CN103489645A - Gel electrolyte for DSSC and preparation method of gel electrolyte - Google Patents
Gel electrolyte for DSSC and preparation method of gel electrolyte Download PDFInfo
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Abstract
The invention relates to a DSSC, in particular to a gel electrolyte for the DSSC and a preparation method of the gel electrolyte. The gel electrolyte for the DSSC is characterized in that the mass ratio of the components of the gel electrolyte is functionalized graphene: ionic polymers: ionic liquid: tert-butylpyridine: iodine simple substances: lithium bis(trifluoromethane sulfonimide)= (0.5-20): (10-50): (50-90): (0.5-5): (0.02-10): (0.02-10). The oxidized graphene modified by the ionic liquid can be well scattered inside the electrolyte, the performance of the electrolyte is improved, and then the photovoltaic conversion efficiency of the DSSC is improved. The prepared gel electrolyte does not contain any traditional toxic solutions, and is low in price, easy to obtain, easy to package, good in stability of the DSSC and high in DSSC efficiency. The assembly programs of the DSSC are few, and cost is low. In the room temperature environment, a xenon lamp is utilized to simulate sunlight, and under the condition of the light intensity being 100mW/cm<2>, the measured photovoltaic conversion efficiency of the DSSC (the effective area being 0.16cm<2>) is as highest as 7.9%.
Description
Technical field
The present invention relates to DSSC, refer in particular to a kind of used by dye sensitization solar battery gel electrolyte and preparation method thereof.
Background technology
DSSC (DSSC) has the advantages such as high efficiency, low cost, is the most promising class solar cell; The sandwich that DSSC is comprised of electrode and electrically-conductive backing plate titanium dioxide porous membrane, photosensitizer (dyestuff), electrolyte (containing oxidation-reduction pair), platinum, wherein, electrolyte is the core component of DSSC, the main transmission redox couple that plays a part, electrolytical performance directly affects solar battery efficiency.
DSSC mainly comprises following a few class with electrolyte: liquid electrolyte, quasi-solid electrolyte (gel electrolyte), solid electrolyte; Traditional liquid electrolyte bag generally contains inorganic or organic iodide, iodine, additive and organic solvent etc., and owing to having, conductivity is high, and the ion diffusion velocity is fast, and to advantages such as porous electrode good penetrability, liquid electrolyte DSSC is widely studied; Yet that traditional organic solvent liquid electrolyte exists is volatile, encapsulation difficulty, poor stability, toxicity reach greatly the shortcomings such as the easy desorption of dyestuff, these drawbacks limit the long-term use of DSSC [Adv. Mater., 2001,13,11,826-830].
Chinese invention patent CN 101205283A discloses a kind of gel-type electrolyte and preparation method thereof, and electrolyte is by iodine, polymethacrylate ionic liquid, polyacrylonitrile, ethylene carbonate, propene carbonate and SiO
2form; This electrolyte preparation method is simple, ionic conductivity is high, and the introducing of polymer makes electrolyte form the seepage that gel has suppressed the organic solvents such as ethylene carbonate, propene carbonate to a certain extent, but still the volatilization of inevitable ethylene carbonate, propene carbonate, cause the decline of battery performance.
It is a kind of good electrolyte that ionic liquid (IL) has the advantages such as low-vapor pressure, wide electrochemical window, high thermal stability and high conductivity, with ionic liquid, replace traditional organic solvent to prepare liquid electrolyte DSSC, can solve the volatile difficult problem of conventional solvent, yet ionic liquid still presents liquid state, take ionic liquid as still there is the encapsulation difficulty in electrolytical DSSC, use for a long time the difficult problem of easy seepage.
Chinese invention patent CN101635200A discloses a kind of dye-sensitized solar cell electrolyte and preparation method thereof: after aggretion type ionic liquid, non-polymeric type ionic liquid, ionic liquid crosslinking agent and initator are mixed, by in-situ polymerization, prepare the quasi-solid polymer gel electrolyte, it is strong that gel electrolyte prepared by the method coheres ability, be easy to encapsulation, simplified the battery assembly program.Yet the photoelectric conversion efficiency of battery remains further to be improved.
