CN105023758A - Ionic liquid gel electrolyte used for dye-sensitized solar cell and preparation method - Google Patents
Ionic liquid gel electrolyte used for dye-sensitized solar cell and preparation method Download PDFInfo
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- Y02E10/542—Dye sensitized solar cells
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Abstract
The invention belongs to the technical field of solar cells, and specifically relates to an ionic liquid gel electrolyte used for a dye-sensitized solar cell. According to the ionic liquid gel electrolyte provided by the invention, ionic liquid is used as a principal part, and a polymer is used as gels, thereby preparing and obtaining an ionic liquid gel electrolyte in a gel state under room temperature. The ionic liquid gel electrolyte has the characteristics of being non-volatile and non-flowing and being good in stability, replaces a liquid electrolyte which is easily volatile and easy to leak used in a traditional dye-sensitized solar cell, and thus the service life of the dye-sensitized solar cell can be greatly prolonged. When the electrolyte is heated to 300 DEG C in nitrogen, mass loss does not occur, and the electrolyte can be stored in air for a long time and is non-volatile. Efficiency of the dye-sensitized solar cell using the electrolyte can reach 5.47%, efficiency attenuation does not occur after the electrolyte is directly exposed to the air to be tested for 400min, and the efficiency can be maintained at 90% of original efficiency after the electrolyte is placed for 30 days under a simple package.
Description
Technical field
The invention belongs to technical field of solar batteries, be specifically related to a kind of electrolyte for DSSC and preparation method thereof.
Background technology
DSSC is a kind of cheapness, high efficiency, the easy electrooptical device prepared that latest developments go out, and has all attracted to pay close attention to widely in academia and industrial quarters
1.Portable DSSC often needs often deformation to occur when using, and easily cause encapsulation not tight, electrolyte leakage or volatilization, make solar cell failure.
Ionic liquid (Ionic liquid), also referred to as low temperature molten salt, refers in room temperature or close to presenting compound that is liquid, that be made up of ion completely under room temperature.Ionic liquid has the advantages such as stable, heat-resisting, non-volatile, nonflammable, electrochemical window is wide, and the fine solvent as a new generation receives and pays close attention to widely, is widely used in electrochemical device
2.The efficiency that a small amount of ionic liquid can improve device is added in DSSC.Also there is researcher to use ionic liquid to prepare the electrolyte of DSSC, achieve good effect
3.But ionic liquid not yet solves the problem of liquid electrolyte easy to leak, flexible, can in tensile means this problem especially serious.Also the method having researcher to pass through to add gel attempts solving electrolytical leakage problems, but this method can not solve electrolytical volatilization problems
4.
The present invention uses polymer that ionic liquid electrolyte is carried out gelation, combines the advantage of the illiquidity of the non-volatile and gel of ionic liquid electrolyte, has prepared the ionic liquid gel electrolyte with excellent stability.This electrolyte greatly can promote the stability of DSSC, promotes its useful life.
Summary of the invention
The object of the present invention is to provide a kind of for the long-life of DSSC, the electrolyte of high stability and preparation method thereof.
Ionic liquid gel electrolyte provided by the invention, comprise solvent, solute and gel, solvent is alkyl substituted imidazole salt ion liquid, and solute is iodine, lithium iodide, KI, 4-tert .-butylpyridine, and gel is Kynoar-hexafluoropropylene copolymer (PVDF-HFP); Wherein, iodine concentration is 0.01-0.2 M, and lithium iodide concentrations is 0-0.5 M, and KI concentration is 0-0.5 M, 4-tert .-butylpyridine concentration is 0-1.5 M, and Kynoar-hexafluoropropylene copolymer accounts for gross mass mark 3-50%; In addition, also containing 1,2-dimethyl-3-propyl group iodate imidazoles (DMPII) that concentration is 0-2M.
In the present invention, described alkyl substituted imidazole salt ion liquid can be 1-methyl-3-propyl group iodate imidazoles (PMII), two (trifluoromethyl sulfonyl) inferior amine salts (BMITFSI) of 1-butyl-3-methylimidazole etc.
Ionic liquid gel electrolyte of the present invention is bis trifluoromethyl sulfimide root (TFSI as anion in the ionic liquid of solvent
-) or iodide ion (I
-), cation is alkyl imidazole salt ion.
Ionic liquid gel electrolyte provided by the invention, be gel under room temperature, can change liquid state into when being heated to 50 ~ 200 degrees Celsius, gel process has invertibity.
Ionic liquid gel provided by the invention, have non-volatile, non-leakage, water-fast, heat-resisting, nonflammable, electrochemical window is wide, the advantages such as good stability.
