CN110364361A - A kind of quantum dot sensitized solar cell and preparation method thereof with graphite phase carbon nitride boundary layer - Google Patents
A kind of quantum dot sensitized solar cell and preparation method thereof with graphite phase carbon nitride boundary layer Download PDFInfo
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- CN110364361A CN110364361A CN201810311306.7A CN201810311306A CN110364361A CN 110364361 A CN110364361 A CN 110364361A CN 201810311306 A CN201810311306 A CN 201810311306A CN 110364361 A CN110364361 A CN 110364361A
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- quantum dot
- boundary layer
- carbon nitride
- phase carbon
- conductive glass
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- 239000002096 quantum dot Substances 0.000 title claims abstract description 107
- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 title claims abstract description 82
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 77
- 229910002804 graphite Inorganic materials 0.000 title claims abstract description 74
- 239000010439 graphite Substances 0.000 title claims abstract description 74
- 238000002360 preparation method Methods 0.000 title claims abstract description 14
- 239000011521 glass Substances 0.000 claims abstract description 109
- 238000006243 chemical reaction Methods 0.000 claims abstract description 62
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims abstract description 39
- 239000003792 electrolyte Substances 0.000 claims abstract description 32
- 238000000034 method Methods 0.000 claims abstract description 28
- 239000000843 powder Substances 0.000 claims abstract description 25
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims abstract description 21
- 239000000178 monomer Substances 0.000 claims abstract description 18
- 239000011259 mixed solution Substances 0.000 claims abstract description 17
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 claims abstract description 16
- VHNQIURBCCNWDN-UHFFFAOYSA-N pyridine-2,6-diamine Chemical compound NC1=CC=CC(N)=N1 VHNQIURBCCNWDN-UHFFFAOYSA-N 0.000 claims abstract description 15
- 239000000203 mixture Substances 0.000 claims abstract description 14
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims abstract description 11
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 claims abstract description 11
- 229910021529 ammonia Inorganic materials 0.000 claims abstract description 10
- 239000000908 ammonium hydroxide Substances 0.000 claims abstract description 9
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 44
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 44
- NPNMHHNXCILFEF-UHFFFAOYSA-N [F].[Sn]=O Chemical compound [F].[Sn]=O NPNMHHNXCILFEF-UHFFFAOYSA-N 0.000 claims description 41
- 235000019441 ethanol Nutrition 0.000 claims description 35
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 28
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 27
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 26
- 239000012298 atmosphere Substances 0.000 claims description 26
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 24
- 238000005245 sintering Methods 0.000 claims description 24
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 claims description 23
- 239000011734 sodium Substances 0.000 claims description 23
- 229910052708 sodium Inorganic materials 0.000 claims description 23
- 229910052757 nitrogen Inorganic materials 0.000 claims description 22
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 20
- 238000010438 heat treatment Methods 0.000 claims description 20
- 239000012528 membrane Substances 0.000 claims description 20
- 239000001301 oxygen Substances 0.000 claims description 20
- 229910052760 oxygen Inorganic materials 0.000 claims description 20
- 239000002002 slurry Substances 0.000 claims description 20
- 239000007788 liquid Substances 0.000 claims description 18
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical group CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 claims description 18
- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 claims description 17
- 239000000919 ceramic Substances 0.000 claims description 16
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 claims description 16
- 238000007747 plating Methods 0.000 claims description 14
- 229910052697 platinum Inorganic materials 0.000 claims description 14
- 239000007789 gas Substances 0.000 claims description 13
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 12
- 229910052980 cadmium sulfide Inorganic materials 0.000 claims description 12
- UMGDCJDMYOKAJW-UHFFFAOYSA-N thiourea Chemical compound NC(N)=S UMGDCJDMYOKAJW-UHFFFAOYSA-N 0.000 claims description 12
- WUPHOULIZUERAE-UHFFFAOYSA-N 3-(oxolan-2-yl)propanoic acid Chemical compound OC(=O)CCC1CCCO1 WUPHOULIZUERAE-UHFFFAOYSA-N 0.000 claims description 11
- 229940116367 cadmium sulfide Drugs 0.000 claims description 11
- 239000003960 organic solvent Substances 0.000 claims description 11
- 230000008569 process Effects 0.000 claims description 11
- 206010070834 Sensitisation Diseases 0.000 claims description 10
- 230000008313 sensitization Effects 0.000 claims description 10
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 9
- 239000006185 dispersion Substances 0.000 claims description 9
- 238000002156 mixing Methods 0.000 claims description 9
- MCMNRKCIXSYSNV-UHFFFAOYSA-N ZrO2 Inorganic materials O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 8
- 239000011812 mixed powder Substances 0.000 claims description 8
- BPUBBGLMJRNUCC-UHFFFAOYSA-N oxygen(2-);tantalum(5+) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ta+5].[Ta+5] BPUBBGLMJRNUCC-UHFFFAOYSA-N 0.000 claims description 8
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 claims description 8
- 239000000243 solution Substances 0.000 claims description 8
- 239000002904 solvent Substances 0.000 claims description 8
- PBCFLUZVCVVTBY-UHFFFAOYSA-N tantalum pentoxide Inorganic materials O=[Ta](=O)O[Ta](=O)=O PBCFLUZVCVVTBY-UHFFFAOYSA-N 0.000 claims description 8
- 238000010792 warming Methods 0.000 claims description 8
- 229920000877 Melamine resin Polymers 0.000 claims description 7
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 7
- UHYPYGJEEGLRJD-UHFFFAOYSA-N cadmium(2+);selenium(2-) Chemical class [Se-2].[Cd+2] UHYPYGJEEGLRJD-UHFFFAOYSA-N 0.000 claims description 7
- 239000004202 carbamide Substances 0.000 claims description 7
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 claims description 7
- PFNQVRZLDWYSCW-UHFFFAOYSA-N (fluoren-9-ylideneamino) n-naphthalen-1-ylcarbamate Chemical compound C12=CC=CC=C2C2=CC=CC=C2C1=NOC(=O)NC1=CC=CC2=CC=CC=C12 PFNQVRZLDWYSCW-UHFFFAOYSA-N 0.000 claims description 6
- MARUHZGHZWCEQU-UHFFFAOYSA-N 5-phenyl-2h-tetrazole Chemical compound C1=CC=CC=C1C1=NNN=N1 MARUHZGHZWCEQU-UHFFFAOYSA-N 0.000 claims description 6
- XZMCDFZZKTWFGF-UHFFFAOYSA-N Cyanamide Chemical compound NC#N XZMCDFZZKTWFGF-UHFFFAOYSA-N 0.000 claims description 6
- LRHPLDYGYMQRHN-UHFFFAOYSA-N N-Butanol Chemical compound CCCCO LRHPLDYGYMQRHN-UHFFFAOYSA-N 0.000 claims description 6
- 239000003795 chemical substances by application Substances 0.000 claims description 6
- QGBSISYHAICWAH-UHFFFAOYSA-N dicyandiamide Chemical compound NC(N)=NC#N QGBSISYHAICWAH-UHFFFAOYSA-N 0.000 claims description 6
- 230000008859 change Effects 0.000 claims description 5
- BDERNNFJNOPAEC-UHFFFAOYSA-N propan-1-ol Chemical compound CCCO BDERNNFJNOPAEC-UHFFFAOYSA-N 0.000 claims description 5
- 239000004408 titanium dioxide Substances 0.000 claims description 5
- SKJCKYVIQGBWTN-UHFFFAOYSA-N (4-hydroxyphenyl) methanesulfonate Chemical compound CS(=O)(=O)OC1=CC=C(O)C=C1 SKJCKYVIQGBWTN-UHFFFAOYSA-N 0.000 claims description 4
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 claims description 4
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 claims description 4
- 229910052793 cadmium Inorganic materials 0.000 claims description 4
