CN108023021B - silicon-Spiro-OMeTAD heterojunction photovoltaic cell and preparation method thereof - Google Patents
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Abstract
The invention relates to a silicon-Spiro-OMeTAD heterojunction photovoltaic cell and a preparation method thereof. The preparation method of the silicon-Spiro-OMeTAD heterojunction photovoltaic cell comprises the following steps: cleaning the n-type silicon substrate; carrying out surface methylation treatment on the n-type silicon substrate; preparing a Spiro-OMeTAD layer; preparing a Spiro-OMeTAD/PEDOT PSS composite layer; preparing a PSS layer; preparing a front electrode; and preparing a back electrode, wherein the Spiro-OMeTAD layer and the Spiro-OMeTAD/PEDOT PSS composite layer both contain zirconium diselenide nanosheets and tantalum diselenide nanosheets. The synergy between layers in the silicon-Spiro-OMeTAD heterojunction photovoltaic cell enables the cell to have excellent photoelectric conversion efficiency.
Description
Technical Field
The invention relates to the technical field of photovoltaic cells, in particular to a silicon-cyclone-OMeTAD heterojunction photovoltaic cell and a preparation method thereof.
Background
With the high development of industry and the continuous increase of population, energy problems become key problems restricting the development of human beings. The solar energy is energy which is accumulated in nuclear fusion in the sun and can be exploded to radiate outwards, and compared with the traditional energy, the solar energy is inexhaustible. How to fully utilize solar energy to make solar energy really replace petrochemical energy becomes the most important source of energy consumption of all mankind, and has become the research focus of people. At present, there are two main ways of utilizing solar energy: photothermal conversion and photoelectric conversion. The most important representative of the photothermal conversion is a solar water heater, and the best application mode of the photoelectric conversion is a solar cell.
The photoelectric conversion efficiency of the monocrystalline silicon solar cell and the polycrystalline silicon solar cell is excellent, the cost of the monocrystalline silicon solar cell and the polycrystalline silicon solar cell is high due to the complex and tedious preparation process of the monocrystalline silicon solar cell and the polycrystalline silicon solar cell, and the problem that the photoelectric conversion efficiency of the amorphous silicon thin film solar cell is attenuated along with the increase of illumination time is not properly solved. The organic-inorganic hybrid silicon heterojunction solar cell attracts people's attention due to simple preparation process, however, the existing organic-inorganic hybrid silicon heterojunction solar cell has low photoelectric conversion efficiency.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provides a silicon-Spiro-OMeTAD heterojunction photovoltaic cell and a preparation method thereof.
In order to achieve the above object, the present invention provides a method for preparing a silicon-Spiro-OMeTAD heterojunction photovoltaic cell, comprising the following steps: (1) cleaning the n-type silicon substrate; (2) passivating the surface of the n-type silicon substrate; (3) preparation of a Spiro-OMeTAD layer: spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets and Spiro-OMeTAD on the front side of the n-type silicon substrate obtained in the step (2), wherein the spin-coating rotation speed is 2000-3000 r/min, and then performing annealing treatment to form the Spiro-OMeTAD layer; (4) preparation of Spiro-OMeTAD/PEDOT PSS composite layer: sequentially spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets and Spiro-OMeTAD and a PEDOT (PSS) solution on the surface of the Spiro-OMeTAD layer at the spin-coating speed of 3500-4000 rpm, and then carrying out annealing treatment to form the Spiro-OMeTAD/PEDOT (PSS) composite layer; (5) preparation of PEDOT: PSS layer: and spin-coating PEDOT on the surface of the Spiro-OMeTAD/PEDOT composite layer: PSS solution, the spin coating speed is 2000-2500 rpm, then annealing treatment is carried out, and the PEDOT PSS layer is formed; (6) preparing a front electrode; (7) preparing a back electrode; wherein the concentration of the zirconium diselenide nanosheets in the mixed solution in the steps (3) and (4) is 0.1-0.5mg/ml, the concentration of the tantalum diselenide nanosheets is 0.1-0.5mg/ml, the concentration of Spiro-OMeTAD is 10-15mg/ml, and the concentration of PEDOT: PSS in the PEDOT: PSS solution in the steps (4) and (5) is 8-12 mg/ml.