Ionic liquid gel electrolyte provided by the invention has excellent performance, non-volatile, non-leakage, water-fast, heat-resisting, nonflammable, electrochemical window is wide, good stability.There is after gel-forming good intensity and flexibility, can self-supporting, and show good elasticity (as Fig. 1 a, 1b).Still there is not weightlessness (as Fig. 1 c) when being heated to 300 degrees Celsius, having showed excellent temperature stability.Ionic liquid gel electrolyte nitrogen under 50 degrees Celsius of constant temperature purges 400 minutes and can not volatilize (as Fig. 1 d), has obvious advantage relative to acetonitrile electrolyte widely used in control group and 3 the most common methoxypropionitrile gel electrolytes.The electrolytical conductivity of ionic liquid gel is 1x10
-8– 1x10
3s/cm.
Ionic liquid gel electrolyte of the present invention is used in DSSC, replaces organic solvent to be the electrolyte of main component, effectively can solve that conventional liquid electrolyte in DSSC is volatile, problem that easy to leak, life-span are short.Meanwhile, the deformable characteristic of gel electrolyte is also more suitable for flexible dye-sensitized solar battery.When using the titanium silk of surface anodization growth titanium dioxide as work electrode, carbon nano-tube or metal platinum are as during to electrode, use DSSC prepared by this electrolyte, its open circuit voltage is 0.3-0.8 V, short-circuit current density is 2-18 mA/cm2, fill factor, curve factor 30%-80%, most effectively reaches 5.47%.Typical case J-V curve is as Fig. 2.Typical electrochemical impedance spectroscopy, as Fig. 3, shows good charge-conduction performance.Meanwhile, this DSSC has excellent thermal stability, is heated to 110 degrees Celsius and can not causes irreversible lesion, as Fig. 4 to device or electrolyte.And have longer useful life, under non-critical enclosed system, preservation can maintain the original efficiency of more than 80%, as Fig. 5 after 30 days.
If electrode is can stretching structure, prepared solar cell also has certain flexibility and tensility, and bending behind efficiency can remain on more than 95%, stretch 25% internal efficiency can keep 95%.
The present invention provides the preparation method of above-mentioned gel electrolyte simultaneously, and concrete steps are as follows:
Alkyl substituted imidazole salt ion liquid is used to be solvent, adding concentration is 0.01-0.2 M elemental iodine, 0-0.5 M lithium iodide, 0-0.5 M KI, 0-1.5 M4-tert .-butylpyridine, the Kynoar-hexafluoropropylene copolymer (PVDF-HFP) of 3-50% mass fraction; Concentration is ionic liquid 1, the 2-dimethyl-3-propyl group iodate imidazoles (DMPII) of 0-2 M.Common heating, and by stirring, the means such as ultrasonic are mixed into homogeneous solution, then cooling makes its gelation, namely obtains ionic liquid gel electrolyte.
Also can with an organic solvent aid dispersion, concrete grammar is: be first jointly dissolved in the organic solvents such as 3-methoxypropionitrile or acetonitrile by all solutes and PVDF-HFP, it is made to disperse by means such as heating, stirring, ultrasonic disperse, the ionic liquid of aequum is added after being uniformly dispersed, hot mixt is added afterwards in convection oven or vacuum drying oven, organic solvent is all volatilized, after cooling, obtains ionic liquid gel electrolyte.
In order to improve electrolytical performance further, guanidine thiocyanate (addition is 0%-5% of ionic liquid) can be added in aforesaid electrolyte, or other additives.
The assembling of battery, gets out work electrode and to electrode, heats above-mentioned electrolyte and make it become low-viscosity (mobile) liquid, being poured between solar cell two electrode, and the electrolyte after cooling in device is gel state.
The present invention compared with prior art has the following advantages:
Prepared electrolyte main component is ionic liquid gel, is flexible, immobilising jelly, has ionic conductivity under room temperature.Non-volatile under normal temperature or heated condition, be heated to 300 degrees Celsius and do not decompose, have excellent stability while using this electrolytical solar cell to have greater efficiency, be much better than conventional liquid electrolyte useful life;
Ionic liquid gel has flexibility and elasticity, with device generation deformation, can avoid the stress accumulation in solid electrolyte and embrittlement risk in deformability and the solar cell that can stretch;
This electrolyte has thermoplasticity, is heated to uniform temperature and can be changed into solution, convenient processing.After heating and melting, low, the good fluidity of viscosity, can infiltrate among electrode gap by capillarity, ensure good contact;
Non-volatile due to ionic liquid, in heating process, there is not volatilization problems in this electrolyte, thus solve the volatilization of gel electrolyte in heating injection process, problem that composition changes, can not be heated for a long time, be conveniently used for more injection technologies.
