CN110400882A - The preparation method and solar energy laminated cell of hetero-junctions perovskite solar battery - Google Patents
The preparation method and solar energy laminated cell of hetero-junctions perovskite solar battery Download PDFInfo
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Abstract
The invention discloses a kind of preparation method of hetero-junctions perovskite solar battery and solar energy laminated cells, it include: that the first conductive layer is prepared using the first sputtering method on the battery functi on layer of perovskite top, the second conductive layer, the power of the power of the first sputtering method less than the second sputtering method are prepared using the second sputtering method on first conductive layer.Substep sputtering method of the present invention prepares conductive layer, can preferably protect perovskite top battery functi on layer, is unlikely to improve the whole yield that battery is reorganized and outfit because sputtering power is excessive and breakdown；Also, it is improved using perovskite solar energy laminated cell stability prepared by this method, photoelectric conversion efficiency is up to 20.19%.
Description
Technical field
The present invention relates to perovskite technical field of solar more particularly to a kind of hetero-junctions perovskite solar batteries
Preparation method and solar energy laminated cell.
Background technique
Perovskite solar battery is due to having outstanding advantages of photoelectric conversion efficiency is high, at low cost, production is simple to become
The research hotspot of area of solar cell, and be the solar battery of current most application prospect.Perovskite sun electricity now
The photoelectric conversion efficiency in pond has reached 23.7%, and can match in excellence or beauty traditional and volume production inorganic thin film solar battery.
But perovskite solar cell stability is poor, greatly limits its development.In order to preferably play
The advantage of perovskite solar battery improves its stability, using perovskite solar battery as top battery and as bottom battery
Silicon substrate or other more mature hull cells be overlapped, formed hetero-junctions HIT (Heterojunction with
Intrinsic Thin-layer) lamination solar cell, mutually learn from other's strong points to offset one's weaknesses, overcomes common perovskite solar battery
The problem of stability deficiency, improves the photoelectric conversion efficiency of perovskite solar battery.
When preparing hetero-junctions perovskite solar energy laminated cell, the function layer surface system in perovskite top battery is needed
Standby one layer of conductive layer, on the one hand can preferably collect carrier, on the other hand can have more with back electrode in contact
Well more fully contact.The preparation method of the conductive layer of perovskite top battery functi on layer surface is magnetron sputtering method, sputtering at present
Power cannot be too low, and otherwise the efficiency of obtained perovskite solar energy laminated cell will be greatly reduced, but if power mistake
Height, it is larger to the functional layer damage of perovskite top battery, and there is the risk of breakdown.
Summary of the invention
In order to solve the above-mentioned technical problems, the present invention provides a kind of preparation sides of hetero-junctions perovskite solar battery
Method and solar energy laminated cell ensure that perovskite solar energy lamination electricity while not damaging perovskite top battery functi on layer
The transfer efficiency in pond.
A kind of preparation method of hetero-junctions perovskite solar battery, comprising:
The first conductive layer is prepared using the first sputtering method in the functional layer of perovskite top battery；
The second conductive layer, the sputtering of first sputtering method are prepared using the second sputtering method on first conductive layer
Power is less than the sputtering power of second sputtering method.
A kind of solar energy laminated cell, including bottom battery and perovskite top battery, perovskite top battery, comprising: suitable
The secondary functional layer being set on the bottom battery, the second sputtering method of the first conductive layer and use using the preparation of the first sputtering method
Second conductive layer of preparation, wherein the sputtering power of first sputtering method is less than the sputtering power of second sputtering method.
Compared with prior art, the invention has the benefit that
1) preparation method of a kind of hetero-junctions perovskite solar battery provided by the present invention, using substep sputtering method,
It is sputtered on the battery functi on layer of perovskite top using relatively low power, can preferably protect perovskite top battery
Functional layer, be unlikely to because sputtering power it is excessive and breakdown, improve battery preparation whole yield.
2) the first conductive layer is sputtered using relatively low power, saves the usage amount of magnetic control spattering target, In
It reduces costs to a certain extent.
3) solar energy laminated cell provided by the present invention, using the system of above-mentioned hetero-junctions perovskite solar battery
The performance of conductive layer prepared by Preparation Method, solar energy laminated cell is improved, and photoelectric conversion efficiency has obtained significantly mentioning
It rises.
Other features and advantages of the present invention will be illustrated in the following description, also, partly becomes from specification
It obtains it is clear that understand through the implementation of the invention.The objectives and other advantages of the invention can be by specification, power
Specifically noted structure is achieved and obtained in sharp claim and attached drawing.
Detailed description of the invention
Attached drawing is used to provide to further understand technical solution of the present invention, and constitutes part of specification, with this
The embodiment of application technical solution for explaining the present invention together, does not constitute the limitation to technical solution of the present invention.
Fig. 1 is perovskite/silicon heterogenous solar energy laminated cell structure chart of 1-4 of the embodiment of the present invention；
Fig. 2 is perovskite/silicon heterogenous solar energy laminated cell structure chart of the embodiment of the present invention 5；
Fig. 3 is perovskite/silicon heterogenous solar energy laminated cell structure chart of the embodiment of the present invention 6；
Fig. 4 is perovskite/silicon heterogenous solar energy laminated cell structure chart of the embodiment of the present invention 7；
Fig. 5 is perovskite/silicon heterogenous solar energy laminated cell structure chart of comparative example 1 of the present invention；
Fig. 6 is perovskite/silicon heterogenous solar energy laminated cell structure chart of comparative example 2 of the present invention；
Fig. 7 is perovskite/silicon heterogenous solar energy laminated cell structure chart of comparative example 3 of the present invention；
Fig. 8 is perovskite/silicon heterogenous solar energy laminated cell structure chart of comparative example 4 of the present invention；
Fig. 9 is perovskite/silicon heterogenous solar energy lamination electricity of 1-3 of the embodiment of the present invention, embodiment 5 and comparative example 1-2
The IV curve graph in pond；
Figure 10 is the flow chart provided by the present invention that conductive layer and top electrode are prepared in perovskite functional layer.
