CN107302057A - Planar structure hybrid solar cell based on antimonous sulfide dense film - Google Patents
Planar structure hybrid solar cell based on antimonous sulfide dense film Download PDFInfo
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Abstract
The invention discloses a kind of planar structure hybrid solar cell based on antimonous sulfide dense film, belong to thin-film material and devices field.The solar cell includes substrate, electron transfer layer, light absorbing layer, hole transmission layer and the metal electrode of electrically conducting transparent, and the light absorbing layer is to use ratio to be 1:1.5 ~ 2.5 SbCl3With thiocarbamide as presoma, densification Sb is prepared by spin coating2S3Film, thickness range is 360 nanometers to 1 micron.The present invention is using fine and close Sb2S3Film is that light absorbing layer constitutes planar structure hybrid solar cell, and with low cost, technique is simple for its, be easy to large area production, relative to meso-hole structure solar cell, based on Sb2S3The planar structure solar cell repeatability of dense film is strong, and the efficiency of battery is more easy to be improved.
Description
Technical field
The invention belongs to thin-film material and devices field, and in particular to a kind of plane based on antimonous sulfide dense film
Structure hybridization solar cell.
Background technology
With the very fast development continually developed with thin-film solar cells of new material, Australian horse in 2002
Fourth professor Green proposes the following material for turning into preferable solar cell and should had the special feature that：Direct band gap is in 1.1-
Between 1.7 eV, with sunshine Spectral matching；Material non-toxic, meets environmental requirement；The constituent content of constituent material enriches, valency
Lattice are cheap；Film preparing technology is easily-controllable and can realize that large area is manufactured；Good electricity conversion and high stability.
But at present, the inorganic material being seen in report hybrid solar cell has toxicity mostly, and
Earth's crust content is also very limited, even if Toxic in high photoelectric transformation efficiency, but the source of raw material and preparation process can be obtained
Pollution of the discharge of matter to environment, is still to limit its wide variety of maximum bottleneck, thus some there is photovoltaic performance, it is relative
Nontoxic, environmentally friendly inorganic compound material causes the interest of researchers.
The A races metal sulfides (A2B3, A=Bi, Sb and B=S, Se) of VA- VI enter people as important semi-conducting material
The visual field.Wherein, antimony trisulfide (Sb2S3) because its superior photoelectric properties is as novel solar battery active layer material.
Sb2S3It is a kind of Binary compound semiconductor with layer structure linked together with (Sb4S6) n octahedrons, with good
Optical property, visible region optical absorption coefficient be more than 5 × 104 cm-1, simultaneously as quantum limitation effect, it is prohibited
Bandwidth is adjustable between 1.7-2.2ev, and material hypotoxicity in itself and rich content are also one kind that it makees battery-active layer
Advantage.
But traditional chemical bath deposition process（CBD）The Sb of preparation2S3Film causes film to exist because there is the introducing of water
The oxide of some antimony, these oxides can cause the generation of defect in film, cause the compound of carrier, reduction battery effect
Rate.And vacuum deposition method prepares Sb2S3Film requires high to experimental facilities, and preparation time is long.
The content of the invention
It is an object of the invention to for above-mentioned Sb2S3The present situation of thin-film solar cells, is based on the invention provides one kind
The planar structure hybrid solar cell of antimonous sulfide dense film.Sb is prepared using spin-coating method2S3Dense film, was prepared
Journey does not have the introducing of water, greatly reduces the presence of the oxide of antimony.On this basis, with Sb2S3Film does light absorbing layer preparation
The organic inorganic hybridization solar cell of planar structure.
To achieve the above object, the present invention is adopted the following technical scheme that：
A kind of planar structure hybrid solar cell based on antimonous sulfide dense film, including oxidic transparent conductive liner
Bottom, electron transfer layer, light absorbing layer, hole transmission layer and metal electrode, the light absorbing layer are the Sb prepared with spin-coating method2S3
Dense film, the thickness of light absorbing layer is 360 nanometers to 1 micron.
The oxidic transparent conductive substrates are FTO, ITO or AZO electro-conductive glass.
The electron transfer layer is smooth TiO2Film.
The hole transmission layer is P3HT films.
The metal electrode is Al or Ag.
