CN105932158A - Linear perovskite solar cell and preparation method thereof - Google Patents

Linear perovskite solar cell and preparation method thereof Download PDF

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CN105932158A
CN105932158A CN201610270624.4A CN201610270624A CN105932158A CN 105932158 A CN105932158 A CN 105932158A CN 201610270624 A CN201610270624 A CN 201610270624A CN 105932158 A CN105932158 A CN 105932158A
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solar cell
perovskite solar
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perovskite
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彭慧胜
丘龙斌
杨嘉桦
何思斯
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Fudan University
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    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
    • H10K30/30—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising bulk heterojunctions, e.g. interpenetrating networks of donor and acceptor material domains
    • H10K30/35—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising bulk heterojunctions, e.g. interpenetrating networks of donor and acceptor material domains comprising inorganic nanostructures, e.g. CdSe nanoparticles
    • H10K30/352—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising bulk heterojunctions, e.g. interpenetrating networks of donor and acceptor material domains comprising inorganic nanostructures, e.g. CdSe nanoparticles the inorganic nanostructures being nanotubes or nanowires, e.g. CdTe nanotubes in P3HT polymer
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    • H10K71/10—Deposition of organic active material
    • H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
    • H10K71/125—Deposition of organic active material using liquid deposition, e.g. spin coating using electrolytic deposition e.g. in-situ electropolymerisation
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Abstract

The invention belongs to the field of a solar cell and specially relates to a linear perovskite solar cell and a preparation method thereof. The method is characterized by taking a titanium wire as an electrode; through an electrochemical deposition method, forming a titanium dioxide nanotube array and a perovskite nanocrystalline active layer in sequence from the axis to the outside; and finally, wrapping a transparent carbon nanotube gate as another electrode to form a flexible braided coaxial linear perovskite solar cell. The open-circuit voltage, short-circuit current density and fill factor of the linear perovskite solar cell are 0.85 V, 16.1 mA cm<2> and 0.5, and the corresponding energy conversion efficiency is 6.8%. The linear perovskite solar cell adopts the transparent carbon nanotube gate as the electrode, and an electron transfer layer and the light active layer are prepared through the electrochemical deposition method; the preparation process is simple and low in cost; the cell has high strength and good flexibility; and through a conventional braiding technique, the linear perovskite solar cell can be braided into fabric or integrated into the clothes, and can serve as a portable power supply device for daily life of people.