Description of symbols
1- hearth electrode, 2- third conductive layer, the silicon heterogenous layer of 3-, 31-N type amorphous silicon layer, the first intrinsic amorphous silicon of 32-
Layer, 33-N type monocrystalline silicon layer, the second intrinsic amorphous silicon layer of 34-, 35-P type amorphous silicon layer, 4- tunnel layer, 5- electron transfer layer,
6- perovskite absorbed layer, 7- hole transmission layer, 8- conductive layer, the first conductive layer of 81-, the second conductive layer of 82-, 9- top electrode,
10- inorganic layer, the 4th conductive layer of 11-
Specific embodiment
In order to make the object, technical scheme and advantages of the embodiment of the invention clearer, below in conjunction with the embodiment of the present invention
Attached drawing, the technical solution of the embodiment of the present invention is clearly and completely described.Obviously, described embodiment is this hair
Bright a part of the embodiment, instead of all the embodiments.Based on described the embodiment of the present invention, the common skill in this field
Art personnel every other embodiment obtained under the premise of being not necessarily to creative work, shall fall within the protection scope of the present invention.
" first ", " second " used in the present invention and similar word are not offered as any sequence, quantity or again
The property wanted, and be used only to distinguish different component parts.
As shown in Figure 10, the preparation method of a kind of hetero-junctions perovskite solar battery provided by the present invention, comprising:
Step S101: the first conductive layer is prepared using the first sputtering method on the battery functi on layer of perovskite top；Step S102: first
The second conductive layer is prepared using the second sputtering method on conductive layer.
In the preparation method, the power of the power of the first sputtering method less than the second sputtering method.First conductive layer is located next to
The functional layer of perovskite top battery is sputtered using the relatively low power of 1kw-2kw, is conducive to protect perovskite top electricity
The functional layer in pond is not breakdown, improves the yield of battery preparation.Second conductive layer uses relatively high more than or equal to 4kw
Power sputtered, peak power also needs to be determined according to the target sputtered, must can bear lower than target
Maximum power.There is the protection of the first conductive layer, it will not be due to the higher sputtering power of the second conductive layer perovskite top electricity
The breakdown of pond functional layer, and can guarantee the performance of the conductive layer of preparation.
Further, shown in Figure 10, a kind of preparation of hetero-junctions perovskite solar battery provided by the present invention
Method can also include: step S101: prepare the first conductive layer using the first sputtering method on the battery functi on layer of perovskite top；
Step S102: the second conductive layer is prepared using the second sputtering method on the first conductive layer；Step S103: on the second conductive layer
Prepare top electrode.The setting of first conductive layer and the second conductive layer can preferably collect carrier, on the other hand can be with
Top electrode more preferably more fully contacts, and improves the transmittability of carrier.
Reaction gas in first sputtering method is using the mixed gas or oxygen of oxygen and argon gas, argon gas and hydrogen
Mixed gas；Reaction gas in second sputtering method uses oxygen and the mixed gas or oxygen of argon gas, argon gas and hydrogen
Mixed gas；The reaction gas of first sputtering method can be identical or not identical with the reaction gas of the second sputtering method, only
Want the oxygen content of the reaction gas of the first sputtering method less than the oxygen content of the reaction gas of the second sputtering method.First sputtering
The oxygen content (flow-rate ratio) of reaction gas is 1.5%-2% in method, and the oxygen content of the second sputtering method reaction gas is 3%-4%,
Oxygen content can change the number of Lacking oxygen in conductive layer, to influence conductive layer to the constraint ability of electronics, using difference
The reaction gas of oxygen content changes the work function of conductive layer, can improve the functional layer of conductive layer Yu perovskite top battery
Contact performance, guarantee the good transmission performance of carrier.
First sputtering method and the second sputtering method are respectively direct current magnetron sputtering process, radio frequency sputtering method, direct current and RF coupling
Any one in sputtering method, plasma sputtering.The sputtering the preparation method of first conductive layer and the second conductive layer can be identical
Can not be identical, as long as the power of the first sputtering method is less than the power of the second sputtering method.
The present invention also provides a kind of solar energy laminated cells, including bottom battery, tunnel layer and the perovskite being sequentially arranged
Battery is pushed up, indsole battery is silica-based solar cell, copper-indium-galliun-selenium film solar cell, telluride chromium thin film solar-electricity
Any one in pond, gallium arsenide film solar battery, perovskite top battery is superimposed with bottom battery, can effectively be changed
The stability of kind perovskite battery, improves the service performance of battery.
It is provided with tunnel layer between bottom battery and perovskite top battery, prevents the PN junction of bottom battery and perovskite top battery
It is directly connected to, influences the performance of laminated cell.The material of tunnel layer include but is not limited to indium-doped tin oxide ITO, nanocrystal silicon,
Tin oxide SnO2Deng and their combination.Preparation method includes but is not limited to magnetron sputtering, hydatogenesis etc..Tunnel layer
With a thickness of 10nm-25nm, few son can be made to be tunneled through while preventing more son drifts.
