CN101894678B - Spongy quantum dot solar cell and preparation method thereof - Google Patents
Spongy quantum dot solar cell and preparation method thereof Download PDFInfo
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- CN101894678B CN101894678B CN2010101930353A CN201010193035A CN101894678B CN 101894678 B CN101894678 B CN 101894678B CN 2010101930353 A CN2010101930353 A CN 2010101930353A CN 201010193035 A CN201010193035 A CN 201010193035A CN 101894678 B CN101894678 B CN 101894678B
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Abstract
The invention provides a novel quantum dot solar cell which integrates a sensitizer and a transmission layer, i.e. quantum dots and oxide nanoparticles in the existing quantum dot solar cell anode structure as a whole, and utilizes the advantages of quantum restriction effect, multi-exciton effect and zonule effect of the quantum dots to increase light absorption, reduce electronic recombination in electronic transmission, and quickly transmit an hole into electrolyte, thus improving photoelectric conversion efficiency of the cell. The invention further provides a preparation method of an anode of a spongy structure stacked by the CdS quantum dots with different porosities. The method has the characteristics of simple process, short reaction time and low reaction temperature.
Description
Technical field
The invention relates to solar cell, relate in particular to quantum dot solar cell and preparation method thereof.
Background technology
Along with people's is to the continuous increase of energy demand and the continuous minimizing of fossil type (coal, oil, natural gas) energy reserve, and seeking alternative new forms of energy sustainable, green non-pollution has become the emphasis problem of scientific research.In numerous alternative energy source (like nuclear energy, wind energy, water ability, tidal energy, solar energy etc.), solar power generation beyond doubt the most people expect and the promising energy.The energy that the sun shines the earth every year is 5.4 * 10
24About J, be equivalent to the whole world and all can use several ten thousand times of the energy every year.Compare with fossil fuel, solar energy is inexhaustible, does not pollute; The use of solar energy can not destroy earth heat balance, and is favourable to ecological protection; Compare with nuclear energy, solar energy is safer, and its application can be to any pollution of environment structure; Compare with water ability, wind energy, the cost of solar energy is lower, and not limited by geographical conditions.Therefore, the utilization of solar energy, especially directly change solar radiation into the research and development of the solar cell of electric energy, received the special concern of countries in the world.
So far, three generations's development has been passed through in the development of solar cell in the world.First generation solar cell is stock with silicon, and conversion efficiency can reach about 15%, has occupied the exhausted vast scale in present photovoltaic cell market; Second generation solar cell, i.e. thin film solar cell, the laboratory conversion efficiency can reach about 30%.But these two kinds of batteries are difficult to far away meet the need of market all because of it costs an arm and a leg.Third generation solar cell, promptly DSSC (DSSCs) is a kind of novel solar cell that gets a good chance of at present.Preceding relatively two battery eliminators, its preparation technology is simple, with low cost, and cost of manufacture is merely 1/5～1/10 of silicon solar cell, and the life-span can reach more than 20 years.The laboratory conversion efficiency can reach about 11%.But the more than ten years have gone over, and its conversion efficiency is still paced up and down about 11%, further improve quite difficulty of transformation efficiency.No matter be silicon solar cell, thin-film solar cells, or all there is 31% the limit in the energy transformation ratio of DSSCs, has hindered the lifting of photoelectric conversion efficiency.The researcher finds to utilize special performances such as the quantum limitation effect of quantum dot, many exciton effects recently; Can break through the power conversion limit of solar cell; Reach 66% transformation efficiency; This has caused research quantum dot solar cell (quantum dot solar cells, upsurge QDSCs).