Preferably, the cleaning of the n-type silicon substrate in the step (1) includes: and ultrasonically cleaning the n-type silicon substrate in acetone, ethanol and deionized water in sequence, and then blowing the n-type silicon substrate by using nitrogen for later use.
Preferably, the surface passivation treatment of the n-type silicon substrate in the step (2) includes: the n-type silicon substrate is subjected to a methylation process to form Si-CH3 bonds to passivate the silicon surface.
Preferably, the annealing temperature of the annealing treatment in the step (3) is 100-110 ℃ and the annealing time is 10-20 minutes; the annealing temperature of the annealing treatment in the step (4) is 90-100 ℃, and the annealing time is 5-10 minutes; the annealing temperature of the annealing treatment in the step (5) is 110-120 ℃, and the annealing time is 10-20 minutes.
Preferably, the front electrode in the step (6) is a silver gate electrode, and the thickness of the front electrode is 100-150 nm.
Preferably, the back electrode in the step (7) is an aluminum electrode, and the thickness of the back electrode is 200 nm-300 nm.
The invention also provides a silicon-Spiro-OMeTAD heterojunction photovoltaic cell which is prepared by the method.
Compared with the prior art, the invention has the following advantages:
in the silicon-Spiro-OMeTAD heterojunction photovoltaic cell, the Spiro-OMeTAD layer contains the zirconium diselenide nanosheets and the tantalum diselenide nanosheets, so that the contact performance between the Si/Spiro-OMeTAD heterojunction can be adjusted, the built-in electric field is improved, the conductivity of the Spiro-OMeTAD layer is improved, the separation and the transmission of electron hole pairs are facilitated, and the open-circuit voltage of the silicon-Spiro-OMeTAD heterojunction photovoltaic cell is improved.
A layer of Spiro-OMeTAD/PEDOT: PSS composite layer is arranged between the Spiro-OMeTAD layer and the PEDOT: PSS layer, the composite layer is formed by spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets, Spiro-OMeTAD and PEDOT: PSS solution in sequence and then annealing together, the zirconium diselenide nanosheets, tantalum diselenide nanosheets, Spiro-OMeTAD and PEDOT: PSS are mixed with each other in the annealing process to form a uniform and compact composite layer, the contact performance between the Spiro-OMeTAD layer and the PEDOT: PSS layer is improved, holes in the Spiro-OMeTAD layer can be rapidly transmitted to the PEDOT: PSS layer through the composite layer and then collected by a front electrode, the short-circuit current and the filling factor of the silicon-Spiro-OMeTAD heterojunction photovoltaic cell are improved, photoelectric conversion can be stably and efficiently carried out, specific process parameters of each step are optimized, the photoelectric conversion efficiency of the silicon-Spiro-OMeTAD heterojunction photovoltaic cell is up to 13.7%.
Drawings
Fig. 1 is a schematic structural diagram of a silicon-Spiro-OMeTAD heterojunction photovoltaic cell of the present invention.
Detailed Description
The preparation method of the silicon-Spiro-OMeTAD heterojunction photovoltaic cell provided by the specific embodiment of the invention comprises the following steps: (1) cleaning the n-type silicon substrate; (2) passivating the surface of the n-type silicon substrate; (3) preparation of a Spiro-OMeTAD layer: spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets and Spiro-OMeTAD on the front side of the n-type silicon substrate obtained in the step (2), wherein the spin-coating rotation speed is 2000-3000 r/min, and then performing annealing treatment to form the Spiro-OMeTAD layer; (4) preparation of Spiro-OMeTAD/PEDOT PSS composite layer: sequentially spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets and Spiro-OMeTAD and a PEDOT (PSS) solution on the surface of the Spiro-OMeTAD layer at the spin-coating speed of 3500-4000 rpm, and then carrying out annealing treatment to form the Spiro-OMeTAD/PEDOT (PSS) composite layer; (5) preparation of PEDOT: PSS layer: and spin-coating PEDOT on the surface of the Spiro-OMeTAD/PEDOT composite layer: PSS solution, the spin coating speed is 2000-2500 rpm, then annealing treatment is carried out, and the PEDOT PSS layer is formed; (6) preparing a front electrode; (7) preparing a back electrode; wherein the concentration of the zirconium diselenide nanosheets in the mixed solution in the steps (3) and (4) is 0.1-0.5mg/ml, the concentration of the tantalum diselenide nanosheets is 0.1-0.5mg/ml, the concentration of Spiro-OMeTAD is 10-15mg/ml, and the concentration of PEDOT: PSS in the PEDOT: PSS solution in the steps (4) and (5) is 8-12 mg/ml.