Perovskite top battery, comprising: the functional layer that is sequentially arranged, using the preparation of the first sputtering method the first conductive layer and
Using the second conductive layer and top electrode layer of the preparation of the second sputtering method.
Functional layer includes the electron transfer layer being sequentially arranged on the battery of bottom, perovskite absorbed layer, hole transmission layer, nothing
Machine layer, or the hole transmission layer including being sequentially arranged on the battery of bottom, perovskite absorbed layer, electron transfer layer, inorganic layer.
Electron transfer layer can extract and transmit electronics, including but not limited to titanium oxide in perovskite absorbed layer light-generated excitons
(TiO2), tin oxide (SnO2), zinc oxide (ZnO), lithium fluoride (LiF), C60 and their combination.Preparation method includes but not
It is limited to solwution method, chemical vapour deposition technique, magnetron sputtering method etc..Electron transfer layer with a thickness of 10nm-500nm.
Perovskite absorbed layer is with ABX3The material of structure, in which:
A is univalent cation, including but not limited to Rb+、Na+、K+、Cs+, HN=CHNH3+(being expressed as FA), CH3NH3+
(being expressed as MA) and their combination；
B is bivalent cation, including but not limited to Sn2+、Pb2+Their combination；
X is selected from halide anion, O2-、S2-And their combination.
It include but is not limited to (Cs) for perovskite absorbed layer of the inventionx(FA)1-xPbI3、(FA)x(MA)1-x PbI3、
(FA)x(MA)1-x PbIyCl1-y、(FAPbI3)x(MAPbBr3)1-xDeng；Wherein x=0-1, y=0-1.
The preparation method of perovskite absorbed layer include but is not limited to spin coating, spraying, blade coating, vapor deposition, chemical vapor deposition,
Gas phase assists liquid phase method, silk-screen printing etc. and their combination.Perovskite absorbed layer with a thickness of 100nm-1000nm.
Hole transmission layer can extract and transmit hole, including but not limited to organic matter in perovskite absorbed layer light-generated excitons
Class material, such as Spiro-OMeTAD (2,2 ', 7,7 '-four [N, N- bis- (4- methoxyphenyl) amino] -9,9 '-spiral shell, two fluorenes)；
Doping metals class organic material, such as the Spiro-OMeTAD of doping lithium salts；Organic metal salt material, such as CuPc；Polymerization
Composition material, such as PTAA (poly- [bis- (4- phenyl) (2,4,6- trimethylphenyl) amine]) etc.；Mineral-type materials, such as iodate
Cuprous (CuI), cuprous sulfocyanide (CuSCN), nickel oxide (NiO) etc.；And their combination.Preparation method includes but unlimited
In blade coating, spin coating, evaporation, gas-phase transport and deposition etc.；Hole transmission layer with a thickness of 10nm-500nm.
Material used by inorganic layer includes but is not limited to SnO2、MoOx(x is 2 or 3), NiO, WO3Deng and their group
It closes.Preparation method includes but is not limited to atomic layer deposition, electron beam evaporation, chemical vapor deposition etc..Inorganic layer with a thickness of
10nm-50nm, to the destruction of electron transfer layer or hole transmission layer and effective biography of electronics when can reduce sputtering
It is defeated.
Optionally, functional layer can also be not provided with inorganic layer, using the directly on electron transfer layer or hole transmission layer
One sputtering method prepares the first conductive layer.
First conductive layer is prepared using the first sputtering method, and the second conductive layer is prepared using the second sputtering method, wherein first splashes
Penetrate sputtering power of the sputtering power less than the second sputtering method of method.
Oxygen content of the oxygen content of the reaction gas of first sputtering method less than the reaction gas of the second sputtering method, oxygen content
Can change Lacking oxygen in conductive layer number, and then work function, sheet resistance and the light transmittance of conductive layer are influenced, so made
In standby hetero-junctions perovskite solar battery: less than the work function of the second conductive layer, first leads the work function of the first conductive layer
The sheet resistance of electric layer is 30 Ω/cm2-60Ω/cm2, the sheet resistance of the second conductive layer is 70 Ω/cm2-100Ω/cm2, and first leads
The light transmittance of electric layer is 60%-90%, and the light transmittance of the second conductive layer is 70%-90%.
The thickness of first conductive layer is set as 20nm-30nm, can when the second conductive layer is sputtered using higher-wattage
The functional layer of perovskite top battery is protected not to be damaged.The thickness of second conductive layer is set as 80nm-280nm, and guarantee is entirely led
The performance of electric layer.
First conductive layer and the second conductive layer respectively include but are not limited to oxide material, such as fluorine-doped tin oxide
(FTO), indium-doped tin oxide (ITO) or Al-Doped ZnO (AZO) etc.；Metal material, such as Au, Al, Pt etc.；Composite material, example
Such as TiO2/Ag/TiO2Deng.
Top electrode includes but is not limited to Au, Ag, Cu, Al, Ni, Cr etc. and their combination.Preparation method include but
It is not limited to evaporation, silk screen print method etc..Push up battery with a thickness of 50nm-200nm.
Bottom battery is described in detail for silicon heterogenous.
The structure of silicon heterogenous bottom battery includes the hearth electrode being sequentially arranged, third conductive layer and silicon heterogenous layer.
