TWI529955B - 具有經選擇性摻雜導電氧化物層之太陽能電池及其製備方法 - Google Patents
具有經選擇性摻雜導電氧化物層之太陽能電池及其製備方法 Download PDFInfo
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- TWI529955B TWI529955B TW103108818A TW103108818A TWI529955B TW I529955 B TWI529955 B TW I529955B TW 103108818 A TW103108818 A TW 103108818A TW 103108818 A TW103108818 A TW 103108818A TW I529955 B TWI529955 B TW I529955B
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- Prior art keywords
- coating
- dopant
- precursor material
- layer
- doped
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Links
- 238000004519 manufacturing process Methods 0.000 title 1
- 238000000576 coating method Methods 0.000 claims description 214
- 239000011248 coating agent Substances 0.000 claims description 209
- 239000000463 material Substances 0.000 claims description 91
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- 229910052731 fluorine Inorganic materials 0.000 claims description 29
- 238000000034 method Methods 0.000 claims description 26
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- 239000011737 fluorine Substances 0.000 claims description 25
- 238000005229 chemical vapour deposition Methods 0.000 claims description 23
- 229910052718 tin Inorganic materials 0.000 claims description 20
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 claims description 20
- 229910001887 tin oxide Inorganic materials 0.000 claims description 20
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- 229910052782 aluminium Inorganic materials 0.000 claims description 10
- 229910052725 zinc Inorganic materials 0.000 claims description 10
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- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 claims description 2
- KTSFMFGEAAANTF-UHFFFAOYSA-N [Cu].[Se].[Se].[In] Chemical compound [Cu].[Se].[Se].[In] KTSFMFGEAAANTF-UHFFFAOYSA-N 0.000 claims description 2
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- 239000010410 layer Substances 0.000 description 99
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- DTQVDTLACAAQTR-UHFFFAOYSA-N Trifluoroacetic acid Chemical compound OC(=O)C(F)(F)F DTQVDTLACAAQTR-UHFFFAOYSA-N 0.000 description 34
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- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 14
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- 229910052760 oxygen Inorganic materials 0.000 description 8
- YMLFYGFCXGNERH-UHFFFAOYSA-K butyltin trichloride Chemical compound CCCC[Sn](Cl)(Cl)Cl YMLFYGFCXGNERH-UHFFFAOYSA-K 0.000 description 7