The preparation method of the planar structure hybrid solar cell based on antimonous sulfide as described above, specifically include with
Lower step：
（1）Cleaning oxidic transparent conductive substrates are simultaneously dried；
（2）The preparation of electron transfer layer：With sol-gel method, whirlpool applies TiO in transparent conductive substrate2Solution；Then TiO2Thoroughly
Bright film is calcined in Muffle furnace high temperature, and calcining heat is 550 DEG C, and calcination time is 60min；
（3）The preparation of light absorbing layer：Under Ar compression rings border, by the Sb prepared2S3Precursor solution whirlpool is applied on the electron transport layer,
Then in thermal station heating make solution react generation Sb2S3；Whirlpool is repeated to apply with heating response step to adjust generation
Sb2S3Film thickness；Temperature is raised again to be made annealing treatment, and makes Sb2S3Thin film crystallization；
（4）The preparation of hole transmission layer：On light absorbing layer surface, whirlpool applies P3HT；
（5）The preparation of electrode：In hole transport layer surface evaporation metal electrode.
Step（3）It is middle to prepare Sb with spin coating method2S3The technological parameter of film is：
Sb2S3Precursor solution：Prepare SbCl3With thiocarbamide as precursor solution, Sb and S mol ratio are 1:1.5~2.5；
Whirlpool is applied：750 revs/min of forward rotating speed, the time is 12s；After walk around speed 3000 revs/min, the time is 60s；
Heating-up temperature：140℃；
Reaction time：10min；
Annealing：Annealing temperature is 340 DEG C, annealing time 15min.
The beneficial effects of the present invention are：
（1）The Sb that the present invention is prepared using spin-coating method2S3Crystalline property is good, miscellaneous few；With Sb2S3Film is light absorbing layer
Short circuit current flow, fill factor, curve factor and the energy conversion efficiency of the hybrid solar cell battery of planar structure have good performance；
（2）The present invention is using fine and close Sb2S3Film is that light absorbing layer constitutes planar structure hybrid solar cell, and its cost is low
Honest and clean, technique is simple, be easy to large area production, relative to meso-hole structure solar cell, based on Sb2S3The planar structure of dense film
Solar cell repeatability is strong, and the efficiency of battery is more easy to be improved.
Brief description of the drawings
Fig. 1 is with Sb2S3Film as light absorbing layer planar structure hybrid solar cell structural representation；1- aluminium electricity
Pole (or silver electrode), 2-P3HT films, 3-Sb2S3Film, 4-TiO2Transparent membrane, 5-FTO electro-conductive glass；
Fig. 2 is Sb2S3Film XRD, and by it and Sb2S3Standard comparison card JP42-1393 is compared；
Fig. 3 is Sb2S3Film energy gap；
Fig. 4 is with the nm of thickness 360 Sb2S3Film is that the hybrid solar cell J-V of planar structure prepared by light absorbing layer is bent
Line；
Fig. 5 is with the nm of thickness 580 Sb2S3Film is that the hybrid solar cell J-V of planar structure prepared by light absorbing layer is bent
Line；
Fig. 6 is the Sb with 1 μm of thickness2S3Film is that the hybrid solar cell J-V of planar structure prepared by light absorbing layer is bent
Line；
Fig. 7 is Sb:S is 1:1.5 Sb2S3Film is that the hybrid solar cell J-V of planar structure prepared by light absorbing layer is bent
Line；
Fig. 8 is Sb:S is 1:2.2 Sb2S3Film is that the hybrid solar cell J-V of planar structure prepared by light absorbing layer is bent
Line；
Fig. 9 is Sb:S is 1:2.5 Sb2S3Film is that the hybrid solar cell J-V of planar structure prepared by light absorbing layer is bent
Line.
Embodiment
The present invention is with Sb2S3Film can use following step system for the hybrid solar cell of the planar structure of light absorbing layer
It is standby：
The preparation of 1 precursor solution
（1）Take 1.37g SbCl3, N-N dimethylformamides are then added dropwise；
（2）To step（1）In solution stirring at normal temperature 30 minutes；
（3）30 minutes thiocarbamides to add 0.675g ~ 1.125g in backward solution of stirring, stirring at normal temperature 30 minutes.