Hearth electrode includes but is not limited to Au, Ag, Cu, Al, Ni, Cr etc. and their combination.Preparation method include but
It is not limited to evaporation, silk screen print method etc..Hearth electrode with a thickness of 50nm-200nm.
Third conductive layer includes but is not limited to oxide material, such as fluorine-doped tin oxide (FTO), indium-doped tin oxide (ITO)
Or Al-Doped ZnO (AZO) etc.；Metal material, such as Au, Al, Pt etc.；High molecular material, such as polyaniline etc.；Composite wood
Material, such as TiO2/Ag/TiO2Deng.Third conductive layer with a thickness of 50nm-500nm.
Silicon heterogenous layer includes being sequentially arranged the non-silicon layer of N-type or P-type non-crystalline silicon layer, the first intrinsic amorphous silicon layer, N-type
Monocrystalline silicon layer, the second intrinsic amorphous silicon layer, P-type non-crystalline silicon layer or the non-silicon layer of N-type.Wherein, n type single crystal silicon layer with a thickness of
90 μm -250 μm, N-type or the non-silicon layer of p-type with a thickness of 3nm-30nm, the first intrinsic amorphous silicon layer with a thickness of 3nm-
10nm, the second intrinsic amorphous silicon layer with a thickness of 3nm-10nm.
It is described in detail in embodiment with the preparation of perovskite/silicon heterogenous solar battery.
Embodiment 1
Perovskite as shown in Figure 1/silicon heterogenous solar energy laminated cell structure chart, including the bottom electricity being sequentially arranged
Pole 1, third conductive layer 2, the non-silicon layer 35 of p-type, the first intrinsic amorphous silicon layer 32, n type single crystal silicon layer 33, the second intrinsic amorphous
Silicon layer 34, N-type non-crystalline silicon layer 31, tunnel layer 4, hole transmission layer 7, perovskite absorbed layer 6, electron transfer layer 5, inorganic layer 10,
First conductive layer 81, the second conductive layer 82, top electrode 9, specific preparation process is as follows:
1): preparing n type single crystal silicon layer: n type single crystal silicon substrate being placed in KOH solution and is corroded, clean, obtain thickness
The n type single crystal silicon layer that degree is 150 μm；
2): enhancing vapour deposition process (PECVD) method of chemistry successively in the back side using plasma of n type single crystal silicon layer
Deposit the first intrinsic amorphous silicon layer and P-type non-crystalline silicon layer, obtain with a thickness of 5nm the first intrinsic non-silicon crystal layer and with a thickness of
The intrinsic non-silicon layer of the p-type of 10nm；
3): the second intrinsic amorphous silicon layer and N-type amorphous silicon being sequentially depositing using PECVD in the front of n type single crystal silicon layer
Layer, obtains the second intrinsic non-silicon layer with a thickness of 5nm and the intrinsic non-silicon layer of N-type with a thickness of 10nm；
4): the magnetron sputtering ITO on the non-silicon layer of p-type obtains the third conductive layer with a thickness of 100nm.
5): hearth electrode Au electrode layer being prepared using vapour deposition method on third conductive layer, with a thickness of 80nm.
6): N being sequentially depositing using PECVD in N-type non-crystalline silicon layer+、P+Crystal silicon tunnel junctions, obtain with a thickness of 10nm's
Tunnel layer.
7): being evaporated in vacuo Spiro-OMeTAD on the tunneling layer, obtain the hole transmission layer with a thickness of 30nm.
8): preparing perovskite absorbed layer on the hole transport layer: on the hole transport layer using lead iodide and cesium bromide
Vacuum thermal evaporation mode obtains the lead iodide with a thickness of 500nm/cesium bromide film layer, then revolves in lead iodide/cesium bromide film layer
The alcohol mixed solution of FAI and FABr is applied, 150 DEG C of annealing obtain perovskite absorbed layer.
9): preparing the mixed layer of C60/FLi by the way of common thermal evaporation on perovskite absorbed layer, obtain thickness
For the electron transfer layer of 50nm.
10): chemical vapor deposition MoO on the electron transport layer3Inorganic layer, with a thickness of 30nm.
11): in MoO3The first conductive layer of ITO, preparation condition are prepared using the first magnetron sputtering method on inorganic layer are as follows:
Reaction gas: oxygen and argon gas, wherein the content of oxygen is 1.5%；Magnetron sputtering power: 1.5kw, with a thickness of
30nm；
12): the second conductive layer of ITO, reaction condition being prepared using the second magnetron sputtering method on the first conductive layer of ITO are as follows:
Oxygen and argon gas, wherein the content of oxygen is 3.5%；Magnetron sputtering power: 4kw, with a thickness of 100nm；
13): top electrode Au electrode layer being prepared using vapour deposition method on the second conductive layer of ITO, with a thickness of 80nm.
Embodiment 2
Perovskite as shown in Figure 1/silicon heterogenous solar energy laminated cell structure chart, specific preparation method is as implemented
Described in the preparation method of example 1, the difference is that:
11): in MoO3On inorganic layer, the first conductive layer of ITO, preparation condition are prepared using the first magnetron sputtering method are as follows:
Reaction gas: oxygen and argon gas, wherein the content of oxygen is 1.8%；Magnetron sputtering power: 1.6kw, with a thickness of
20nm。
12): the second conductive layer of ITO, reaction condition being prepared using the second magnetron sputtering method on the first conductive layer of ITO are as follows:
Oxygen and argon gas, wherein the content of oxygen is 3.0%；Magnetron sputtering power: 4.5kw, with a thickness of 150nm.