- 239000010936 titanium Substances 0.000 description 6
- 239000011701 zinc Substances 0.000 description 6
- 238000000149 argon plasma sintering Methods 0.000 description 5
- 238000001514 detection method Methods 0.000 description 5
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- 229910052715 tantalum Inorganic materials 0.000 description 3
- BNEMLSQAJOPTGK-UHFFFAOYSA-N zinc;dioxido(oxo)tin Chemical compound [Zn+2].[O-][Sn]([O-])=O BNEMLSQAJOPTGK-UHFFFAOYSA-N 0.000 description 3
- GSJBKPNSLRKRNR-UHFFFAOYSA-N $l^{2}-stannanylidenetin Chemical compound [Sn].[Sn] GSJBKPNSLRKRNR-UHFFFAOYSA-N 0.000 description 2
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- 150000004706 metal oxides Chemical class 0.000 description 2
- 229910052750 molybdenum Inorganic materials 0.000 description 2
- 239000000178 monomer Substances 0.000 description 2
- 229910052758 niobium Inorganic materials 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 2
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- TVSZGZNGPRDODL-UHFFFAOYSA-H hexafluorotungsten tungsten Chemical compound [W].F[W](F)(F)(F)(F)F TVSZGZNGPRDODL-UHFFFAOYSA-H 0.000 description 1
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Classifications
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- H—ELECTRICITY
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- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
- H01L31/0256—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by the material
- H01L31/0264—Inorganic materials
- H01L31/032—Inorganic materials including, apart from doping materials or other impurities, only compounds not provided for in groups H01L31/0272 - H01L31/0312
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- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
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- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
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- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
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- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C17/00—Surface treatment of glass, not in the form of fibres or filaments, by coating
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- C03C17/3602—Surface treatment of glass, not in the form of fibres or filaments, by coating with at least two coatings having different compositions at least one coating being a metal the metal being present as a layer