The advantage of quantum dot solar cell comes from: (1) quantum limitation effect: when the semiconductor grain size was close with its exciton Bohr radius, system can be with and be split into the series of discrete quantum level.Quantum dot is applied on the solar cell, can regulates and control its extinction wavelength through the size of selecting the different materials that can be with and controlling particle diameter, it is interior to the absorbing of sunlight to be implemented in wideer wave-length coverage, sees Yu, W.W.; Peng, X.Angew.Chem.Int.Ed.2002,41,2368.(2) many exciton effects: when the yardstick of semi-conducting material is reduced to quantum dot,, cause the chance of auger effect and anti-process thereof collision ionization to increase greatly because the limited and incident electronics of charge carrier-hole enclosed pasture effect strengthens.In quanta point material, single photon will produce a plurality of excitons through the collision ionization.(3) little band effect: semi-conducting material can produce the phenomenon that can be with division after quantization, between each quantum dot, can produce many tiny and continuous energy levels, is called little band.This level structure can reduce thermionic cooldown rate, and for hot electron provides many good conduction and collects the path, hot electron can outwards be spread out of at the higher energy level place, therefore can obtain higher photovoltage.Quantum dot is extinction in the visible region, can be used as the sensitizer of DSSC, and the advantage of quantum dot aspect light absorption is because its quantum limitation effect.Can utilize hot electron collision photon to produce a plurality of hole-electron pairs with quantum dot.And quantum dot has high extinction coefficient, thereby it can reduce total efficient that dark current can improve solar cell.
But the structure of the existing QDSCs of existing quantum dot solar cell all is to have inherited the thinking of traditional DSSCs, is substituted with organic dye with quantum dot, receives sunlight, produces photoelectron, through the transmission of light anode, arrives FTO charge-trapping end.There is following problem in this structure: the transmission loss of (1) light induced electron is big.Photo-generated carrier produces the back and injects oxide particle, approximately will be through 10
3-10
6Individual nano particle could arrive passive electrode, and light induced electron takes place compound through the blemish place of the nano particle of being everlasting.(2) hole transport difficulty.With respect to dye sensitizing agent, the hole is relatively slow from quantum dot importing electrolyte.See that from root this is that G.J.Phys.Chem.C 2008,112 owing to due to the difference of electronics and hole density of electronic states on conduction band and valence band, see Hodes, 17778.With the n N-type semiconductor N is example; The density of states of the density of states in hole electronics on the conduction band on the quantum dot valence band; With respect to the electronics injection process; It is disadvantageous on dynamics that the hole imports electrolyte, is led until then in the hole, and the quantum dot of oxidation state is difficult to absorb once more photon and produces electron-hole pair.In addition, if the hole can not be led away smoothly, the quantum dot of oxidation state is unsettled in electrolyte, and photoetch can take place, and is dissolved in the electrolyte gradually.Therefore, the transmission in hole has restricted the separation of charge of QDSCs, thereby has restricted the lifting of its electricity conversion.(3) efficiency of light absorption is low.In DSSCs, dye molecule forms monolayer outside sull, and too much dye molecule not only can not increase the absorption to sunlight, but also can cause the cancellation of photo-generated carrier.Similar with DSSCs, the best lift-launch amount of QDSCs also is an absorption monolayer quantum dot outside transport layer.Because mostly quanta point material is narrow gap semiconductor, it is compound that interband takes place the electron-hole pair that under illumination, produces easily, also takes place compound during light induced electron transmits between quantum dot easily.But, outside transport layer, can only carry the individual layer quantum dot and limit effective absorption and the utilization of quantum dot sunlight.
So reasonably design the structure of solar cell, the advantage of effectively utilizing quantum dot and being had is the direction of the light of solar cell development.
Summary of the invention
The objective of the invention is to overcome the deficiency of prior art; Providing a kind of unites two into one sensitizer (quantum dot) in the present quantum dot solar cell anode construction and transport layer (oxide nano particles); Utilize the advantage of the quantum limitation effect of quantum dot, many exciton effects and little band effect; Thereby can increase light absorption, reduce electron recombination in the electric transmission, and can rapidly the hole be passed to the electricity conversion of raising battery in the electrolyte; And it is simple to have technology, spongy quantum dot solar cell that the reaction time is short, temperature is low and preparation method thereof.