Embodiment 3
Perovskite as shown in Figure 1/silicon heterogenous solar energy laminated cell structure chart, specific preparation method is as implemented
Described in the preparation method of example 1, the difference is that:
11): in MoO3On inorganic layer, the first conductive layer of ITO, preparation condition are prepared using the first magnetron sputtering method are as follows:
Reaction gas: oxygen and argon gas, wherein the content of oxygen is 2.0%；Magnetron sputtering power: 2kw, with a thickness of
25nm。
12): the second conductive layer of ITO, reaction condition being prepared using the second magnetron sputtering method on the first conductive layer of ITO are as follows:
Oxygen and argon gas, wherein the content of oxygen is 4.0%；Magnetron sputtering power: 4.5kw, with a thickness of 260nm.
Embodiment 4
Perovskite as shown in Figure 1/silicon heterogenous solar energy laminated cell structure chart, specific preparation method is as implemented
Described in the preparation method of example 1, the difference is that:
11): in MoO3Inorganic layer prepares the first conductive layer of ITO, preparation condition using the first magnetron sputtering method are as follows:
Reaction gas: oxygen, argon gas and hydrogen, wherein the content of oxygen is 1.7%；Magnetron sputtering power: 1.9kw is thick
Degree is 28nm.
12): the second conductive layer of FTO, reaction condition being prepared using the second magnetron sputtering method on the first conductive layer of ITO are as follows:
Oxygen and argon gas, wherein the content of oxygen is 3.8%；Magnetron sputtering power: 4.4kw, with a thickness of 80nm.
Embodiment 5
Perovskite as shown in Figure 2/silicon heterogenous solar energy laminated cell structure chart, including the bottom electricity set gradually
Pole 1, third conductive layer 2, the non-silicon layer 31 of N-type, the first intrinsic amorphous silicon layer 32, n type single crystal silicon layer 33, the second intrinsic amorphous
Silicon layer 34, P-type non-crystalline silicon layer 35, tunnel layer 4, electron transfer layer 5, perovskite absorbed layer 6, hole transmission layer 7, inorganic layer 10,
First conductive layer 81, the second conductive layer 82, top electrode 9, specific preparation process is as follows:
1): preparing n type single crystal silicon layer: n type single crystal silicon substrate being placed in KOH solution and is corroded, clean, obtain thickness
The n type single crystal silicon layer that degree is 100 μm.
2): the first intrinsic amorphous silicon layer and N-type amorphous silicon being sequentially depositing using PECVD at the back side of n type single crystal silicon layer
Layer, obtains the first intrinsic non-silicon crystal layer with a thickness of 8nm and the intrinsic non-silicon layer of N-type with a thickness of 10nm.
3): the second intrinsic amorphous silicon layer and P-type non-crystalline silicon being sequentially depositing using PECVD in the front of n type single crystal silicon layer
Layer, obtains the second intrinsic non-silicon layer with a thickness of 8nm and the intrinsic non-silicon layer of p-type with a thickness of 10nm.
4): the magnetron sputtering AZO on the non-silicon layer of N-type obtains the third conductive layer with a thickness of 100nm.
5): hearth electrode Ag electrode layer being prepared using vapour deposition method on third conductive layer, with a thickness of 80nm.
6): P being sequentially depositing using PECVD on P-type non-crystalline silicon layer+、N+Nanocrystal silicon tunnel junctions, obtain with a thickness of
The tunnel layer of 10nm.
7): spin coating SnO on the tunneling layer2, obtain the electron transfer layer with a thickness of 100nm.
8): preparing perovskite absorbed layer on the electron transport layer: on the electron transport layer using lead iodide and cesium bromide
Vacuum thermal evaporation mode obtains the lead iodide with a thickness of 500nm/cesium bromide film layer, then revolves in lead iodide/cesium bromide film layer
Apply the alcohol mixed solution of FAI and FABr, 150 DEG C of annealing.
9): the spin coating PTAA on perovskite absorbed layer obtains the hole transmission layer with a thickness of 100nm.
10): on the hole transport layer, chemical vapor deposition MoO3Inorganic protective layer, with a thickness of 30nm.
11): in MoO3Inorganic layer prepares the first conductive layer of AZO, preparation condition using the first magnetron sputtering method are as follows:
Reaction gas: oxygen and argon gas, wherein the content of oxygen is 1.6%；Magnetron sputtering power: 1.8kw, with a thickness of
20nm。
12): the second conductive layer of AZO, reaction condition being prepared using the second magnetron sputtering method on the first conductive layer of AZO are as follows:
Oxygen and argon gas, wherein the content of oxygen is 3.6%；Magnetron sputtering power: 4.2kw, with a thickness of 120nm.
13): top electrode Au electrode layer being prepared using vapour deposition method on the second conductive layer of AZO, with a thickness of 80nm.
