CN107785173A - It is a kind of be applied to low light condition under quantum dot sensitized solar cell to electrode material and preparation method thereof - Google Patents

It is a kind of be applied to low light condition under quantum dot sensitized solar cell to electrode material and preparation method thereof Download PDF

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Publication number
CN107785173A
CN107785173A CN201610769647.XA CN201610769647A CN107785173A CN 107785173 A CN107785173 A CN 107785173A CN 201610769647 A CN201610769647 A CN 201610769647A CN 107785173 A CN107785173 A CN 107785173A
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rgo
mos
quantum dot
electrode
solar cell
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历凤燕
甄苗苗
金占斌
赖培冬
许林
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Northeastern University China
Northeast Normal University
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Northeast Normal University
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
    • H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
    • H01G9/20—Light-sensitive devices
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
    • H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
    • H01G9/004—Details
    • H01G9/04—Electrodes or formation of dielectric layers thereon
    • H01G9/042—Electrodes or formation of dielectric layers thereon characterised by the material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
    • H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
    • H01G9/20—Light-sensitive devices
    • H01G9/2022—Light-sensitive devices characterized by he counter electrode
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • 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

Abstract

The present invention provide it is a kind of be applied to low light condition under quantum dot sensitized solar cell to electrode material and preparation method thereof.To electrode by conductive substrates and Mo2S/RGO films form.Preparation process is as follows：Sodium molybdate, thiocarbamide and graphite oxide are dissolved in distilled water, then mixed solution is transferred in water heating kettle and reacted.After reaction terminates, product is centrifuged, washed, drying, and obtains MoS2/RGO.By MoS obtained above2/ RGO is deposited on paired electrode processed in conductive substrates.MoS provided by the invention2/ RGO is simple to electrode material preparation method, has higher stability and catalytic performance, and be easy to the encapsulation of battery.Using MoS2/ RGO has very high photoelectric transformation efficiency to the quantum dot sensitized solar cell of electrode assembling under low light condition, in 25mW/cm2Light intensity under up to 6.23%, used suitable for cloudy day, haze sky and low Rizhao Area.

