
And contain I
3 -/ I
2The quasi-solid electrolyte of oxidation-reduction pair is between liquid electrolyte and solid electrolyte, have the advantage of liquid electrolyte and solid electrolyte concurrently, both overcome the problem of the solvent leakage of liquid electrolyte, the high ionic conductivity that liquid electrolyte is arranged again becomes the important development direction of dye sensitized nano crystal salar battery.
Quasi-solid electrolyte normally adds some additives by liquid electrolyte makes its gelation.The additive of having reported has micromolecule gel rubber material, high-molecular gel material and some nano particles.The polymeric additive of having reported at present has fluorine-containing copolymer (polysiloxanes of P (VDF-HFP), polyacrylonitrile (PAN), polyethylene glycol oxide grafting, glycan etc.
Summary of the invention
Summary of the invention
The object of the present invention is to provide a kind of dye sensitized nano crystal salar battery based on polymer-doped quasi-solid electrolyte material and preparation method thereof, to solve the leakage problem of solvent, under the prerequisite of not obvious reduction solar cell photoelectric conversion efficiency, increase substantially the useful life of solar cell.
The dye sensitized nano crystal salar battery that the present invention proposes, on the surface of the wide bandgap semiconductor nanometer crystal film that has adsorbed photosensitizer, assemble polymer-doped quasi-solid electrolyte material, its two sides is the electro-conductive glass that is coated with platinum layer, forms sandwich shape, and its structure as shown in Figure 1.Wherein, the dye sensitized nano crystal film is a work electrode, and the electro-conductive glass of platinum plating layer is to electrode, and carries out simplified package with paraffin.
Wide bandgap semiconductor nanometer crystal film of the present invention adopts the titanium dioxide nanocrystalline film, photosensitizer adopts cis-two thiocyanate radical-two (4,4 '-dicarboxylic acids-2,2 ' bipyridine) closes ruthenium cis-dithiocyanato bis (4,4 '-dicarboxy-2,2 '-bipyridine) ruthenium (being called for short the N3 dyestuff) and cis-two thiocyanate radical-4,4 '-dicarboxylic acids-2,2 ' bipyridine-4,4 '-dihexyl-2,2 ' bipyridine closes ruthenium cis-dithiocyanato 4,4 '-dicarboxy-2,2 '-bipyridine-4,4 '-dinonyl-2,2 '-bipyridineruthenium (being called for short the Z907 dyestuff)
Said polymer of the present invention is the macromolecule of polyethers, as the copolymer (as P123 etc.) of polyethylene glycol oxide (PEO), PPOX (PPO), ethylene oxide and propylene oxide.
The preparation method of dye sensitized nano crystal salar battery of the present invention is as follows, the quasi-solid electrolyte that the macromolecule of assembling polyethers mixes on the surface of the wide bandgap semiconductor nanometer crystal film that passes through dye sensitization, electro-conductive glass with platinum plating is placed on the semiconductor nano epitaxial of dye sensitization then, promptly constitute the sandwich type dye sensitized nano crystal salar battery, and encapsulate with paraffin, its structure is as shown in Figure 1.
In the said method, the wide bandgap semiconductor nanometer crystal film is a nano titanium dioxide film.
In the said method, the preparation process of semiconductor nano epitaxial is as follows: with granularity is that the colloidal tio 2 of 1-50 nanometer is coated on and forms broad stopband nano titanium oxide epitaxial on the transparent conductive substrate, 200-600 ℃ of following roasting 15 minutes to 12 hours, cooling back repetitive operation was until the broad stopband nano titanium oxide epitaxial that obtains the 1-50 micron.Wherein transparent conductive substrate is a tin ash electro-conductive glass of mixing fluorine.
In the said method, the step of dye sensitization is as follows: the nano titanium oxide epitaxial is put into baking oven heated 10-120 minute down in 100-250 ℃, being immersed in concentration when being cooled to 25-100 ℃ is 10
-5-10
-3Sensitization in 2-48 hour in the N3 of mol or the Z907 dyestuff.After sensitization is finished, take out sensitization film and wash with corresponding solvent, remove the dyestuff of not absorption and dry up.
In the said method, the step of assembling polyethers macromolecule dopant material is as follows: polymer dissolution is being contained 0.1-0.5 mol I
2, 0.1-0.5 mol I
-0.5-1.0 mol 4-tert .-butylpyridine, 0.5-1.0 in the solution of mol 1-methyl-acetonitrile, propene carbonate, methoxyacetonitrile or the acetonitrile of 3-propyl imidazole salt and the mixture of propene carbonate, make it gelation, thereby the formation quasi-solid electrolyte, wherein the mass content of polyethers macromolecule in solution is 1-10%.