- C03C17/3668—Surface treatment of glass, not in the form of fibres or filaments, by coating with at least two coatings having different compositions at least one coating being a metal the metal being present as a layer the multilayer coating having electrical properties
- C03C17/3678—Surface treatment of glass, not in the form of fibres or filaments, by coating with at least two coatings having different compositions at least one coating being a metal the metal being present as a layer the multilayer coating having electrical properties specially adapted for use in solar cells
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- C—CHEMISTRY; METALLURGY
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- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/22—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the deposition of inorganic material, other than metallic material
- C23C16/30—Deposition of compounds, mixtures or solid solutions, e.g. borides, carbides, nitrides
- C23C16/40—Oxides
- C23C16/407—Oxides of zinc, germanium, cadmium, indium, tin, thallium or bismuth
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- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
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- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/44—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the method of coating
- C23C16/54—Apparatus specially adapted for continuous coating
- C23C16/545—Apparatus specially adapted for continuous coating for coating elongated substrates
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/02—Details
- H01L31/0224—Electrodes
- H01L31/022466—Electrodes made of transparent conductive layers, e.g. TCO, ITO layers
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- H—ELECTRICITY
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Description
本發明概言之係關於太陽能電池(例如光伏打(PV)電池)，且更具體而言關於具有經選擇性摻雜透明導電氧化物層之太陽能電池及其製備方法。
太陽能電池或光伏打(PV)電池係將太陽光直接轉換成電之電子器件。照在太陽能電池上之光產生電流及電壓二者來產生電力。在太陽能電池中，來自太陽光之光子擊中太陽能電池且被半導體材料吸附。電子自其原子被撞散，從而產生電位差。電流流經材料來消除電位差。由於太陽能電池之特殊組成，僅允許電子在單方向上移動。
習用非晶型矽薄膜太陽能電池通常包含在其上方提供底層之玻璃基板(蓋板)、透明導電氧化物(TCO)接觸層及具有p-n接面之非晶型矽薄膜活性層。後金屬層起反射器及背接觸之作用。TCO層較佳具有不規則表面以增加光散射。在太陽能電池中，使用光散射或「混濁度」來捕獲電池作用區中之光。電池中捕獲之光越多，可獲得之效率越高。然而，混濁度不可大至對光穿過TCO層之透明度造成不利影響。因此，光捕獲係嘗試改良太陽能電池之效率時之重要問題且在薄膜電池設計中尤為重要。亦期望TCO層高度透明以容許最大量之太陽能輻射穿過矽層。作為一般規則，到達半導體材料之光子越多，電池
之效率越高。此外，TCO層應高度導電以允許電池中之電子容易轉移。此導電性可藉由向TCO材料中添加摻雜物材料來增強。
TCO層係太陽能電池性能之重要因素。TCO材料較佳應具有高導電率(即，低片電阻)、電磁波譜期望區域中之高透明度，且應具有高混濁度以促進光散射。然而，該等因素彼此交織。例如，導電率取決於摻雜物濃度及TCO層之厚度。然而，增加摻雜物濃度或TCO層厚度通常會減小TCO層之透明度。此外，表面粗糙度(光散射)通常隨塗層厚度而增加。然而，增加塗層厚度通常會減小穿過塗層之透射率(尤其可見光透射率)。因此，在選擇太陽能電池之TCO層時必須衡量該等因素中每一者之影響及相互作用。