Wherein the cleaning of the n-type silicon substrate in the step (1) comprises: and ultrasonically cleaning the n-type silicon substrate in acetone, ethanol and deionized water in sequence, and then blowing the n-type silicon substrate by using nitrogen for later use. The surface passivation treatment of the n-type silicon substrate in the step (2) includes: the n-type silicon substrate is subjected to a methylation process to form Si-CH3 bonds to passivate the silicon surface. The annealing temperature of the annealing treatment in the step (3) is 100-110 ℃ and the annealing time is 10-20 minutes; the annealing temperature of the annealing treatment in the step (4) is 90-100 ℃, and the annealing time is 5-10 minutes; the annealing temperature of the annealing treatment in the step (5) is 110-120 ℃, and the annealing time is 10-20 minutes. The front electrode in the step (6) is a silver gate electrode, and the thickness of the front electrode is 100-150 nm. The back electrode in the step (7) is an aluminum electrode, and the thickness of the back electrode is 200 nm-300 nm.
As shown in fig. 1, the silicon-Spiro-OMeTAD heterojunction photovoltaic cell prepared by the method comprises a back electrode 1, an n-type silicon substrate 2, a Spiro-OMeTAD layer 3, a Spiro-OMeTAD/PEDOT: PSS composite layer 4, a PEDOT: PSS layer 5 and a front electrode 6 from bottom to top.
Example 1:
a preparation method of a silicon-Spiro-OMeTAD heterojunction photovoltaic cell comprises the following steps: (1) cleaning the n-type silicon substrate; (2) passivating the surface of the n-type silicon substrate; (3) preparation of a Spiro-OMeTAD layer: spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets and Spiro-OMeTAD on the front side of the n-type silicon substrate obtained in the step (2), wherein the spin-coating rotation speed is 2500 rpm, and then performing annealing treatment to form a Spiro-OMeTAD layer; (4) preparation of Spiro-OMeTAD/PEDOT PSS composite layer: sequentially spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets and Spiro-OMeTAD and a PEDOT (PSS) solution on the surface of the Spiro-OMeTAD layer at the spin-coating speed of 3800 r/min, and then carrying out annealing treatment to form the Spiro-OMeTAD/PEDOT (PSS) composite layer; (5) preparation of PEDOT: PSS layer: and spin-coating PEDOT on the surface of the Spiro-OMeTAD/PEDOT composite layer: the PSS solution is spin-coated at 2300 rpm, and then annealing treatment is carried out to form the PEDOT, namely the PSS layer; (6) preparing a front electrode; (7) preparing a back electrode; wherein the concentration of zirconium diselenide nanosheets in the mixed solution in steps (3) and (4) is 0.3mg/ml, the concentration of tantalum diselenide nanosheets is 0.3mg/ml, the concentration of Spiro-OMeTAD is 12mg/ml, and the concentration of PEDOT: PSS in the PEDOT: PSS solution in steps (4) and (5) is 10 mg/ml.