Description

A kind of wire perovskite solar cell and preparation method thereof
Technical field
The invention belongs to technical field of solar batteries, be specifically related to a kind of wire perovskite (CH3NH3PbI3) solar cell and preparation method thereof.
Background technology
In recent years, convert the solar into the wire solar cell of electric energy due to its light weight, flexibility, can weave, the feature such as low cost, cause the extensive concern of people.So far, people mainly concentrate research wire DSSC and linear polymer solar cell.DSSC needs to use electrolyte to be transferred in hole electrode, and the wire solar cell of report is based primarily upon liquid electrolyte at present, there is the challenge such as easily leakage, volatile, encapsulation difficulty；DSSC based on solid electrolyte and polymer solar battery efficiency are below 4%, the development of serious restriction wire solar cell and application.Development in recent years goes out a class novel Organic leadP trihalid CH3NH3PbI3Solar cell, in the time less than 5 years, photoelectric transformation efficiency increases to above 20% from initial about 3.8%.As a comparison, it is respectively 13% and 10.6% through the research of longer-term, the DSSC of planar structure and polymer solar battery high-photoelectric transformation efficiency at present.Based on above-mentioned perovskite material, it is possible to obtain high efficiency all solid state wire perovskite solar cell.
Simultaneously, use oriented transparent CNT grid as transparency electrode, ordered arrangement due to wherein CNT, oriented transparent CNT grid maintain the excellent electricity of single-root carbon nano-tube and chemical property well, thus there is high electrical conductivity, hot strength, it is widely used in structure function material and photoelectric device.Current result of study shows, aligned carbon nanotube grid can use as transparency electrode in perovskite solar cell.Compared to electrode material (such as wire and the polymer fiber scribbling conductive layer) conventional in wire solar cell, CNT grid both can overcome the defect that wire flexibility is poor, quality heavy and cladding area is little, it is also possible to the problem overcoming the polymer fiber structural stability difference scribbling conductive layer.
The present invention prepare a kind of based on high-quality, high coverage rate perovskite active material wire perovskite CH3NH3PbI3Solar cell, wherein titanium silk is as an electrode, titanic oxide electronic transport layer is obtained by electrochemical deposition method, then perovskite active layer material is prepared by cathode run, finally parcel transparent carbon nanotube grid are as another electrode, form the coaxial wire perovskite solar cell that a kind of flexibility can weave.Compared to the preparation method of other wire solar cells, this method achieves the pattern control of titanium dioxide and perovskite, and low cost, easily prepares.
Summary of the invention
The perovskite CH that it is an object of the invention to provide a kind of structure-controllable, can weave3NH3PbI3Solar cell and preparation method thereof.
Wire perovskite CH provided by the present invention3NH3PbI3Solar cell, is based on transparent carbon nanotube grid flexible to weave coaxial wire perovskite solar cell, and its negative pole is titanium silk, as electroplated electrode；Another one electrode is oriented transparent CNT grid, at outer layer.Electron transfer layer (titanium dioxide) and photoactive layer (perovskite CH is clipped between two electrodes3NH3PbI3), form the coaxial wire perovskite solar cell that flexibility can weave.This wire battery has good pliability and woven performance, has the integration of height, and whole device can be woven into fabric easily or be integrated in other fabric.
The present invention provides the preparation method of above-mentioned wire perovskite solar cell, using a titanium silk as electrode, utilize electrochemical deposition method, Nano tube array of titanium dioxide is outwards sequentially formed by axle center, the nanocrystalline active layer of perovskite, finally parcel transparent carbon nanotube grid are as another electrode, form the coaxial wire perovskite solar cell that a kind of flexibility can weave.Concretely comprise the following steps:
(1) titanic oxide electronic transport layer is prepared
It is negative electrode using titanium silk as anode, platinum electrode, is placed in containing 0.1-0.4M NH4In the glycerine of F, water (volume ratio of G & W is 1:2-3:1) mixed solution, and at two ends plus the voltage of 10-50 V；After rinsing with water, anneal at 300-550 DEG C 30-60min by titanium silk；The titanium silk after annealing is immersed the TiCl of 15-40 mM again4In solution, at 60-90 DEG C, keep 20-35 min；Afterwards, anneal at titanium silk being placed in 300-550 DEG C 20-50 min；
