CN103489645B - A kind of used by dye sensitization solar battery gel electrolyte and preparation method thereof - Google Patents
A kind of used by dye sensitization solar battery gel electrolyte and preparation method thereof Download PDFInfo
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Abstract
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, it is characterised in that: gel electrolyte component according to mass ratio is: functionalization graphene: Ionomer: ionic liquid: tert .-butylpyridine: elemental iodine: double trifluoromethanesulfonic acid imide li=0.5-20:10-50:50-90:0.5-5:0.02-10:0.02-10.Graphene oxide through Ionic Liquid Modified can be good at being dispersed in inside electrolyte, improves the performance of electrolyte, thus improves the photoelectric transformation efficiency of DSSC.Gel electrolyte prepared by the present invention does not contains any traditional toxic solvent, cheap and easy to get, easily encapsulates, the good stability of battery, and battery efficiency is high.Battery assembly program is few, low cost.At room temperature environment, use xenon lamp simulated solar irradiation, light intensity 100mW/cm2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is up to 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 advantage such as high efficiency, low cost, is the most promising class solaode；The sandwich that electrode and electrically-conductive backing plate are made up of by DSSC titanium dioxide porous membrane, photosensitizer (dyestuff), electrolyte (containing oxidation-reduction pair), platinum, wherein, electrolyte is the core component of DSSC, acting primarily as the effect of transmission redox couple, the performance of electrolyte directly affects solar battery efficiency.
DSSC electrolyte mainly includes following a few class: liquid electrolyte, quasi-solid electrolyte (gel electrolyte), solid electrolyte；Traditional liquid electrolyte bag typically contains inorganic or organic iodide, iodine, additive and organic solvent etc., high owing to having electrical conductivity, and ion diffusion velocity is fast, and to advantages such as porous electrode good penetrability, liquid electrolyte DSSC is widely studied；But, traditional organic solvent liquid electrolyte exists that volatile, encapsulation difficulty, poor stability, toxicity is big and the shortcoming such as the easy desorption of dyestuff, and these shortcomings limit the life-time service [Adv. Mater., 2001,13,11,826-830] of DSSC.
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, Allyl carbonate and SiO2Composition；This electrolyte preparation method is simple, ionic conductivity is high, and the introducing of polymer makes electrolyte form gel and inhibits the seepage of the organic solvent such as ethylene carbonate, Allyl carbonate to a certain extent, but still inevitable ethylene carbonate, the volatilization of Allyl 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, traditional organic solvent is replaced to prepare liquid electrolyte DSSC with ionic liquid, the volatile difficult problem of conventional solvent can be solved, but ionic liquid still presents liquid, still there is encapsulation difficulty, the long-time difficult problem using easy seepage in the DSSC with ionic liquid as electrolyte.
Chinese invention patent CN101635200A discloses a kind of dye-sensitized solar cell electrolyte and preparation method thereof: prepare Quasi-solid-state polymer gel electrolyte by in-situ polymerization after aggretion type ionic liquid, non-polymeric ionic liquid, ionic liquid cross-linking agent and initiator mix homogeneously, it is strong that gel electrolyte prepared by the method coheres ability, it is prone to encapsulation, simplifies battery assembly program.But, the photoelectric transformation efficiency of battery needs to be improved further.
In electrolyte based on ionic liquid, add inorganic nano material contribute to electrolyte and be internally formed network channel (the Chem. Mater. continuously transmitting ion
2010, 22, 1807 1813), it is favorably improved the electrical conductivity of electrolyte, Graphene and derivant thereof are the carbon nanomaterials that a class is novel, electric property due to its uniqueness, in DSSC field, there is great application prospect, graphene oxide (GO) is the derivant of Graphene, multiple reactive group is contained on surface, although having good dispersibility in water, but its application in the organic systems such as gel-form solid polymer electrolyte of bad dispersibility and the relatively low drawbacks limit of heat stability in organic solvent, it is carried out rational functional modification, contribute to giving 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 the used solution of the problems referred to above: used by dye sensitization solar battery gel electrolyte, it is characterised 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 characterised 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 characterised in that: component according to mass ratio is: Ionic Liquid Modified graphene oxide: Ionomer: ionic liquid: tert .-butylpyridine: double 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 characterised in that: component according to mass ratio is: Ionic Liquid Modified graphene oxide: Ionomer: ionic liquid: tert .-butylpyridine: elemental iodine: double 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, BF4,
PF6, CF3SO3, C2F5SO3,
N(SO2CF3)2And CF3One in COO, R2For H, methyl, ethyl, isopropyl, the one in phenyl.