2 substrate processings
The substrate used in experiment is electro-conductive glass（ITO electro-conductive glass or transparent flexible plastic, FTO electro-conductive glass or transparent soft
Property plastics, AZO electro-conductive glass or transparent flexible plastic, are commercially available prod or known technology）, substrate should be entered first before the test
Row cleaning.Electro-conductive glass piece is cut into suitable shape size, cleaned up with cleaning agent, then running water is rinsed, and is gone
Ionized water is rinsed, then place it in ultrasonic cleaner successively with deionized water, ethanol, acetone, acetone and
Ethanol is respectively cleaned by ultrasonic 15 minutes, and last baking box drying can obtain the substrate of clean surface.
Film whirlpool applies technical process
（1）The Conducting Glass for scribbling electron transfer layer is positioned on glue evenning table, suction piece is evacuated with mechanical pump；
（2）Glue evenning table parameter is set to：750 revs/min of forward rotating speed, the time is 12s, after walk around speed 3000 revs/min,
Time is 60s；
（3）Take appropriate Sb2S3Precursor solution is dripped on substrate, and opening whirlpool applies button；
（4）The Sb that whirlpool is coated2S3Film is placed on 140 DEG C of heating 10min in thermal station, the aobvious red of reacted film；
（5）After print cooling, pass through repeat step（3）（4）Obtain 360 nanometers to 1 micron of Sb2S3Film；
（6）Then in inert gas（Ar gas）Under, the print prepared is subjected to annealing 15min at 340 DEG C；
（7）After the completion of, remove sample from thermal station.
It is prepared by solar cell
（1）The preparation of electron transfer layer：Conducting Glass is positioned on glue evenning table, suction piece is evacuated with mechanical pump, is taken appropriate
TiO2Precursor solution is dripped on substrate, the TiO that whirlpool is coated2Film places 550 DEG C of calcining 60min in Muffle furnace；
（2）The preparation of light absorbing layer：As described in 3；
（3）The preparation of hole transmission layer：Sol evenning machine spin coating P3HT is used on light absorbing layer.
（4）The preparation of electrode：Evaporated metal aluminium or silver on P3HT.
Material and device performance test
In order to verify the Sb of preparation2S3The characteristic of film thing phase, we utilize X-ray diffractometer（XRD）Crystal orientation survey is carried out to him
Examination.
In order to evaluate Sb2S3Film as the hybrid solar cell of the planar structure of light absorbing layer photovoltaic property, we
The test of J-V curves has been carried out to it using Keithley SMU testers.
The present invention is further described with reference to test result, the description is intended merely to better illustrate with spin coating legal system
Standby Sb2S3Film as the hybrid solar cell of the planar structure of light absorbing layer feasibility.The present invention is not limited to here
Described particular example and embodiment.Any those of skill in the art are easy to do not departing from spirit of the invention and model
It is further improved in the case of enclosing and perfect, both falls within protection scope of the present invention.
Sb2S3Film characterization and performance test：
Test one：
（1）Clean sheet glass：First glass slide is put into and fills cleaning agent（Such as found person who is not a member of any political party's liquid detergent）Solution in soak
10 minutes, clear water was rinsed after then cleaning repeatedly；Then it is processed by shot blasting with polishing powder；Then be respectively put into equipped with go from
It is ultrasonic 15 minutes respectively in Zi Shui, an acetone and an alcohol vessel；It is finally putting into 100 degree of drying in baking oven；
（2）Prepare Sb2S3Film：Take 1.37g SbCl3With 0.9g thiocarbamides（Sb:S is 1:2）Sb2S3Precursor solution whirlpool is applied to
In substrate of glass, condition of work is：750 revs/min of forward rotating speed, the time is 12s, after walk around 3000 revs/min of speed, the time is
60s；The Sb that whirlpool is coated2S3Film heats 10min in thermal station at 140 DEG C, then 340 DEG C of annealings under Ar compression rings border
15min；
（3）Film is tested using X-ray diffractometer, material XRD illustrates as shown in Figure 2：Entered using JP42-1393
Row is compared, and characteristic peak can be matched substantially, and miscellaneous characteristic peak is seldom, illustrates that the crystallinity of material is higher, impurity content
It is few.