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 claims description 4
- ZXEKIIBDNHEJCQ-UHFFFAOYSA-N isobutanol Chemical compound CC(C)CO ZXEKIIBDNHEJCQ-UHFFFAOYSA-N 0.000 claims description 4
- OCGWQDWYSQAFTO-UHFFFAOYSA-N tellanylidenelead Chemical compound [Pb]=[Te] OCGWQDWYSQAFTO-UHFFFAOYSA-N 0.000 claims description 4
- 239000011787 zinc oxide Substances 0.000 claims description 4
- 229910052799 carbon Inorganic materials 0.000 claims description 3
- 150000001875 compounds Chemical class 0.000 claims description 3
- 239000003504 photosensitizing agent Substances 0.000 claims description 3
- GGYFMLJDMAMTAB-UHFFFAOYSA-N selanylidenelead Chemical compound [Pb]=[Se] GGYFMLJDMAMTAB-UHFFFAOYSA-N 0.000 claims description 3
- 150000001298 alcohols Chemical class 0.000 claims description 2
- ZULTVNRFZRQYKL-UHFFFAOYSA-M fluorotin Chemical compound [Sn]F ZULTVNRFZRQYKL-UHFFFAOYSA-M 0.000 claims description 2
- 235000011187 glycerol Nutrition 0.000 claims description 2
- 230000035484 reaction time Effects 0.000 claims description 2
- BUGBHKTXTAQXES-UHFFFAOYSA-N Selenium Chemical compound [Se] BUGBHKTXTAQXES-UHFFFAOYSA-N 0.000 claims 1
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims 1
- 238000001816 cooling Methods 0.000 claims 1
- 238000004321 preservation Methods 0.000 claims 1
- 238000007789 sealing Methods 0.000 claims 1
- 229910052711 selenium Inorganic materials 0.000 claims 1
- 239000011669 selenium Substances 0.000 claims 1
- 239000011701 zinc Substances 0.000 claims 1
- 229910052725 zinc Inorganic materials 0.000 claims 1
- 238000002604 ultrasonography Methods 0.000 abstract description 2
- 230000000712 assembly Effects 0.000 abstract 1
- 238000000429 assembly Methods 0.000 abstract 1
- 238000001027 hydrothermal synthesis Methods 0.000 abstract 1
- 239000010410 layer Substances 0.000 description 54
- 239000008367 deionised water Substances 0.000 description 13
- 229910021641 deionized water Inorganic materials 0.000 description 13
- 238000002791 soaking Methods 0.000 description 12
- 239000004575 stone Substances 0.000 description 8
- 238000011160 research Methods 0.000 description 7
- 238000012360 testing method Methods 0.000 description 7
- 230000009466 transformation Effects 0.000 description 7
- 239000002202 Polyethylene glycol Substances 0.000 description 6
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 6
- 239000007864 aqueous solution Substances 0.000 description 6
- 238000000227 grinding Methods 0.000 description 6
- 238000005259 measurement Methods 0.000 description 6
- 239000004570 mortar (masonry) Substances 0.000 description 6
- 229920001223 polyethylene glycol Polymers 0.000 description 6
- 238000012545 processing Methods 0.000 description 6
- 239000002344 surface layer Substances 0.000 description 6
- 238000004506 ultrasonic cleaning Methods 0.000 description 6
- 239000005864 Sulphur Substances 0.000 description 5
- 238000007790 scraping Methods 0.000 description 5
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 4
- 241000790917 Dioxys <bee> Species 0.000 description 4
- 230000005611 electricity Effects 0.000 description 3
- 230000007246 mechanism Effects 0.000 description 3
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 2
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 2
- 229910052786 argon Inorganic materials 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 2
- 239000011229 interlayer Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 239000002086 nanomaterial Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 239000000758 substrate Substances 0.000 description 2
- 229910052719 titanium Inorganic materials 0.000 description 2
- 239000010936 titanium Substances 0.000 description 2
- 238000004073 vulcanization Methods 0.000 description 2
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 1
- 241000209140 Triticum Species 0.000 description 1
- 235000021307 Triticum Nutrition 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 238000013019 agitation Methods 0.000 description 1
- FRLJSGOEGLARCA-UHFFFAOYSA-N cadmium sulfide Chemical compound [S-2].[Cd+2] FRLJSGOEGLARCA-UHFFFAOYSA-N 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 235000013312 flour Nutrition 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 125000000524 functional group Chemical group 0.000 description 1
- 239000008187 granular material Substances 0.000 description 1
- 238000011065 in-situ storage Methods 0.000 description 1
- MRNHPUHPBOKKQT-UHFFFAOYSA-N indium;tin;hydrate Chemical compound O.[In].[Sn] MRNHPUHPBOKKQT-UHFFFAOYSA-N 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 230000010534 mechanism of action Effects 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- 230000001376 precipitating effect Effects 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000009738 saturating Methods 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- XSOKHXFFCGXDJZ-UHFFFAOYSA-N telluride(2-) Chemical compound [Te-2] XSOKHXFFCGXDJZ-UHFFFAOYSA-N 0.000 description 1
- 238000012876 topography Methods 0.000 description 1
- RMZAYIKUYWXQPB-UHFFFAOYSA-N trioctylphosphane Chemical compound CCCCCCCCP(CCCCCCCC)CCCCCCCC RMZAYIKUYWXQPB-UHFFFAOYSA-N 0.000 description 1
- ZMBHCYHQLYEYDV-UHFFFAOYSA-N trioctylphosphine oxide Chemical compound CCCCCCCCP(=O)(CCCCCCCC)CCCCCCCC ZMBHCYHQLYEYDV-UHFFFAOYSA-N 0.000 description 1
- 238000005303 weighing Methods 0.000 description 1
- GTLQJUQHDTWYJC-UHFFFAOYSA-N zinc;selenium(2-) Chemical compound [Zn+2].[Se-2] GTLQJUQHDTWYJC-UHFFFAOYSA-N 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G13/00—Apparatus specially adapted for manufacturing capacitors; Processes specially adapted for manufacturing capacitors not provided for in groups H01G4/00 - H01G11/00
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/20—Light-sensitive devices
- H01G9/2027—Light-sensitive devices comprising an oxide semiconductor electrode
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/20—Light-sensitive devices
- H01G9/2027—Light-sensitive devices comprising an oxide semiconductor electrode
- H01G9/2031—Light-sensitive devices comprising an oxide semiconductor electrode comprising titanium oxide, e.g. TiO2
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/20—Light-sensitive devices
- H01G9/2027—Light-sensitive devices comprising an oxide semiconductor electrode
- H01G9/204—Light-sensitive devices comprising an oxide semiconductor electrode comprising zinc oxides, e.g. ZnO
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
- Y02E10/542—Dye sensitized solar cells
Landscapes
- Engineering & Computer Science (AREA)
- Power Engineering (AREA)
- Microelectronics & Electronic Packaging (AREA)
- Manufacturing & Machinery (AREA)
- Hybrid Cells (AREA)
- Photovoltaic Devices (AREA)
Abstract
The present invention discloses a kind of quantum dot sensitized solar cell and preparation method thereof with graphite phase carbon nitride boundary layer.The battery by electro-conductive glass, graphite phase carbon nitride boundary layer, oxide porous film, quantum dot light sensitizer, electrolyte and forms electrode.Electro-conductive glass is subjected to hydro-thermal process in nitrogenous organic monomer and the mixed solution of 2,6-diaminopyridine;The mix powder being made of nitrogenous organic monomer, elemental sulfur and phenol is heat-treated in conductive glass surface and in ammonia, pyrolytic reaction occurs at high temperature for mix powder, graphite phase carbon nitride boundary layer is generated in conductive glass surface, it goes to clean with the method for ammonium hydroxide ultrasound, obtain the graphite phase carbon nitride boundary layer of high quality, oxide porous film is prepared again, and through techniques such as quantum dot sensitized-battery assemblies.The setting of graphite phase carbon nitride boundary layer in the present invention improves photoelectric conversion efficiency to inhibit the defeated reaction of back pass in quantum dot sensitized solar cell.