Add network channel (the Chem. Mater. 2010 that inorganic nano material contributes to the continuous transmission of the inner formation of electrolyte ion in the electrolyte based on ionic liquid, 22, 1807 – 1813), contribute to improve electrolytical conductivity, Graphene and derivative thereof are the novel carbon nanomaterials of a class, due to its unique electric property, there is great application prospect in the DSSC field, graphene oxide (GO) is the derivative of Graphene, multiple reactive group is contained on surface, although there is good dispersiveness in water, but the drawbacks limit that bad dispersibility and thermal stability are lower in organic solvent its application in the organic systems such as gel-form solid polymer electrolyte, it is carried out to rational functional modification, contribute to give full play to its performance.
Summary of the invention
The invention provides a kind of based on Ionic Liquid Modified graphene oxide/ionic liquid Recombination gel electrolyte and preparation method thereof, for DSSC.
The present invention is directed to solution that the problems referred to above adopt: the used by dye sensitization solar battery gel electrolyte is characterized in that: component according to mass ratio is: Ionic Liquid Modified graphene oxide: Ionomer: ionic liquid: tert .-butylpyridine=0.5-20:10-50:50-90:0.5-5.
Further used by dye sensitization solar battery gel electrolyte, it is characterized in that: component according to mass ratio is: Ionic Liquid Modified graphene oxide: Ionomer: ionic liquid: tert .-butylpyridine: elemental iodine=0.5-20:10-50:50-90:0.5-5:0.02-10.
Further used by dye sensitization solar battery gel electrolyte, it is characterized in that: component according to mass ratio is: Ionic Liquid Modified graphene oxide: Ionomer: ionic liquid: tert .-butylpyridine: two trifluoromethanesulfonic acid imide lis: 0.5-20:10-50:50-90; 0.5-5:0.02-10.
Further used by dye sensitization solar battery gel electrolyte, it is characterized in that: component according to mass ratio is: Ionic Liquid Modified graphene oxide: Ionomer: ionic liquid: tert .-butylpyridine: elemental iodine: two trifluoromethanesulfonic acid imide lis: 0.5-20:10-50:50-90:0.5-5:0.02-10:0.02-10.
The structure of described Ionic Liquid Modified function graphene oxide (preparation method with reference to Chem. Commun., 2009,3880 – 3882) is:
Wherein Y is Br, I, SCN, N (CN)
2, C (CN)
3, B (CN)
4, BF
4, PF
6, CF
3sO
3, C
2f
5sO
3, N (SO
2cF
3)
2and CF
3a kind of in COO, R
2for H, methyl, ethyl, isopropyl, a kind of in phenyl.
Described Ionomer is:
or
in a kind of, m=0-9 wherein, X is respectively I, Br, Cl, SCN, N (CN)
2, C (CN)
3, B (CN)
4, BF
4, PF
6, CF
3sO
3, C
2f
5sO
3, [N (SO
2cF
3)
2] and CF
3a kind of in COO, R is H, methyl, ethyl, isopropyl, a kind of in phenyl.
Described ionic liquid is
in one or two or more kinds by mixture of any mass ratio, s=0-5 wherein, Z is I, SCN, N (CN)
2, C (CN)
3, B (CN)
4, BF
4, PF
6, CF
3sO
3, C
2f
5sO
3, [N (SO
2cF
3)
2] and CF
3a kind of in COO, R
1for H, methyl, ethyl, a kind of in isopropyl and phenyl.
The used for solar batteries gel electrolyte of above-mentioned preparation, it is characterized in that: by Ionic Liquid Modified function graphene oxide and Ionomer, ionic liquid, tert .-butylpyridine is mixed according to described ratio, or by Ionic Liquid Modified function graphene oxide and Ionomer, ionic liquid, tert .-butylpyridine and elemental iodine mix according to described ratio, or by Ionic Liquid Modified function graphene oxide and Ionomer, ionic liquid, tert .-butylpyridine and two trifluoromethanesulfonic acid imide li mix according to described ratio, or by Ionic Liquid Modified function graphene oxide and Ionomer, ionic liquid, tert .-butylpyridine, elemental iodine and two trifluoromethanesulfonic acid imide li mix according to described ratio
,60 ~ 120
oat the C temperature, airtight stirring and dissolving 2 ~ 12 hours, form even gel electrolyte, drip to while hot or be expelled between light anode dyestuff titanium dioxide film and Pt electrode, by heating, vacuumize to process and make gel electrolyte be penetrated into fully in the titanium dioxide film perforated membrane, then encapsulate and makes the solid-state full ionic liquid gel solar cell of standard.
