CN102254583B - Iodine-doped carbon material serving as cathode of dye-sensitized solar cell - Google Patents
Iodine-doped carbon material serving as cathode of dye-sensitized solar cell Download PDFInfo
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- CN102254583B CN102254583B CN 201110083182 CN201110083182A CN102254583B CN 102254583 B CN102254583 B CN 102254583B CN 201110083182 CN201110083182 CN 201110083182 CN 201110083182 A CN201110083182 A CN 201110083182A CN 102254583 B CN102254583 B CN 102254583B
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
- Y02E10/542—Dye sensitized solar cells
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
- Y02E10/549—Organic PV cells
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Abstract
The invention discloses an iodine-doped carbon material serving as a cathode of a dye-sensitized solar cell. The material is iodine-doped graphite structure carbon, iodine-doped non-graphite structure carbon or an iodine-doped carbon material which is formed by sintering marine biomass respectively, wherein iodine accounts for 1 to 10 weight percent of the material, carbon accounts for 70 to 90 weight percent of the material, and hydrogen accounts for 0 to 5 weight percent of the material. The invention also discloses a preparation method and application of the material. The iodine-doped carbon material serving as the cathode of the solar cell has excellent performance, the solar conversion efficiency is equivalent to that of a platinum electrode, and the iodine-doped carbon material has the advantages of low cost, simple preparation method and the like.
Description
Technical field
The present invention relates to a kind of iodine doping carbon material.
The invention still further relates to above-mentioned iodine doping carbon preparation methods.
The invention still further relates to the application of above-mentioned iodine doping carbon material in DSSC.
Background technology
Along with the development of society, human more and more higher for the demand of the energy, the non-renewable fossil energy of generally using can't satisfy human needs at present.Therefore how effectively to utilize the key subjects that just become energy field such as reproducible novel energies such as solar energy, biomass energies.Based on this, development of new, the power conversion device of solar energy or biomass energy becomes one of research focus efficiently.
Solar energy is that new energy development utilizes most active fields.Solar cell in the market mainly is two kinds of monocrystalline silicon and polysilicons.But the problem of these two kinds of solar cell maximums is the process conditions harshness, and manufacturing cost is too high, is unfavorable for extensive use.And the nano-TiO that occur the nineties in last century
2Organic semiconductor composite solar battery and organic/polymer solar battery, process conditions are simple, and cost is lower, might become the upstart of 21 century solar cell.It is solar cell that DSSC very likely replaces traditional silicon, becomes the leading of following solar cell.
Since 1991 come out, just caused people's extensive concern based on the DSSC of porous titanium oxide, zinc oxide nanocrystalline material.DSSC is owing to its cheap relatively price, and simple manufacturing process and higher efficient might become the leading of following solar cell.Its light-electric switching mechanism is: the nanocrystalline porous film with high-specific surface area can adsorb a lot of individual layer dye molecules and absorb sunlight, and the sensitizer molecule transits to excitation state by absorbing luminous energy, because the unsteadiness of excitation state, sensitizer molecule and TiO
2The surface interacts, and electronics transits to very soon than low-lying level TiO
2Conduction band, enter TiO
2The electronics of conduction band will finally enter conducting film, then by external loop, produce photoelectric current.Simultaneously, be in the dye molecule of oxidation state by the iodide ion I in the electrolyte
-Ground state is got back in oxidation, and I
-Be reduced to I
3-, I
3-The very fast electronics that is entered from negative electrode is oxidized to I
-Constituted a circulation.
Negative electrode also plays an important role in DSSC.In real work, DSSC can produce polarization phenomena owing to there is electric current to pass through negative electrode if the cathode catalysis performance is low, forms overpotential, causes the loss of electromotive force, has reduced the performance of battery.Therefore, the preparation of conventional cathode generally uses the electro-conductive glass sheet as matrix, adopts distinct methods to plate different materials such as graphite, platinum or conducting polymer, and wherein the effect of platinum plating is better, but cost is higher, complex process.About existing patent report in the quick magnificent solar-electricity pool cathode of dyestuff be at present: 200410037799.8 nickel-base alloy electrode, 200510105677.2 mesoporous metal electrode, 200610135370.1 the metallic graphite carbon combination electrode, 200710009239.5 conductive polymer electrodes, 200710133450.8,200710177810.4 and 200610114581.7 mesoporous carbon is to electrode, 200910068409.6 metal nitride is to electrode etc.