The present invention is achieved through following technical proposals.
Spongy quantum dot solar cell; Comprise cadmium sulfide CdS quantum dot anode, electrolyte and platinum cathode; Said cadmium sulfide CdS quantum dot anode has sensitizer and transport layer; Said cadmium sulfide CdS quantum dot anode construction is that sensitizer and transport layer are uniting two into one of quantum dot and oxide nano particles, is the spongy porous three-dimensional structure of quantum dot composition.
The preparation method of spongy quantum dot solar cell has following steps:
(1) with the FTO glass (SnO of doped with fluorine
2Electro-conductive glass) is equipped with one deck TiO through being coated with legal system
2Seed Layer is annealed it 1 hour in 500 ℃ then;
(2) isopyknic aqueous solution of preparation 0.025～0.05mol/L cadmium acetate and 0.075～0.15mol/L thiocarbamide; By ammonia concn in the overall reaction solution is that the amount of 1.6～2.2mol/L adds ammoniacal liquor in the aqueous solution of cadmium acetate; Utilize ultrasonic wave to carry out sonicated; The aqueous solution with the thiocarbamide for preparing adds subsequently, and adding neopelex dressing agent mixes as reaction solution;
(3) the FTO glass after step (1) annealing is placed the agitated reactor that fills step (2) reaction solution, utilize hydro thermal method under 120 ℃ of temperature, to react and prepared spongy CdS quantum dot thin layer in 2～11 hours;
(4) take out the light anode prepare and the spongy CdS film that obtains carried out annealing in process;
The spongy anode material that (5) will obtain immerses the N3 dyestuff and soaked 1～2 hour, use the sarin Surlyn heat sealing film that Du Pont is produced to be made into the frame shape structure of definite shape and be clipped in work electrode and the Pt electrode between, after the heating with cell package together;
(6) electrolyte after under vacuum action, pouring into, utilizes sarin Surlyn heat sealing film with it sealing through the aperture of Pt electrode reservation equally, makes spongy quantum dot solar cell.
The invention has the beneficial effects as follows that a kind of preparation technology is provided is simple, the spongy quantum dot solar cell that the reaction time is short, temperature is low, design is ingenious, novel; In a creative way light-sensitive material and transferring material are united two into one, the absorption that has increased light has also improved the transmission performance of electronics simultaneously.
Though the spongy quantum dot solar cell of new structure is without optimizing but obtained 1.61% photoelectric conversion efficiency, thereby lay a good foundation for later application.Simultaneously, this mentality of designing also provides new direction for the research and development of quantum dot solar cell.
Description of drawings
Fig. 1 is the electron scanning micrograph of overlooking for spongy CdS quantum dot anode;
Fig. 2 is the side-looking electron scanning micrograph for spongy CdS quantum dot anode;
Fig. 3 is the stereoscan photograph of the spongy CdS quantum dot anode of 1.6mol/L ammonia concn preparation;
Fig. 4 is the stereoscan photograph of the spongy CdS quantum dot anode of 1.8mol/L ammonia concn preparation;
Fig. 5 is the stereoscan photograph of the spongy CdS quantum dot anode of 2.0mol/L ammonia concn preparation;
Fig. 6 is the stereoscan photograph of the spongy CdS quantum dot anode of 2.2mol/L ammonia concn preparation.
Embodiment
The chemical pure raw material that the raw materials used employing of the present invention is commercially available.
In preparation method of the present invention, thiocarbamide is excessive, and thiocarbamide not only provides the sulphur source, and it is further grown up can be coated on the prevention of CdS outside.Neopelex is a kind of anionic surfactant commonly used, can be effectively and metal cation form complex, thereby the growing up of restriction particle.And the CdS quantum dot that forms can form the branch vesicular texture through the effect of hydrogen bond.Thiocarbamide can resolve into NH under the condition of alkalescence
3, CO
2And S
2-, along with the decomposition of thiocarbamide, CO
2Can come out internally Deng gas; The anode material of the loose structure that this like this quantum dot is piled up has formed, and referring to Fig. 1 and Fig. 2, is the electron scanning micrograph of spongy CdS quantum dot anode; Fig. 1 is for overlooking stereoscan photograph, and Fig. 2 is the side stereoscan photograph.Ammoniacal liquor can promote thiocarbamide to decompose, so along with the increase of ammonia vol, the CdS particle will be grown up, and the hole is also many more.