Wherein the cleaning of the n-type silicon substrate in the step (1) comprises: and ultrasonically cleaning the n-type silicon substrate in acetone, ethanol and deionized water in sequence, and then blowing the n-type silicon substrate by using nitrogen for later use. The surface passivation treatment of the n-type silicon substrate in the step (2) includes: the n-type silicon substrate is subjected to a methylation process to form Si-CH3 bonds to passivate the silicon surface. The annealing temperature of the annealing treatment in the step (3) is 105 ℃ and the annealing time is 15 minutes; the annealing temperature of the annealing treatment in the step (4) is 95 ℃, and the annealing time is 7 minutes; the annealing temperature of the annealing treatment in the step (5) is 115 ℃, and the annealing time is 15 minutes. The front electrode in the step (6) is a silver gate electrode, and the thickness of the front electrode is 120 nm. The back electrode in the step (7) is an aluminum electrode, and the thickness of the back electrode is 270 nm.
The open-circuit voltage of the silicon-Spiro-OMeTAD heterojunction photovoltaic cell prepared by the method is 0.6V, and the short-circuit current is 30.5mA/cm2The fill factor was 0.75, and the photoelectric conversion efficiency was 13.7%.
Example 2
A preparation method of a silicon-Spiro-OMeTAD heterojunction photovoltaic cell comprises the following steps: (1) cleaning the n-type silicon substrate; (2) passivating the surface of the n-type silicon substrate; (3) preparation of a Spiro-OMeTAD layer: spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets and Spiro-OMeTAD on the front side of the n-type silicon substrate obtained in the step (2), wherein the spin-coating rotation speed is 2000-3000 r/min, and then performing annealing treatment to form the Spiro-OMeTAD layer; (4) preparation of Spiro-OMeTAD/PEDOT PSS composite layer: sequentially spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets and Spiro-OMeTAD and a PEDOT (PSS) solution on the surface of the Spiro-OMeTAD layer at the spin-coating speed of 3500 rpm, and then carrying out annealing treatment to form the Spiro-OMeTAD/PEDOT (PSS) composite layer; (5) preparation of PEDOT: PSS layer: and spin-coating PEDOT on the surface of the Spiro-OMeTAD/PEDOT composite layer: PSS solution, the spin coating speed is 2000 r/min, then annealing treatment is carried out, and the PEDOT, PSS layer is formed; (6) preparing a front electrode; (7) preparing a back electrode; wherein the concentration of zirconium diselenide nanosheets in the mixed solution in steps (3) and (4) is 0.1mg/ml, the concentration of tantalum diselenide nanosheets is 0.1mg/ml, the concentration of Spiro-OMeTAD is 10mg/ml, and the concentration of PEDOT: PSS in the PEDOT: PSS solution in steps (4) and (5) is 8 mg/ml.
Wherein the cleaning of the n-type silicon substrate in the step (1) comprises: and ultrasonically cleaning the n-type silicon substrate in acetone, ethanol and deionized water in sequence, and then blowing the n-type silicon substrate by using nitrogen for later use. The surface passivation treatment of the n-type silicon substrate in the step (2) includes: the n-type silicon substrate is subjected to a methylation process to form Si-CH3 bonds to passivate the silicon surface. The annealing temperature of the annealing treatment in the step (3) is 100 ℃ and the annealing time is 10 minutes; the annealing temperature of the annealing treatment in the step (4) is 90 ℃, and the annealing time is 5 minutes; the annealing temperature of the annealing treatment in the step (5) is 110 ℃, and the annealing time is 20 minutes. The front electrode in the step (6) is a silver gate electrode, and the thickness of the front electrode is 100 nanometers. The back electrode in the step (7) is an aluminum electrode, and the thickness of the back electrode is 200 nm.
The open-circuit voltage of the silicon-Spiro-OMeTAD heterojunction photovoltaic cell prepared by the method is 0.58V, and the short-circuit current is 29mA/cm2The fill factor was 0.7 and the photoelectric conversion efficiency was 11.8%.