業內期望提供其中可更容易地選擇導電率、透射率及光散射之TCO層。業內亦期望提供提供太陽能電池之其中可更容易地控制該等因素之TCO層的方法。業內亦期望提供具有該TCO層之太陽能電池。
太陽能電池包括具有第一表面及第二表面之第一基板。在第二表面之至少一部分上方提供第一導電層，其中第一導電層包括納入摻雜物材料之透明導電氧化物層。摻雜物材料選擇性分佈在導電層中。在透明第一導電層上方提供半導體層。在半導體層之至少一部分上方提供第二導電層。
製備具有透明導電氧化物層且摻雜物在該層中選擇性分佈之經塗覆基板的方法包括，將氧化物前驅物材料及摻雜物前驅物材料選擇性供應至多單元化學氣相沈積塗覆機之每一塗覆單元，其中選擇所供應摻雜物材料之量以改變所得塗層中之摻雜物含量對塗層深度。
化學氣相沈積系統包括至少一台具有複數個塗覆單元之塗覆機，其中將塗覆單元連接至一或多個包括至少一種氧化物前驅物材料及至少一種摻雜物材料之塗層供應源。在較佳實施例中，將塗覆單元
個別地連接至包括至少一種氧化物前驅物材料及至少一種摻雜物材料之各別塗層供應源。
製備具有塗層且摻雜物在該塗層中選擇性分佈之經塗覆基板的方法包括：將塗層前驅物材料供應至多單元化學氣相沈積塗覆機之塗覆單元；將摻雜物前驅物材料供應至多單元化學氣相沈積塗覆機之塗覆單元；控制塗層前驅物材料及摻雜物前驅物材料中至少一者之供應以在塗覆單元處定義具有摻雜物前驅物材料對塗層前驅物材料之所選比率的塗層組合物；及將塗層組合物沈積至基板上以形成經摻雜塗層。選擇摻雜物前驅物材料對塗層前驅物材料之比率，以定義所得經摻雜塗層之期望摻雜物含量對塗層深度輪廓。
可將塗覆單元之至少一部分個別地連接至塗層前驅物供應及摻雜物前驅物供應。
10‧‧‧太陽能電池
12‧‧‧第一(外)基板
14‧‧‧第一(外)主表面
16‧‧‧第二(內)主表面
18‧‧‧可選底塗層
20‧‧‧第一導電層
22‧‧‧半導體層
24‧‧‧第二導電層
26‧‧‧可選第二(內)基板
50‧‧‧化學氣相沈積塗覆系統
52‧‧‧熔融金屬(錫)錫浴/第一塗覆機
54‧‧‧第二塗覆機
56‧‧‧玻璃基板
60‧‧‧塗層前驅物供應
62‧‧‧摻雜物前驅物供應
A1‧‧‧塗覆單元
A2‧‧‧塗覆單元
A3‧‧‧塗覆單元
B1‧‧‧塗覆單元
B2‧‧‧塗覆單元
B3‧‧‧塗覆單元
B4‧‧‧塗覆單元
B5‧‧‧塗覆單元
B6‧‧‧塗覆單元
B7‧‧‧塗覆單元
在結合附圖考慮時，自以下描述將完全理解本發明。
圖1係納入本發明特徵之太陽能電池之側面剖視圖(未按比例)；圖2係納入本發明特徵之化學氣相沈積(CVD)塗覆系統之側面透視圖(未按比例)；圖3係實例1之TFA流(lb/hr)對單元編號之圖；圖4係實例1之F/Sn比率對塗層深度之圖；圖5係實例2之TFA流(lb/hr)對單元編號之圖；圖6係實例2之F/Sn比率對塗層深度之圖；圖7係實例3之TFA流(lb/hr)對單元編號之圖；圖8係實例3之F/Sn比率對塗層深度之圖；圖9係實例4之TFA流(lb/hr)對單元編號之圖；圖10係實例4之F/Sn比率對塗層深度之圖；圖11係實例5之氟及錫含量對塗層深度之圖；
圖12係實例5之F/Sn比率對塗層深度之圖；圖13係實例6樣品1之錫、氧及氟含量對塗層深度之圖；圖14係實例6樣品2之錫、氧及氟含量對塗層深度之圖；圖15係實例6樣品3之錫、氧及氟含量對塗層深度之圖；圖16係實例6之混濁度%對塗層厚度之圖；圖17係實例6之片電阻對塗層厚度之圖；圖18係實例6之混濁度對波長之圖。
如本文所使用之空間或方向術語(例如「左」、「右」、「內部」、「外部」、「上方」、「下方」及諸如此類)係指如圖式中所展示之本發明。然而，應理解，本發明可設想多種替代性定向，且因此該等術語不應視為具有限制性。此外，如本文所使用，用於本說明書及申請專利範圍中之表示尺寸、物理特徵、處理參數、成份量、反應條件及諸如此類之所有數值在所有情況下皆應理解為經術語「約」修飾。因此，除非指明相反之情形，否則下列說明書及申請專利範圍中所闡釋之數值皆可端視本發明尋求獲得之期望特性而變化。最低限度且並非企圖將等效教義之應用限於申請專利範圍之範疇，每一數值應至少根據所報告有效數位的數值且藉由使用普通捨入技術來解釋。此外，本文所揭示之所有範圍皆應理解為涵蓋其中所包含之開始及結束範圍值以及任何及所有子範圍。例如，所述範圍「1至10」應視為包含介於(且包含)最小值1與最大值10之間的任何及所有子範圍；即，以最小值1或較大值開始且以最大值10或較小值結束之所有子範圍，例如，1至3.3、4.7至7.5、5.5至10及諸如此類。此外，如本文所使用之術語「在上方形成」、「在上方沈積」、「在上方提供」或「位於上方」意指於表面上形成、沈積、提供或定位但未必與該表面直接接觸。例如，在基板「上方形成」之塗層並不排除存在位於所形成塗層與基板間之
一或多個相同或不同組成之其他塗層或膜。如本文所使用之術語「聚合物」或「聚合物的」包含寡聚物、均聚物、共聚物及三元共聚物，例如自兩種或更多種類型之單體或聚合物形成之聚合物。術語「可見區」或「可見光」係指具有介於380nm至760nm範圍內之波長之電磁輻射。術語「紅外區」或「紅外輻射」係指具有介於大於760nm至100,000nm範圍內之波長之電磁輻射。術語「紫外區」或「紫外輻射」意指具有介於200nm至小於380nm範圍內之波長之電磁能。術語「微波區」或「微波輻射」係指具有介於300百萬赫至300吉赫範圍內之頻率之電磁輻射。此外，本文中所提及之所有文件(例如(但不限於)已頒佈專利及專利申請案)應視為其全文皆「以引用方式併入本文中」。在以下論述中，折射率值係針對550奈米(nm)參考波長之彼等。術語「膜」係指具有期望或所選組成之塗層之區域。「層」包括一或多個「膜」。「塗層」或「塗層堆疊」包括一或多個「層」。
儘管將針對在太陽能電池中之應用闡述本發明，但應理解本發明並不限於在太陽能電池中之應用，且可用於其他應用，例如建築上釉、有機發光二極體或太陽能控制透明度。