Description

It is a kind of be applied to low light condition under quantum dot sensitized solar cell to electrode material And preparation method thereof
Technical field
The invention belongs to technical field of solar batteries, is related to a kind of suitable for quantum dot sensitized solar energy under low light condition Battery to electrode material and preparation method thereof.
Background technology
Solar energy is that the ideal for the environment and energy problem for solving facing mankind is new as a kind of pure regenerative resource The energy.1991, MichaelProfessor etc. is in research and development DSSC (Dye-Sensitized Solar Cells, are abbreviated as DSSCs) aspect achieve breakthrough [1].But for DSSCs, however it remains dyestuff Cost is high, and titanium dioxide easily makes dyestuff photodissociation, and dyestuff spectral region is relatively narrow, and Dye Adsorption rate improves a series of restrictions such as difficulty Factor.Recent studies have indicated that the inorganic semiconductor material of narrow band gap can replace dyestuff as sensitizer, if by these material controls System is in the range of quantum effect, then as quantum dot sensitizer.Quanta point material compared with conventional dyes, have it is cheap, Many advantages, such as absorption region is broad and relatively stable.The highest theoretical cell effect of quantum dot sensitized solar cell (QDSSCs) Rate can reach 66%, and this breaches the energy conversion limit (31%) of existing solar cell, it has also become before receiving much attention Along field.
Effect to electrode is to collect the redox reaction in electronics and catalytic electrolysis matter, and this is required to electrode material Existing good electric conductivity has catalytic action again.Noble metal such as Pt, Au, Ag etc. can serve as to electrode material.More vulcanizations Thing electrolyte is the most frequently used electrolyte of sulfide quantum dots sensitization solar battery.However, Pt is to electricity in more sulphur electrolyte The charge transfer resistance on pole surface is larger, and the electric charge transfer speed of electro-catalysis reduction result in larger overpotential slowly so that Pt It is relatively low to catalytic activity of the electrode in quantum dot sensitized solar cell.In addition, the S in more sulphur electrolyte2- be easily absorbing Surface to Pt to electrode, makes Pt be poisoned, and reduces its catalytic activity.Therefore, non-Pt efficient, stably, cheap is developed It is one of key issue for lifting quantum dot sensitization solar battery efficiency to electrode material.
In recent years, researcher has carried out extensive work to find the alternative materials of Pt electrodes, and research finds that metal vulcanizes Thing (CuS, Cu2S, CoS, PbS etc.) as quantum dot sensitized solar cell there is excellent catalytic effect to electrode, wherein Cu2S is the most prominent to the performance of electrode.But Cu2S is prepared to the method for electrode generally use copper corrosion, prepared by this method Cu2The shortcomings of S existence and stabilities are poor, easily come off, are not easy to encapsulate, and copper sheet substrate is easily by more sulphur electrolyte corrosions, and quantum Point sensitization solar battery descends by force photoelectric transformation efficiency relatively low in dim light, can not be used in cloudy day, haze sky and low Rizhao Area. Therefore, in the technical field, urgent need develop it is a kind of there is good electric conductivity and catalytic performance, and inexpensively, stably, easily encapsulate And suitable under low light condition to electrode material.
The content of the invention
It is an object of the invention to overcome present in prior art it is poor to electrode stability, be not easy to encapsulate, copper sheet substrate A kind of easily by more sulphur electrolyte corrosions the problems such as, there is provided Mo for quantum dot sensitized solar cell2S/RGO to electrode and its Preparation method.Mo2The faster charge transport properties of catalytic performance and RGO excellent S, can effectively reduce the quantum dot sensitized sun The interface impedance of energy battery, improves its photoelectric transformation efficiency.The method have the characteristics that with this quantum dot to electrode assembling Sensitization solar battery has very high photoelectric transformation efficiency under low light condition, suitable for cloudy day, haze sky and low sunshine Area uses.
Technical scheme is used by the present invention solves the technical problem：The quantum dot sensitized sun under a kind of low light condition The preparation method of energy counter electrode of battery, comprises the following steps：
MoS2/ RGO is prepared by hydro-thermal method：By 1mmol Na2MoO4·2H2O and 5mmol thiocarbamides are dissolved in 60mL distilled water, 0.01 graphite oxide is added into the solution.Then mixed solution is transferred in 100mL water heating kettles, in 210 DEG C of temperature strip 24h is reacted under part.Black precipitate is obtained, is cooled to room temperature, is centrifuged, distillation water washing 3 times, is placed in 80 DEG C of baking ovens and dries 12h, obtain the MoS that average-size is 0.6 μm2/ RGO microballoons；