Test two：
（1）Clean glass：With test one；
（2）Prepare Sb2S3Film：With test one；
（3）The optical absorptive character explanation of film is as shown in Figure 3：Energy gap is 1.72eV, it was demonstrated that the film of preparation is met
Requirement of the battery to optical property.
Embodiment 1：
（1）Clean FTO sheet glass：First glass slide is put into and fills cleaning agent（Such as found person who is not a member of any political party's liquid detergent）Solution in soak
Bubble 10 minutes, clear water is rinsed after then cleaning repeatedly；Then it is processed by shot blasting with polishing powder；Then it is respectively put into be equipped with and goes
It is ultrasonic 15 minutes respectively in the vessel of ionized water, an acetone and an alcohol；100 degree of drying are finally putting into baking oven to eliminate
Stress；
（2）The preparation of electron transfer layer：By TiO2Precursor solution whirlpool is applied in FTO substrate of glass, 750 revs/min of forward rotating speed
Clock, the time is 12s, after walk around speed 4000 revs/min, the time is 30s；The TiO that whirlpool is coated2Film is 550 DEG C in Muffle furnace
Lower calcining 60min；
（3）The preparation of light absorbing layer：Take 1.37g SbCl3With 0.9g thiocarbamides（Sb:S is 1:2）Sb2S3Precursor solution, whirlpool is applied
In in electro-conductive glass substrate, condition of work is：750 revs/min of forward rotating speed, the time is 12s, after walk around speed 3000 revs/min,
Time is 60s；The Sb that whirlpool is coated2S3Film heats 10min in thermal station at 140 DEG C, then under Ar compression rings border 340 DEG C move back
Fire processing 15min, Sb2S3Thickness is 360 nm；
（4）It is prepared by hole transmission layer：Claim P3HT 15 milligrams with electronic balance, instill 1.0 milliliters of chlorobenzene；Then it has been placed on temperature
On the magnetic stirring apparatus for spending control, 30 DEG C are stirred 24 hours, and sol evenning machine spin coating P3HT is used on light absorbing layer, and condition of work is：
600 revs/min of forward rotating speed, the time is 9s, after walk around speed 1500 revs/min, the time is 30s；
（5）The preparation of electrode：The evaporated metal aluminium on P3HT.
Battery performance illustrates as shown in Figure 4：Open-circuit voltage is：0.336V, the short circuit current flow of battery is：2.03mA/
cm2, fill factor, curve factor is：28.5%, energy conversion efficiency is：0.12%.
Embodiment 2：
（1）Clean FTO sheet glass：Be the same as Example 1；
（2）The preparation of electron transfer layer：Be the same as Example 1；
（3）The preparation of light absorbing layer：Take 1.37g SbCl3With 0.9g thiocarbamides（Sb:S is 1:2）Sb2S3Precursor solution, whirlpool is applied
In in electro-conductive glass substrate, condition of work is：750 revs/min of forward rotating speed, the time is 12s, after walk around speed 3000 revs/min,
Time is 60s；The Sb that whirlpool is coated2S3Film heats 10min in thermal station at 140 DEG C；Whirlpool is repeated to apply and heating response step,
In Sb2S3Whirlpool applies one layer of Sb again on film2S3Film, then under Ar compression rings border 340 DEG C annealing 15min, Sb2S3Thickness is
580 nm；
（4）It is prepared by hole transmission layer：Be the same as Example 1；
（5）The preparation of electrode：Be the same as Example 1.
Battery performance explanation is as shown in Figure 5：Open-circuit voltage is：0.44 V, the short circuit current flow of battery is：7.3 mA/cm2,
Fill factor, curve factor is：36.1%, energy conversion efficiency is：1.16%.
Embodiment 3：
（1）Clean FTO sheet glass：Be the same as Example 1；
（2）The preparation of electron transfer layer：Be the same as Example 1；
（3）The preparation of light absorbing layer：Take 1.37g SbCl3With 0.9g thiocarbamides（Sb:S is 1:2）Sb2S3Precursor solution, is applied to
In electro-conductive glass substrate, condition of work is：750 revs/min of forward rotating speed, the time is 12s, after walk around speed 3000 revs/min, when
Between be 60s；The Sb that whirlpool is coated2S3Film heats 10min in thermal station at 140 DEG C；Whirlpool is repeated two more times to apply and heating response step
Suddenly, then under Ar compression rings border 340 DEG C annealing 15min, Sb2S3Thickness is 1 μm；
（4）It is prepared by hole transmission layer：Be the same as Example 1；
（5）The preparation of electrode：Be the same as Example 1.