Beneficial effect of the present invention is:
The present invention proposes a kind of Ionic Liquid Modified graphene oxide/ionic liquid composite gel electrolyte and preparation method thereof, Ionic Liquid Modified has improved the dispersive property of graphene oxide in ionic liquid electrolyte.By adding the Ionic Liquid Modified graphene oxide, the performance of gel electrolyte is improved, and is conducive to prepare the DSSC of high electricity conversion.
Embodiment
Below in conjunction with specific embodiment, technical scheme of the present invention is further described.
Embodiment mono-:
The Ionic Liquid Modified graphene oxide
preparation (list of references Chem. Commun., 2009,3880 – 3882):
Step 1: the preparation of ionic liquid
By 2.20g 3-propantheline bromide hydrobromide and 0.79g 1-methylimidazole back flow reaction 24 hours in 25ml ethyl acetate, with ethyl acetate, wash twice, rotary evaporation obtains amido ionic liquid 1-(3-aminopropyl)-3-methylimidazole bromine except desolventizing, adds the Li[N (SO of slightly excessive (mol measures excessive 5%)
2cF
3)
2] (2.90g) carry out anion exchange, room temperature reaction 12 hours, obtaining anion after centrifugal, washing (using distilled water), drying is N (SO
2cF
3)
2 -ionic liquid (IL-NH
2), with reference to the method, prepared by the ionic liquid of other structure.
Step 2: the preparation of Ionic Liquid Modified graphene oxide
The graphene oxide sheet solid 50mg that will make by the Hummers method is distributed in 100ml water, and ultrasonic aid dispersion obtains the graphene oxide hydrosol after 30 minutes.Add 100mg KOH in the graphene oxide hydrosol, 200mg IL-NH
2, mixed liquor, 80 ℃ of lower back flow reaction 24 hours, centrifugal, washing (using distilled water), is drying to obtain to the Ionic Liquid Modified graphene oxide, with reference to the method, prepared by the Ionic Liquid Modified graphene oxide of other structure.
Embodiment bis-:
Will
0.08g,
0.40g,
1.10g, tert .-butylpyridine 0.01g, elemental iodine 0.005g, two trifluoromethanesulfonic acid imide li 0.005g are 60
ounder C, mix and blend 12h, obtain gel electrolyte, drips to while hot between light anode dyestuff titanium dioxide film and Pt electrode, by the vacuum filling technology, prepares gel electrolyte DSSC, at ambient temperature, uses the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 5.7%.
Embodiment tri-:
Will
0.06g,
0.60g,,
1.40g, tert .-butylpyridine 0.05g, elemental iodine 0.02g, two trifluoromethanesulfonic acid imide li 0.04g, 75
ounder C, mix and blend 8h, obtain gel electrolyte, drips to while hot between light anode dyestuff titanium dioxide film and Pt electrode, by the vacuum filling technology, prepares gel electrolyte DSSC, at ambient temperature, uses the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 6.2%.
Embodiment tetra-:
0.15g,
0.25g,
0.75g, tert .-butylpyridine 0.05g, elemental iodine 0.05g, two trifluoromethanesulfonic acid imide li 0.05g, 85
ounder C, mix and blend 4h, obtain gel electrolyte, drip to while hot between light anode dyestuff titanium dioxide film and Pt electrode, further heating makes gel electrolyte be penetrated into fully in the titanium dioxide film perforated membrane, prepares gel electrolyte DSSC by the vacuum filling technology, at ambient temperature, use the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 6.5%.
Embodiment five:
Will
0.08g,
0.40g,
1.00g, tert .-butylpyridine 0.09g, elemental iodine 0.09g, two trifluoromethanesulfonic acid imide li 0.06g, 95
ounder C, mix and blend 2h, obtain gel electrolyte, drips to while hot between light anode dyestuff titanium dioxide film and Pt electrode, by the vacuum filling technology, prepares gel electrolyte DSSC.At ambient temperature, use the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 6.9%.