Description
Technical field
The present invention relates to a kind of quantum dot sensitized solar cells and preparation method thereof, in particular, being related to one kind in conduction
One boundary layer being made of graphite phase carbon nitride is set between glass and oxide porous film, to prevent electro-conductive glass and electricity
The contact of solution liquid improves quantum dot sensitized solar cell and its preparation side of photoelectric conversion efficiency to inhibit the defeated reaction of back pass
Method belongs to technical field of solar cells.
Background technique
Solar energy is most possibly replaced due to having the characteristics that " reserves are huge, the time is permanent, environmental-friendly, widely applicable "
For fossil fuel, become the ideal energy form of human future.Currently, people are the manufacture sun using the main method of solar energy
Battery converts solar energy into electric energy and is used.In miscellaneous solar cell, quantum dot sensitized solar cell due to
With many advantages such as photoelectric conversion efficiency is high, preparation process is simple, the prices of raw materials are cheap, receive various countries researcher's
Common concern.
Although quantum dot sensitized solar cell has above-mentioned many advantages, its photoelectric conversion efficiency and business application
Standard is compared and is had a certain gap.Influence the reason of its efficiency further increases first is that back pass existing for inside battery is defeated anti-
It answers.Specifically, quantum dot sensitized solar cell is usually by electro-conductive glass, oxide porous film, quantum dot light sensitizer, electricity
It solves liquid and electrode is formed.And electrolyte therein can be penetrated at electro-conductive glass by the hole in oxide porous film,
And it is compound with the light induced electron generation on electro-conductive glass, form the defeated reaction of so-called back pass.With quantum dot sensitized solar cell
In for the most commonly used more sulphur electrolyte (mixed solution of vulcanized sodium and elemental sulfur), the equation of the defeated reaction of back pass is
[(2x-2)e-+Sx 2-→xS2-], reaction mechanism is as shown in Figure 1.Back pass is defeated to react the effective output for greatly reducing light induced electron,
The photoelectric conversion efficiency of battery is seriously affected.
It can be seen that prevent contact of the electrolyte with electro-conductive glass, answering for light induced electron and electrolyte can be effectively reduced
It closes, inhibits the defeated reaction of back pass, improve the photoelectric conversion efficiency of quantum dot sensitized solar cell.Using in electro-conductive glass and oxide
The method that a boundary layer is arranged between perforated membrane can achieve said effect, but wherein the selection of interlayer materials is for most
The influence of whole battery performance is most important.
Summary of the invention
It is an object of the invention to overcome in the prior art quantum dot sensitized solar cell since the defeated reaction of back pass reduces it
The problem of photoelectric properties, provides a kind of quantum dot sensitized solar cell and preparation method thereof with high light photoelectric transformation efficiency.
The purpose of the present invention is achieved by following technical proposals:
A kind of quantum dot sensitized solar cell with graphite phase carbon nitride boundary layer, from bottom to top by electro-conductive glass, stone
Black phase carbon nitride boundary layer, oxide porous film, quantum dot light sensitizer, electrolyte and to electrode form.
The electro-conductive glass is one of indium tin oxide electro-conductive glass or fluorine tin-oxide electro-conductive glass.
The graphite phase carbon nitride boundary layer is arranged between electro-conductive glass and oxide porous film, with a thickness of 50-
150nm, graphite phase carbon nitride boundary layer are made of graphite phase carbon nitride nanometer sheet, thickness preferably 60-100nm.
The oxide porous film is titanium dioxide porous membrane, stannic oxide perforated membrane, zinc oxide porous film, zirconium dioxide
One of perforated membrane or tantalum pentoxide perforated membrane.
The quantum dot light sensitizer is CdSe quantum dots, cadmiumsulfide quantum dot, cadmium telluride quantum dot, zinc selenide quantum
One in point, ZnS quantum dots, zinc telluride quantum dot, lead selenide quantum dot, vulcanized lead quantum dot or lead telluride quantum dot
Kind.
The electrolyte be vulcanized sodium and elemental sulfur solution, wherein solvent be first alcohol and water mixed solution, methanol and
The volume ratio of water is (1:3)-(3:1), and the molar concentration of vulcanized sodium is 0.1-0.5molL-1, the molar concentration of elemental sulfur is
0.3-0.7mol·L-1, i.e., vulcanized sodium and elemental sulfur are dispersed in mixed solution, the molar concentration of vulcanized sodium (is uniformly divided
The vulcanization na concn being dispersed in mixed solution) it is 0.1-0.5molL-1, elemental sulfur molar concentration (be dispersed in mixing it is molten
Simple substance sulphur concentration in liquid) it is 0.3-0.7molL-1。
In the fluorine tin-oxide electro-conductive glass to indium tin oxide electro-conductive glass or platinum plating that electrode is platinum plating
It is a kind of.
Prepare have graphite phase carbon nitride boundary layer quantum dot sensitized solar cell method, as steps described below into
Row:
Step 1, electro-conductive glass is placed in the autoclave bottom equipped with mixed solution and keeps it conductive up, it is close
It is honored as a queen to be placed under 100-160 degrees Celsius and be reacted, wherein mixed solution is that nitrogenous organic monomer, 2,6-diaminopyridine are equal
Even be dispersed in alcohol organic solvent is prepared, and nitrogenous organic monomer is 10-50 mass parts, and 2,6-diaminopyridine is
50-90 mass parts, alcohol organic solvent be 100-120 parts by volume, nitrogenous organic monomer be melamine, cyanamide, dicyandiamide,
One of urea or thiocarbamide;
In step 1, alcohol organic solvent is the alcohol organic solvent being in a liquid state under 20-25 degrees Celsius of room temperature, such as first
One of alcohol, ethyl alcohol, propyl alcohol, butanol, ethylene glycol, glycerine, isopropanol or isobutanol.
In step 1, nitrogenous organic monomer is 20-35 mass parts, and 2,6-diaminopyridine is 70-80 mass parts, alcohol
Class organic solvent is 100-120 parts by volume, and each mass parts are 1mg, and each parts by volume is 1ml.
In step 1, nitrogenous organic monomer, 2,6-diaminopyridine are dispersed in alcohol organic solvent, in 30-
Ultrasonic mixing 6-10h at 50 DEG C.
In step 1, the electro-conductive glass is in indium tin oxide electro-conductive glass or fluorine tin-oxide electro-conductive glass
It is a kind of.
In step 1, reaction temperature is 120-150 degrees Celsius, and the reaction time is 1-5 hours, preferably 3-5 hours.
In step 1, it to after reaction take out electro-conductive glass, and is cleaned 3-5 times with deionized water.
Step 2, the electro-conductive glass handled by step 1 is placed in ceramic crucible bottom and keeps it conductive up, it will
Mixed-powder is laid on conducting surface, then ceramic crucible is placed in tube-type atmosphere furnace, and pyrolytic reaction is carried out in ammonia atmosphere,
From 20-25 degrees Celsius of room temperature with 5-25 DEG C of min-1Heating rate be warming up to 400-600 DEG C and keep the temperature 1-6 hours, with furnace
20-25 degrees Celsius are cooled to room temperature, wherein mixed-powder is by the nitrogenous organic monomer of 50-130 mass parts, 20-40 mass parts simple substance
Sulphur and 5-25 mass parts phenol composition, nitrogenous organic monomer are one in melamine, cyanamide, dicyandiamide, urea or thiocarbamide
Kind;
In step 2, from 20-25 degrees Celsius of room temperature with 5-10 DEG C of min-1Heating rate be warming up to 460-550 DEG C
And 2-4 hours are kept the temperature, cool to 20-25 degrees Celsius of room temperature with the furnace.