Example 3
A preparation method of a silicon-Spiro-OMeTAD heterojunction photovoltaic cell comprises the following steps: (1) cleaning the n-type silicon substrate; (2) passivating the surface of the n-type silicon substrate; (3) preparation of a Spiro-OMeTAD layer: spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets and Spiro-OMeTAD on the front side of the n-type silicon substrate obtained in the step (2), wherein the spin-coating rotation speed is 2000-3000 r/min, and then performing annealing treatment to form the Spiro-OMeTAD layer; (4) preparation of Spiro-OMeTAD/PEDOT PSS composite layer: sequentially spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets and Spiro-OMeTAD and a PEDOT (PSS) solution on the surface of the Spiro-OMeTAD layer at the spin-coating speed of 4000 revolutions per minute, and then carrying out annealing treatment to form the Spiro-OMeTAD/PEDOT (PSS) composite layer; (5) preparation of PEDOT: PSS layer: and spin-coating PEDOT on the surface of the Spiro-OMeTAD/PEDOT composite layer: PSS solution, the spin coating speed is 2500 rpm, then annealing treatment is carried out, and the PEDOT, PSS layer is formed; (6) preparing a front electrode; (7) preparing a back electrode; wherein the concentration of zirconium diselenide nanosheets in the mixed solution in steps (3) and (4) is 0.5mg/ml, the concentration of tantalum diselenide nanosheets is 0.5mg/ml, the concentration of Spiro-OMeTAD is 15mg/ml, and the concentration of PEDOT: PSS in the PEDOT: PSS solution in steps (4) and (5) is 12 mg/ml.
Wherein the cleaning of the n-type silicon substrate in the step (1) comprises: and ultrasonically cleaning the n-type silicon substrate in acetone, ethanol and deionized water in sequence, and then blowing the n-type silicon substrate by using nitrogen for later use. The surface passivation treatment of the n-type silicon substrate in the step (2) includes: the n-type silicon substrate is subjected to a methylation process to form Si-CH3 bonds to passivate the silicon surface. The annealing temperature of the annealing treatment in the step (3) is 110 ℃ and the annealing time is 15 minutes; the annealing temperature of the annealing treatment in the step (4) is 100 ℃, and the annealing time is 10 minutes; the annealing temperature of the annealing treatment in the step (5) is 120 ℃, and the annealing time is 20 minutes. The front electrode in the step (6) is a silver gate electrode, and the thickness of the front electrode is 150 nm. The back electrode in the step (7) is an aluminum electrode, and the thickness of the back electrode is 300 nanometers.
The open-circuit voltage of the silicon-Spiro-OMeTAD heterojunction photovoltaic cell prepared by the method is 0.57V, and the short-circuit current is 28.5mA/cm2The fill factor was 0.67, and the photoelectric conversion efficiency was 10.9%.
Comparative example:
by way of comparison, a method of fabricating a silicon-Spiro-OMeTAD heterojunction photovoltaic cell, comprising the steps of: (1) cleaning the n-type silicon substrate; (2) passivating the surface of the n-type silicon substrate; (3) preparation of a Spiro-OMeTAD layer: spin-coating a Spiro-OMeTAD solution on the front surface of the n-type silicon substrate obtained in the step (2), wherein the spin-coating rotation speed is 2500 rpm, and then performing annealing treatment to form the Spiro-OMeTAD layer; (4) preparation of PEDOT: PSS layer: and (3) spin coating PEDOT on the surface of the Spiro-OMeTAD layer: the PSS solution is spin-coated at 2300 rpm, and then annealing treatment is carried out to form the PEDOT, namely the PSS layer; (5) preparing a front electrode; (6) preparing a back electrode; wherein the concentration of Spiro-OMeTAD in the Spiro-OMeTAD solution is 12mg/ml, and the concentration of PEDOT to PSS in the PEDOT to PSS solution is 10 mg/ml.
Wherein the cleaning of the n-type silicon substrate in the step (1) comprises: and ultrasonically cleaning the n-type silicon substrate in acetone, ethanol and deionized water in sequence, and then blowing the n-type silicon substrate by using nitrogen for later use. The surface passivation treatment of the n-type silicon substrate in the step (2) includes: the n-type silicon substrate is subjected to a methylation process to form Si-CH3 bonds to passivate the silicon surface. The annealing temperature of the annealing treatment in the step (3) is 105 ℃ and the annealing time is 15 minutes; the annealing temperature of the annealing treatment in the step (4) is 115 ℃, and the annealing time is 25 minutes. The front electrode in the step (5) is a silver gate electrode, and the thickness of the front electrode is 120 nm. The back electrode in the step (6) is an aluminum electrode, and the thickness of the back electrode is 270 nm.