Embodiment six:
Will
0.06g,
0.20g,
1.20g, tert .-butylpyridine 0.10g, elemental iodine 0.12g, 80
ounder C, mix and blend 7h, obtain gel electrolyte, drips to while hot between light anode dyestuff titanium dioxide film and Pt electrode, by the vacuum filling technology, prepares gel electrolyte DSSC, at ambient temperature, uses the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 7.2%.
Embodiment seven:
Will
0.10g,
0.50g,
0.50g, tert .-butylpyridine 0.03g, two trifluoromethanesulfonic acid imide li 0.05g, 90
ounder C, mix and blend 12h, obtain gel electrolyte, drips to while hot between light anode dyestuff titanium dioxide film and Pt electrode, by the vacuum filling technology, prepares gel electrolyte DSSC, at ambient temperature, uses the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 6.2%.
Embodiment eight:
Will
0.20g,
0.40g,
1.60g, tert .-butylpyridine 0.10g, elemental iodine 0.12g, two trifluoromethanesulfonic acid imide li 0.08g, 120
ounder C, mix and blend 3h, obtain gel electrolyte, drips to while hot between light anode dyestuff titanium dioxide film and Pt electrode, by the vacuum filling technology, prepares gel electrolyte DSSC, at ambient temperature, uses the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 5.9%.
Embodiment nine:
Will
0.12g,
0.12g,
0.48g,
0.40g, tert .-butylpyridine 0.02g, elemental iodine 0.02g, two trifluoromethanesulfonic acid imide li 0.06g, 60
ounder C, mix and blend 12h, obtain gel electrolyte, drips to while hot between light anode dyestuff titanium dioxide film and Pt electrode, by the vacuum filling technology, prepares gel electrolyte DSSC, at ambient temperature, uses the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 7.2%.
Embodiment ten:
Will
0.20g,
0.20g,
0.40g,
0.40g, tert .-butylpyridine 0.04g, elemental iodine 0.10g, two trifluoromethanesulfonic acid imide li 0.10g, 110
ounder C, mix and blend 4h, obtain gel electrolyte, drip to while hot between light anode dyestuff titanium dioxide film and Pt electrode, further heating makes gel electrolyte be penetrated into fully in the titanium dioxide film perforated membrane, prepares gel electrolyte DSSC by the vacuum filling technology, at ambient temperature, use the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 7.9%.
Embodiment 11:
Will
0.10g,
0.20g,
0.40g,
0.30g, tert .-butylpyridine 0.03g, 75
ounder C, mix and blend 12h, obtain gel electrolyte, drips to while hot between light anode dyestuff titanium dioxide film and Pt electrode, by the vacuum filling technology, prepares gel electrolyte DSSC.At ambient temperature, use the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 5.2%.
Embodiment 12:
Will
0.20g,
0.50g,
0.50 g, tert .-butylpyridine 0.03g, elemental iodine 0.02g, two trifluoromethanesulfonic acid imide li 0.06g, 100
ounder C, mix and blend 12h, obtain gel electrolyte, drips to while hot between light anode dyestuff titanium dioxide film and Pt electrode, by the vacuum filling technology, prepares gel electrolyte DSSC, at ambient temperature, uses the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 7.0%.
Embodiment 13:
Will
0.20g,
0.40g,
0.60 g, tert .-butylpyridine 0.03g, elemental iodine 0.02g, 100
ounder C, mix and blend 12h, obtain gel electrolyte, drips to while hot between light anode dyestuff titanium dioxide film and Pt electrode, by the vacuum filling technology, prepares gel electrolyte DSSC, at ambient temperature, uses the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 6.6%.
Embodiment 14:
Will
0.20g,
0.30g,
0.30g,
0.40g, tert .-butylpyridine 0.03g, elemental iodine 0.10g, two trifluoromethanesulfonic acid imide li 0.10g, 110
ounder C, mix and blend 4h, obtain gel electrolyte, drip to while hot between light anode dyestuff titanium dioxide film and Pt electrode, further heating makes gel electrolyte be penetrated into fully in the titanium dioxide film perforated membrane, prepares gel electrolyte DSSC by the vacuum filling technology, at ambient temperature, use the xenon lamp simulated solar irradiation, light intensity 100mW/cm
2under condition, record battery (effective area 0.16cm
2) photoelectric conversion efficiency is 7.5%.