In step 2, mixed-powder is by the nitrogenous organic monomer of 60-120 mass parts, 25-35 mass parts elemental sulfur and 10-20
Mass parts phenol composition, each mass parts are 1mg.
In step 2, mixed-powder is laid on conducting surface, with a thickness of 1-3mm.
Step 3, the electro-conductive glass handled by step 2 is placed in ammonium hydroxide and is cleaned by ultrasonic, in electro-conductive glass table
Wheat flour obtains graphite phase carbon nitride boundary layer;
In step 3, the mass concentration of ammonia is 100-300mgml in ammonium hydroxide-1, it is cleaned by ultrasonic 1-5min.
Step 4, the slurry containing oxide powder is coated in and has graphite phase carbon nitride interface by what step 3 was handled
The conductive glass surface of layer obtains oxide porous film through sintering after slurry is dry, and during the sintering process, atmosphere used is oxygen
The molar ratio of the mixed gas of gas and nitrogen, oxygen and nitrogen is (1:5)-(5:1), from 20-25 degrees Celsius of room temperature with 10-30
℃·min-1Heating rate be warming up to 300-400 DEG C and keep the temperature 30-120min, cool to 20-25 degrees Celsius of room temperature with the furnace;
In step 4, the oxide powder is titania powder, stannic oxide powder, Zinc oxide powder, titanium dioxide
One of zirconium powder or tantalum pentoxide powder.
In step 4, during the sintering process, atmosphere used is the mixed gas of oxygen and nitrogen, and oxygen and nitrogen rub
You are than being (1:3)-(3:1), from 20-25 degrees Celsius of room temperature with 10-20 DEG C of min-1Heating rate be warming up to 340-380 DEG C
And 40-80min is kept the temperature, cool to 20-25 degrees Celsius of room temperature with the furnace.
Step 5, the obtained conduction with graphite phase carbon nitride boundary layer and oxide porous film will be handled by step 4
Glass immerses in quantum dot light sensitization agent dispersing liquid carries out quantum dot sensitized, obtained light anode under the conditions of being protected from light;
In steps of 5, it is cleaned 3-5 times after sensitization with ethyl alcohol.
In steps of 5, the quantum dot light sensitizer in quantum dot light sensitization agent dispersing liquid is CdSe quantum dots, cadmium sulfide
Quantum dot, cadmium telluride quantum dot, zinc selenide quantum dot, ZnS quantum dots, zinc telluride quantum dot, lead selenide quantum dot, vulcanization
One of lead quantum dot or lead telluride quantum dot, solvent are n-hexane, and the mass concentration of quantum dot is 5-30mgml-1It is molten
Agent.In steps of 5, quantum dot sensitized holding 4-6h is carried out under the conditions of being protected from light in quantum dot light sensitization agent dispersing liquid.
Step 6, it by light anode obtained in step 5 and electrolyte, be packaged together to electrode, is finally made with stone
The quantum dot sensitized solar cell of black phase carbon nitride boundary layer.
In step 6, electrolyte is the solution of vulcanized sodium and elemental sulfur, and wherein solvent is the mixed solution of first alcohol and water,
The volume ratio of first alcohol and water is (1:3)-(3:1), and the molar concentration of vulcanized sodium is 0.1-0.5molL-1, elemental sulfur it is mole dense
Degree is 0.3-0.7molL-1。
In step 6, to the fluorine tin-oxide conduction glass of indium tin oxide electro-conductive glass or platinum plating that electrode is platinum plating
One of glass.
Provided preparation method can form a complete, fine and close graphite-phase in conductive glass surface through the invention
Nitrogenize carbon boundary layer.By taking embodiment 1 as an example, observes and finds through field emission scanning electron microscope (Japanese firm, S4800 type):
Prepared graphite phase carbon nitride boundary layer is made of (attached drawing 3b) dense granule, and surface topography is clearly distinguishable from tin indium oxide
Electro-conductive glass (attached drawing 3a).It is measured by atomic force microscope (Asylum Research company, the U.S., MFP-3D-SA type)
Arrive: prepared graphite phase carbon nitride boundary layer with a thickness of 50nm.Through X-ray diffractometer (Japanese Tokyo company, Rigaku
D/max 2500v/pc type) test discovery: prepared boundary layer is to occur two spies at 13.1 ° and 27.3 ° in angle of diffraction
Diffraction maximum is levied, (100) and (002) crystal face of graphite phase carbon nitride is corresponded respectively to, has further confirmed that the boundary layer by graphite
Phase carbon nitride composition, as shown in Fig. 4.
The graphite phase carbon nitride nanometer sheet that the present invention utilizes is a kind of New Two Dimensional nano material that developed recently gets up, tool
There are ideal two-dimensional nanostructure, excellent optical property, surface functional group abundant.It is introduced as interlayer materials saturating
The more complete and good boundary layer of electric conductivity is capable of forming between bright conductive substrates and sull (to be prepared in situ and set
Set), compound (effectively prevent the contact of electrolyte and conductive substrates) of the light induced electron with electrolyte can be effectively reduced, inhibit
The defeated reaction of back pass, the defeated reaction of back pass so as to which quantum dot sensitized solar cell is effectively reduced, improves the quantum dot sensitized sun
The photoelectric conversion performance of battery improves its photoelectric conversion efficiency, and the mechanism of action is as shown in Fig. 2, i.e. graphite phase carbon nitride interface
Application of the layer in quantum dot sensitized solar cell, photoelectric conversion efficiency are 1.5-2.2 times originally.
Detailed description of the invention
Fig. 1 is the defeated reaction mechanism schematic diagram of quantum dot sensitized solar cell back pass, wherein 1: electro-conductive glass;2: photoproduction electricity
Son;3: the oxide porous film of absorption quantum dot photosensitizer;4: the S in electrolytex 2-Ion;5: the S in electrolyte2-Ion.
Fig. 2 is that graphite phase carbon nitride boundary layer inhibits the mechanism of the defeated reaction of back pass in quantum dot sensitized solar cell to illustrate
Figure, wherein 1: electro-conductive glass;2: light induced electron;3: graphite phase carbon nitride boundary layer;4: the oxidation of absorption quantum dot photosensitizer
Object perforated membrane;5: the S in electrolytex 2-Ion;6: the S in electrolyte2-Ion.
Fig. 3 is the SEM photograph of indium tin oxide electro-conductive glass and graphite phase carbon nitride interface layer surfaces pattern, wherein a: indium
Tin-oxide electro-conductive glass;B: graphite phase carbon nitride boundary layer.
Fig. 4 is the X-ray diffraction spectrum of graphite phase carbon nitride boundary layer.
Fig. 5 is the Flied emission transmission electron microscope photo of cadmiumsulfide quantum dot.
Specific embodiment
Technical solution of the present invention is further illustrated combined with specific embodiments below.
Reference implementation example
Quantum dot of the present invention is prepared by solvent thermal reaction, is carried out by taking cadmiumsulfide quantum dot as an example below
Illustrate:
(1) 0.114g caddy, 0.2g trioctyl phosphine oxide are put into the three-neck flask of a 50ml, under protection of argon gas
It is heated to 220 DEG C and keeps the temperature 30min, keep magnetic agitation in the process, form colorless and transparent cadmium presoma.
(2) 0.16g elemental sulfur, 5ml tri octyl phosphine are put into the vial with rubber stopper of a 10ml.Mixture
Flaxen sulphur presoma is formed after ultrasound 10min under protection of argon gas.
(3) sulphur presoma is rapidly injected in cadmium presoma, and the temperature of reaction system is risen to 300 DEG C, keep the temperature 1h.