Relative to polymeric ionic liquid electrolyte, this technical operation is simple, does not need in cell manufacturing process, introduce complicated chemical reaction, simplifies preparation process.
Accompanying drawing explanation
Fig. 1, a, b, the optical photograph of ionic liquid gel electrolyte under nature and case of bending; C, the electrolytical thermal gravimetric analysis curve of ionic liquid gel; D, ionic liquid gel electrolyte and other two kinds of widely used electrolytical volatility contrast, and measure reduced gravity situations when nitrogen purges at 50 c.
Fig. 2, uses the J-V curve of the electrolytical solar cell of ionic liquid gel.
Fig. 3, uses electrochemical impedance spectroscopy (EIS) curve of the electrolytical solar cell of ionic liquid gel.
Fig. 4, ionic liquid gel electrolyte and acetonitrile are the conventional liquid electrolyte efficiency (η) of solvent and original efficiency (η
0) ratio is in the contrast of heating condition.
Fig. 5, after simple and easy encapsulation, ionic liquid gel electrolyte and acetonitrile are the conventional liquid electrolyte efficiency (η) of solvent and original efficiency (η
0) contrast of ratio in 30 days.
Embodiment
Embodiment 1, the electrolytical preparation of ionic liquid gel
Ionic liquid 1-methyl-3-propyl group iodate imidazoles (PMII) is used to be solvent, add the elemental iodine that concentration is 0.05 M, 0.05 M lithium iodide, 0.05 M KI, 0.5 M 4-tert .-butylpyridine, the Kynoar-hexafluoropropylene copolymer (PVDF-HFP) of 20wt%, jointly heat and is mixed into homogeneous solution by stirring, the means such as ultrasonic, cooling becomes gel again, is ionic liquid gel electrolyte.
Prepared solar cell (work electrode effective area 0.12 cm
2) open circuit voltage is 0.6 V, short-circuit current density is 9 mA/cm
2, fill factor, curve factor 60%, efficiency 3.24%.This solar cell has excellent thermal stability, is heated to 120 degrees Celsius and can not causes irreversible lesion to device or electrolyte, places 30 days behind efficiencies and keeps more than 90%.
DSSC uses the titanium silk that grown titania nanotube to be work electrode, and N719 is dyestuff, and carbon nano-tube is as to electrode.The J-V curve of solar cell records under AM1.5 solar simulator, and solar simulator used is Oriel-94023 type, with Keithley 2400 source table, and 1000WXe lamp.
Embodiment 2, uses two (trifluoromethyl sulfonyl) inferior amine salt (BMITFSI) of ionic liquid 1-butyl-3-methyl imidazolium to be solvent, adds the elemental iodine that concentration is 0.05 M, 0.2 M KI.Kynoar-the hexafluoropropylene copolymer (PVDF-HFP) of 20wt%, jointly heat and is mixed into homogeneous solution by stirring, the means such as ultrasonic, then cools and become gel, is ionic liquid gel electrolyte.
Prepared solar cell (work electrode effective area 0.12 cm
2) open circuit voltage is 0.65 V, short-circuit current density is 12 mA/cm
2, fill factor, curve factor 55%, efficiency 4.29%.This solar cell has excellent thermal stability, is heated to 120 degrees Celsius and can not causes irreversible lesion to device or electrolyte, places 30 days behind efficiencies and keeps more than 90%.
DSSC uses the titanium silk that grown titania nanotube to be work electrode, and N719 is dyestuff, and platinum filament is as to electrode.Method of testing is with embodiment 1.
Embodiment 3, two (trifluoromethyl sulfonyl) inferior amine salt (BMITFSI) of ionic liquid 1-butyl-3-methyl imidazolium is used to be solvent, add the elemental iodine that concentration is 0.05 M, 0.2 M lithium iodide, 0.2 M KI, 0.5 M ionic liquid 1, 2-dimethyl-3-propyl group iodate imidazoles (DMPII), Kynoar-the hexafluoropropylene copolymer (PVDF-HFP) of 20wt%, first all solutes and PVDF-HFP are dissolved in the organic solvents such as 3-methoxypropionitrile or acetonitrile jointly, by heating, stir, the means such as ultrasonic disperse make it disperse, the ionic liquid of aequum is added after being uniformly dispersed, hot mixt is added afterwards in convection oven or vacuum drying oven, organic solvent is all volatilized, add 0.5 M4-tert .-butylpyridine more in the molten state to stir, ionic liquid gel electrolyte is obtained after cooling.
Prepared solar cell (work electrode effective area 0.12 cm
2) open circuit voltage is 0.7 V, short-circuit current density is 13 mA/cm
2, fill factor, curve factor 61%, efficiency 5.47%.This solar cell has excellent thermal stability, is heated to 110 degrees Celsius and can not causes irreversible lesion to device or electrolyte, places 30 days behind efficiencies and keeps more than 85%.