Embodiment 6
Perovskite as shown in Figure 3/silicon heterogenous solar energy laminated cell structure chart, including the bottom electricity set gradually
Pole 1, third conductive layer 2, the non-silicon layer 35 of p-type, the first intrinsic amorphous silicon layer 32, n type single crystal silicon layer 33, the second intrinsic amorphous
Silicon layer 34, N-type non-crystalline silicon layer 31, tunnel layer 4, hole transmission layer 7, perovskite absorbed layer 6, electron transfer layer 5,81- first are led
Electric layer, the second conductive layer of 82-, top electrode 9, specific preparation process is as follows:
1): preparing n type single crystal silicon layer: n type single crystal silicon substrate being placed in KOH solution and is corroded, clean, obtain thickness
The n type single crystal silicon layer that degree is 100 μm；
2): the first intrinsic amorphous silicon layer and P-type non-crystalline silicon being sequentially depositing using PECVD at the back side of n type single crystal silicon layer
Layer, obtains the first intrinsic non-silicon crystal layer with a thickness of 8nm and the intrinsic non-silicon layer of p-type with a thickness of 8nm；
3): the second intrinsic amorphous silicon layer and N-type amorphous silicon being sequentially depositing using PECVD in the front of n type single crystal silicon layer
Layer, obtains the second intrinsic non-silicon layer with a thickness of 8nm and the intrinsic non-silicon layer of N-type with a thickness of 8nm；
4): the magnetron sputtering FTO on the non-silicon layer of p-type obtains the third conductive layer with a thickness of 100nm.
5): hearth electrode Au electrode layer being prepared using vapour deposition method on third conductive layer, with a thickness of 80nm.
6): N being sequentially depositing using PECVD in N-type non-crystalline silicon layer+、P+Crystal silicon tunnel junctions, obtain with a thickness of 10nm's
Tunnel layer.
7): being evaporated in vacuo Spiro-OMeTAD on the tunneling layer, obtain the hole transmission layer with a thickness of 30nm.
8): preparing perovskite absorbed layer on the hole transport layer: on the hole transport layer using lead iodide and cesium bromide
Vacuum thermal evaporation mode obtains the lead iodide with a thickness of 500nm/cesium bromide film layer, then revolves in lead iodide/cesium bromide film layer
The alcohol mixed solution of FAI and FABr is applied, 150 DEG C of annealing obtain perovskite absorbed layer.
9): preparing the mixed layer of C60/FLi by the way of common thermal evaporation on perovskite absorbed layer, obtain thickness
For the electron transfer layer of 50nm.
10): the first conductive layer of FTO, preparation condition being prepared using the first magnetron sputtering method on the electron transport layer are as follows:
Reaction gas: oxygen and argon gas, wherein the content of oxygen is 1.3%；Magnetron sputtering power: 1.6kw, with a thickness of
22nm；
11): the second conductive layer of FTO, reaction condition being prepared using the second magnetron sputtering method on the first conductive layer of FTO are as follows:
Oxygen and argon gas, wherein the content of oxygen is 3.5%；Magnetron sputtering power: 4kw, with a thickness of 80nm；
12): top electrode Au electrode layer being prepared using vapour deposition method on the second conductive layer of FTO, with a thickness of 80nm.
Embodiment 7
Perovskite as shown in Figure 4/silicon heterogenous solar energy laminated cell structure chart, including the bottom electricity being sequentially arranged
Pole 1, third conductive layer 2, the non-silicon layer 31 of N-type, the first intrinsic amorphous silicon layer 32, n type single crystal silicon layer 33, the second intrinsic amorphous
Silicon layer 34, P-type non-crystalline silicon layer 35, tunnel layer 4, electron transfer layer 5, perovskite absorbed layer 6, hole transmission layer 7,81- first are led
Electric layer, the second conductive layer of 82-, top electrode 9, specific preparation process is as follows:
1): preparing n type single crystal silicon layer: n type single crystal silicon substrate being placed in KOH solution and is corroded, clean, obtain thickness
The n type single crystal silicon layer that degree is 150 μm；
2): the first intrinsic amorphous silicon layer and N-type amorphous silicon being sequentially depositing using PECVD at the back side of n type single crystal silicon layer
Layer, obtains the first intrinsic non-silicon crystal layer with a thickness of 5nm and the intrinsic non-silicon layer of N-type with a thickness of 10nm；
3): the second intrinsic amorphous silicon layer and P-type non-crystalline silicon being sequentially depositing using PECVD in the front of n type single crystal silicon layer
Layer, obtains the second intrinsic non-silicon layer with a thickness of 5nm and the intrinsic non-silicon layer of p-type with a thickness of 10nm；
4): the magnetron sputtering ITO on the non-silicon layer of N-type obtains the third conductive layer with a thickness of 100nm.
5): hearth electrode Ag electrode layer being prepared using vapour deposition method on third conductive layer, with a thickness of 80nm.
6): P being sequentially depositing using PECVD on P-type non-crystalline silicon layer+、N+Nanocrystal silicon tunnel junctions, obtain with a thickness of
The tunnel layer of 10nm.
7): spin coating SnO on the tunneling layer2, obtain the electron transfer layer with a thickness of 100nm.
8): preparing perovskite absorbed layer on the electron transport layer: on the electron transport layer using lead iodide and cesium bromide
Vacuum thermal evaporation mode obtains the lead iodide with a thickness of 500nm/cesium bromide film layer, then revolves in lead iodide/cesium bromide film layer
Apply the alcohol mixed solution of FAI and FABr, 150 DEG C of annealing.
9): the spin coating PTAA on perovskite absorbed layer obtains the hole transmission layer with a thickness of 100nm.
10): the first conductive layer of AZO, preparation condition being prepared using the first magnetron sputtering method on the hole transport layer are as follows:
Reaction gas: oxygen and argon gas, wherein the content of oxygen is 1.6%；Magnetron sputtering power: 1.7kw, with a thickness of
26nm。
11): the second conductive layer of AZO, reaction condition being prepared using the second magnetron sputtering method on the first conductive layer of AZO are as follows:
Oxygen and argon gas, wherein the content of oxygen is 3.2%；Magnetron sputtering power: 4.2kw, with a thickness of 150nm.