(4) to after reaction, 20ml ethyl alcohol, which is added in reaction solution, precipitates cadmiumsulfide quantum dot, the precipitating of generation
Be centrifuged, dry after powdered cadmiumsulfide quantum dot is made, it is spare.
Found using Flied emission transmission electron microscope observation: prepared cadmiumsulfide quantum dot crystallinity is high, dispersed
Good, uniform particle sizes (about 5nm), as shown in Fig. 5.
The powdered quantum dot for weighing required quality when in use is dissolved in n-hexane, and quantum dot light sensitizer can be obtained
Dispersion liquid.
Embodiment 1
(1) by the 2,6-diaminopyridine co-dissolve of the melamine of 10mg and 50mg in the methanol of 100ml, and will
System ultrasonic mixing 6h at 30 DEG C.
(2) mixed solution that step (1) obtains is transferred in the autoclave that a volume is 150ml, it then will be a piece of
Indium tin oxide electro-conductive glass is put into the autoclave base, and keeps it conductive up.After autoclave is sealed, it is placed in 100
It is reacted at a temperature of DEG C, time 3h.It is cleaned three times to after reaction take out electro-conductive glass, and with deionized water.
(3) a ceramic crucible bottom will be lain against by the indium tin oxide electro-conductive glass of step (2) processing, and kept
It is conductive up.Then, the mix powder being made of 50mg melamine, 20mg elemental sulfur and 5mg phenol is laid in
Indium tin oxide conductive glass surface.After again, ceramic crucible is placed in the middle position of a tube-type atmosphere furnace, in ammonia gas
Pyrolytic reaction is carried out in atmosphere, heating rate is 5 DEG C of min-1, reaction temperature is 400 DEG C, soaking time 2h.
(4) to after reaction taking out indium tin oxide electro-conductive glass in step (3), it is then placed into mass concentration
For 100mgml-1Ammonium hydroxide in carry out ultrasonic cleaning 1min, graphite phase carbon nitride interface finally is made in conductive glass surface
Layer.It is obtained by atomic force microscope (Asylum Research company, the U.S., MFP-3D-SA type) measurement: prepared graphite
Phase carbon nitride boundary layer with a thickness of 50nm.
(5) 1.5g titania powder, 0.5g polyethylene glycol (number-average molecular weight 20000) and 50ml deionized water is common
It is put into agate mortar, obtains titania slurry after grinding 30min.Then, titania slurry is coated using scraping embrane method
In the indium tin oxide conductive glass surface for having graphite phase carbon nitride boundary layer, after slurry is dry, dioxy is obtained through sintering
Change titanium perforated membrane.During the sintering process, atmosphere used is the mixed gas of oxygen and nitrogen, and the molar ratio of oxygen and nitrogen is
(1:5), heating rate are 10 DEG C of min-1, sintering temperature is 300 DEG C, soaking time 30min.
(6) by step (5) indium tin oxide obtained for having graphite phase carbon nitride boundary layer and titanium dioxide porous membrane
It is 5mgml that electro-conductive glass, which immerses mass concentration,-1CdSe quantum dots n-hexane dispersion liquid in, and protected under the conditions of being protected from light
4h is held, is cleaned three times after taking-up with ethyl alcohol, light anode is made.
(7) it by light anode obtained in step (6) and electrolyte, be packaged together to electrode, is finally made with stone
The CdSe quantum dots of black phase carbon nitride boundary layer are sensitized solar cell.Wherein, electrolyte be vulcanized sodium and elemental sulfur methanol/
Aqueous solution, the volume ratio of first alcohol and water are (1:3), and the molar concentration of vulcanized sodium is 0.1molL-1, the molar concentration of elemental sulfur
For 0.3molL-1, it is the indium tin oxide electro-conductive glass of platinum plating to electrode.
In AM1.5 (energy density 100mWcm-2) simulated solar irradiation under test, the photoelectric conversion efficiency of the battery
Be 13.4%, and under equal conditions the obtained CdSe quantum dots sensitization solar cell without graphite phase carbon nitride boundary layer light
Photoelectric transformation efficiency is only 6.7%.
Embodiment 2
(1) by the 2,6-diaminopyridine co-dissolve of the cyanamide of 20mg and 60mg in the ethyl alcohol of 100ml, and by system
The ultrasonic mixing 7h at 35 DEG C.
(2) mixed solution that step (1) obtains is transferred in the autoclave that a volume is 150ml, it then will be a piece of
Fluorine tin-oxide electro-conductive glass is put into the autoclave base, and keeps it conductive up.After autoclave is sealed, it is placed in 110
It is reacted at a temperature of DEG C, time 3.5h.To after reaction take out electro-conductive glass, and three are cleaned with deionized water
Time.
(3) a ceramic crucible bottom will be lain against by the fluorine tin-oxide electro-conductive glass of step (2) processing, and kept
It is conductive up.Then, the mix powder being made of 70mg cyanamide, 25mg elemental sulfur and 10mg phenol is laid in fluorine tin
Oxide conducting glass surface.After again, ceramic crucible is placed in the middle position of a tube-type atmosphere furnace, in ammonia atmosphere
Pyrolytic reaction is carried out, heating rate is 10 DEG C of min-1, reaction temperature is 450 DEG C, soaking time 2.5h.
(4) to after reaction taking out fluorine tin-oxide electro-conductive glass in step (3), it is then placed into mass concentration
For 150mgml-1Ammonium hydroxide in carry out ultrasonic cleaning 2min, graphite phase carbon nitride interface finally is made in conductive glass surface
Layer.It is obtained by atomic force microscope (Asylum Research company, the U.S., MFP-3D-SA type) measurement: prepared graphite
Phase carbon nitride boundary layer with a thickness of 80nm.
(5) 1.5g stannic oxide powder, 0.5g polyethylene glycol (number-average molecular weight 20000) and 50ml deionized water is common
It is put into agate mortar, obtains stannic oxide slurry after grinding 30min.Then, stannic oxide slurry is coated using scraping embrane method
In the fluorine tin-oxide conductive glass surface for having graphite phase carbon nitride boundary layer, after slurry is dry, dioxy is obtained through sintering
Change tin perforated membrane.During the sintering process, atmosphere used is the mixed gas of oxygen and nitrogen, and the molar ratio of oxygen and nitrogen is
(1:3), heating rate are 15 DEG C of min-1, sintering temperature is 325 DEG C, soaking time 40min.
(6) by step (5) the fluorine tin-oxide obtained for having graphite phase carbon nitride boundary layer and stannic oxide perforated membrane
It is 10mgml that electro-conductive glass, which immerses mass concentration,-1Cadmiumsulfide quantum dot n-hexane dispersion liquid in, and under the conditions of being protected from light
4.5h is kept, is cleaned three times after taking-up with ethyl alcohol, light anode is made.
(7) it by light anode obtained in step (6) and electrolyte, be packaged together to electrode, is finally made with stone
The cadmiumsulfide quantum dot sensitized solar cell of black phase carbon nitride boundary layer.Wherein, electrolyte be vulcanized sodium and elemental sulfur methanol/
Aqueous solution, the volume ratio of first alcohol and water are (1:2), and the molar concentration of vulcanized sodium is 0.2molL-1, the molar concentration of elemental sulfur
For 0.4molL-1, it is the fluorine tin-oxide electro-conductive glass of platinum plating to electrode.
In AM1.5 (energy density 100mWcm-2) simulated solar irradiation under test, the photoelectric conversion efficiency of the battery
Be 13.8%, and under equal conditions the obtained cadmiumsulfide quantum dot sensitized solar cell without graphite phase carbon nitride boundary layer light
Photoelectric transformation efficiency is only 7.1%.
Embodiment 3
(1) by the 2,6-diaminopyridine co-dissolve of the dicyandiamide of 30mg and 70mg in the propyl alcohol of 100ml, and by body
Lie in ultrasonic mixing 8h at 40 DEG C.