納入本發明特徵之實例性太陽能電池10展示於圖1中。太陽能電池10包含具有第一(外)主表面14及第二(內)主表面16之第一(外)基板12。「外」意指表面面向入射輻射，例如太陽光。可選底塗層18可位於第二表面16上方。第一導電層20(例如TCO層)位於第二表面16上方(例如在底塗層18(若存在)上)。半導體層22位於TCO層20上方。第二導電層24位於半導體層22上方。例如，第二導電層24可為金屬層或含金屬之層。可選第二(內)基板26位於第二導電層24上方。
在本發明之廣泛實踐中，第一基板12(及可選第二基板26，若存在)可包含具有任何期望特徵之任何期望材料。例如，第一基板12可對可見光透明或半透明。「透明」意指具有大於0%至100%之可見光透
射率。另一選擇為，第一基板12可半透明。「半透明」意指允許電磁能(例如可見光)穿過但使此能量擴散以使觀察者相對側之物體並不清晰可見。適宜材料之實例包含(但不限於)塑膠基板(例如丙烯酸聚合物，例如聚丙烯酸酯；聚甲基丙烯酸烷基酯，例如聚甲基丙烯酸甲酯、聚甲基丙烯酸乙酯、聚甲基丙烯酸丙酯及諸如此類；聚胺基甲酸酯；聚碳酸酯；聚對苯二甲酸烷基酯，例如聚對苯二甲酸乙二酯(PET)、聚對苯二甲酸丙二酯、聚對苯二甲酸丁二酯及諸如此類；含有聚矽烷之聚合物；或用於製備該等材料之任何單體之共聚物或其任何混合物)；玻璃基板；或上述任一者之混合物或組合。例如，第一基板12可包含習用鈉鈣矽酸鹽玻璃、硼矽酸鹽玻璃或鑲鉛玻璃。玻璃可為透明玻璃。「透明玻璃」意指無色或無色彩玻璃。另一選擇為，玻璃可為有色或彩色玻璃。玻璃可為退火或熱處理玻璃。如本文所使用之術語「熱處理」意指回火或至少部分回火。玻璃可具有任何類型(例如習用浮製玻璃)，且可為具有任何光學特性(例如任何值之可見透射率、紫外透射率、紅外透射率及/或總太陽能透射率)之任何組成。「浮製玻璃」意指藉由其中將熔融玻璃沈積至熔融金屬浴(例如熔融錫)上之習用浮製製程形成之玻璃。玻璃之底側(即與熔融錫浴接觸之側)通常稱為「錫側」，且玻璃之頂側通常稱為「空氣側」。玻璃之錫側可具有少量納入玻璃表面中之錫。可用於本發明實踐之玻璃之非限制性實例包含Solargreen®、Solextra®、GL-20®、GL-35TM、Solarbronze®、Starphire®、Solarphire®、Solarphire PV®及Solargray®玻璃，其皆可自Pittsburgh,Pennsylvania之PPG Industries公司購得。
第一基板12可具有任何期望尺寸，例如長度、寬度、形狀或厚度。例如，第一基板12可為平坦、彎曲，或具有平坦及彎曲部分二者。在一個非限制性實施例中，第一基板12可具有介於以下範圍內之
厚度：0.5mm至10mm，例如1mm至5mm，例如2mm至4mm，例如3mm至4mm。
第一基板12可在550奈米(nm)之參考波長及2mm之參考厚度下具有高可見光透射率。「高可見光透射率」意指在550nm下之可見光透射率大於或等於85%，例如大於或等於87%，例如大於或等於90%，例如大於或等於91%，例如大於或等於92%，例如大於或等於93%。
可選底塗層18(若存在)可為單層，或具有第一層及第一層上方之第二層之多層塗層。底塗層18可在第一基板12與上覆塗層之間提供障壁。已知二氧化矽可提供良好障壁特性，尤其作為鈉離子擴散出玻璃基板之障壁。或者，底塗層18可係兩種或更多種氧化物(例如選自矽、鈦、鋁、錫、鋯、磷之氧化物)之混合物。氧化物可以任何期望比例存在。底塗層18(若存在)之第二層可為均質塗層。或者，第二層可為梯度塗層，且該塗層之至少兩種成份之相對比例隨塗層厚度而變化。
TCO層20包括至少一個導電氧化物層，例如經摻雜氧化物層。例如，TCO層20可包含一或多種氧化物材料，例如(但不限於)Zn、Fe、Mn、Al、Ce、Sn、Sb、Hf、Zr、Ni、Zn、Bi、Ti、Co、Cr、Si、In中一或多者之一或多種氧化物，或該等材料中兩者或更多者之合金(例如錫酸鋅)。TCO層20亦可包含一或多種摻雜物材料，例如(但不限於)F、In、Al、P、Cu、Mo、Ta、Ti、Ni、Nb、W及/或Sb。
TCO層20可具有以下厚度：大於200nm，例如大於250nm，例如大於350nm，例如大於380nm，例如大於400nm，例如大於420nm，例如大於470nm，例如大於500nm，例如大於600nm。例如，TCO層可具有介於以下範圍內之厚度：350nm至1,000nm，例如400nm至800nm，例如500nm至700nm，例如600nm至700nm。
TCO層20可具有以下表面電阻率(片電阻)：小於20歐姆/平方
(Ω/□)，例如小於15Ω/□，例如小於14Ω/□，例如小於13.5Ω/□，例如小於13Ω/□，例如小於12Ω/□，例如小於11Ω/□，例如小於10Ω/□。
TCO層20可具有介於以下範圍內之表面粗糙度(RMS)：5nm至60nm，例如5nm至40nm，例如5nm至30nm，例如10nm至30nm，例如10nm至20nm，例如10nm至15nm，例如11nm至15nm。第一底塗層之表面粗糙度將小於TCO層20之表面粗糙度。
在較佳實施例中，TCO層20係氟經摻雜錫氧化物塗層，且氟係以下列量存在：基於塗層之總重量小於20wt.%，例如小於15wt.%，例如小於13wt.%，例如小於10wt.%，例如小於5wt.%，例如小於4wt.%，例如小於2wt.%，例如小於1wt.%。TCO層20可為非晶型、結晶或至少部分結晶。然而，與先前TCO層不同，本發明之TCO層在整個塗層厚度內不必具有均勻的摻雜輪廓。在本發明實踐中，可藉由下文所闡述之TCO層形成製程選擇或改變TCO層之所選區域中之摻雜物含量。
在一較佳實施例中，TCO層20包括氟摻雜錫氧化物且具有介於以下範圍內之厚度：350nm至1,000nm，例如400nm至800nm，例如500nm至700nm，例如600nm至700nm，例如650nm。