Described Ionomer is:OrIn one, wherein m=0-9, X are respectively I, Br, Cl, SCN, N (CN)2,
C(CN)3, B(CN)4, BF4, PF6, CF3SO3,
C2F5SO3, [N(SO2CF3)2] and CF3One in COO, R is H, methyl, ethyl, isopropyl, the one in phenyl.
Described ionic liquid isIn one or two or more kinds by the mixture of any mass ratio, wherein s=0-5, Z are I, SCN, N (CN)2,
C(CN)3, B(CN)4, BF4, PF6, CF3SO3,
C2F5SO3, [N(SO2CF3)2] and CF3One in COO, R1For the one in H, methyl, ethyl, isopropyl and phenyl.
The gel electrolyte used for solar batteries of above-mentioned preparation, it is characterized in that: by Ionic Liquid Modified function graphene oxide and Ionomer, ionic liquid, tert .-butylpyridine mixes 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 double 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 double trifluoromethanesulfonic acid imide li mix according to described ratio,60 ~ 120oAt a temperature of C, airtight stirring and dissolving 2 ~ 12 hours, form homogeneous gel electrolyte, drip to or be expelled between light anode dyestuff titanium dioxide film and Pt electrode while hot, being processed by heating, evacuation makes gel electrolyte completely penetrate in titanium dioxide film perforated membrane, then is packaged preparing quasi-solid-state full ionic liquid gel solaode.
The beneficial effects 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, and Ionic Liquid Modified improves graphene oxide dispersive property in ionic liquid electrolyte.By adding Ionic Liquid Modified graphene oxide, the performance of gel electrolyte is improved, and is conducive to preparing the DSSC of high electricity conversion.
Detailed description of the invention
Below in conjunction with specific embodiment, technical scheme is further described.
Embodiment one:
Ionic Liquid Modified graphene oxidePreparation (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. is back flow reaction 24 hours in 25ml ethyl acetate, twice is washed by ethyl acetate, rotary evaporation removes solvent and obtains amido ionic liquid 1-(3-aminopropyl)-3-Methylimidazole. bromine, adds the Li [N (SO little over amount (mol amount excess 5%)2CF3)2] (2.90g) carry out anion exchange, room temperature reaction 12 hours, centrifugal, washing (with distilled water), dried i.e. to obtain anion be N (SO2CF3)2 -Ionic liquid (IL-NH2), the ionic liquid of other structure is prepared with reference to the method.
Step 2: the preparation of Ionic Liquid Modified graphene oxide
Being distributed in 100ml water by the graphene oxide lamellar solid 50mg prepared by Hummers method, ultrasonic wave added obtains the graphene oxide hydrosol after disperseing 30 minutes.100mg KOH, 200mg is added in the graphene oxide hydrosol
IL-NH2, by mixed liquor back flow reaction 24 hours at 80 DEG C, it being centrifuged, wash (with distilled water), be drying to obtain Ionic Liquid Modified graphene oxide, the Ionic Liquid Modified graphene oxide of other structure is prepared with reference to the method.
Embodiment two:
Will0.08g
,0.40g,1.10g, tert .-butylpyridine 0.01g, elemental iodine 0.005g, double trifluoromethanesulfonic acid imide li 0.005g are 60oUnder C, mix and blend 12h, obtain gel electrolyte, drip between light anode dyestuff titanium dioxide film and Pt electrode while hot, prepare gel electrolyte DSSC by vacuum filling technology, at ambient temperature, use xenon lamp simulated solar irradiation, light intensity 100mW/cm2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 5.7%.
Embodiment three:
Will0.06g,0.60g,1.40g, tert .-butylpyridine 0.05g, elemental iodine 0.02g, double trifluoromethanesulfonic acid imide li 0.04g, 75oUnder C, mix and blend 8h, obtain gel electrolyte, drip between light anode dyestuff titanium dioxide film and Pt electrode while hot, prepare gel electrolyte DSSC by vacuum filling technology, at ambient temperature, use xenon lamp simulated solar irradiation, light intensity 100mW/cm2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 6.2%.
Embodiment four:
0.15g,0.25g,0.75g, tert .-butylpyridine 0.05g, elemental iodine 0.05g, double trifluoromethanesulfonic acid imide li 0.05g, 85oUnder C, mix and blend 4h, obtain gel electrolyte, drip between light anode dyestuff titanium dioxide film and Pt electrode while hot, heating makes gel electrolyte completely penetrate in titanium dioxide film perforated membrane further, prepares gel electrolyte DSSC by vacuum filling technology, at ambient temperature, use xenon lamp simulated solar irradiation, light intensity 100mW/cm2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 6.5%.