(2) mixed solution that step (1) obtains is transferred in the autoclave that a volume is 150ml, it then will be a piece of
Fluorine tin-oxide electro-conductive glass is put into the autoclave base, and keeps it conductive up.After autoclave is sealed, it is placed in 120
It is reacted at a temperature of DEG C, time 4h.It is cleaned three times to after reaction take out electro-conductive glass, and with deionized water.
(3) a ceramic crucible bottom will be lain against by the fluorine tin-oxide electro-conductive glass of step (2) processing, and kept
It is conductive up.Then, the mix powder being made of 90mg dicyandiamide, 30mg elemental sulfur and 15mg phenol is laid in fluorine
Tin-oxide conductive glass surface.After again, ceramic crucible is placed in the middle position of a tube-type atmosphere furnace, in ammonia atmosphere
Middle carry out pyrolytic reaction, heating rate are 15 DEG C of min-1, reaction temperature is 500 DEG C, soaking time 3h.
(4) to after reaction taking out fluorine tin-oxide electro-conductive glass in step (3), it is then placed into mass concentration
For 200mgml-1Ammonium hydroxide in carry out ultrasonic cleaning 3min, graphite phase carbon nitride interface finally is made in conductive glass surface
Layer.It is obtained by atomic force microscope (Asylum Research company, the U.S., MFP-3D-SA type) measurement: prepared graphite
Phase carbon nitride boundary layer with a thickness of 110nm.
(5) 1.5g Zinc oxide powder, 0.5g polyethylene glycol (number-average molecular weight 20000) and 50ml deionized water are put jointly
Enter in agate mortar, obtains zinc oxide slurry after grinding 30min.Then, using scrape embrane method by zinc oxide slurry be coated in have
The fluorine tin-oxide conductive glass surface of graphite phase carbon nitride boundary layer obtains zinc oxide porous through sintering after slurry is dry
Film.During the sintering process, atmosphere used is the mixed gas of oxygen and nitrogen, and the molar ratio of oxygen and nitrogen is (1:1), heating
Rate is 20 DEG C of min-1, sintering temperature is 350 DEG C, soaking time 50min.
(6) step (5) the fluorine tin-oxide obtained with graphite phase carbon nitride boundary layer and zinc oxide porous film is led
It is 15mgml that electric glass, which immerses mass concentration,-1Cadmium telluride quantum dot n-hexane dispersion liquid in, and protected under the conditions of being protected from light
5h is held, is cleaned three times after taking-up with ethyl alcohol, light anode is made.
(7) it by light anode obtained in step (6) and electrolyte, be packaged together to electrode, is finally made with stone
The cadmium telluride quantum dot of black phase carbon nitride boundary layer is sensitized solar cell.Wherein, electrolyte be vulcanized sodium and elemental sulfur methanol/
Aqueous solution, the volume ratio of first alcohol and water are (1:1), and the molar concentration of vulcanized sodium is 0.3molL-1, the molar concentration of elemental sulfur
For 0.5molL-1, it is the fluorine tin-oxide electro-conductive glass of platinum plating to electrode.
In AM1.5 (energy density 100mWcm-2) simulated solar irradiation under test, the photoelectric conversion efficiency of the battery
Be 12.2%, and under equal conditions the obtained cadmium telluride quantum dot sensitization solar cell without graphite phase carbon nitride boundary layer light
Photoelectric transformation efficiency is only 6.5%.
Embodiment 4
(1) by the 2,6-diaminopyridine co-dissolve of the urea of 40mg and 80mg in the butanol of 100ml, and by system
The ultrasonic mixing 9h at 45 DEG C.
(2) mixed solution that step (1) obtains is transferred in the autoclave that a volume is 150ml, it then will be a piece of
Fluorine tin-oxide electro-conductive glass is put into the autoclave base, and keeps it conductive up.After autoclave is sealed, it is placed in 130
It is reacted at a temperature of DEG C, time 4.5h.To after reaction take out electro-conductive glass, and three are cleaned with deionized water
Time.
(3) a ceramic crucible bottom will be lain against by the fluorine tin-oxide electro-conductive glass of step (2) processing, and kept
It is conductive up.Then, the mix powder being made of 110mg thiocarbamide, 35mg elemental sulfur and 20mg phenol is laid in fluorine
Tin-oxide conductive glass surface.After again, ceramic crucible is placed in the middle position of a tube-type atmosphere furnace, in ammonia atmosphere
Middle carry out pyrolytic reaction, heating rate are 20 DEG C of min-1, reaction temperature is 550 DEG C, soaking time 3.5h.
(4) to after reaction taking out fluorine tin-oxide electro-conductive glass in step (3), it is then placed into mass concentration
For 250mgml-1Ammonium hydroxide in carry out ultrasonic cleaning 4min, graphite phase carbon nitride interface finally is made in conductive glass surface
Layer.It is obtained by atomic force microscope (Asylum Research company, the U.S., MFP-3D-SA type) measurement: prepared graphite
Phase carbon nitride boundary layer with a thickness of 150nm.
(5) 1.5g Zirconium dioxide powder, 0.5g polyethylene glycol (number-average molecular weight 20000) and 50ml deionized water is common
It is put into agate mortar, obtains zirconium dioxide slurry after grinding 30min.Then, zirconium dioxide slurry is coated using scraping embrane method
In the fluorine tin-oxide conductive glass surface for having graphite phase carbon nitride boundary layer, after slurry is dry, dioxy is obtained through sintering
Change zirconium perforated membrane.During the sintering process, atmosphere used is the mixed gas of oxygen and nitrogen, and the molar ratio of oxygen and nitrogen is
(3:1), heating rate are 25 DEG C of min-1, sintering temperature is 375 DEG C, soaking time 60min.
(6) by step (5) the fluorine tin-oxide obtained for having graphite phase carbon nitride boundary layer and zirconium dioxide perforated membrane
It is 20mgml that electro-conductive glass, which immerses mass concentration,-1Zinc selenide quantum dot n-hexane dispersion liquid in, and under the conditions of being protected from light
5.5h is kept, is cleaned three times after taking-up with ethyl alcohol, light anode is made.
(7) it by light anode obtained in step (6) and electrolyte, be packaged together to electrode, is finally made with stone
The zinc selenide quantum dot of black phase carbon nitride boundary layer is sensitized solar cell.Wherein, electrolyte be vulcanized sodium and elemental sulfur methanol/
Aqueous solution, the volume ratio of first alcohol and water are (2:1), and the molar concentration of vulcanized sodium is 0.4molL-1, the molar concentration of elemental sulfur
For 0.6molL-1, it is the fluorine tin-oxide electro-conductive glass of platinum plating to electrode.
In AM1.5 (energy density 100mWcm-2) simulated solar irradiation under test, the photoelectric conversion efficiency of the battery
Be 16.2%, and under equal conditions the obtained zinc selenide quantum dot sensitization solar cell without graphite phase carbon nitride boundary layer light
Photoelectric transformation efficiency is only 7.1%.
Embodiment 5
(1) by the 2,6-diaminopyridine co-dissolve of the thiocarbamide of 50mg and 90mg in the ethylene glycol of 100ml, and by body
Lie in ultrasonic mixing 10h at 50 DEG C.
(2) mixed solution that step (1) obtains is transferred in the autoclave that a volume is 150ml, it then will be a piece of
Fluorine tin-oxide electro-conductive glass is put into the autoclave base, and keeps it conductive up.After autoclave is sealed, it is placed in 140
It is reacted at a temperature of DEG C, time 5h.It is cleaned three times to after reaction take out electro-conductive glass, and with deionized water.