Battery performance explanation is as shown in Figure 6：Open-circuit voltage is：0.42V, the short circuit current flow of battery is：4.6mA/cm2, fill out
Filling the factor is：34.9%, energy conversion efficiency is：0.68%.
Embodiment 4：
（1）Clean FTO sheet glass：Be the same as Example 1；
（2）The preparation of electron transfer layer：Be the same as Example 1；
（3）The preparation of light absorbing layer：Take 1.37g SbCl3With 0.675g thiocarbamides（Sb:S is 1:1.5）Sb2S3Precursor solution
Whirlpool is applied in electro-conductive glass substrate, and condition of work is：750 revs/min of forward rotating speed, the time is 12s, after walk around speed 3000 turns/
Minute, the time is 60s；The Sb that whirlpool is coated2S3Film heats 10min in thermal station at 140 DEG C；Whirlpool is repeated twice to apply and heating
Reactions steps, whirlpool applies two layers of Sb2S3Film, then under Ar compression rings border 340 DEG C annealing 15min；
（4）It is prepared by hole transmission layer：Be the same as Example 1；
（5）The preparation of electrode：Be the same as Example 1.
Battery performance explanation is as shown in Figure 7：Open-circuit voltage is：0.41V, the short circuit current flow of battery is：5.6mA/cm2, fill out
Filling the factor is：39.2%, energy conversion efficiency is：0.9%.
Embodiment 5：
（1）Clean FTO sheet glass：Be the same as Example 1；
（2）The preparation of electron transfer layer：Be the same as Example 1；
（3）The preparation of light absorbing layer：Take 1.37g SbCl3With 0.99g thiocarbamides（Sb:S is 1:2.2）Sb2S3Precursor solution whirlpool
It is applied in electro-conductive glass substrate, condition of work is：750 revs/min of forward rotating speed, the time is 12s, after walk around speed 3000 revs/min
Clock, the time is 60s；The Sb that whirlpool is coated2S3Film heats 10min in thermal station at 140 DEG C；It is repeated twice whirlpool and applies anti-with heating
Step is answered, whirlpool applies two layers of Sb2S3Film, then under Ar compression rings border 340 DEG C annealing 15min；
（4）It is prepared by hole transmission layer：Be the same as Example 1；
（5）The preparation of electrode：Be the same as Example 1.
Battery performance explanation is as shown in Figure 8：Open-circuit voltage is：0.44V, the short circuit current flow of battery is：7.3mA/cm2, fill out
Filling the factor is：36.1%, energy conversion efficiency is：1.16%.
Embodiment 6：
（1）Clean FTO sheet glass：Be the same as Example 1；
（2）The preparation of electron transfer layer：Be the same as Example 1；
（3）The preparation of light absorbing layer：Take 1.37g SbCl3With 1.125g thiocarbamides（Sb:S is 1:2.5）Sb2S3Precursor solution
Whirlpool is applied in electro-conductive glass substrate, and condition of work is：750 revs/min of forward rotating speed, the time is 12s, after walk around speed 3000 turns/
Minute, the time is 60s；The Sb that whirlpool is coated2S3Film heats 10min in thermal station at 140 DEG C；Whirlpool is repeated twice to apply and heating
Reactions steps, two layers of Sb of spin coating2S3Film, then under Ar compression rings border 340 DEG C annealing 15min；
（4）It is prepared by hole transmission layer：Be the same as Example 1；
（5）The preparation of electrode：Be the same as Example 1.
Battery performance explanation is as shown in Figure 9：Open-circuit voltage is：0.42V, the short circuit current flow of battery is：6mA/cm2, filling
The factor is：38.6%, energy conversion efficiency is：0.97%.
The foregoing is only presently preferred embodiments of the present invention, all equivalent changes done according to scope of the present invention patent with
Modification, should all belong to the covering scope of the present invention.