Summary of the invention
The object of the present invention is to provide a kind of iodine doping carbon material.
Another purpose of the present invention is to provide a kind of method for preparing above-mentioned iodine doping carbon material.
For achieving the above object, iodine doping carbon material provided by the invention is respectively the iodine doping carbon material that iodine doped graphite structural carbon, iodine mix non-graphite-structure carbon and burnt till by the marine organisms matter that contains iodine; Wherein content of iodine is the 1%-10% of weight ratio, and carbon content is weight ratio 70-90%.
Described iodine doping carbon material wherein, contains the hydrogen that weight ratio is 0-5%.
Described iodine doping carbon material, wherein, the temperature of burning till is 500-1200 ℃.
The method of the above-mentioned iodine doping carbon of preparation provided by the invention material, with graphite matter carbon, non-graphite matter carbon or marine organisms matter and iodine in the mixed atmosphere of nitrogen or nitrogen and hydrogen in 500-1200 ℃ of following sintering, iodine is doped in the material with carbon element, and can makes this material with carbon element have good electrical conductivity.In 50-70 ℃, place, the iodine volatilization of remnants is complete.Also can adopt solution reaction to prepare iodine doped graphite structural carbon material, that is: iodine is dissolved in the ethanol, add graphite matter carbon and stir down at 35-50 ℃, prepare iodine doped graphite structural carbon material.
Described iodine doping carbon preparation methods, wherein, graphite matter carbon is Graphene, and non-graphite matter charcoal is carbon black, and the marine organisms matter that contains iodine is sea-tangle, marine alga etc.
Iodine doping carbon material of the present invention can be as the negative electrode of DSSC, and iodine doping carbon material is coated onto on the electro-conductive glass as negative electrode, uses the semi-conducting material that is adsorbed with dye molecule to be galvanic anode.Wherein, can also add carbon black in the iodine doping carbon material as negative electrode, the weight ratio of iodine doping carbon material and carbon black can be controlled 1: 8-10.
Semi-conducting material as galvanic anode is TiO
2, ZnO or WO
3In one or more; Dye molecule is N3, N719, N749 or phyllins.
The invention has the advantages that:
1, iodine doping carbon material of the present invention is that the solar conversion efficiency of the DSSC made of negative electrode is all higher, and good stability.
2, to prepare the technology of iodine doping carbon material simple in the present invention, and cost is low.
Description of drawings
Fig. 1 is the sem photograph of graphene oxide of the present invention and iodine 3 hours prepared iodine doped graphenes of 900 ℃ of following sintering under blanket of nitrogen.
Fig. 2 is that the present invention is dissolved in the sem photographs that add graphite oxide 48 hours prepared iodine doped graphenes of stirring under 50 ℃ in the absolute ethyl alcohol then with iodine.
Fig. 3 is the sem photograph that contains the iodine material with carbon element that the present invention prepares with marine organisms matter.
Fig. 4 is that embodiment is the I-V curve chart of the DSSC of negative electrode preparation with iodine doped graphite lamella.
Fig. 5 is embodiment is mixed into the DSSC of negative electrode preparation with iodine doped graphite lamella and carbon black I-V curve chart.
Fig. 6 is that embodiment is the I-V curve chart of the DSSC of negative electrode preparation with the iodine doping carbon black.
Fig. 7 is embodiment with the iodine doping carbon material of sea-tangle sintering is the I-V curve chart of the DSSC of negative electrode preparation.
Embodiment
The objective of the invention is by seeking the cathode material of new low-cost DSSC, with the transformation efficiency that improves DSSC and the production cost that reduces DSSC.