By 0.25g MoS2/ RGO and 0.06g polyethylene glycol is dissolved in 0.5mL ethanol, ultrasonic 30min, is prepared into slurry Material；
Above-mentioned slurry is uniformly coated in conductive substrates using blade coating, spin coating or the method for silk-screen printing, Ran Houjing 30min is heat-treated under 400 DEG C of argon gas atmospheres, it is thin to electrode to form the quantum dot sensitized solar cell that thickness is 10~20 μm Film；
Conductive substrates of the present invention are indium oxide (ITO) glass mixed F tin ash (FTO) or mix Sn.
Compared with prior art, it is used to replace MoS of the tradition to electrode the invention provides a kind of2/ RGO is to electrode material And preparation method, advantage of the invention is that：
1) with traditional Pt to electrode and Cu2S compares to electrode, MoS2/ RGO is shown to electrode in more sulphur electrolyte More excellent catalytic performance.The faster charge transport properties of RGO, the interface of quantum dot sensitized solar cell can be effectively reduced Impedance, improve its photoelectric transformation efficiency.
2) Cu prepared with copper corrosion method2S compares to electrode, MoS prepared by the present invention2/ RGO is to electrode in more sulphur electricity Xie Zhizhong has higher stability, and is easy to the encapsulation of battery.
3) MoS is used2/ RGO has very high light to the quantum dot sensitized solar cell of electrode assembling under low light condition Photoelectric transformation efficiency, used suitable for cloudy day, haze sky and low Rizhao Area.
Brief description of the drawings
Fig. 1 is MoS2The ESEM (a, b) and transmission electron microscope picture (c, d) of/RGO microballoons.
Fig. 2 is MoS2Cross-sectional scans electron microscopes (a) and EDX energy spectrum diagram (b) of/the RGO to electrode.
Fig. 3 is MoS2The X-ray powder diffraction figure of/RGO microballoons.
Fig. 4 is MoS2The x-ray photoelectron energy spectrum diagram of/RGO microballoons.
Fig. 5 is the MoS using the present invention2The quantum dot sensitized solar cell that/RGO forms to electrode is in different light intensity bars Photoelectric current-photovoltage curve under part.
Embodiment
In order to further illustrate the present invention, following embodiment is enumerated, but it is not intended to limit each accessory claim and determined The invention scope of justice.
Specific embodiment 1：
(1) MoS is prepared2/ RGO is to electrode
1) substrate is cleaned
FTO electro-conductive glass substrate is first cleaned with washing powder, dried up, is then immersed in the isopropanol heat containing KOH 12h in saturated solution, removes the dust and grease of FTO substrate surfaces, then uses deionized water respectively, acetone, each ultrasound of ethanol 15min, finally dry up standby.
2)MoS2The preparation of/RGO composites
By 1mmol Na2MoO4·2H2O and 5mmol thiocarbamides are dissolved in 60mL distilled water, and 0.01g oxidations are added into the solution Graphite.Then mixed solution is transferred in 100mL water heating kettles, reacts 24h under 210 DEG C of temperature conditionss.Black is obtained to sink Form sediment, be cooled to room temperature, centrifuge, distillation water washing 3 times, be placed in 80 DEG C of baking ovens and dry 12h.
3)MoS2Preparations of/the RGO to electrode slurry
By 0.25g MoS2/ RGO and 0.06g polyethylene glycol is dissolved in 0.5mL ethanol, ultrasonic 30min, after being uniformly dispersed Obtain slurry.
4) MoS is prepared using knife coating2/ RGO is to electrode
Area and film thickness are scratched in the FTO controls cleaned with 3M glue, then slurry is added dropwise on FTO, it is light with knife One layer gently is scraped, obtained membrane electrode is calcined into 30min at 400 DEG C, to increase the attachment degree of film.
(2) the tubulose TiO of CdS quantum dot sensitization is prepared2Light anode (TiO2/CdS)
1) hydro-thermal method prepares TiO2Nanotube
0.6mL isopropyl titanates (TTIP) are added in 30mL 5M HCl (37%) solution, stir 5min, Ran Houzhuan Move on in 50mL reactor, by 2 × 2cm2FTO is tilted and is put into, 150 DEG C of reaction 14h.It is natural with deionized water rinsing after taking-up Dry；In the HCl that the slice, thin piece that upper step obtains is invaded to 30mL 6.67M, 150 DEG C of reaction 7h, sample uses deionized water after taking out Rinse, 450 DEG C of calcining 30min.
2) deposition of CdS quantum dot
The method (SILAR) deposited using continuous ionic layer：Configure 0.5M Cd (NO3)2Ethanol solution, and 0.5M Na2S first alcohol and water (1:1) solution；First by TiO2Nano-tube array membrane sample immerses Cd (NO3)2Solution 2min, taking-up ethanol Rinse, treat that sample dries, then sample is immersed into Na2S solution 2min, take out with corresponding solvent washing and dry.It is repeatedly above-mentioned Process, circulate five times, the TiO of deposition CdS quantum dot is prepared2Film of Nano tube array, 300 DEG C of calcining 30min.