半導體層22可係任何習用太陽能電池半導體材料，例如結晶矽。實例包含單晶矽、多晶矽及非晶型矽。半導體材料之其他實例包含碲化鎘及銅銦硒化物/硫化物。在典型矽太陽能電池中，磷摻雜(n型)矽之層處於較稠硼摻雜(p型)矽之頂部。在小p-n接面處產生電場，從而在將電池連接至電負載時產生電流之流動。非晶型矽層22可具有介於以下範圍內之厚度：200nm至1,000nm，例如200nm至800nm，例如300nm至500nm，例如300nm至400nm，例如350nm。
第二導電層24可係金屬層或含金屬之層，且可包含一或多種金屬氧化物材料。適宜金屬氧化物材料之實例包含(但不限於)Zn、Fe、
Mn、Al、Ce、Sn、Sb、Hf、Zr、Ni、Zn、Bi、Ti、Co、Cr、Si、In中一或多者之氧化物或該等材料中兩者或更多者之合金(例如錫酸鋅)。含金屬之層24可具有介於以下範圍內之厚度：50nm至500nm，例如50nm至300nm，例如50nm至200nm，例如100nm至200nm，例如150nm。
可選第二基板26(若存在)可具有上文針對第一基板12闡述之任何材料。第一基板12與第二基板26可具有相同或不同材料且可具有相同或不同厚度。
底塗層18、TCO層20、半導體層22及第二導電層24可藉由任何習用方法在基板12之至少一部分上方形成，該等方法係例如(但不限於)噴霧熱解、化學氣相沈積(CVD)或磁控濺鍍真空沈積(MSVD)。各層皆可藉由相同方法形成或不同層可藉由不同方法形成。例如，可選底塗層18及TCO層20可藉由CVD方法形成。在CVD方法中，將前驅物組合物攜載於載體氣體(例如氮氣)中，且引導至加熱基板。在本發明之一實踐中，TCO層20係藉由如下文所闡述之熔融錫浴中之CVD塗覆系統形成。
在本發明且圖解說明於圖2中之一較佳實踐中，使用位於習用浮製玻璃製程之熔融金屬(錫)錫浴51中之CVD塗覆系統50來沈積TCO層20。CVD塗覆系統50可具有一台塗覆機或複數台塗覆機。在圖2所展示之實施例中，塗覆系統具有第一CVD塗覆機52及第二CVD塗覆機54。然而，可使用任何期望數量之塗覆機。每一塗覆機52及54具有複數個塗覆單元(例如，塗覆狹槽)，以在玻璃基板56沿熔融金屬浴中之熔融金屬頂部移動時將塗層材料供應至下伏玻璃基板56上。熟習此項技術者將充分理解CVD塗覆機及習用浮製玻璃製程之一般結構及操作，且因此未進行詳細闡述。
在所圖解說明之實施例中，第一塗覆機52具有三個塗覆單元A1-A3，且第二塗覆機54具有七個塗覆單元B1-B7。此單元編號隨意且經呈現僅用於幫助論述下文所闡述之製程。可將每一塗覆單元連接至歧管以將塗層組合物供應至玻璃。另一選擇為，可將一或多個單元或一組單元個別地連接至塗層前驅物之供應及/或摻雜物前驅物材料之供應。該等連接可經由管道、導管或任何其他習用方法來實施。在圖2中，第二塗覆機54之塗覆單元B1-B7各自個別地連接至各別塗層前驅物供應60及摻雜物前驅物供應62。第一塗覆機52亦可以類似方式來組態。在本發明之一實踐中，可使用第一塗覆機52將底塗層施加在玻璃上，且可使用第二塗覆機54來供應具有所選摻雜物輪廓之頂塗層(例如TCO塗層)，如下文所闡述。儘管在圖2所圖解說明之較佳實施例中，每一塗覆單元係個別地連接至塗層前驅物供應60及摻雜物前驅物供應62，但應理解若期望用於具體塗層組態，則可藉由例如歧管將兩個或更多個單元連接至相同的塗層前驅物供應60。此外，若期望，若為期望最終塗層組合物可接受，則可將摻雜物前驅物供應62可操作地連接至兩個或更多個塗層前驅物供應60導管。
塗層前驅物供應60係含有前驅物材料之來源或容器，該等前驅物材料在引導至熱玻璃56上時反應或分解以形成期望組成之塗層。為形成氧化物塗層，塗層前驅物材料可包含在引導至熱玻璃56上時與氧反應或組合以形成氧化物之材料。材料之實例包含Zn、Fe、Mn、Al、Ce、Sn、Sb、Hf、Zr、Ni、Zn、Bi、Ti、Co、Cr、Si、In中一或多者之氧化物或該等材料中兩者或更多者之合金(例如錫酸鋅)的前驅物。該等前驅物材料市面有售且可基於期望塗覆組成來選擇。例如，單丁基三氯化錫(MBTC)係錫氧化物塗層之前驅物，正矽酸四乙酯(TEOS)係二氧化矽塗層之前驅物，三異丁基鋁(TIBAL)係氧化鋁塗層之前驅物。
摻雜物前驅物供應62係含有欲在將塗層材料沈積至玻璃表面上之前與塗層前驅物材料混合之材料或摻雜物之來源或容器。常用摻雜物材料包含F、In、Al、P、Cu、Mo、Ta、Ti、Ni、Nb、W及/或Sb。例如，六氟化鎢係鎢之前驅物，三氟乙酸(TFA)係氟之前驅物。該等前驅物材料市面有售且可基於期望摻雜物來選擇。
可在各塗覆單元藉由選擇或改變供應至塗覆機之個別單元之多個塗層供應之塗層前驅物材料與摻雜物前驅物材料的量或比率來改變供應至玻璃56上之塗層組合物。例如且為說明之目的，可將各單元連接至氧化錫前驅物材料(例如MBTC)之供應作為塗層前驅物供應60及氟前驅物材料(例如TFA)之供應作為摻雜物前驅物供應62。如將瞭解，亦可將該等單元連接至CVD塗覆製程之其他典型供應，例如載體氣體供應(例如氮或氧)及水源供應等。然而，為易於論述，未明確顯示該等其他來源。可根據特別目的之需要，藉由改變各單元之塗層組份(例如塗層前驅物與摻雜物前驅物)之比率來控制所得塗層之摻雜物濃度。
例如，對於習用太陽能電池，期望TCO層之外表面導電(即具有低片電阻)。在先前方法中，此係藉由將導電摻雜物添加至塗層前驅物材料中以形成塗層組合物及然後將塗層組合物施加至玻璃表面上達成。所得塗層具有在整個塗層中均勻分佈之摻雜物。儘管此塗層具有導電外表面，但遠離外表面定位於塗層較深處之摻雜物對塗層之表面導電率貢獻極小且實際上對整體塗層透明度不利。在本發明中，摻雜物濃度可偏向或選擇性限於TCO塗層之外部(上部分)以提供期望片電阻，但不存在於塗層之深度中以防對該層之透射率造成不利影響。
或者，若期望氧化錫塗層之外表面具有高片電阻但該塗層導電，則可優先添加摻雜物材料以靠近塗層底部且不存在於該層頂部附近。