In the said method, described polyethers macromolecular compound can be polyethylene glycol oxide (PEO), PPOX (PPO), ethylene oxide and propylene oxide (P
123Deng) copolymer.
The Optical Electro-Chemistry of dye sensitized nano crystal salar battery of the present invention is measured according to two traditional electrode systems and is measured, radiation source be 1000W solar simulator (1.5AM) (Oriel, USA).Photoelectric current and photovoltage output are measured by Keithley2400 digital source table (U.S. Keithley company).
Polymer-doped dye sensitized nano crystal salar battery quasi-solid electrolyte of the present invention makes it gelation at the polymer of the certain content of dissolving of traditional liquid electrolyte and forms.The advantage of polymer-doped dye sensitized nano crystal salar battery quasi-solid electrolyte is: the formation of polymer gel network configuration, effectively solved the leakage problem of liquid electrolyte, both can not obvious reduction cell photoelectric transformation efficiency, can prolong the useful life of dye sensitized nano crystal salar battery again significantly.For example, after 140 hours, the photoelectric conversion efficiency of the dye sensitized nano crystal salar battery of liquid electrolyte has reduced by 50%, and based on polymer-doped quasi-solid electrolyte the photoelectric conversion efficiency of dye sensitized nano crystal salar battery only be reduced to 5% from 5.3%.
Description of drawings
Fig. 1 adopts solar battery apparatus figure of the present invention.
Fig. 2 is based on photoelectric current (I)-photovoltage (V) curve of the DSSC of liquid electrolyte.
Fig. 3 is based on photoelectric current (I)-photovoltage (V) curve of the DSSC of the quasi-solid electrolyte of 8.6% doping polyoxyethylene (PEO) doping.
Fig. 4 is based on photoelectric current (I)-photovoltage (V) curve of the DSSC of the quasi-solid electrolyte of 8.6% polyoxypropylene (PPO) doping.
Fig. 5 is based on 8.6% poly-(oxygen ethene-oxypropylene-oxygen ethene) (P
123) photoelectric current (I)-photovoltage (V) curve of DSSC of the quasi-solid electrolyte that mixes.
The normalized stability of Fig. 6 based on the liquid electrolyte DSSC.
The stability of the DSSC of the normalized quasi-solid electrolyte based on 8.6% doping polyoxyethylene (PEO) of Fig. 7.
The stability of the DSSC of the normalized quasi-solid electrolyte based on 8.6% polyoxyethylene (PPO) of Fig. 8.
Fig. 9 is normalized based on 8.6% poly-(oxygen ethene-oxypropylene-oxygen ethene) (P
123) the stability of DSSC of quasi-solid electrolyte.
Number in the figure: 1 is electro-conductive glass, and 2 is nano crystal semiconductor, and 3 is N3 or Z907 dyestuff, and 4 is polymer-doped quasi-solid electrolyte, and 5 is platinized platinum, and 6 is electro-conductive glass.
Embodiment
Embodiment 1: with a titanium dioxide nanocrystalline membrane electrode 5 * 10
-4Soak sensitization in 24 hours in the ethanolic solution of mol N3 dyestuff.Drip the 0.1ml quasi-solid electrolyte again and (consist of 0.1 mol I
20.1 mol LiI, 0.5 mol 4-tert .-butylpyridine, 0.6 mol 1-methyl-3-propyl imidazole salt, acetonitrile/propene carbonate of the PEO of 8.6% (mass fraction) (volume ratio=1: 1) solution), then the ito glass of a slice platinum plating is placed on dye sensitization the nano titanium oxide epitaxial on, assemble out DSSC and measure.At 100mW/cm
2White light under record battery the open circuit photovoltage be that 628mV, short-circuit photocurrent are 11.2mA/cm
2, fill factor, curve factor is 0.67, energy conversion efficiency is 4.7%, place 400h after, the energy conversion efficiency of this solar cell reduces by 75%.
Embodiment 2: with a titanium dioxide nanocrystalline membrane electrode 5 * 10
-4Soak sensitization in 24 hours in the ethanolic solution of mol N3 dyestuff.Drip the 0.1ml quasi-solid electrolyte again and (consist of 0.1 mol I
20.1 mol LiI, 0.5 mol 4-tert .-butylpyridine, 0.6 mol 1-methyl-3-propyl imidazole salt, acetonitrile/propene carbonate of the PEO of 8.6% (mass fraction) (volume ratio=1: 1) solution), then the ito glass of a slice platinum plating is placed on dye sensitization the nano titanium oxide epitaxial on, assemble out DSSC and measure.At 100mW/cm
2White light under record battery the open circuit photovoltage be that 673mV, short-circuit photocurrent are 10.1mA/cm
2, fill factor, curve factor is 0.72, energy conversion efficiency is 4.9%, place 400h after, the energy conversion efficiency of this solar cell reduces by 30%.