For this reason, the invention discloses a kind of iodine doping carbon material as the negative electrode of DSSC, comprise graphited and non-graphitized iodine doping carbon material, as by the iodine doped graphene of graphene oxide by high temperature doping iodine or solution reaction preparation, cross the iodine doping carbon black of high temperature iodine doping preparation and the iodine doping carbon material that is formed by marine organisms matter high temperature sintering by carbon black.
The method for preparing the DSSC negative electrode with iodine doping carbon material of the present invention is this class material to be ground be coated onto on the electro-conductive glass after back adding binder mixes.
Iodine doping carbon of the present invention as the light anode of the prepared DSSC of negative electrode for being adsorbed with dye molecule and semi-conducting material, as TiO
2, ZnO or WO
3Deng.Dye molecule is to have high absorption efficiency as complex N3, the N719 of second bipyridine ruthenium, N749 etc., and nonmetal pigment such as phyllins with the energy level of semi-conducting material coupling and to sunlight
Iodine doping carbon material of the present invention is the solar cell of negative electrode preparation, uses the TO that is adsorbed with dye molecule
2Be galvanic anode, iodine doping carbon material has higher activity as the general material with carbon element of negative electrode of DSSC, and its mechanism may be because iodine doping carbon material can reduce the polarization phenomena of photocathode.About the preparation of iodine doping carbon material among the present invention and the present document of performance and the patent that are used as the photocathode material of DSSC are not all appeared in the newspapers.
The invention is characterized in:
1) these iodine doping carbon preparation methods are simple, and can adopt the diverse ways preparation.
2) layer structure of both having preserved graphitized carbon by the iodine doped graphite carbon of graphene oxide high temperature sintering preparation has bigger specific surface and has conductivity and catalytic activity preferably, can prepare greater efficiency battery cheaply.Iodine doping carbon material by the ungraphitised carbon preparation has improved its catalytic activity owing to having introduced I, and prepared cell efficient also improves a lot.
3) the prepared iodine doping carbon material of the present invention can mix the cathode material as DSSC in varing proportions with carbon black, like this can be by regulating conductivity and the activity that I shared ratio in negative electrode is regulated cathode material, can improve the consumption that Solar cell performance can reduce iodine doping carbon material again, reduce cost.
By the following examples and by reference to the accompanying drawings the present invention is described in detail.
Embodiment 1: be the DSSC of negative electrode preparation with iodine doped graphite lamella
With 200mg oxidized graphite flake layer and 1g iodine 900 ℃ of following sintering 3 hours under the blanket of nitrogen in tube furnace, in 70 ℃ baking oven, placed 48 hours then, allow remaining iodine volatilization fully, measured iodine atom content is 3.43%.Then the iodine doped graphene is coated onto on the electro-conductive glass as negative electrode, uses the TO that is adsorbed with dye molecule
2Be galvanic anode, dye molecule is N719.
Fig. 1 is the sem photograph of the iodine doped graphene of embodiment 1 preparation.Gained I-V curve as shown in Figure 4, electricity conversion reaches 2.95%, and the electricity conversion of doped graphene only is not 0.06%, platinum electrode is the electricity conversion 4.6% of negative electrode under the equal conditions.
Embodiment 2: prepare the iodine doped graphene with solution reaction
Iodine is dissolved in the ethanol, and graphene oxide is distributed in the water, and reaction was 24 hours under both mixed 50-100 ℃, used a large amount of ethanol centrifuge washings then, and is dry in 50 ℃ of baking ovens.
Fig. 2 is the sem photograph of the iodine doped graphene of embodiment 2 preparations.
Embodiment 3: the DSSC that is mixed into the negative electrode preparation with iodine doped graphite lamella and carbon black
Iodine doped graphite lamella preparation method is with embodiment 1, iodine doped graphite lamella and carbon black mixed with 1: 10 ratio of weight ratio to be coated onto on the electro-conductive glass be negative electrode, uses the TO that is adsorbed with dye molecule
2Be galvanic anode, dye molecule is N719.Gained I-V curve as shown in Figure 5, electricity conversion reaches 5.9%, and the electricity conversion of pure carbon black only is 2.1%, platinum electrode is the electricity conversion 4.6% of negative electrode under the equal conditions.