(3) a ceramic crucible bottom will be lain against by the fluorine tin-oxide electro-conductive glass of step (2) processing, and kept
It is conductive up.Then, the mix powder being made of 130mg urea, 40mg elemental sulfur and 25mg phenol is laid in fluorine
Tin-oxide conductive glass surface.After again, ceramic crucible is placed in the middle position of a tube-type atmosphere furnace, in ammonia atmosphere
Middle carry out pyrolytic reaction, heating rate are 25 DEG C of min-1, reaction temperature is 600 DEG C, soaking time 4h.
(4) to after reaction taking out fluorine tin-oxide electro-conductive glass in step (3), it is then placed into mass concentration
For 300mgml-1Ammonium hydroxide in carry out ultrasonic cleaning 5min, graphite phase carbon nitride interface finally is made in conductive glass surface
Layer.It is obtained by atomic force microscope (Asylum Research company, the U.S., MFP-3D-SA type) measurement: prepared graphite
Phase carbon nitride boundary layer with a thickness of 90nm.
(5) 1.5g tantalum pentoxide powder, 0.5g polyethylene glycol (number-average molecular weight 20000) and 50ml deionized water is total
With being put into agate mortar, zirconium dioxide slurry is obtained after grinding 30min.Then, using scraping embrane method for tantalum pentoxide slurry
Coated in the fluorine tin-oxide conductive glass surface for having graphite phase carbon nitride boundary layer, after slurry is dry, obtained through sintering
Tantalum pentoxide perforated membrane.During the sintering process, atmosphere used is the mixed gas of oxygen and nitrogen, mole of oxygen and nitrogen
Than for (5:1), heating rate is 30 DEG C of min-1, sintering temperature is 400 DEG C, soaking time 70min.
(6) step (5) the fluorine tin obtained with graphite phase carbon nitride boundary layer and tantalum pentoxide perforated membrane is aoxidized
It is 25mgml that object electro-conductive glass, which immerses mass concentration,-1ZnS quantum dots n-hexane dispersion liquid in, and in being protected from light condition
Lower holding 6h is cleaned three times after taking-up with ethyl alcohol, and light anode is made.
(7) it by light anode obtained in step (6) and electrolyte, be packaged together to electrode, is finally made with stone
The ZnS quantum dots of black phase carbon nitride boundary layer are sensitized solar cell.Wherein, electrolyte be vulcanized sodium and elemental sulfur methanol/
Aqueous solution, the volume ratio of first alcohol and water are (3:1), and the molar concentration of vulcanized sodium is 0.5molL-1, the molar concentration of elemental sulfur
For 0.7molL-1, it is the fluorine tin-oxide electro-conductive glass of platinum plating to electrode.
In AM1.5 (energy density 100mWcm-2) simulated solar irradiation under test, the photoelectric conversion efficiency of the battery
Be 11.2%, and under equal conditions the obtained ZnS quantum dots sensitization solar cell without graphite phase carbon nitride boundary layer light
Photoelectric transformation efficiency is only 5.8%.
Embodiment 6
(1) by the 2,6-diaminopyridine co-dissolve of the melamine of 10mg and 50mg in the methanol of 100ml, and will
System ultrasonic mixing 6h at 30 DEG C.
(2) mixed solution that step (1) obtains is transferred in the autoclave that a volume is 150ml, it then will be a piece of
Fluorine tin-oxide electro-conductive glass is put into the autoclave base, and keeps it conductive up.After autoclave is sealed, it is placed in 100
It is reacted at a temperature of DEG C, time 3h.It is cleaned three times to after reaction take out electro-conductive glass, and with deionized water.
(3) a ceramic crucible bottom will be lain against by the fluorine tin-oxide electro-conductive glass of step (2) processing, and kept
It is conductive up.Then, the mix powder being made of 110mg urea, 35mg elemental sulfur and 20mg phenol is laid in fluorine
Tin-oxide conductive glass surface.After again, ceramic crucible is placed in the middle position of a tube-type atmosphere furnace, in ammonia atmosphere
Middle carry out pyrolytic reaction, heating rate are 5 DEG C of min-1, reaction temperature is 400 DEG C, soaking time 2h.
(4) to after reaction taking out fluorine tin-oxide electro-conductive glass in step (3), it is then placed into mass concentration
For 100mgml-1Ammonium hydroxide in carry out ultrasonic cleaning 1min, graphite phase carbon nitride interface finally is made in conductive glass surface
Layer.It is obtained by atomic force microscope (Asylum Research company, the U.S., MFP-3D-SA type) measurement: prepared graphite
Phase carbon nitride boundary layer with a thickness of 65nm.
(5) 1.5g titania powder, 0.5g polyethylene glycol (number-average molecular weight 20000) and 50ml deionized water is common
It is put into agate mortar, obtains titania slurry after grinding 30min.Then, titania slurry is coated using scraping embrane method
In the fluorine tin-oxide conductive glass surface for having graphite phase carbon nitride boundary layer, after slurry is dry, dioxy is obtained through sintering
Change titanium perforated membrane.During the sintering process, atmosphere used is the mixed gas of oxygen and nitrogen, and the molar ratio of oxygen and nitrogen is
(1:5), heating rate are 10 DEG C of min-1, sintering temperature is 300 DEG C, soaking time 30min.
(6) by step (5) the fluorine tin-oxide obtained for having graphite phase carbon nitride boundary layer and titanium dioxide porous membrane
It is 5mgml that electro-conductive glass, which immerses mass concentration,-1CdSe quantum dots n-hexane dispersion liquid in, and protected under the conditions of being protected from light
4h is held, is cleaned three times after taking-up with ethyl alcohol, light anode is made.
(7) it by light anode obtained in step (6) and electrolyte, be packaged together to electrode, is finally made with stone
The CdSe quantum dots of black phase carbon nitride boundary layer are sensitized solar cell.Wherein, electrolyte be vulcanized sodium and elemental sulfur methanol/
Aqueous solution, the volume ratio of first alcohol and water are (1:3), and the molar concentration of vulcanized sodium is 0.1molL-1, the molar concentration of elemental sulfur
For 0.3molL-1, it is the fluorine tin-oxide electro-conductive glass of platinum plating to electrode.
In AM1.5 (energy density 100mWcm-2) simulated solar irradiation under test, the photoelectric conversion efficiency of the battery
Be 11.4%, and under equal conditions the obtained CdSe quantum dots sensitization solar cell without graphite phase carbon nitride boundary layer light
Photoelectric transformation efficiency is only 6.9%.
Content carries out the adjustment of technological parameter according to the present invention, the preparation of solar cell of the present invention can be achieved, and show
The performance almost the same with embodiment out.Illustrative description is done to the present invention above, it should which explanation is not departing from this
In the case where the core of invention, any simple deformation, modification or other skilled in the art can not spend creativeness
The equivalent replacement of labour each falls within protection scope of the present invention.
Claims (10)
1. a kind of quantum dot sensitized solar cell with graphite phase carbon nitride boundary layer, which is characterized in that from bottom to top by leading
Electric glass, graphite phase carbon nitride boundary layer, oxide porous film, quantum dot light sensitizer, electrolyte and to electrode form;It is described
Graphite phase carbon nitride boundary layer is arranged between electro-conductive glass and oxide porous film, with a thickness of 50-150nm, graphite-phase nitridation
Carbon boundary layer is made of graphite phase carbon nitride nanometer sheet;Oxide porous film be titanium dioxide porous membrane, stannic oxide perforated membrane,
One of zinc oxide porous film, zirconium dioxide perforated membrane or tantalum pentoxide perforated membrane;Quantum dot light sensitizer is selenizing
Cadmium quantum dot, cadmiumsulfide quantum dot, cadmium telluride quantum dot, zinc selenide quantum dot, ZnS quantum dots, zinc telluride quantum dot, selenium
Change one of lead quantum dot, vulcanized lead quantum dot or lead telluride quantum dot;The electrolyte is vulcanized sodium and elemental sulfur
Solution, wherein solvent is the mixed solution of first alcohol and water, and the volume ratio of first alcohol and water is (1:3)-(3:1), mole of vulcanized sodium
Concentration is 0.1-0.5molL-1, the molar concentration of elemental sulfur is 0.3-0.7molL-1。
2. a kind of quantum dot sensitized solar cell with graphite phase carbon nitride boundary layer according to claim 1, special
Sign is, graphite phase carbon nitride interfacial layer thickness preferably 60-100nm.