Embodiment 3: with a titanium dioxide nanocrystalline membrane electrode 5 * 10
-4Soak sensitization in 24 hours in the ethanolic solution of mol N3 dyestuff.Drip the 0.1ml quasi-solid electrolyte again and (consist of 0.1 mol I
20.1 mol LiI, 0.5 mol 4-tert .-butylpyridine, 0.6 mol 1-methyl-3-propyl imidazole salt, acetonitrile/propene carbonate of the PPO of 8.6% (mass fraction) (volume ratio=1: 1) solution), then the ito glass of a slice platinum plating is placed on dye sensitization the nano titanium oxide epitaxial on, assemble out DSSC and measure.At 100mW/cm
2White light under record battery the open circuit photovoltage be that 629mV, short-circuit photocurrent are 12.2mA/cm
2, fill factor, curve factor is 0.65, energy conversion efficiency is 5.0%, place 400h after, this solar energy conversion efficiency reduces by 25%.
Embodiment 4: with a titanium dioxide nanocrystalline membrane electrode 5 * 10
-4Soak sensitization in 24 hours in the ethanolic solution of mol N3 dyestuff.Drip the 0.1ml quasi-solid electrolyte again and (consist of 0.1 mol I
2, 0.1 mol LiI, 0.5 mol 4-tert .-butylpyridine, 0.6 mol 1-methyl-3-propyl imidazole salt, the P of 8.6% (mass fraction)
123Acetonitrile/propene carbonate (volume ratio=1: 1) solution), then the ito glass of a slice platinum plating is placed on dye sensitization the nano titanium oxide epitaxial on, assemble out DSSC and measure.At 100mW/cm
2White light under record battery the open circuit photovoltage be that 694mV, short-circuit photocurrent are 11.2mA/cm
2, fill factor, curve factor is 0.68, energy conversion efficiency 5.3%, place 400h after, the energy conversion efficiency of this solar cell reduces by 18%.
Embodiment 5: with a titanium dioxide nanocrystalline membrane electrode 5 * 10
-5Soak sensitization in 48 hours in the ethanolic solution of mol Z907 dyestuff.Drip 0.05 milliliter and contain 0.5 mol I
20.5 mol LiI, 1.0 mol 4-tert .-butylpyridine, 1.0 mol 1-methyl-3-propyl imidazole salt, the carbonic allyl ester solution of the PEO of 3% (mass fraction), then the ito glass of a slice platinum plating is placed on dye sensitization the nano titanium oxide epitaxial on, measure with clamp.At 100mW/cm
2White light under record battery the open circuit photovoltage be that 650mV, short-circuit photocurrent are 12.3mA/cm
2, fill factor, curve factor is 0.68, energy conversion efficiency 5.4%.After placing 400h, the energy conversion efficiency of this solar cell reduces by 15%.
Embodiment 6: with a titanium dioxide nanocrystalline membrane electrode 1 * 10
-3Soak sensitization in 2 hours in the ethanolic solution of mol Z907 dyestuff.Drip 0.05 milliliter and contain 0.1 mol I
20.1 mol LiI, 0.5 mol 4-tert .-butylpyridine, 0.8 mol 1-methyl-3-propyl imidazole salt, the methoxyacetonitrile solution of the PPO of 10% (mass fraction), then the ito glass of a slice platinum plating is placed on dye sensitization the nano titanium oxide epitaxial on, measure with clamp.At 100mW/cm
2White light under record battery the open circuit photovoltage be that 633mV, short-circuit photocurrent are 11.2mA/cm
2, fill factor, curve factor is 0.64, energy conversion efficiency 4.5%, place 400h after, the energy conversion efficiency of this solar cell reduces by 15%.
Embodiment 7: with a titanium dioxide nanocrystalline membrane electrode 1 * 10
-4Soak sensitization in 12 hours in the ethanolic solution of mol Z907 dyestuff.Drip 0.05 milliliter and contain 0.05 mol I
2, 0.05 mol LiI, 0.1 mol 4-tert .-butylpyridine, 0.1 mol 1-methyl-3-propyl imidazole salt, the P of 5% (mass fraction)
123Acetonitrile solution, then the ito glass of a slice platinum plating is placed on dye sensitization the nano titanium oxide epitaxial on, measure with clamp.At 100mW/cm
2White light under record battery the open circuit photovoltage be that 625mV, short-circuit photocurrent are 15.8mA/cm
2, fill factor, curve factor is 0.65, energy conversion efficiency 6.4%.The energy conversion efficiency of this solar cell reduces by 30%.