Embodiment five:
Will0.08g,
0.40g,1.00g, tert .-butylpyridine 0.09g, elemental iodine 0.09g, double trifluoromethanesulfonic acid imide li 0.06g, 95oUnder C, mix and blend 2h, obtain gel electrolyte, drip to while hot, between light anode dyestuff titanium dioxide film and Pt electrode, prepare gel electrolyte DSSC by vacuum filling technology.At ambient temperature, xenon lamp simulated solar irradiation, light intensity 100mW/cm are used2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 6.9%.
Embodiment six:
Will0.06g,
0.20g,1.20g, tert .-butylpyridine 0.10g, elemental iodine 0.12g, 80oUnder C, mix and blend 7h, obtain gel electrolyte, drip between light anode dyestuff titanium dioxide film and Pt electrode while hot, prepare gel electrolyte DSSC by vacuum filling technology, at ambient temperature, use xenon lamp simulated solar irradiation, light intensity 100mW/cm2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 7.2%.
Embodiment seven:
Will0.10g,0.50g,0.50g, tert .-butylpyridine 0.03g, double trifluoromethanesulfonic acid imide li 0.05g, 90oUnder C, mix and blend 12h, obtain gel electrolyte, drip between light anode dyestuff titanium dioxide film and Pt electrode while hot, prepare gel electrolyte DSSC by vacuum filling technology, at ambient temperature, use xenon lamp simulated solar irradiation, light intensity 100mW/cm2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 6.2%.
Embodiment eight:
Will0.20g,
0.40g,1.60g, tert .-butylpyridine 0.10g, elemental iodine 0.12g, double trifluoromethanesulfonic acid imide li 0.08g, 120oUnder C, mix and blend 3h, obtain gel electrolyte, drip between light anode dyestuff titanium dioxide film and Pt electrode while hot, prepare gel electrolyte DSSC by vacuum filling technology, at ambient temperature, use xenon lamp simulated solar irradiation, light intensity 100mW/cm2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 5.9%.
Embodiment nine:
Will0.12g,
0.12g,0.48g,0.40g, tert .-butylpyridine 0.02g, elemental iodine 0.02g, double trifluoromethanesulfonic acid imide li 0.06g, 60oUnder C, mix and blend 12h, obtain gel electrolyte, drip between light anode dyestuff titanium dioxide film and Pt electrode while hot, prepare gel electrolyte DSSC by vacuum filling technology, at ambient temperature, use xenon lamp simulated solar irradiation, light intensity 100mW/cm2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 7.2%.
Embodiment ten:
Will0.20g,0.20g,0.40g,0.40g, tert .-butylpyridine 0.04g, elemental iodine 0.10g, double trifluoromethanesulfonic acid imide li 0.10g, 110oUnder C, mix and blend 4h, obtain gel electrolyte, drip between light anode dyestuff titanium dioxide film and Pt electrode while hot, heating makes gel electrolyte completely penetrate in titanium dioxide film perforated membrane further, prepares gel electrolyte DSSC by vacuum filling technology, at ambient temperature, use xenon lamp simulated solar irradiation, light intensity 100mW/cm2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 7.9%.
Embodiment 11:
Will0.10g,0.20g,
0.40g,0.30g, tert .-butylpyridine 0.03g, 75oUnder C, mix and blend 12h, obtain gel electrolyte, drip to while hot, between light anode dyestuff titanium dioxide film and Pt electrode, prepare gel electrolyte DSSC by vacuum filling technology.At ambient temperature, xenon lamp simulated solar irradiation, light intensity 100mW/cm are used2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 5.2%.
Embodiment 12:
Will0.20g,0.50g,0.50
G, tert .-butylpyridine 0.03g, elemental iodine 0.02g, double trifluoromethanesulfonic acid imide li 0.06g, 100oUnder C, mix and blend 12h, obtain gel electrolyte, drip between light anode dyestuff titanium dioxide film and Pt electrode while hot, prepare gel electrolyte DSSC by vacuum filling technology, at ambient temperature, use xenon lamp simulated solar irradiation, light intensity 100mW/cm2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 7.0%.