3) ZnS is passivated
Its method synsedimentary CdS, simply solution change 0.1M Zn (NO into3)2The aqueous solution and 0.1M Na2S first alcohol and water (1: 1) solution, frequency of depositing are 3 times.
(3) assembling quantum dot sensitization solar battery and test
By ZnS/CdS/TiO2Light anode and MoS2/ RGO is put well to electrodes face, is then fixed both sides with clip, is used Sealing compound seals bottom, electrolyte solution is injected at top end opening, electrolyte solution composition is 0.5M Na2S、0.125M S and 0.2M KC1 mixed solution, solvent are 3 by volume ratio:7 methanol and deionized water composition.Finally with glue stick by top Aperture seals the preparation that can complete quantum dot sensitization solar battery.The battery assembled is in 100mW/cm2(AM's 1.5) Electric current-voltage curve is tested under simulated solar irradiation.
Specific embodiment 2：
(1) MoS is prepared2/ RGO is to electrode
With embodiment 1.
(2) TiO of the tubulose of CdS quantum dot sensitization is prepared2Light anode (TiO2/CdS)
With embodiment 1.
(3) assembling quantum dot sensitization solar battery and test
By ZnS/CdS/TiO2Light anode and MoS2/ RGO is put well to electrodes face, is then fixed both sides with clip, is used Sealing compound seals bottom, electrolyte solution is injected at top end opening, electrolyte solution composition is 0.5M Na2S、0.125M S and 0.2M KC1 mixed solution, solvent are 3 by volume ratio:7 methanol and deionized water composition.Finally with glue stick by top Aperture seals the preparation that can complete quantum dot sensitization solar battery.The battery assembled is in 50mW/cm2The mould of (AM 1.5) Intend testing electric current-voltage curve under sunshine.
Specific embodiment 3：
(1) MoS is prepared2/ RGO is to electrode
With embodiment 1.
(2) TiO of the tubulose of CdS quantum dot sensitization is prepared2Light anode (TiO2/CdS)
With embodiment 1.
(3) assembling quantum dot sensitization solar battery and test
By ZnS/CdS/TiO2Light anode and MoS2/ RGO is put well to electrodes face, is then fixed both sides with clip, is used Sealing compound seals bottom, electrolyte solution is injected at top end opening, electrolyte solution composition is 0.5M Na2S、0.125M S and 0.2M KC1 mixed solution, solvent are 3 by volume ratio:7 methanol and deionized water composition.Finally with glue stick by top Aperture seals the preparation that can complete quantum dot sensitization solar battery.The battery assembled is in 25mW/cm2The mould of (AM 1.5) Intend testing electric current-voltage curve under sunshine.
Fig. 1 is MoS2The ESEM (a, b) and transmission electron microscope picture (c, d) of/RGO microballoons.As can be seen from the figure MoS2For Closelypacked petal microballoon, is carried on stratiform RGO.MoS2The average-size of/RGO microballoons is 600nm.From high-resolution 0.62nm spacing of lattice is can see in transmission electron microscope picture, corresponding to hexagonal crystal system MoS2(002) crystal face.
Fig. 2 is MoS2Cross-sectional scans electron microscopes (a) and EDX energy spectrum diagram (b) of/the RGO to electrode.Wherein cross-sectional scans Electronic Speculum The bright lower thickness that suggested the formation of to electrode of chart is 14.6 μm of MoS2/ RGO is to electrode film.EDX energy spectrum diagrams are demonstrated right In electrode film, Mo, S, C, and the presence of tetra- kinds of elements of O.
Fig. 3 is MoS2The X-ray powder diffraction figure of/RGO microballoons.Characteristic peak in 2 θ=33 and 58 ° of positions corresponds to MoS2Six (100) and (110) crystal face of prismatic crystal phase.Because the content of graphene is seldom and its diffraction is very weak, so not seeing C in spectrogram Characteristic diffraction peak.
Fig. 4 is MoS2The x-ray photoelectron energy spectrum diagram of/RGO microballoons.As illustrated, Mo, S, C, and O in sample be present Characteristic peak, show MoS2The presence of each element in/RGO composites.In high-resolution XPS spectrum figure, Mo3d5/2 and Mo 3d3/2 combination can respectively appear in 228.2 and 231.4eV, and this is exactly MoS2Middle Mo4+Characteristic peaks.In addition, C1s XPS Spectrogram shows 284.6,285.9 and 288.5eV absworption peak, corresponds to sp respectively2The carbon of hydridization and and the combination of carbon that is connected of oxygen Can, such as OH- and COOH-.
Fig. 5 is the MoS using the present invention2Quantum dot sensitized solar cell photoelectric stream-photoelectricity that/RGO forms to electrode Buckle line.When light intensity is 100mW/cm2And 50mW/cm2When, open-circuit voltage is respectively 0.84,0.82V, and short circuit current is respectively 7.79 7.27mA/cm2, conversion efficiency is respectively 2.21 and 4.32%.When light intensity is reduced to 25mW/cm2When, conversion efficiency is up to 6.23% (as shown in Table 1).
Table one：By MoS2Photoelectricity of the quantum dot sensitized solar cell that/RGO forms to electrode under different light-intensity conditions Performance parameter
MoS2/RGO Jsc(mAcm-2) Voc(V) FF PCE (%)
25mW/cm2 5.77 0.75 0.36 6.23
50mW/cm2 7.27 0.82 0.36 4.32
100mW/cm2 7.79 0.84 0.34 2.21