Embodiment 4: be the DSSC of negative electrode preparation with the iodine doping carbon black
With 200mg carbon black and 1g iodine 900 ℃ of following sintering 3 hours in the blanket of nitrogen in tube furnace, in 70 ℃ baking oven, placed 48 hours then, allow remaining iodine volatilization fully.Then the iodate carbon black is coated onto on the electro-conductive glass as negative electrode, uses the TO that is adsorbed with dye molecule
2Be galvanic anode, dye molecule is N719.Gained I-V curve as shown in Figure 6, electricity conversion reaches 4.1%, and the electricity conversion of pure carbon black only is 2.1%, platinum electrode is the electricity conversion 4.6% of negative electrode under the equal conditions.
Embodiment 5: the iodine doping carbon material with the sea-tangle sintering is the DSSC of negative electrode preparation
Since sea-tangle (or marine alga) thus in contain abundant I with sea-tangle at high temperature sintering can obtain a kind of iodate material with carbon element that is rich in iodine.Be specially the sea-tangle wash clean, then in the gaseous mixture of the arbitrary proportion of hydrogen and argon gas in 700-1200 ℃ of scope sintering 4 hours.Fig. 3 is the sem photograph that contains the iodine material with carbon element of embodiment 5 usefulness marine organisms matter preparation.Prepared iodine doping carbon material is coated onto on the electro-conductive glass as negative electrode, uses the TO that is adsorbed with dye molecule
2Be galvanic anode, dye molecule is N719.Gained I-V curve as shown in Figure 7, electricity conversion reaches 5.6%, platinum electrode is the electricity conversion 6.1% of negative electrode.
Claims (7)
1. iodine doping carbon material that is used as the DSSC negative electrode, be respectively iodine doped graphene, iodine doping carbon black or the iodine doping carbon material that burnt till by the marine organisms matter that contains iodine, described marine organisms matter is one or both of sea-tangle, marine alga, and the temperature of burning till is 500-1200 ℃; Wherein content of iodine is the 1%-10% of weight ratio, and carbon content is weight ratio 70%-90%.
2. iodine doping carbon material according to claim 1 wherein, contains the hydrogen that weight ratio is 0-5%.
3. method for preparing the described iodine doping carbon of claim 1 material, with Graphene, carbon black or marine organisms matter and iodine in the mixed atmosphere of nitrogen or nitrogen and hydrogen in 500-1200 ℃ of sintering, place in 50-70 ℃, the iodine volatilization of remnants is complete.
4. the application of the described iodine doping carbon of claim 1 material in DSSC is coated onto on the electro-conductive glass iodine doping carbon material as negative electrode, uses the semi-conducting material that is adsorbed with dye molecule to be galvanic anode.
5. application according to claim 4 wherein, has carbon black as adding in the iodine doping carbon material of negative electrode.
6. application according to claim 4 wherein, is TiO as the semi-conducting material of galvanic anode
2, ZnO or WO
3In one or more.
7. application according to claim 4, wherein, dye molecule is N3, N719, N749 or phyllins.
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|---|---|---|---|
| CN 201110083182 CN102254583B (en) | 2011-03-30 | 2011-03-30 | Iodine-doped carbon material serving as cathode of dye-sensitized solar cell |
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| CN103111312B (en) * | 2013-02-04 | 2014-11-05 | 温州大学 | Chlorine-doped graphene and preparation method and application thereof |
| CN106207255B (en) * | 2015-05-06 | 2018-10-30 | 南开大学 | Organic electrolyte system lithium iodine secondary cell and preparation method thereof |
| CN109557140B (en) * | 2018-11-08 | 2021-02-19 | 深圳大学 | N3 doped ZnO material, preparation method thereof and ethanol sensor |
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| CN101591014B (en) * | 2009-06-30 | 2010-12-29 | 湖北大学 | Method for realizing large-scale preparation of monolayer oxidized graphene |
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