The open-circuit voltage of the silicon-Spiro-OMeTAD heterojunction photovoltaic cell is 0.53V, and the short-circuit current is 24.6mA/cm2The fill factor was 0.55, and the photoelectric conversion efficiency was 7.2%.
While the foregoing is directed to the preferred embodiment of the present invention, it will be understood by those skilled in the art that various changes and modifications may be made without departing from the spirit and scope of the invention.
Claims (6)
1. A preparation method of a silicon-Spiro-OMeTAD heterojunction photovoltaic cell is characterized by comprising the following steps: the method comprises the following steps:
(1) cleaning the n-type silicon substrate;
(2) passivating the surface of the n-type silicon substrate;
(3) preparation of a Spiro-OMeTAD layer: spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets and Spiro-OMeTAD on the front side of the n-type silicon substrate obtained in the step (2), wherein the spin-coating rotation speed is 2000-3000 r/min, and then performing annealing treatment to form the Spiro-OMeTAD layer;
(4) preparation of Spiro-OMeTAD/PEDOT PSS composite layer: sequentially spin-coating a mixed solution containing zirconium diselenide nanosheets, tantalum diselenide nanosheets and Spiro-OMeTAD and a PEDOT (PSS) solution on the surface of the Spiro-OMeTAD layer at the spin-coating speed of 3500-4000 rpm, and then carrying out annealing treatment to form the Spiro-OMeTAD/PEDOT (PSS) composite layer;
(5) preparation of PEDOT: PSS layer: and spin-coating PEDOT on the surface of the Spiro-OMeTAD/PEDOT composite layer: PSS solution, the spin coating speed is 2000-2500 rpm, then annealing treatment is carried out, and the PEDOT PSS layer is formed;
(6) preparing a front electrode;
(7) preparing a back electrode;
wherein the concentration of the zirconium diselenide nanosheets in the mixed solution in the steps (3) and (4) is 0.1-0.5mg/ml, the concentration of the tantalum diselenide nanosheets is 0.1-0.5mg/ml, the concentration of Spiro-OMeTAD is 10-15mg/ml, and the concentration of PEDOT: PSS in the PEDOT solution in the steps (4) and (5) is 8-12 mg/ml; wherein the annealing temperature of the annealing treatment in the step (3) is 100-110 ℃ and the annealing time is 10-20 minutes; the annealing temperature of the annealing treatment in the step (4) is 90-100 ℃, and the annealing time is 5-10 minutes; the annealing temperature of the annealing treatment in the step (5) is 110-120 ℃, and the annealing time is 10-20 minutes.
2. The method of preparing a silicon-Spiro-OMeTAD heterojunction photovoltaic cell of claim 1, wherein: the cleaning of the n-type silicon substrate in the step (1) includes: and ultrasonically cleaning the n-type silicon substrate in acetone, ethanol and deionized water in sequence, and then blowing the n-type silicon substrate by using nitrogen for later use.
3. The method of preparing a silicon-Spiro-OMeTAD heterojunction photovoltaic cell of claim 1, wherein: the surface passivation treatment of the n-type silicon substrate in the step (2) includes: the n-type silicon substrate is subjected to a methylation process to form Si-CH3 bonds to passivate the silicon surface.
4. The method of preparing a silicon-Spiro-OMeTAD heterojunction photovoltaic cell of claim 1, wherein: the front electrode in the step (6) is a silver gate electrode, and the thickness of the front electrode is 100-150 nm.
5. The method of preparing a silicon-Spiro-OMeTAD heterojunction photovoltaic cell of claim 1, wherein: the back electrode in the step (7) is an aluminum electrode, and the thickness of the back electrode is 200 nm-300 nm.
6. A silicon-Spiro-OMeTAD heterojunction photovoltaic cell, wherein the silicon-Spiro-OMeTAD heterojunction photovoltaic cell is a silicon-Spiro-OMeTAD heterojunction photovoltaic cell formed by a method according to any one of claims 1 to 5.
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