Because the spongelike structure of the CdS through Hydrothermal Growth has a large amount of micropores, thereby can help the immersion of liquid electrolyte, helps leading away of hole.
This is that quantum dot and the oxide nano particles battery design that unites two into one has not only increased the absorption of light with sensitizer and transport layer, and has reduced the loss of electronics in transmission.
The highest electronics occupied orbital (HOMO) of N3 dyestuff is positioned at CdS valence band and electrolyte also between the ortho states energy level.After the CdS quantum dot light was according to the generation charge carrier, the hole was delivered in the electrolyte through the HOMO of N3 dyestuff.Simultaneously, the N3 dyestuff also is good sensitising agent, under illumination, also can produce electron-hole pair, and the excitation state electronics is delivered in the CdS quantum dot through the lowest unoccupied molecular orbital (LUMO) of dye molecule, improves photoelectron density.The N3 dyestuff that is adsorbed in CdS quantum dot surface plays the double action of sensitization and hole transport.
Specific embodiment is following:
Embodiment 1
FTO glass is equipped with one deck TiO through being coated with legal system
2Seed Layer, then with its 500 ℃ annealing 1 hour subsequent use.Isopyknic aqueous solution of preparation 0.05mol/L cadmium acetate and 0.15mol/L thiocarbamide; By ammonia concn in the overall reaction solution is that the amount of 1.6mol/L adds in the aqueous solution of cadmium acetate and utilizes ultrasonic wave to handle and makes its mixing; Subsequently the thiourea solution for preparing is added, and add the neopelex dressing agent simultaneously and mix as reaction solution.TiO will be arranged
2The FTO glass of Seed Layer places the agitated reactor that fills reaction solution, under 120 ℃ of reaction temperatures, reacts to prepare spongy CdS quantum dot thin layer in 2～11 hours, takes out the light anode prepare and the spongy CdS film that obtains is carried out annealing in process.Can be seen by Fig. 3 having obtained spongelike structure, hole is more.The spongy anode material that obtains is immersed the N3 dyestuff soaked about 1 hour, use the Surlyn heat sealing film that Du Pont is produced to be made into the frame shape structure of definite shape and be clipped in work electrode and the Pt electrode between, after the heating with cell package together.The aperture that electrolyte is reserved through the Pt electrode after under vacuum action, pouring into, utilizes Surlyn heat sealing film that Du Pont produces with it sealing equally, thereby prepares a novel solar cell,
Embodiment 2
In the same agitated reactor; Isopyknic aqueous solution of preparation 0.05mol/L cadmium acetate and 0.15mol/L thiocarbamide; By ammonia concn in the overall reaction solution is that the amount of 1.8mol/L adds in the aqueous solution of cadmium acetate and utilizes ultrasonic wave to carry out sonicated; The aqueous solution with thiocarbamide adds subsequently, and adding neopelex dressing agent mixes as reaction solution.FTO glass is placed the agitated reactor that fills reaction solution; Under 120 ℃ of reaction temperatures, react and prepared spongy CdS quantum dot thin layer in 2～11 hours, can see, obtained the spongelike structure of porous by Fig. 4; And the quantity in hole and hole are increasing, and porosity is bigger.The annealing back is assembled into battery by top method.
