CN112614938B - All-inorganic composite hole transport layer with energy level gradient, battery and preparation method - Google Patents
All-inorganic composite hole transport layer with energy level gradient, battery and preparation method Download PDFInfo
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Abstract
The invention discloses an all-inorganic composite hole transport layer with energy level gradient, a battery and a preparation method, wherein a layer of P-type inorganic material V is inserted between an ITO transparent electrode and a NiOx hole transport layer 2 O 5 Construction of an all-inorganic composite hole transport layer V 2 O 5 /NiO X And an energy level gradient is formed in the composite hole transport layer structure so as to enhance a built-in electric field, promote carrier transmission and reduce the non-radiative recombination probability of interface carriers.
Description
Technical Field
The invention belongs to the field of photoelectric conversion devices, relates to a charge transport material of a thin film solar cell (perovskite solar cell, dye sensitized solar cell and the like), and in particular relates to an all-inorganic composite hole transport layer with energy level gradient, a cell and a preparation method.
Background
In the period of ten years, the photoelectric conversion efficiency of the n-i-p structure device of the perovskite solar cell is rapidly improved from 3.8% to 25.5%, and the perovskite solar cell is outstanding in the photovoltaic field. However, the photoelectric conversion efficiency of the p-i-n structure device remains behind. The inorganic hole transport material commonly used for p-i-n structure devices is NiOx, which has good stability and band structure matching with perovskite materials. Although NiOx exhibits the property of a P-type semiconductor, the concentration of the multi-electrons (holes) is lower, the Fermi level is far away from VBM, the built-in electric field strength is weaker, the probability of non-radiative recombination of an interface is increased, and the energy loss of the interface is increased. Thus, further improvements in the photovoltaic performance of the device require optimized interface energy levels and charge extraction capabilities.
Disclosure of Invention
The invention aims to provide an all-inorganic composite hole transport layer with energy level gradient, a battery and a preparation method thereof, so as to overcome the problems in the prior art, and the invention adopts low-temperature preparation of V 2 O 5 /NiO X The all-inorganic composite hole transport layer forms an energy level gradient, enhances a built-in electric field, promotes interface charge extraction, reduces interface non-radiative recombination probability, and improves the photovoltaic performance of the device.
In order to achieve the above purpose, the invention adopts the following technical scheme:
an all-inorganic composite hole transport layer with an energy level gradient includes a first charge transport layer disposed on a transparent electrode substrate, and a second charge transport layer disposed on the first charge transport layer; the first charge transport layer is obtained by spin coating a vanadium tris (isopropoxide) oxide precursor solution on a transparent electrode substrate, followed by hot plate annealing, and the second charge transport layer is obtained by spin coating a NiOx ink on the first charge transport layer, followed by hot plate annealing.
Further, after the transparent electrode substrate (1) is spin-coated with the vanadium tris (isopropoxide) oxide precursor liquid, the annealing temperature of a hot plate is 120 ℃ and the time is 10min; after spin coating the NiOx ink on the first charge transport layer, the hot plate anneal temperature was 140 ℃ for 1h.
Further, the thickness of the first charge transport layer is 10nm; the thickness of the second charge transport layer was 15nm.
A method for preparing an all-inorganic composite hole transport layer with energy level gradient, comprising the following steps:
step 1: spin-coating a tri (isopropoxy) vanadium oxide precursor liquid on a transparent electrode substrate, and then annealing the transparent electrode substrate by a hot plate to obtain a first charge transport layer;
step 2: and spin-coating NiOx ink on the first charge transport layer, and then annealing by a hot plate to obtain a second charge transport layer, wherein the first charge transport layer and the second charge transport layer jointly form an all-inorganic composite hole transport layer with energy level gradient.
Further, in the step 1, the annealing temperature of the hot plate is 120 ℃ and the time is 10min; and in the step 2, the annealing temperature of the hot plate is 140 ℃ and the time is 1h.
Further, the thickness of the first charge transport layer is 10nm; the thickness of the second charge transport layer was 15nm.
A perovskite solar cell, comprising a transparent electrode substrate, an all-inorganic composite hole transport layer with energy level gradient, a perovskite absorption layer, a third charge transport layer and a metal back electrode which are sequentially arranged from bottom to top, wherein the all-inorganic composite hole transport layer with energy level gradient comprises a first charge transport layer arranged on the transparent electrode substrate and a second charge transport layer arranged on the first charge transport layer; the first charge transport layer is obtained by spin coating a vanadium tris (isopropoxide) oxide precursor solution on a transparent electrode substrate, followed by hot plate annealing, and the second charge transport layer is obtained by spin coating a NiOx ink on the first charge transport layer, followed by hot plate annealing.