Embodiment 13:
Will0.20g,
0.40g,0.60
G, tert .-butylpyridine 0.03g, elemental iodine 0.02g, 100oUnder C, mix and blend 12h, obtain gel electrolyte, drip between light anode dyestuff titanium dioxide film and Pt electrode while hot, prepare gel electrolyte DSSC by vacuum filling technology, at ambient temperature, use xenon lamp simulated solar irradiation, light intensity 100mW/cm2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 6.6%.
Embodiment 14:
Will0.20g,
0.30g,0.30g,0.40g, tert .-butylpyridine 0.03g, elemental iodine 0.10g, double trifluoromethanesulfonic acid imide li 0.10g, 110oUnder C, mix and blend 4h, obtain gel electrolyte, drip between light anode dyestuff titanium dioxide film and Pt electrode while hot, heating makes gel electrolyte completely penetrate in titanium dioxide film perforated membrane further, prepares gel electrolyte DSSC by vacuum filling technology, at ambient temperature, use xenon lamp simulated solar irradiation, light intensity 100mW/cm2Under the conditions of, record battery (effective area 0.16cm2) photoelectric transformation efficiency is 7.5%.
Claims (6)
1. a used by dye sensitization solar battery gel electrolyte, it is characterised in that: component according to mass ratio is: Ionic Liquid Modified
Graphene oxide: Ionomer: ionic liquid: tert .-butylpyridine: double trifluoromethanesulfonic acid imide lis: 0.5-20:10-
50:50-90；0.5-5:0.02-10.
2. a used by dye sensitization solar battery gel electrolyte, it is characterised in that: component according to mass ratio is: Ionic Liquid Modified
Graphene oxide: Ionomer: ionic liquid: tert .-butylpyridine: elemental iodine: double trifluoromethanesulfonic acid imide lis:
0.5-20:10-50:50-90:0.5-5:0.02-10:0.02-10.
3. a kind of used by dye sensitization solar battery gel electrolyte as claimed in claim 1 or 2, it is characterised in that: described
The structure of Ionic Liquid Modified function graphene oxide be:
Wherein Y is Br, I, SCN, N (CN)2,C(CN)3,B(CN)4,BF4,PF6,CF3SO3,C2F5SO3,N(SO2CF3)2With
CF3One in COO, R2For H, methyl, ethyl, isopropyl, the one in phenyl.
4. a kind of used by dye sensitization solar battery gel electrolyte as claimed in claim 1 or 2, it is characterised in that: described
Ionomer is:In one, wherein m=0-9,
X is respectively I, Br, Cl, SCN, N (CN)2,C(CN)3,B(CN)4,BF4,PF6,CF3SO3,C2F5SO3,[N(SO2CF3)2]
And CF3One in COO, R is H, methyl, ethyl, isopropyl, the one in phenyl.
5. a kind of used by dye sensitization solar battery gel electrolyte as claimed in claim 1 or 2, it is characterised in that: described
Ionic liquid isIn one or two or more kinds by the mixture of any mass ratio, wherein s=0-5, Z are I,
SCN,N(CN)2,C(CN)3,B(CN)4,BF4,PF6,CF3SO3,C2F5SO3,[N(SO2CF3)2] and CF3One in COO,
R1For the one in H, methyl, ethyl, isopropyl and phenyl.
6. a kind of used by dye sensitization solar battery gel electrolyte as claimed in claim 1 or 2, it is characterised in that preparation method
As follows: by Ionic Liquid Modified function graphene oxide and Ionomer, ionic liquid, tert .-butylpyridine and double fluoroform
Sulfonic acid imide li mixes according to described ratio, or by Ionic Liquid Modified function graphene oxide and Ionomer, ion
Liquid, tert .-butylpyridine, elemental iodine and double trifluoromethanesulfonic acid imide li mix according to described ratio, 60～120 DEG C of temperature
Under, airtight stirring and dissolving 2～12 hours, form homogeneous gel electrolyte, drip to or be expelled to light anode dyestuff dioxy while hot
Change between titanium film and Pt electrode, processed by heating, evacuation and make gel electrolyte completely penetrate titanium dioxide film porous
In film, then it is packaged preparing quasi-solid-state full ionic liquid gel solaode.
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| CN103971949B (en) * | 2013-02-04 | 2019-04-26 | 南开大学 | Ionic liquid gel electrolyte system and supercapacitor containing the system |
| CN105244537B (en) * | 2015-10-16 | 2017-07-14 | 江苏科技大学 | A kind of method that doping prepares composite polymer electrolyte film |
| CN114702752B (en) * | 2022-04-07 | 2022-11-18 | 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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