(2) perovskite CH is prepared3NH3PbI photoactive layer
It is anode using the titanium silk aoxidized prepared by step (1) as negative electrode, platinum electrode, is placed in containing 0.5-3 mM Pb (NO3)2With 0.1-0.3 M H2O2Solution in, at 3-7 mA/cm2Current density under be energized；Anneal at this titanium silk is placed in 150-300 DEG C 20-60 min；Then, it is dipped in the HI solution of 0.05-0.3 M；It is dried 45-70 min at being placed in 75-95 DEG C again, naturally cools to room temperature；
Afterwards, sample is immersed containing 10-70mg/mL CH3NH3I Aqueous isopropanol in, after 0.5-10min take out；30 min are processed at being placed in 75-95 DEG C again；
(3) oriented transparent CNT gate electrode is prepared
Using chemical vapour deposition technique, in tube furnace, synthesis can spinning carbon nano pipe array；Can wrap in the sample surfaces processed through step (2), (3) by spinning carbon nano pipe array, form electrode.
In the present invention, can can be synthesized in tube furnace by chemical vapour deposition technique by spinning carbon nano pipe array, typical synthetic method is, with the silicon chip of electron-beam evaporation iron (1.2 nm)/alundum (Al2O3) (3nm) as catalyst, as carbon source, (flow is 90 ± 45 to ethene Sccm), Ar(400 ± 200 sccm) and H2(30 ± 15 Sccm) it is carrier gas, reacts at 730-760 DEG C.Can spinning array height by control growth time control in 170～350 μm.Transparent carbon nanotube grid are directly pulled straight from carbon nano pipe array by blade, and the thickness of CNT grid can be controlled in 15-40 Nm every layer.
The photovoltaic performance test of wire perovskite solar cell.Wire solar cell uses solar simulator (Oriel-Sol3A 94023A equipped with a 450 W Xe lamp and an AM1.5 Filter) simulation AM1.5 sunshine, light intensity is 100mW/cm2Under record batteryI-VCurve.
In an embodiment, open-circuit voltage, short-circuit current density and the fill factor, curve factor of this wire perovskite solar cell is respectively 0.85 V, 16.1 mA cm-2With 0.5, corresponding energy conversion efficiency is 6.8%.
It is an advantage of the current invention that:
Perovskite CH3NH3PbI3There is the highest absorptivity, the excellent properties such as electron diffusion length so that battery just can fully absorb incident light under conditions of sufficiently thin, and can effectively transmit separation electron hole pair.On the basis of wire solar cell before, its preparation method is improved by we, and by controlling the pattern of each layer, final efficiency has reached 6.8%.Battery has high intensity and good pliability, and its performance does not changes with the change of incident angle of light.By traditional knitting skill, this wire solar cell can be woven into fabric or be integrated in clothes, can be applied in daily life as portable electric supply installation.
Accompanying drawing explanation
Fig. 1 is structure and the preparation process schematic diagram of wire perovskite solar cell.
Fig. 2 is the SEM image of wire perovskite solar cell.It can be seen that the tubular structure of titanium dioxide and the dense arrangement of perovskite.Wherein, a, b are respectively top graph and the side view of Nano tube array of titanium dioxide；C, d are respectively top graph and the side view of lead iodide nano-chip arrays；E, f are respectively the nanocrystalline top graph of perovskite and side view；G, h are respectively top graph and the side view of aligned carbon nanotube electrode.
Fig. 3 is the current density voltage curve of the wire perovskite solar cell of different titanium dioxide length of tube and different calcium titanium ore layer thickness.Wherein, a is the wire perovskite solar cell Current density-voltage line taking of different titanium dioxide length of tube；B is the current density voltage curve of the wire perovskite solar cell of different calcium titanium ore layer thickness.
Fig. 4 is crooked test schematic diagram and the result of wire perovskite solar cell.Wherein, a is the wire perovskite solar cell of knotting；B is the wire perovskite solar cell of distortion；C is that wire perovskite solar cell photovoltaic performance is along with the change of number of twists.
Fig. 5 is the SEM image being covered with transparent carbon nanotube gate electrode sample.
Detailed description of the invention
The present invention provides aligned carbon nanotube grid, the condition of electrochemical deposition preparation present situation perovskite solar cell and preparation technology.
(1) preparation of transparent carbon nanotube grid