或期望塗層之幾個區域具有摻雜物材料多於其他區域，此亦可藉由將摻雜物材料選擇性添加至CVD塗覆機之所選單元達成。
儘管在上述較佳實施例中，個別塗層前驅物供應60及摻雜物前驅物供應62與塗覆單元流體連通，但亦可將個別塗覆單元各連接至單一塗層來源，該塗層來源具有塗層前驅物材料及摻雜物前驅物材料之混合物，在連接至不同塗覆單元之不同塗層來源之間該等組份之比率不同。
提供以下實例來說明本發明之多個非限制性態樣。然而，應理解本發明並不限於該等特定實例。
以下實例說明使用氧化錫塗層前驅物材料(MBTC)及氟摻雜物前驅物材料(TFA)形成之氟摻雜氧化錫塗層。然而，應理解此僅為說明本發明之一般概念且本發明並不限於該等特定材料。
以下實例中之每一者使用具有3.2mm厚度之透明玻璃基板。藉由如上文所闡述之第二塗覆機54沈積TCO塗層以具有665nm之厚度。使用單元B1-B7。每一單元皆具有52.3磅/小時(lb/hr)之錫前驅物(MBTC)流速及14.6 lb/hr之水流速。每一單元之氟前驅物(TFA)之量係如每一實例中所闡述來變化。在實例中，在圖2中玻璃移動為左至右。即，單元B7係玻璃56所遇到之第二塗覆機54之第一作用單元，且單元B1係玻璃所遇到之最後單元。形成塗層後，使用x射線光電發射光譜對塗層實施濺鍍探測以確定氟濃度對塗層深度之變化。濺鍍時間指示深度，且1秒之濺鍍時間等於約1.5埃。
TFA係如圖3所闡釋供應至每一單元。此實例對每一單元使用均一的TFA流速。對塗層實施濺鍍探測且結果展示於圖4中。如自圖4可見，氟濃度在整個塗層深度上相對均勻。TCO塗層具有8.6Ω/□之片
電阻、82.6%之光透射率及0.96%之混濁度。
TFA係如圖5中所闡釋供應至每一單元。此實例使用較低之初始TFA流速。對塗層實施濺鍍探測且結果展示於圖6中。如可見，氟濃度在塗層之底部較低且在塗層之頂部較高。TCO塗層具有8.8Ω/□之片電阻、82.8%之光透射率及0.79%之混濁度。
TFA係如圖7中所闡釋供應至每一單元。此實例使用較高之初始TFA流速及較低之最終流速。對塗層實施濺鍍探測且結果展示於圖8中。如可見，氟濃度在塗層之底部較高且在塗層之頂部較低。TCO塗層具有9.4Ω/□之片電阻、82.1%之光透射率及1.09%之混濁度。
TFA係如圖9中所闡釋供應至每一單元。此實例使用低初始TFA流速、中間流速及隨後高流速。對塗層實施濺鍍探測且結果展示於圖10中。如可見，氟濃度在塗層之底部較低且在塗層之頂部較高，並在塗層中間附近具有過渡區。TCO塗層具有9.0Ω/□之片電阻、82.7%之光透射率及0.80%之混濁度。
此實例展示氟組合物之離散步階變化隨塗層深度變化之TCO塗層。基板係3.2mm透明玻璃且塗層具有385nm之厚度。使用六個塗覆機單元。MBTC流速為43.6 lb/hr，且水流速為7.9 lb/hr。TFA流速在單元5中為8.2 lb/hr，在單元1及3中為14.03 lb/hr，且在單元2、4及6中為0 lb/hr。塗層具有圖11中所展示之組成輪廓。圖12展示塗層之F/Sn比率對深度。在塗層中形成氟組合物之離散區域。TCO塗層具有21.0Ω/□之片電阻、84.1%之光透射率及0.70%之混濁度。
此實例說明具有氟組合物之步階變化隨深度變化之TCO以能夠控制混濁度，同時維持恆定片電阻。玻璃為具有4.0mm厚度之低鐵玻璃。使用八個塗覆單元。第一塗覆機之單元A3在此實例中表示為「單元8」，且單元1-7係指上文所闡述之單元B1-B7。每一單元皆具有如表1中所展示之MBTC、水及TFA流速。所有值皆係以1bs/hr表示。
該等塗層具有表2中所展示之混濁度及片電阻值。厚度值係以nm表示，混濁度係以%表示，且片電阻係以歐姆/平方表示。
圖13係展示樣品1之氧、錫及氟對深度之圖。圖14係展示樣品2之氧、錫及氟含量對深度之圖。圖15係展示樣品3之氧、錫及氟含量對深度之圖。
圖16展示樣品1-3之總層厚度對混濁度。如可見，隨厚度增加，混濁度增加。圖17展示樣品1-3之塗層厚度對片電阻。如可見，片電阻甚至在塗層厚度增加時仍保持相對恆定。圖18係樣品1-3之透射混濁度對波長之圖。
彼等熟習此項技術者將容易地瞭解，可在不背離上述描述中所
揭示之概念下對本發明作出修改。因此，本文詳細闡述之具體實施例僅出於說明之目的且不限於本發明之範疇，本發明之範疇係隨附申請專利範圍所給予之全寬度及其任何及所有等效內容。
10‧‧‧太陽能電池
12‧‧‧第一(外)基板
14‧‧‧第一(外)主表面
16‧‧‧第二(內)主表面
18‧‧‧可選底塗層
20‧‧‧第一導電層
22‧‧‧半導體層
24‧‧‧第二導電層
26‧‧‧可選第二(內)基板
Claims (21)
- 一種製備經塗覆基板之方法，該基板具有塗層且摻雜物選擇性分佈於該塗層中，該方法包括以下步驟：將塗層前驅物材料供應至多單元化學氣相沈積塗覆機之塗覆單元；將摻雜物前驅物材料供應至多單元化學氣相沈積塗覆機之塗覆單元；控制該塗層前驅物材料與該摻雜物前驅物材料中至少一者之供應，以界定該等塗覆單元中具有所選比率之該摻雜物前驅物材料對該塗層前驅物材料之塗層組合物；及將該塗層組合物沈積至基板上以形成經摻雜塗層，其中選擇該摻雜物前驅物材料對該塗層前驅物材料之比率，以界定所得經摻雜塗層之期望摻雜物含量對塗層深度輪廓(profile)；其中，該期望摻雜物含量對該塗層深度輪廓係不均勻分佈；且其中，摻雜物含量在該經摻雜塗層之頂部低於該經摻雜塗層之底部附近，或在該經摻雜塗層之中間區域高於該經摻雜塗層之頂部或底部。
- 如請求項1之方法，其中將該等塗覆單元之至少一部分個別地連接至塗層前驅物供應及摻雜物前驅物供應。
- 如請求項1之方法，其中該塗層係透明導電氧化物層。
- 如請求項1之方法，其中該塗層前驅物材料包括用於氧化物塗層之前驅物材料，包括Zn、Fe、Mn、Al、Ce、Sn、Sb、Hf、Zr、Ni、Zn、Bi、Ti、Co、Cr、Si、In中之一或多者，或該等材料中 兩者或更多者之合金。
- 如請求項1之方法，其中該摻雜物前驅物材料包括至少一種選自F、In、Al、P及Sb之摻雜物。