A method of fabricating a perovskite solar cell comprising the steps of:
step 1: taking an ITO glass substrate, sequentially and respectively carrying out ultrasonic treatment by using deionized water, acetone and isopropanol, blow-drying by using nitrogen flow, and then cleaning by using ultraviolet light to obtain a transparent electrode substrate;
step 2: spin-coating a tri (isopropoxy) vanadium oxide precursor liquid on a transparent electrode substrate, and then annealing the transparent electrode substrate by a hot plate to obtain a first charge transport layer;
step 3: spin-coating NiOx ink on the first charge transport layer, and then annealing by a hot plate to obtain a second charge transport layer, wherein the first charge transport layer and the second charge transport layer jointly form an all-inorganic composite hole transport layer with energy level gradient;
step 4: preparing a perovskite light absorption layer in the second charge transport layer, wherein the perovskite light absorption layer is made of an organic-inorganic hybrid metal halide perovskite material;
step 5: preparation of C on perovskite light absorption layer by vapor deposition 60 BCP as a third charge transport layer;
step 6: and preparing an Ag layer serving as a metal back electrode on the third charge transport layer by adopting an evaporation mode.
Further, the annealing temperature of the hot plate in the step 2 is 120 ℃ and the time is 10min; and in the step 3, the annealing temperature of the hot plate is 140 ℃ and the time is 1h.
Further, the thickness of the first charge transport layer is 10nm; the thickness of the second charge transport layer was 15nm; the thickness of the perovskite light absorption layer is 700-800nm, C in the third charge transport layer 60 The thickness is 45nm, the thickness of BCP is 8nm, and the thickness of the metal back electrode is 80-100nm.
Compared with the prior art, the invention has the following beneficial technical effects:
the invention inserts a layer of P-type inorganic material V between the transparent electrode substrate and the NiOx hole transport layer 2 O 5 Construction of an all-inorganic composite hole transport layer V 2 O 5 /NiO X ，NiO X The valance band peak of 5.2eV, V 2 O 5 Is 5.0eV, due to the energy level gradient at the two layers of valence band, will be at V 2 O 5 /NiO X The interface forms a built-in electric field, and the existence of electric field driving force promotes the charge transmission process at the interface, so that the non-radiative recombination of carriers is reduced.
The battery prepared by the all-inorganic composite hole transport layer with the energy level gradient can form a built-in electric field due to the energy level gradient, promote charge transport and reduce the non-radiative recombination probability of unfavorable carriers in the device; secondly, the all-inorganic composite hole transport material has good stability, so that the stability of the device is improved; finally, the all-inorganic composite hole transport layer with the structure can be prepared and obtained under the low-temperature condition, so that the preparation process is more energy-saving and is suitable for flexible substrates with poor temperature tolerance.
Drawings
FIG. 1 is a schematic diagram of a perovskite solar cell;
fig. 2 is a schematic diagram of a partial energy level of a perovskite solar cell.
101, a transparent electrode substrate; 102. a first charge transport layer; 103. a second charge transport layer; 104. a perovskite light absorbing layer; 105. a third charge transport layer; 106. a metal back electrode.
Detailed Description
In describing embodiments of the present invention, specific terminology is employed for the sake of clarity. However, the invention is not intended to be limited to the specific terminology so selected. It is to be understood that each specific element includes all technical equivalents which operate in a similar manner to accomplish a similar purpose.
The invention inserts a layer of P-type inorganic material V between an ITO transparent electrode (transparent electrode substrate 101) and a NiOx hole transport layer (second charge transport layer 103) 2 O 5 Construction of an all-inorganic composite hole transport layer V 2 O 5 /NiO X ，NiO X Is 5.2eV，V 2 O 5 Is 5.0eV, due to the energy level gradient at the two layers of valence band, will be at V 2 O 5 /NiO X The interface forms a built-in electric field, and the existence of electric field driving force promotes the charge transmission process at the interface, so that the non-radiative recombination of carriers is reduced.
Specifically, the invention spin-coats triisopropoxy vanadium oxide precursor liquid on a transparent electrode substrate 101, and then carries out hot plate annealing, wherein the hot plate annealing temperature is 120 ℃ and the time is 10min, so as to obtain a first charge transport layer 102; and spin-coating NiOx ink on the first charge transport layer 102, and then carrying out hot plate annealing at 140 ℃ for 1h to obtain a second charge transport layer 103, wherein the thicknesses of the first charge transport layer 102 and the second charge transport layer 103 are respectively 10nm and 15nm, and the first charge transport layer 102 and the second charge transport layer 103 jointly form an all-inorganic composite hole transport layer with energy level gradient.