Embodiment 3
In the same agitated reactor; Isopyknic aqueous solution of preparation 0.05mol/L cadmium acetate and 0.15mol/L thiocarbamide; By ammonia concn in the overall reaction solution is that the amount of 2.0mol/L adds in the aqueous solution of cadmium acetate and utilizes ultrasonic wave to carry out sonicated; The aqueous solution with the thiocarbamide for preparing adds subsequently, and adding neopelex dressing agent mixes as reaction solution.FTO is placed the agitated reactor that fills reaction solution, under 120 ℃ of reaction temperatures, react and prepared spongy CdS quantum dot thin layer in 2～11 hours, can see, obtained the spongelike structure of porous, and the quantity in hole and hole continue increasing by Fig. 5.The annealing back is assembled into battery by top method.
Embodiment 4
In the same agitated reactor; Isopyknic aqueous solution of preparation 0.05mol/L cadmium acetate and 0.15mol/L thiocarbamide; By ammonia concn in the overall reaction solution is that the amount of 2.2mol/L adds in the aqueous solution of cadmium acetate and utilizes ultrasonic wave to carry out sonicated; The aqueous solution with the thiocarbamide for preparing adds subsequently, and adding neopelex dressing agent mixes as reaction solution.FTO is placed the agitated reactor that fills reaction solution; Under 120 ℃ of reaction temperatures, react and prepared spongy CdS quantum dot thin layer in 2～11 hours, can see, obtained the spongelike structure of porous by Fig. 6; And it is maximum that the quantity in hole and hole reach, and porosity is maximum.The annealing back is assembled into battery by top method.
Claims (2)
1. spongy quantum dot solar cell; Comprise cadmium sulfide CdS quantum dot anode, electrolyte and platinum cathode; Said cadmium sulfide CdS quantum dot anode has sensitizer and transport layer; It is characterized in that said cadmium sulfide CdS quantum dot anode construction is that sensitizer and transport layer are uniting two into one of quantum dot and oxide nano particles, be the spongy porous three-dimensional structure of quantum dot composition.
2. the preparation method of the spongy quantum dot solar cell of claim 1 is characterized in that, has following steps:
(1) with the FTO glass (SnO of doped with fluorine
2Electro-conductive glass) is equipped with layer of titanium dioxide TiO through being coated with legal system
2Seed Layer is annealed it 1 hour in 500 ℃ then;
(2) isopyknic aqueous solution of preparation 0.025～0.05mol/L cadmium acetate and 0.075～0.15mol/L thiocarbamide; By ammonia concn in the overall reaction solution is that the amount of 1.6～2.2mol/L adds ammoniacal liquor in the aqueous solution of cadmium acetate; Utilize ultrasonic wave to carry out sonicated; The aqueous solution with the thiocarbamide for preparing adds subsequently, and adding neopelex dressing agent mixes as reaction solution;
(3) the FTO glass after step (1) annealing is placed the agitated reactor that fills step (2) reaction solution, utilize hydro thermal method under 120 ℃ of temperature, to react and prepared spongy CdS quantum dot thin layer in 2～11 hours;
(4) take out the light anode prepare and the spongy CdS film that obtains carried out annealing in process;
The spongy anode material that (5) will obtain immerses the N3 dyestuff and soaked 1～2 hour, with sarin Surlyn heat sealing film be made into the frame shape structure of definite shape and be clipped in work electrode and the Pt electrode between, after the heating with cell package together;
(6) electrolyte after under vacuum action, pouring into, utilizes sarin Surlyn heat sealing film with it sealing through the aperture of Pt electrode reservation equally, makes spongy quantum dot solar cell.
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| CN102543465B (en) * | 2011-12-15 | 2014-04-30 | 天津大学 | CdS single crystal nanowire solar battery and preparation method of the same |
| CN103094539B (en) * | 2012-11-28 | 2014-12-03 | 上海大学 | Preparation method of tin dioxide quantum dot graphene sheet composite |
| CN103730536B (en) * | 2013-12-25 | 2016-09-14 | 南昌航空大学 | The preparation of a kind of rare-earth sulfide quantum dot solar cell and application thereof |
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