12): top electrode Au electrode layer being prepared using vapour deposition method on the second conductive layer of AZO, with a thickness of 80nm.
Comparative example 1
Perovskite as shown in Figure 5/silicon heterogenous solar energy laminated cell structure chart, including the bottom electricity set gradually
Pole 1, third conductive layer 2, the non-silicon layer 35 of p-type, the first intrinsic amorphous silicon layer 32, n type single crystal silicon layer 33, the second intrinsic amorphous
Silicon layer 34, N-type non-crystalline silicon layer 31, tunnel layer 4, hole transmission layer 7, perovskite absorbed layer 6, electron transfer layer 5, inorganic layer 10,
4th conductive layer 11, top electrode 9, specific preparation method as described in the preparation method of embodiment 1, the difference is that:
11): in MoO3On inorganic layer, magnetron sputtering prepares the 4th conductive layer of ITO, preparation condition are as follows:
Reaction gas: oxygen and argon gas, wherein the content of oxygen is 3.5%；Magnetron sputtering power: 4kw, with a thickness of
130nm。
12): on the 4th conductive layer of ITO, vacuum evaporation prepares top electrode Ag back electrode layer, with a thickness of 80nm.
Comparative example 2
Perovskite as shown in FIG. 6/silicon heterogenous solar energy laminated cell structure chart, including the bottom electricity set gradually
Pole 1, third conductive layer 2, the non-silicon layer 31 of N-type, the first intrinsic amorphous silicon layer 32, n type single crystal silicon layer 33, the second intrinsic amorphous
Silicon layer 34, P-type non-crystalline silicon layer 35, tunnel layer 4, electron transfer layer 5, perovskite absorbed layer 6, hole transmission layer 7, inorganic layer 10,
4th conductive layer 11, top electrode 9, specific preparation method as described in the preparation method of embodiment 5, the difference is that:
11): in MoO3On inorganic layer, magnetron sputtering method prepares the 4th conductive layer of AZO, preparation condition are as follows:
Reaction gas: oxygen and argon gas, wherein the content of oxygen is 3.6%；Magnetron sputtering power: 4.2kw, with a thickness of
140nm。
12): top electrode Au electrode layer being prepared using vapour deposition method on the 4th conductive layer of AZO, with a thickness of 80nm.
Comparative example 3
Perovskite as shown in Figure 7/silicon heterogenous solar energy laminated cell structure chart, including the bottom electricity set gradually
Pole 1, third conductive layer 2, the non-silicon layer 35 of p-type, the first intrinsic amorphous silicon layer 32, n type single crystal silicon layer 33, the second intrinsic amorphous
Silicon layer 34, N-type non-crystalline silicon layer 31, tunnel layer 4, hole transmission layer 7, perovskite absorbed layer 6, electron transfer layer the 5, the 4th are conductive
Layer 11, top electrode 9, specific preparation step is as described in Example 6, the difference is that:
10): the 4th conductive layer of FTO, preparation condition being prepared using magnetron sputtering method on the electron transport layer are as follows:
Reaction gas: oxygen and argon gas, wherein the content of oxygen is 3.5%；Magnetron sputtering power: 4kw, with a thickness of
102nm；
11): top electrode Au electrode layer being prepared using vapour deposition method on the 4th conductive layer of FTO, with a thickness of 80nm.
Comparative example 4
Perovskite as shown in Figure 8/silicon heterogenous solar energy laminated cell structure chart, including the bottom electricity being sequentially arranged
Pole 1, third conductive layer 2, the non-silicon layer 31 of N-type, the first intrinsic amorphous silicon layer 32, n type single crystal silicon layer 33, the second intrinsic amorphous
Silicon layer 34, P-type non-crystalline silicon layer 35, tunnel layer 4, electron transfer layer 5, perovskite absorbed layer 6, hole transmission layer the 7, the 4th are conductive
Layer 11, top electrode 9, specific preparation step is as described in Example 7, the difference is that:
10): the 4th conductive layer of AZO, preparation condition being prepared using magnetron sputtering method on the hole transport layer are as follows:
Reaction gas: oxygen and argon gas, wherein the content of oxygen is 3.2%；Magnetron sputtering power: 4.2kw, with a thickness of
176nm。
11): top electrode Au electrode layer being prepared using vapour deposition method on the 4th conductive layer of AZO, with a thickness of 80nm.