The invention also provides a perovskite solar cell shown in figure 1, which structurally comprises the following parts:
1. transparent electrode substrate 101: ITO glass substrate, the area of which is not limited (in this example, 2X 2cm 2 ) The commercial products of the products with large-scale mass production can be directly used. Before use, the surface of the substrate is treated by deionized water, acetone and isopropanol respectively for 15 minutes in sequence, and then dried by nitrogen flow, and cleaned by an ultraviolet cleaner for 10 minutes;
2. first charge transport layer 102: spin-coating a tris (isopropoxy) vanadium oxide precursor solution on an ITO glass substrate, and then annealing the glass substrate by a hot plate (120 ℃ for 10 min); the thickness of the first charge transport layer 102 is 10nm;
the precursor solution is a vanadium tri (isopropoxy) oxide isopropanol solution, and the vanadium tri (isopropoxy) oxide and isopropanol are mixed according to the volume ratio of 1:200 to obtain the vanadium tri (isopropoxy) oxide isopropanol. The solute is vanadium tris (isopropoxide) oxide and the solvent is isopropanol.
3. Second charge transport layer 103: spin-coating NiOx ink on the substrate of the first charge transport layer 102, and then carrying out hot plate annealing at 140 ℃ for 1h to obtain a second charge transport layer 103; the thickness of the second charge transport layer 103 is 15nm;
NiOx can be prepared in different ways, and the X values of the differently prepared species will generally vary, so the use of X to denote that P-type doping of the species is achieved.
The NiOx nanocrystalline powder related by the invention is prepared by adopting a chemical precipitation method, and is concretely as follows:
a) 5.81g of nickel nitrate hexahydrate was dissolved in 20mL of deionized water to obtain a greenish black solution;
b) Aqueous NaOH solution (10 mol L) -1 ) Dropwise adding the solution, continuously stirring until the pH value is 10, and continuously stirring for 20min to obtain light green precipitate;
c) Repeatedly cleaning the precipitate with deionized water for 3 times, washing off excessive impurities, vacuum drying at 80 ℃ overnight to obtain light green powder, calcining the powder at 275 ℃ for 2 hours to obtain black powder, and grinding the powder to be uniform to obtain NiOx nanocrystalline powder.
d) Adding 1mL of deionized water into 20-30mg of the NiOx nanocrystalline powder, and performing ultrasonic dispersion to obtain the NiOx ink.
4. Perovskite light absorbing layer 104: the organic-inorganic hybrid metal halide perovskite material is adopted as the light absorption material, the components of the perovskite light absorption layer 104 are not limited, and the preparation mode is also not limited; the thickness of the perovskite light absorption layer 104 is 700-800nm;
5. third charge transport layer 105: preparation of C by vapor deposition 60 BCP as a third charge transport layer; wherein C is 60 45nm thick and 8nm thick BCP;
6. metal back electrode 106: and preparing 80-100nm Ag serving as a metal back electrode by adopting an evaporation mode.
FIG. 2 is a partial energy level diagram of a perovskite solar cell including an all-inorganic composite hole transport layer, as can be seen from FIG. 2, niO X The valence band of (2) is 5.2eV, V 2 O 5 Is 5.0eV, due to the energy level gradient at the two-layer valence band, will be at V 2 O 5 /NiO X The interface forms a built-in electric field, and the electric field driving force is formed, so that the charge transmission process at the interface is promoted, and carriers are non-radiativeThe sexual recombination is reduced.
Claims (8)
1. An all-inorganic composite hole transport layer having an energy level gradient, characterized by comprising a first charge transport layer (102) disposed on a transparent electrode substrate (101), and a second charge transport layer (103) disposed on the first charge transport layer (102); the first charge transmission layer (102) is obtained by spin coating a tri (isopropoxy) vanadium oxide precursor liquid on a transparent electrode substrate (101) and then hot plate annealing, and the second charge transmission layer (103) is obtained by spin coating NiOx ink on the first charge transmission layer (102) and then hot plate annealing;
after the transparent electrode substrate (101) is spin-coated with the vanadium tri (isopropoxide) oxide precursor liquid, the annealing temperature of a hot plate is 120 ℃ and the time is 10min; after NiOx ink is spin-coated on the first charge transport layer (102), the annealing temperature of a hot plate is 140 ℃ and the time is 1h;
the first charge transport layer (102) has a thickness of 10nm; the thickness of the second charge transport layer (103) is 15nm.