Can spinning carbon nano pipe array by chemical vapour deposition technique synthetically prepared in tube furnace, typical synthetic method is, with the silicon chip of electron-beam evaporation iron (1.2 nm)/alundum (Al2O3) (3nm) as catalyst, as carbon source, (flow is 90 ± 45 to ethene Sccm), Ar(400 ± 200 sccm) and H2(30 ± 15 Sccm) it is carrier gas, reacts at 740 DEG C.Can spinning array height by control growth time control in 170～350 μm.Transparent carbon nanotube grid are directly pulled straight from carbon nano pipe array by blade, and the thickness of CNT grid can be controlled in 20 nm every layer.
(2) preparation of titanic oxide electronic transport layer
It is negative electrode using titanium silk as anode, platinum electrode, is placed in containing 0.1-0.4M NH4In the glycerine of F, water (volume ratio is 1:2-3:1) mixed solution, and at two ends plus the voltage of 10-50 V；After rinsing with water, anneal at 300-550 DEG C 30-60min by titanium silk；The titanium silk after annealing is immersed the TiCl of 15-40 mM again4In solution, at 60-90 DEG C, keep 20-35 min；Afterwards, anneal at titanium silk being placed in 300-550 DEG C 20-50 min.
(3) perovskite CH3NH3The preparation of PbI photoactive layer
It is anode using the titanium silk aoxidized prepared by step (2) method as negative electrode, platinum electrode, is placed in containing 0.5-3 mM Pb (NO3)2With 0.1-0.3 M H2O2Solution in, at 3-7 mA/cm2Current density under be energized；Anneal at this titanium silk is placed in 150-300 DEG C 20-60 min；Then, it is dipped in the HI solution of 0.05-0.3 M；It is dried 45-70 min at being placed in 75-95 DEG C again, naturally cools to room temperature；
Afterwards, sample is immersed containing 10-70mg/mL CH3NH3I Aqueous isopropanol in, after 0.5-10min take out；30 min are processed at being placed in 75-95 DEG C again.
(4) preparation of oriented transparent CNT gate electrode
Using chemical vapour deposition technique, concrete grammar is shown in (1), and in tube furnace, synthesis can spinning carbon nano pipe array.This can be wrapped on the sample surfaces sequentially processed according to (2) (3) method by spinning array, form electrode.
Embodiment 1 :Deposition has the silicon chip of iron (1.2nm)/alundum (Al2O3) (3nm) to be catalyst, ethene is as carbon source (flow is 90sccm), argon gas (400sccm) and hydrogen (30sccm) are carrier gas, react at 740 DEG C, can spinning array height about 250 μm.The titanium silk of cleaning-drying, is placed in containing 0.27M In the glycerine of NH4F, water (volume ratio is 1:1) mixed solution, and add that at two ends the voltage of 20 V carries out anodic oxidation；It is placed in containing 3 mM Pb (NO3)2With 0.2 M H2O2Solution in, at 7mA/cm2Current density under carry out cathodic reduction；Immerse 0.05 again The HI solution of M forms PbI；It is finally putting into 20 mg/mL M CH3NH3The aqueous isopropanol of I carries out dipping, and finally cladding transparent carbon nanotube gate electrode forms wire battery.
Embodiment 2 :Deposition has iron (1.1 nm)/alundum (Al2O3) (3nm) silicon chip is catalyst, and ethene is as carbon source (flow is 90sccm), and argon gas (400sccm) and hydrogen (30sccm) are carrier gas, reacts at 760 DEG C, can spinning array height about 300 μm.The titanium silk of cleaning-drying, is placed in the glycerine containing 0.27M NH4F, water (volume ratio is 1:2) mixed solution, and adds that at two ends the voltage of 30 V carries out anodic oxidation；It is placed in containing 2 mM Pb (NO3)2With 0.2 M H2O2Solution in, at 5mA/cm2Current density under carry out cathodic reduction；The HI solution immersing 0.1 M again forms PbI；It is finally putting into 40 mg/mL CH3NH3I Aqueous isopropanol carry out dipping, finally cladding transparent carbon nanotube gate electrode forms wire battery.
Embodiment 3 :Deposition has the silicon chip of iron (1.2nm)/alundum (Al2O3) (3nm) to be catalyst, ethene is as carbon source (flow is 90sccm), argon gas (400sccm) and hydrogen (30sccm) are carrier gas, react at 740 DEG C, can spinning array height about 250 μm.The titanium silk of cleaning-drying, is placed in containing 0.27M In the glycerine of NH4F, water (volume ratio is 1:1) mixed solution, and add that at two ends the voltage of 10V carries out anodic oxidation；It is placed in containing 2 mM Pb (NO3)2With 0.2 M H2O2Solution in, at 3 mA/cm2Current density under carry out cathodic reduction；Immerse 0.3 M again HI solution formed PbI；It is finally putting into 70 mg/mL CH3NH3The aqueous isopropanol of I carries out dipping, and finally cladding transparent carbon nanotube gate electrode forms wire battery.
In sum, the present invention is prepared for a kind of wire perovskite CH based on electrochemical deposition method3NH3PbI3Preparation method of solar battery, uses specific electrochemical deposition condition to prepare the material of specific morphology, finally obtains high performance calcium titanium ore solar cell.This wire battery has good pliability and woven performance, has the integration of height, and whole device can be woven into fabric easily or be integrated in other fabric.