3. a kind of quantum dot sensitized solar cell with graphite phase carbon nitride boundary layer according to claim 1 or 2,
It is characterized in that, the electro-conductive glass is one of indium tin oxide electro-conductive glass or fluorine tin-oxide electro-conductive glass.
4. a kind of quantum dot sensitized solar cell with graphite phase carbon nitride boundary layer according to claim 1 or 2,
It is characterized in that, to one in the fluorine tin-oxide electro-conductive glass of indium tin oxide electro-conductive glass or platinum plating that electrode is platinum plating
Kind.
5. a kind of preparation method of the quantum dot sensitized solar cell with graphite phase carbon nitride boundary layer, which is characterized in that press
It is carried out according to following step:
Step 1, electro-conductive glass is placed in the autoclave bottom equipped with mixed solution and keeps it conductive up, after sealing
It is placed under 100-160 degrees Celsius and is reacted, wherein mixed solution is nitrogenous organic monomer, 2,6-diaminopyridine is uniformly divided
It is dispersed in alcohol organic solvent and is prepared, nitrogenous organic monomer is 10-50 mass parts, and 2,6-diaminopyridine is 50-90
Mass parts, alcohol organic solvent be 100-120 parts by volume, nitrogenous organic monomer be melamine, cyanamide, dicyandiamide, urea or
One of person's thiocarbamide;
Step 2, the electro-conductive glass handled by step 1 is placed in ceramic crucible bottom and keeps it conductive up, will mixed
Powder is laid on conducting surface, then ceramic crucible is placed in tube-type atmosphere furnace, and pyrolytic reaction is carried out in ammonia atmosphere, from room
20-25 degrees Celsius of temperature is with 5-25 DEG C of min-1Heating rate be warming up to 400-600 DEG C and keep the temperature 1-6 hours, furnace cooling
To 20-25 degrees Celsius of room temperature, wherein mixed-powder by the nitrogenous organic monomer of 50-130 mass parts, 20-40 mass parts elemental sulfur and
5-25 mass parts phenol composition, nitrogenous organic monomer are one of melamine, cyanamide, dicyandiamide, urea or thiocarbamide;
Step 3, the electro-conductive glass handled by step 2 is placed in ammonium hydroxide and is cleaned by ultrasonic, in conductive glass surface system
Obtain graphite phase carbon nitride boundary layer;
Step 4, by the slurry containing oxide powder be coated in by step 3 handle with graphite phase carbon nitride boundary layer
Conductive glass surface obtains oxide porous film through sintering after slurry is dry, during the sintering process, atmosphere used be oxygen and
The molar ratio of the mixed gas of nitrogen, oxygen and nitrogen is (1:5)-(5:1), from 20-25 degrees Celsius of room temperature with 10-30 DEG C
min-1Heating rate be warming up to 300-400 DEG C and keep the temperature 30-120min, cool to 20-25 degrees Celsius of room temperature with the furnace;
Step 5, the obtained electro-conductive glass with graphite phase carbon nitride boundary layer and oxide porous film will be handled by step 4
It immerses in quantum dot light sensitization agent dispersing liquid and carries out quantum dot sensitized, obtained light anode under the conditions of being protected from light;
Step 6, it by light anode obtained in step 5 and electrolyte, be packaged together to electrode, is finally made with graphite-phase
Nitrogenize the quantum dot sensitized solar cell of carbon boundary layer.
6. a kind of preparation of quantum dot sensitized solar cell with graphite phase carbon nitride boundary layer according to claim 5
Method, which is characterized in that in step 1, alcohol organic solvent is that the alcohols that is in a liquid state is organic molten under 20-25 degrees Celsius of room temperature
Agent, such as one of methanol, ethyl alcohol, propyl alcohol, butanol, ethylene glycol, glycerine, isopropanol or isobutanol;Nitrogenous organic monomer
For 20-35 mass parts, 2,6-diaminopyridine is 70-80 mass parts, and alcohol organic solvent is 100-120 parts by volume;It will contain
Nitrogen organic monomer, 2,6-diaminopyridine are dispersed in alcohol organic solvent, the ultrasonic mixing 6-10h at 30-50 DEG C;It leads
Electric glass is one of indium tin oxide electro-conductive glass or fluorine tin-oxide electro-conductive glass;Reaction temperature is taken the photograph for 120-150
Family name's degree, reaction time are 1-5 hours, preferably 3-5 hours.
7. a kind of preparation of quantum dot sensitized solar cell with graphite phase carbon nitride boundary layer according to claim 5
Method, which is characterized in that in step 2, from 20-25 degrees Celsius of room temperature with 5-10 DEG C of min-1Heating rate be warming up to
460-550 DEG C and heat preservation 2-4 hours, cool to 20-25 degrees Celsius of room temperature with the furnace;Mixed-powder is contained by 60-120 mass parts
Nitrogen organic monomer, 25-35 mass parts elemental sulfur and 10-20 mass parts phenol composition, mixed-powder is laid on conducting surface, thick
Degree is 1-3mm;In step 3, the mass concentration of ammonia is 100-300mgml in ammonium hydroxide-1, it is cleaned by ultrasonic 1-5min.
8. a kind of preparation of quantum dot sensitized solar cell with graphite phase carbon nitride boundary layer according to claim 5
Method, which is characterized in that in step 4, the oxide powder is titania powder, stannic oxide powder, oxide powder and zinc
One of end, Zirconium dioxide powder or tantalum pentoxide powder;During the sintering process, atmosphere used is oxygen and nitrogen
The molar ratio of mixed gas, oxygen and nitrogen is (1:3)-(3:1), from 20-25 degrees Celsius of room temperature with 10-20 DEG C of min-1's
Heating rate is warming up to 340-380 DEG C and keeps the temperature 40-80min, cools to 20-25 degrees Celsius of room temperature with the furnace;In steps of 5, it measures
Son point photosensitizer dispersion liquid in quantum dot light sensitizer be CdSe quantum dots, cadmiumsulfide quantum dot, cadmium telluride quantum dot,
Zinc selenide quantum dot, ZnS quantum dots, zinc telluride quantum dot, lead selenide quantum dot, vulcanized lead quantum dot or lead telluride amount
One of son point, solvent is n-hexane, and the mass concentration of quantum dot is 5-30mgml-1Solvent, in quantum dot light sensitizer
Quantum dot sensitized holding 4-6h is carried out in dispersion liquid under the conditions of being protected from light.
9. a kind of preparation of quantum dot sensitized solar cell with graphite phase carbon nitride boundary layer according to claim 5
Method, which is characterized in that in step 6, electrolyte is the solution of vulcanized sodium and elemental sulfur, and wherein solvent is the mixed of first alcohol and water
Solution is closed, the volume ratio of first alcohol and water is (1:3)-(3:1), and the molar concentration of vulcanized sodium is 0.1-0.5molL-1, elemental sulfur
Molar concentration be 0.3-0.7molL-1, the fluorine tin of indium tin oxide electro-conductive glass or platinum plating that electrode is platinum plating is aoxidized
One of object electro-conductive glass.
10. application of the graphite phase carbon nitride boundary layer in quantum dot sensitized solar cell, which is characterized in that reduce light induced electron
It is compound with electrolyte, inhibit the defeated reaction of back pass, improves 1.5-2.2 times that photoelectric conversion efficiency is original.
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