2. A method of preparing an all-inorganic composite hole transport layer having an energy level gradient as set forth in claim 1, comprising the steps of:
step 1: spin-coating a tri (isopropoxy) vanadium oxide precursor liquid on a transparent electrode substrate (101), and then annealing by a hot plate to obtain a first charge transport layer (102);
step 2: and spin-coating NiOx ink on the first charge transfer layer (102), and then carrying out hot plate annealing to obtain a second charge transfer layer (103), wherein the first charge transfer layer (102) and the second charge transfer layer (103) jointly form an all-inorganic composite hole transfer layer with energy level gradient.
3. The method for preparing an all-inorganic composite hole transport layer with energy level gradient according to claim 2, wherein the annealing temperature of the hot plate in step 1 is 120 ℃ for 10min; and in the step 2, the annealing temperature of the hot plate is 140 ℃ and the time is 1h.
4. The method for producing an all-inorganic composite hole transport layer with energy level gradient according to claim 2, wherein the thickness of the first charge transport layer (102) is 10nm; the thickness of the second charge transport layer (103) is 15nm.
5. A perovskite solar cell based on an all-inorganic composite hole transport layer with energy level gradient according to claim 1, characterized by comprising a transparent electrode substrate (101), an all-inorganic composite hole transport layer with energy level gradient, a perovskite absorption layer (104), a third charge transport layer (105) and a metal back electrode (106) which are arranged in sequence from bottom to top, wherein the all-inorganic composite hole transport layer with energy level gradient comprises a first charge transport layer (102) arranged on the transparent electrode substrate (101), and a second charge transport layer (103) arranged on the first charge transport layer (102); the first charge transport layer (102) is obtained by spin coating a tri (isopropoxy) vanadium oxide precursor liquid on a transparent electrode substrate (101) and then hot plate annealing, and the second charge transport layer (103) is obtained by spin coating NiOx ink on the first charge transport layer (102) and then hot plate annealing.
6. A method of fabricating a perovskite solar cell as claimed in claim 5, comprising the steps of:
step 1: taking an ITO glass substrate, sequentially and respectively carrying out ultrasonic treatment by using deionized water, acetone and isopropanol, drying by using nitrogen flow, and then cleaning by using ultraviolet light to obtain a transparent electrode substrate (101);
step 2: spin-coating a tri (isopropoxy) vanadium oxide precursor liquid on a transparent electrode substrate (101), and then annealing by a hot plate to obtain a first charge transport layer (102);
step 3: spin-coating NiOx ink on the first charge transfer layer (102), and then carrying out hot plate annealing to obtain a second charge transfer layer (103), wherein the first charge transfer layer (102) and the second charge transfer layer (103) jointly form an all-inorganic composite hole transfer layer with energy level gradient;
step 4: preparing a perovskite light absorption layer (104) on the second charge transport layer (103), wherein the perovskite light absorption layer (104) adopts an organic-inorganic hybrid metal halide perovskite material;
step 5: preparation of C on perovskite light absorbing layer (104) by vapor deposition 60 BCP as a third charge transport layer (105);
step 6: an Ag layer is prepared on the third charge transport layer (105) by vapor deposition as a metal back electrode (106).
7. The method for manufacturing a perovskite solar cell according to claim 6, wherein the annealing temperature of the thermal plate in the step 2 is 120 ℃ for 10min; and in the step 3, the annealing temperature of the hot plate is 140 ℃ and the time is 1h.
8. The method of manufacturing a perovskite solar cell according to claim 6, wherein the thickness of the first charge transport layer (102) is 10nm; the thickness of the second charge transport layer (103) is 15nm; the perovskite light absorption layer (104) has a thickness of 700-800nm, and C is contained in the third charge transport layer (105) 60 The thickness is 45nm, the thickness of BCP is 8nm, and the thickness of the metal back electrode (106) is 80-100nm.
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| CN115084395B (en) * | 2022-08-22 | 2022-11-15 | 中国华能集团清洁能源技术研究院有限公司 | Perovskite absorption layer/hole transport layer interface processing method and perovskite solar cell |
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| CN106654016A (en) * | 2016-12-16 | 2017-05-10 | 深圳大学 | Organic photoelectric device and preparation method thereof and composition with hole transport performance |
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| CN110098336A (en) * | 2019-06-11 | 2019-08-06 | 中国矿业大学 | A kind of perovskite battery and preparation method thereof based on full-inorganic charge transmission film |
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