Claims (3)

1. a linear flexible can weave perovskite solar cell, it is characterised in that its negative pole is titanium silk, as electroplated electrode；Another one electrode is oriented transparent CNT grid；Titanic oxide electronic transport layer and perovskite CH is clipped between two electrodes3NH3PbI3Photoactive layer, forms the coaxial wire perovskite solar cell that flexibility can weave.
2. a linear flexible as claimed in claim 1 can weave the preparation method of perovskite solar cell, it is characterised in that concretely comprises the following steps:
(1) titanic oxide electronic transport layer is prepared
It is negative electrode using titanium silk as anode, platinum electrode, is placed in containing 0.1-0.4M NH4In the glycerine of F, water mixed solution, and at two ends plus the voltage of 10-50 V；After rinsing with water, anneal at 300-550 DEG C 30-60min by titanium silk；The titanium silk after annealing is immersed the TiCl of 15-40 mM again4In solution, at 60-90 DEG C, keep 20-35min；Afterwards, anneal at titanium silk being placed in 300-550 DEG C 20-50min；
(2) perovskite CH is prepared3NH3PbI photoactive layer
It is anode using the titanium silk aoxidized prepared by step (1) as negative electrode, platinum electrode, is placed in containing 0.5-3mM Pb (NO3)2With 0.1-0.3 M H2O2Solution in, at 3-7mA/cm2Current density under be energized；Anneal at this titanium silk is placed in 150-300 DEG C 20-60 min；Then, it is dipped in the HI solution of 0.05-0.3 M；It is dried 45-70 min at being placed in 75-95 DEG C again, naturally cools to room temperature；
Afterwards, sample is immersed containing 10-70mg/mL CH3NH3I Aqueous isopropanol in, after 0.5-10min take out；30 are processed at being placed in 75-95 DEG C again min；
(3) oriented transparent CNT gate electrode is prepared
Using chemical vapour deposition technique, in tube furnace, synthesis can spinning carbon nano pipe array；Can wrap in the sample surfaces processed through step (2), (3) by spinning carbon nano pipe array, form gate electrode.
Linear flexible the most according to claim 2 can weave the preparation method of perovskite solar cell, it is characterized in that being synthesized in tube furnace by chemical vapour deposition technique by spinning carbon nano pipe array, concretely comprise the following steps: with the silicon chip of electron-beam evaporation iron/alundum (Al2O3) as catalyst, ethene is as carbon source, carbon source flow is 90 ± 45 sccm, Ar and H2For carrier gas, Ar is 400 ± 200 Sccm, H2It is 30 ± 15 sccm；React at 730-760 DEG C；Can spinning array height by control growth time control in 170-350 μm；Transparent carbon nanotube grid are directly pulled straight from carbon nano pipe array by blade, and the THICKNESS CONTROL of CNT grid is 15-40 nm every layer.
CN201610270624.4A 2016-04-27 2016-04-27 Linear perovskite solar cell and preparation method thereof Pending CN105932158A (en)

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN106571426A (en) * 2016-10-26 2017-04-19 陕西师范大学 Perovskite cell using titanium dioxide nanotube array as electron transport layer and preparation method thereof
CN110896129A (en) * 2018-09-13 2020-03-20 中国科学院大连化学物理研究所 Multi-exciton dissociation heterojunction based on perovskite nanocrystalline and acene molecular material
CN113862712A (en) * 2021-09-15 2021-12-31 中山大学 Preparation method of lead-containing or bismuth-containing perovskite nanocrystal

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN106571426A (en) * 2016-10-26 2017-04-19 陕西师范大学 Perovskite cell using titanium dioxide nanotube array as electron transport layer and preparation method thereof
CN106571426B (en) * 2016-10-26 2020-05-12 陕西师范大学 Perovskite battery with titanium dioxide nanotube array as electron transport layer and preparation method thereof
CN110896129A (en) * 2018-09-13 2020-03-20 中国科学院大连化学物理研究所 Multi-exciton dissociation heterojunction based on perovskite nanocrystalline and acene molecular material
CN113862712A (en) * 2021-09-15 2021-12-31 中山大学 Preparation method of lead-containing or bismuth-containing perovskite nanocrystal
CN113862712B (en) * 2021-09-15 2023-12-01 中山大学 Preparation method of lead-containing or bismuth-containing perovskite nanocrystals

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