- 如請求項1之方法，其包含控制該塗層前驅物材料與該摻雜物前驅物材料中至少一者之供應，以使該摻雜物在氧化錫層內不均勻分佈。
- 如請求項1之方法，其中該塗層前驅物材料包括氧化錫前驅物以形成氧化錫層，且該摻雜物前驅物材料包括氟前驅物。
- 如請求項7之方法，其中氟含量在該氧化錫層之頂部高於該氧化錫層之底部附近。
- 如請求項7之方法，其中該氟含量在該氧化錫層之頂部低於該氧化錫層之該底部附近。
- 如請求項7之方法，其中該氟含量在該氧化錫層之該中間區域高於該氧化錫層之該頂部或底部。
- 一種太陽能電池，其包括：第一基板，其具有第一表面及第二表面；第一導電層，其在該第二表面之至少一部分上方，其中該第一導電層係納入摻雜物材料之透明導電氧化物層，其中該摻雜物材料選擇性分佈在該導電層中，且其中該摻雜物材料在該第一導電層之頂部低於該第一導電層之底部附近，或在該第一導電層之中間區域高於該第一導電層之頂部或底部；半導體層，其在該透明第一導電層上方；及第二導電層，其在該半導體層之至少一部分上方。
- 如請求項11之太陽能電池，其進一步包括介於該第二表面與該第一導電層間之底塗層。
- 如請求項11之太陽能電池，其進一步包括該第二導電層上方之第二基板。
- 如請求項11之太陽能電池，其中該第一導電層包括Zn、Fe、Mn、Al、Ce、Sn、Sb、Hf、Zr、Ni、Zn、Bi、Ti、Co、Cr、Si、In中一或多者之氧化物，或該等材料中兩者或更多者之合金。
- 如請求項14之太陽能電池，其中該第一導電層包括至少一種選自F、In、Al、P及Sb之摻雜物。
- 如請求項15之太陽能電池，其中該第一導電層包括氟摻雜之氧化錫層。
- 如請求項16之太陽能電池，其中該氟在該氧化錫層內不均勻分佈。
- 如請求項17之太陽能電池，其中氟含量在該氧化錫層之頂部高於該氧化錫層之底部附近。
- 如請求項11之太陽能電池，其中該半導體層係選自單晶矽、多晶矽、非晶型矽、碲化鎘及銅銦硒化物/硫化物。
- 一種化學氣相沈積系統，其包括：至少一個具有多個塗覆單元之塗覆機，其中該等塗覆單元係個別地連接至各別包括至少一種氧化物前驅物材料及至少一種摻雜物材料之塗層供應源。
- 一種製備經塗覆基板之方法，該基板具有塗層且摻雜物選擇性分佈於該塗層中，該方法包括以下步驟：將塗層前驅物材料供應至多單元化學氣相沈積塗覆機之塗覆單元；將摻雜物前驅物材料供應至多單元化學氣相沈積塗覆機之塗覆單元； 控制該塗層前驅物材料與該摻雜物前驅物材料中至少一者之供應，以界定該等塗覆單元中具有所選比率之該摻雜物前驅物材料對該塗層前驅物材料之塗層組合物；及將該塗層組合物沈積至基板上以形成經摻雜塗層，其中選擇該摻雜物前驅物材料對該塗層前驅物材料之比率，以界定所得經摻雜塗層之期望摻雜物含量對塗層深度輪廓；其中，該期望摻雜物含量對該塗層深度輪廓係不均勻分佈；且其中，摻雜物含量在該經摻雜塗層之底部附近之該經摻雜塗層之第一部分高於該經摻雜塗層之中間區域；且其中該摻雜物含量在該經摻雜塗層之底部附近之該經摻雜塗層之第二部分低於該經摻雜塗層之中間區域。
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| US201361777316P | 2013-03-12 | 2013-03-12 | |
| US14/200,443 US20140311573A1 (en) | 2013-03-12 | 2014-03-07 | Solar Cell With Selectively Doped Conductive Oxide Layer And Method Of Making The Same |
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| US10672920B2 (en) | 2015-03-12 | 2020-06-02 | Vitro Flat Glass Llc | Article with buffer layer |
| US20200392012A1 (en) * | 2019-06-17 | 2020-12-17 | Oregon State University | Solution deposition of metal salts to form metal oxides |
| JP7179338B2 (ja) * | 2019-08-19 | 2022-11-29 | 株式会社ユニバーサルエンターテインメント | 遊技機 |
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Also Published As
| Publication number | Publication date |
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| TW201505194A (zh) | 2015-02-01 |
| US20140311573A1 (en) | 2014-10-23 |
| WO2014164434A1 (en) | 2014-10-09 |
| JP2018040059A (ja) | 2018-03-15 |
| US20180190844A1 (en) | 2018-07-05 |
| CN108807566A (zh) | 2018-11-13 |
| JP2019149557A (ja) | 2019-09-05 |
| US11031514B2 (en) | 2021-06-08 |
| JP2016517630A (ja) | 2016-06-16 |
| KR20150119017A (ko) | 2015-10-23 |
| CN105074937A (zh) | 2015-11-18 |
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