Claims (8)
1, a kind of dye sensitized nano crystal salar battery, it is characterized in that on the surface of the wide bandgap semiconductor nanometer crystal film that has adsorbed photosensitizer, assembling the quasi-solid electrolyte material that the polyethers macromolecule mixes, its two sides is the electro-conductive glass that is coated with platinum layer, form sandwich shape, wherein the dye sensitized nano crystal film is a work electrode, and the electro-conductive glass of platinum plating layer is to electrode; The polyethers macromolecule is the copolymer of polyethylene glycol oxide, PPOX, ethylene oxide and propylene oxide.
2, dye sensitized nano crystal salar battery according to claim 1 is characterized in that the wide bandgap semiconductor nanometer crystal film is the titanium dioxide nanocrystalline film.
3, dye sensitized nano crystal salar battery according to claim 1 is characterized in that said photosensitizer is N3 or Z907 dyestuff.
4, a kind of preparation method as one of claim 1-3 described dye sensitized nano crystal salar battery, the macromolecule doping quasi-solid electrolyte that it is characterized in that assembling polyethers on the surface of the wide bandgap semiconductor nanometer crystal film that passes through dye sensitization, electro-conductive glass with platinum plating is placed on the semiconductor nano epitaxial of dye sensitization then, use clamp, promptly constitute the sandwich type dye sensitized nano crystal salar battery, and encapsulate with paraffin.
5, the preparation method of dye sensitized nano crystal salar battery according to claim 4, the macromolecule that it is characterized in that the assembling polyethers high molecular step of mixing is as follows: polymer dissolution is containing 0.1-0.5 mol I
2, 0.1-0.5 mol I
-0.5-1.0 mol 4-tert .-butylpyridine, 0.5-1.0 in the solution of mol 1-methyl-acetonitrile, propene carbonate, methoxyacetonitrile or the acetonitrile of 3-propyl imidazole salt and the mixture of propene carbonate, make it gelation, thereby the formation quasi-solid electrolyte, wherein the mass content of polyethers macromolecule in solution is 1-10%.
6, the preparation method of dye sensitized nano crystal salar battery according to claim 4, the preparation process that it is characterized in that the semiconductor nano epitaxial is as follows: with granularity is that the colloidal tio 2 of 1-50 nanometer is coated on and forms broad stopband nano titanium oxide epitaxial on the transparent conductive substrate, 200-600 ℃ of following roasting 15 minutes to 12 hours, cooling back repetitive operation was until the broad stopband nano titanium oxide epitaxial that obtains the 1-50 micron.
7, the preparation method of dye sensitized nano crystal salar battery according to claim 4 is characterized in that said polyethers macromolecule adopts the copolymer of polyethylene glycol oxide, PPOX or ethylene oxide and propylene oxide.
8, the preparation method of dye sensitized nano crystal salar battery according to claim 4, the method for sensitizing that it is characterized in that nanometer crystal film is: the nano titanium oxide epitaxial is put into baking oven heated 10-120 minute down in 100-250 ℃, being immersed in concentration when being cooled to 25-100 ℃ is 10
-5-10
-3Sensitization in 2-48 hour in the N3 of mol or the Z907 dyestuff.
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| CN1320663C true CN1320663C (en) | 2007-06-06 |
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| CN100423314C (en) * | 2005-09-01 | 2008-10-01 | 复旦大学 | Dye sensitization nanocrystalline solar battery based on dendroid compounds and its preparing method |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH1166953A (en) * | 1997-08-22 | 1999-03-09 | Sumitomo Metal Mining Co Ltd | Conductive adhesive and usage thereof |
| JP2003217690A (en) * | 2002-01-18 | 2003-07-31 | Nippon Shokubai Co Ltd | Dye-sensitized solar battery |
| CN1468909A (en) * | 2002-07-16 | 2004-01-21 | 中国科学院化学研究所 | Gel-type solid polymer electrolyte and its prepn |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH1166953A (en) * | 1997-08-22 | 1999-03-09 | Sumitomo Metal Mining Co Ltd | Conductive adhesive and usage thereof |
| JP2003217690A (en) * | 2002-01-18 | 2003-07-31 | Nippon Shokubai Co Ltd | Dye-sensitized solar battery |
| CN1468909A (en) * | 2002-07-16 | 2004-01-21 | 中国科学院化学研究所 | Gel-type solid polymer electrolyte and its prepn |
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