DSSC uses the titanium silk that grown titania nanotube to be work electrode, and N719 is dyestuff, and carbon nano-tube is as to electrode.Method of testing is with embodiment 1.
list of references
1. Oregan, B.; Gratzel, M., A low-cost, high-efficiency solar-cell based on dye-sensitized colloidal TiO2 films.
Nature 1991, 353(6346), 737-740.
2. Rogers, R. D.; Seddon, K. R., Ionic liquids--solvents of the future？
Science 2003, 302(5646), 792-793.
3. Kuang, D.; Wang, P.; Ito, S.; Zakeeruddin, S. M.; Gr?tzel, M., Stable mesoscopic dye-sensitized solar cells based on tetracyanoborate ionic liquid electrolyte.
J Am Chem Soc 2006, 128(24), 7732-7733.
4. Kang, M. G.; Kim, K. M.; Ryu, K. S.; Chang, S. H.; Park, N. G.; Hong, J. S.; Kim, K. J., Dye-sensitized TiO2 solar cells using polymer gel electrolytes based on PVdF-HFP.
J Electrochem Soc 2004, 151(7), E257-E260.
5. Pan, S.; Yang, Z.; Li, H.; Qiu, L.; Sun, H.; Peng, H., Efficient Dye-Sensitized Photovoltaic Wires Based on an Organic Redox Electrolyte.
J Am Chem Soc 2013, 135(29), 10622-10625.
6. Jiang, K.; Li, Q.; Fan, S., Nanotechnology: Spinning continuous carbon nanotube yarns.
Nature 2002, 419(6909), 801-801.
7. Sun, H.; Yang, Z.; Chen, X.; Qiu, L.; You, X.; Chen, P.; Peng, H., Photovoltaic Wire with High Efficiency Attached onto and Detached from a Substrate Using a Magnetic Field.
Angew Chem Int Ed 2013, 52(32), 8276-8280.。
Claims (5)
1. the ionic liquid gel electrolyte for DSSC, comprise solvent, solute and gel, it is characterized in that, solvent is alkyl substituted imidazole salt ion liquid, solute is iodine, lithium iodide, KI, 4-tert .-butylpyridine, and gel is Kynoar-hexafluoropropylene copolymer; Wherein, iodine concentration is 0.01-0.2 M, and lithium iodide concentrations is 0-0.5 M, and KI concentration is 0-0.5 M, 4-tert .-butylpyridine concentration is 0-1.5 M, and Kynoar-hexafluoropropylene copolymer accounts for gross mass mark 3-50%; In addition, also containing ionic liquid 1, the 2-dimethyl-3-propyl group iodate imidazoles that concentration is 0-2M.
2. ionic liquid gel electrolyte according to claim 1, is characterized in that described alkyl substituted imidazole salt ion liquid is 1-methyl-3-propyl group iodate imidazoles, two (trifluoromethyl sulfonyl) inferior amine salt of 1-butyl-3-methylimidazole.
3. ionic liquid gel electrolyte according to claim 1 and 2, be gel under it is characterized in that room temperature, change liquid state into when being heated to 50 ~ 200 degrees Celsius, gel process has invertibity.
4. ionic liquid gel electrolyte according to claim 1 or 2, it is characterized in that in the ionic liquid as solvent, anion is bis trifluoromethyl sulfimide root or iodide ion, cation is alkyl imidazole salt ion.
5. the ionic liquid gel electrolyte preparation method as described in one of claim 1-4, is characterized in that concrete steps are as follows:
Use alkyl substituted imidazole salt ion liquid to be solvent, adding concentration is 0.01-0.2 M elemental iodine, 0-0.5 M lithium iodide, 0-1.5 M4-tert .-butylpyridine, the Kynoar-hexafluoropropylene copolymer of 3-50% mass fraction; 0-2 M ionic liquid 1,2-dimethyl-3-propyl group iodate imidazoles; Common heating, and by stirring or ultrasonic, be mixed into homogeneous solution, then cooling makes its gelation, namely obtains ionic liquid gel electrolyte;
Or, first all solutes and Kynoar-hexafluoropropylene copolymer are dissolved in 3-methoxypropionitrile or acetonitrile organic solvents jointly, by heating, stir or ultrasonic disperse means, make it be uniformly dispersed, then add ionic liquid 1, the 2-dimethyl-3-propyl group iodate imidazoles of aequum, in convection oven or vacuum drying oven, add hot mixt, organic solvent is all volatilized, after cooling, namely obtains required ionic liquid gel electrolyte.
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Application publication date: 20151104 |