Claims (8)
1. a used by dye sensitization solar battery gel electrolyte, it is characterized in that: component according to mass ratio is: Ionic Liquid Modified graphene oxide: Ionomer: ionic liquid: tert .-butylpyridine=0.5-20:10-50:50-90:0.5-5.
2. a kind of used by dye sensitization solar battery gel electrolyte as claimed in claim 1, it is characterized in that: component according to mass ratio is: Ionic Liquid Modified graphene oxide: Ionomer: ionic liquid: tert .-butylpyridine: elemental iodine=0.5-20:10-50:50-90:0.5-5:0.02-10.
3. a kind of used by dye sensitization solar battery gel electrolyte as claimed in claim 1, it is characterized in that: component according to mass ratio is: Ionic Liquid Modified graphene oxide: Ionomer: ionic liquid: tert .-butylpyridine: two trifluoromethanesulfonic acid imide lis: 0.5-20:10-50:50-90; 0.5-5:0.02-10.
4. a kind of used by dye sensitization solar battery gel electrolyte as claimed in claim 1, it is characterized in that: component according to mass ratio is: Ionic Liquid Modified graphene oxide: Ionomer: ionic liquid: tert .-butylpyridine: elemental iodine: two trifluoromethanesulfonic acid imide lis: 0.5-20:10-50:50-90:0.5-5:0.02-10:0.02-10.
5. a kind of used by dye sensitization solar battery gel electrolyte as claimed in claim 1, it is characterized in that: the structure of described Ionic Liquid Modified function graphene oxide is:
Wherein Y is Br, I, SCN, N (CN)
2, C (CN)
3, B (CN)
4, BF
4, PF
6, CF
3sO
3, C
2f
5sO
3, N (SO
2cF
3)
2and CF
3a kind of in COO, R
2for H, methyl, ethyl, isopropyl, a kind of in phenyl.
6. a kind of used by dye sensitization solar battery gel electrolyte as claimed in claim 1, it is characterized in that: described Ionomer is:
or
in a kind of, m=0-9 wherein, X is respectively I, Br, Cl, SCN, N (CN)
2, C (CN)
3, B (CN)
4, BF
4, PF
6, CF
3sO
3, C
2f
5sO
3, [N (SO
2cF
3)
2] and CF
3a kind of in COO, R is H, methyl, ethyl, isopropyl, a kind of in phenyl.
7. a kind of used by dye sensitization solar battery gel electrolyte as claimed in claim 1, it is characterized in that: described ionic liquid is
in one or two or more kinds by mixture of any mass ratio, s=0-5 wherein, Z is I, SCN, N (CN)
2, C (CN)
3, B (CN)
4, BF
4, PF
6, CF
3sO
3, C
2f
5sO
3, [N (SO
2cF
3)
2] and CF
3a kind of in COO, R
1for H, methyl, ethyl, a kind of in isopropyl and phenyl.
8. the preparation method of a kind of used by dye sensitization solar battery gel electrolyte as claimed in claim 1, it is characterized in that: by Ionic Liquid Modified function graphene oxide and Ionomer, ionic liquid, tert .-butylpyridine is mixed according to described ratio, or by Ionic Liquid Modified function graphene oxide and Ionomer, ionic liquid, tert .-butylpyridine and elemental iodine mix according to described ratio, or by Ionic Liquid Modified function graphene oxide and Ionomer, ionic liquid, tert .-butylpyridine and two trifluoromethanesulfonic acid imide li mix according to described ratio, or by Ionic Liquid Modified function graphene oxide and Ionomer, ionic liquid, tert .-butylpyridine, elemental iodine and two trifluoromethanesulfonic acid imide li mix according to described ratio, 60 ~ 120
oat the C temperature, airtight stirring and dissolving 2 ~ 12 hours, form even gel electrolyte, drip to while hot or be expelled between light anode dyestuff titanium dioxide film and Pt electrode, by heating, vacuumize to process and make gel electrolyte be penetrated into fully in the titanium dioxide film perforated membrane, then encapsulate and makes the solid-state full ionic liquid gel solar cell of standard.
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CN114702752A (en) * | 2022-04-07 | 2022-07-05 | 中山市华洋塑胶颜料有限公司 | Graphene composite plastic for heat dissipation and preparation method thereof |
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