Claims (9)
1. a kind of planar structure hybrid solar cell based on antimonous sulfide dense film, including oxidic transparent conductive liner
Bottom, electron transfer layer, light absorbing layer, hole transmission layer and metal electrode, it is characterised in that：The light absorbing layer is with spin-coating method
The Sb of preparation2S3Dense film, the thickness of light absorbing layer is 360 nanometers to 1 micron.
2. the planar structure hybrid solar cell according to claim 1 based on antimonous sulfide, it is characterised in that：Institute
Oxidic transparent conductive substrates are stated for FTO, ITO or AZO electro-conductive glass.
3. the planar structure hybrid solar cell according to claim 1 based on antimonous sulfide, it is characterised in that：Institute
Electron transfer layer is stated for smooth TiO2Film.
4. the planar structure hybrid solar cell according to claim 1 based on antimonous sulfide, it is characterised in that：Institute
Hole transmission layer is stated for P3HT films.
5. the planar structure hybrid solar cell according to claim 1 based on antimonous sulfide, it is characterised in that：Institute
Metal electrode is stated for Al or Ag.
6. the preparation method of the planar structure hybrid solar cell according to claim 1 based on antimonous sulfide, its
It is characterised by：Specifically include following steps：
（1）Cleaning oxidic transparent conductive substrates are simultaneously dried；
（2）The preparation of electron transfer layer：With sol-gel method, whirlpool applies TiO in transparent conductive substrate2Solution；Then TiO2Thoroughly
Bright film is calcined in Muffle furnace high temperature；
（3）The preparation of light absorbing layer：In an inert atmosphere, by the Sb prepared2S3Precursor solution whirlpool is coated in electron transfer layer
On, then in thermal station heating make solution react generation Sb2S3；Whirlpool is repeated to apply with heating response step to adjust generation
Sb2S3Film thickness；Temperature is raised again to be made annealing treatment, and makes Sb2S3Thin film crystallization；
（4）The preparation of hole transmission layer：On light absorbing layer surface, whirlpool applies P3HT；
（5）The preparation of electrode：In hole transport layer surface evaporation metal electrode.
7. preparation method according to claim 6, it is characterised in that：Step（3）It is middle to prepare Sb with spin coating method2S3Film
Technological parameter be：
Sb2S3Precursor solution：Prepare SbCl3With thiocarbamide as precursor solution, Sb and S mol ratio are 1:1.5~2.5；
Whirlpool is applied：750 revs/min of forward rotating speed, the time is 12s；After walk around speed 3000 revs/min, the time is 60s；
Heating-up temperature：140℃；
Reaction time：10min；
Annealing：Annealing temperature is 340 DEG C, annealing time 15min.
8. preparation method according to claim 6, it is characterised in that：Step（2）Middle calcining heat is 550 DEG C, during calcining
Between be 60min.
9. preparation method according to claim 6, it is characterised in that：Step（3）Described inert gas is Ar gas.
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| CN108899377A (en) * | 2018-07-17 | 2018-11-27 | 福州大学 | A kind of thin-film solar cells and preparation method thereof of Ti doping antimony trisulfide |
| CN109037034A (en) * | 2018-07-26 | 2018-12-18 | 深圳清华大学研究院 | Selenizing Sb film and preparation method thereof, the solar battery using it |
| CN109473552A (en) * | 2018-10-30 | 2019-03-15 | 深圳大学 | A kind of solar battery and preparation method thereof based on solwution method |
| CN109473551A (en) * | 2018-10-30 | 2019-03-15 | 深圳大学 | A kind of solar battery and preparation method thereof based on double source vapor deposition |
| CN110676331A (en) * | 2019-08-30 | 2020-01-10 | 中山大学 | Preparation method of antimony sulfide thin film based on alcohol solvent and application of antimony sulfide thin film in solar cell |
| CN113097314A (en) * | 2021-03-31 | 2021-07-09 | 福州大学 | Flexible antimony sulfide thin-film solar cell and preparation method thereof |
| CN114380952A (en) * | 2021-12-27 | 2022-04-22 | 湖南工业大学 | Near-infrared photoinduced quick self-healing conductive hydrogel and preparation method and application thereof |
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