Experimental result and analysis
The characterization of perovskite solar cell module: perovskite solar battery prepared in embodiment uses
Keithley2400SMU, AM 1.5Gsolar irradiation are in 100mW/cm2Light source under carry out device detection, gained
Test data is as shown in table 1 below:
1 perovskite solar cell properties of table test table
| Current density (mA/cm2) | Voltage (V) | Fill factor (%) | PCE (%) | |
| Embodiment 1 | 17.89 | 1.6668 | 59.99 | 17.89 |
| Embodiment 2 | 19.55 | 1.6225 | 58.21 | 18.46 |
| Embodiment 3 | 19.81 | 1.7006 | 59.95 | 20.19 |
| Embodiment 4 | 18.03 | 1.6019 | 58.51 | 17.91 |
| Embodiment 5 | 17.37 | 1.5948 | 67.12 | 18.80 |
| Embodiment 6 | 16.31 | 1.5273 | 58.31 | 16.77 |
| Embodiment 7 | 16.96 | 1.5565 | 57.29 | 16.60 |
| Comparative example 1 | 20.31 | 1.4489 | 42.77 | 10.00 |
| Comparative example 2 | 17.24 | 1.5270 | 35.35 | 9.31 |
| Comparative example 3 | 16.56 | 1.5061 | 55.47 | 7.40 |
| Comparative example 4 | 12.49 | 1.5798 | 53.25 | 4.95 |
Embodiment 1-5 is prepared by the preparation method using hetero-junctions perovskite solar battery provided by the present invention
Solar energy laminated cell.By embodiment 1 and comparative example 1, embodiment 5 and comparative example 2 it was found that, embodiment 1 and 5
Fill factor be apparently higher than comparative example 1 and 2, illustrate to prepare solar energy laminated cell using method provided by the present invention
When, it is smaller to the damage of the functional layer of perovskite battery.In comparative example 1 and 2, perovskite top battery functi on layer surface by
It destroys, the photoelectric conversion efficiency of prepared laminated cell rapidly declines.
In embodiment 1-5, the electric conductivity of different conductive layers is different, and wherein ITO performance is relatively preferable, and current density is most
Height, prepared perovskite/silicon heterogenous battery photoelectric conversion efficiency is up to 20.19%.
Inorganic layer is eliminated in embodiment 6 and embodiment 7, in the presence of no inorganic layer, using institute of the present invention
The preparation method of offer protects other functional layers (electron transfer layer, hole biography of perovskite battery to a certain extent
Defeated layer and perovskite absorbed layer), photoelectric conversion efficiency compared to for comparative example 3 and 4 have be obviously improved.
Although disclosed herein embodiment it is as above, the content only for ease of understanding the present invention and use
Embodiment, be not intended to limit the invention.Technical staff in any fields of the present invention, is not departing from the present invention
Under the premise of disclosed spirit and scope, any modification and variation, but this can be carried out in the form and details of implementation
The scope of patent protection of invention, still should be subject to the scope of the claims as defined in the appended claims.
Claims (13)
1. a kind of preparation method of hetero-junctions perovskite solar battery characterized by comprising
The first conductive layer is prepared using the first sputtering method in the functional layer of perovskite top battery；
The second conductive layer is prepared using the second sputtering method on first conductive layer, the sputtering power of first sputtering method is small
In the sputtering power of second sputtering method.
2. the preparation method of hetero-junctions perovskite solar battery according to claim 1, which is characterized in that described
After preparing the second conductive layer using the second sputtering method on one conductive layer, the method, further includes:
Top electrode is prepared on the second conductive layer.
3. the preparation method of hetero-junctions perovskite solar battery according to claim 1 or 2, which is characterized in that described
The power of first sputtering method is 1kw-2kw, and the power of second sputtering method is greater than or equal to 4kw.
4. the preparation method of hetero-junctions perovskite solar battery according to claim 3, which is characterized in that described first
The reaction gas of sputtering method is mixed gas or oxygen, the mixed gas of argon gas and hydrogen of oxygen and argon gas；
The reaction gas of second sputtering method is the mixing of the mixed gas or oxygen, argon gas and hydrogen of oxygen and argon gas
Gas.
5. the preparation method of hetero-junctions perovskite solar battery according to claim 4, which is characterized in that described first
The oxygen content of the reaction gas of sputtering method is less than the oxygen content of the reaction gas of second sputtering method.
6. the preparation method of hetero-junctions perovskite solar battery according to claim 5, which is characterized in that described first
The oxygen content of the reaction gas of sputtering method is 1.5%-2%, and the oxygen content of the reaction gas of second sputtering method is 3%-
4%.
7. a kind of solar energy laminated cell, including bottom battery and perovskite top battery, which is characterized in that the perovskite top electricity
Pond, comprising: be sequentially arranged on the bottom battery functional layer, using the first conductive layer of the first sputtering method preparation and using the
Second conductive layer of two sputtering methods preparation, wherein the sputtering power of first sputtering method is less than the sputtering of second sputtering method
Power.
8. solar energy laminated cell according to claim 7, which is characterized in that the functional layer include electron transfer layer,
Perovskite absorbed layer, hole transmission layer and inorganic layer, first conductive layer are set on the inorganic layer.
9. solar energy laminated cell according to claim 7, which is characterized in that perovskite top battery further includes top electricity
Pole, the top electrode are set on second conductive layer.
10. according to the described in any item solar energy laminated cells of claim 7-9, which is characterized in that first conductive layer
With a thickness of 20nm-30nm, second conductive layer with a thickness of 80nm-280nm.
11. solar energy laminated cell according to claim 7, which is characterized in that the work function of first conductive layer is small
In the work function of second conductive layer.
12. solar energy laminated cell according to claim 11, which is characterized in that the sheet resistance of first conductive layer is 30
Ω/cm2-60Ω/cm2, the sheet resistance of second conductive layer is 70 Ω/cm2-100Ω/cm2。
13. solar energy laminated cell according to claim 12, which is characterized in that the light transmittance of first conductive layer is
60%-90%, the light transmittance of second conductive layer are 70%-90%.
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| CN115996583A (en) * | 2023-03-24 | 2023-04-21 | 西安电子科技大学 | Perovskite/silicon laminated solar cell and preparation method thereof |
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| CN115996583A (en) * | 2023-03-24 | 2023-04-21 | 西安电子科技大学 | Perovskite/silicon laminated solar cell and preparation method thereof |
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