Claims (5)

  1. It is used for quantum dot sensitized solar cell under low light condition 1. a kind of electrode material and preparation method thereof, its feature existed In comprising the following steps：
    1)MoS2/ RGO is prepared by hydro-thermal method：By 1mmol Na2MoO4·2H2O and 5mmol thiocarbamides are dissolved in 60mL distilled water, to 0.01 graphite oxide is added in the solution；Then mixed solution is transferred in 100mL water heating kettles, in 210 DEG C of temperature conditionss Lower reaction 24h；Black precipitate is obtained, is cooled to room temperature, is centrifuged, distillation water washing 3 times, is placed in 80 DEG C of baking ovens and dries 12h, obtain the MoS that average-size is 0.6 μm2/ RGO microballoons；
    2) by 0.25g MoS2/ RGO and 0.06g polyethylene glycol is dissolved in 0.5mL ethanol, ultrasonic 30min, is prepared into slurry；
    3) above-mentioned slurry is uniformly coated in conductive substrates using blade coating, spin coating or the method for silk-screen printing, then through 400 30min is heat-treated under DEG C argon gas atmosphere, forms quantum dot sensitized solar cell that thickness is 10~20 μm to electrode film.
  2. 2. preparation method according to claim 1, it is characterised in that：Described conductive substrates are to mix F tin ash (FTO) or Sn indium oxide (ITO) glass is mixed.
  3. 3. preparation method according to claim 1, it is characterised in that：Mo in the step 16+Source can be Na2MoO4· 2H2O or (NH4)6Mo7O24·4H2O, S2-Source can be thiocarbamide or Na2S。
  4. A kind of 4. MoS for being used for quantum dot sensitized solar cell as claimed in claim 12Applications of/the RGO to electrode, it is special Sign is：MoS2/ RGO is to electrode and the tubulose TiO of CdS quantum dot sensitization2Light anode, more sulphur electrolyte composition are quantum dot sensitized Solar cell.
  5. A kind of 5. low light condition as claimed in claim 1, it is characterised in that：Light intensity<100mW/cm2。
CN201610769647.XA 2016-08-30 2016-08-30 It is a kind of be applied to low light condition under quantum dot sensitized solar cell to electrode material and preparation method thereof Pending CN107785173A (en)

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Application publication date: 20180309