JP2014096569A - 銅・インジウム・ガリウム・セレニウム(cigs)または銅・亜鉛・錫・硫黄(czts)系薄膜型太陽電池及びその製造方法 - Google Patents
銅・インジウム・ガリウム・セレニウム(cigs)または銅・亜鉛・錫・硫黄(czts)系薄膜型太陽電池及びその製造方法 Download PDFInfo
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- copper
- thin film
- selenium
- tin
- indium
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- 239000010949 copper Substances 0.000 title claims abstract description 158
- 229910052802 copper Inorganic materials 0.000 title claims abstract description 137
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 title claims abstract description 136
- 239000010409 thin film Substances 0.000 title claims abstract description 116
- 239000011669 selenium Substances 0.000 title claims abstract description 68
- 239000011701 zinc Substances 0.000 title claims abstract description 60
- BUGBHKTXTAQXES-UHFFFAOYSA-N Selenium Chemical compound [Se] BUGBHKTXTAQXES-UHFFFAOYSA-N 0.000 title claims abstract description 58
- 229910052711 selenium Inorganic materials 0.000 title claims abstract description 58
- 229910052738 indium Inorganic materials 0.000 title claims abstract description 50
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 title claims abstract description 50
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 title claims abstract description 49
- 229910052733 gallium Inorganic materials 0.000 title claims abstract description 49
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 title claims abstract description 47
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 title claims abstract description 47
- 229910052717 sulfur Inorganic materials 0.000 title claims abstract description 47
- 239000011593 sulfur Substances 0.000 title claims abstract description 47
- 229910052718 tin Inorganic materials 0.000 title claims abstract description 47
- 229910052725 zinc Inorganic materials 0.000 title claims abstract description 47
- 238000004519 manufacturing process Methods 0.000 title claims description 46
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims abstract description 56
- 229910052750 molybdenum Inorganic materials 0.000 claims abstract description 56
- 239000011733 molybdenum Substances 0.000 claims abstract description 56
- 230000031700 light absorption Effects 0.000 claims abstract description 27
- 239000000203 mixture Substances 0.000 claims abstract description 22
- 238000000034 method Methods 0.000 claims description 61
- 239000011135 tin Substances 0.000 claims description 53
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 claims description 45
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 24
- 239000000843 powder Substances 0.000 claims description 24
- 239000000758 substrate Substances 0.000 claims description 23
- 238000005229 chemical vapour deposition Methods 0.000 claims description 20
- 238000004544 sputter deposition Methods 0.000 claims description 15
- 238000000576 coating method Methods 0.000 claims description 14
- 239000011787 zinc oxide Substances 0.000 claims description 12
- 238000010894 electron beam technology Methods 0.000 claims description 10
- 230000008569 process Effects 0.000 claims description 9
- 239000011248 coating agent Substances 0.000 claims description 8
- 238000010438 heat treatment Methods 0.000 claims description 8
- 238000000224 chemical solution deposition Methods 0.000 claims description 7
- 229910052751 metal Inorganic materials 0.000 claims description 6
- 239000002184 metal Substances 0.000 claims description 6
- 238000007650 screen-printing Methods 0.000 claims description 6
- 238000007606 doctor blade method Methods 0.000 claims description 5
- 238000010422 painting Methods 0.000 claims description 5
- 238000004528 spin coating Methods 0.000 claims description 5
- 238000005507 spraying Methods 0.000 claims description 5
- 239000000919 ceramic Substances 0.000 claims description 3
- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 claims description 3
- 239000000463 material Substances 0.000 claims description 3
- 229920000642 polymer Polymers 0.000 claims description 3
- SBIBMFFZSBJNJF-UHFFFAOYSA-N selenium;zinc Chemical compound [Se]=[Zn] SBIBMFFZSBJNJF-UHFFFAOYSA-N 0.000 claims description 3
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 claims description 3
- 229910001887 tin oxide Inorganic materials 0.000 claims description 3
- WILFBXOGIULNAF-UHFFFAOYSA-N copper sulfanylidenetin zinc Chemical compound [Sn]=S.[Zn].[Cu] WILFBXOGIULNAF-UHFFFAOYSA-N 0.000 claims description 2
- 238000004070 electrodeposition Methods 0.000 claims description 2
- 238000007738 vacuum evaporation Methods 0.000 claims description 2
- 238000007740 vapor deposition Methods 0.000 claims description 2
- MHWZQNGIEIYAQJ-UHFFFAOYSA-N molybdenum diselenide Chemical compound [Se]=[Mo]=[Se] MHWZQNGIEIYAQJ-UHFFFAOYSA-N 0.000 abstract description 28
- 238000006243 chemical reaction Methods 0.000 abstract description 13
- 230000008859 change Effects 0.000 abstract description 4
- 230000015572 biosynthetic process Effects 0.000 description 13
- 230000000052 comparative effect Effects 0.000 description 9
- 239000007789 gas Substances 0.000 description 8
- 238000002441 X-ray diffraction Methods 0.000 description 7
- 238000000151 deposition Methods 0.000 description 6
- 238000012360 testing method Methods 0.000 description 6
- 238000010586 diagram Methods 0.000 description 5
- 230000032798 delamination Effects 0.000 description 4
- 239000011521 glass Substances 0.000 description 4
- 229910016001 MoSe Inorganic materials 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 2
- 239000012300 argon atmosphere Substances 0.000 description 2
- 239000012298 atmosphere Substances 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- QXYJCZRRLLQGCR-UHFFFAOYSA-N dioxomolybdenum Chemical compound O=[Mo]=O QXYJCZRRLLQGCR-UHFFFAOYSA-N 0.000 description 2
- 238000012545 processing Methods 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 229910052710 silicon Inorganic materials 0.000 description 2
- 239000010703 silicon Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000006835 compression Effects 0.000 description 1
- 238000007906 compression Methods 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 150000001879 copper Chemical class 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000000280 densification Methods 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 239000012153 distilled water Substances 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 239000010408 film Substances 0.000 description 1
- QNWMNMIVDYETIG-UHFFFAOYSA-N gallium(ii) selenide Chemical compound [Se]=[Ga] QNWMNMIVDYETIG-UHFFFAOYSA-N 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000012423 maintenance Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 238000012261 overproduction Methods 0.000 description 1
- 230000005622 photoelectricity Effects 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 238000007747 plating Methods 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 238000001552 radio frequency sputter deposition Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 239000005361 soda-lime glass Substances 0.000 description 1
- 238000002207 thermal evaporation Methods 0.000 description 1
- 238000001771 vacuum deposition Methods 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
Classifications
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- 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
- H01L31/0322—Inorganic materials including, apart from doping materials or other impurities, only compounds not provided for in groups H01L31/0272 - H01L31/0312 comprising only AIBIIICVI chalcopyrite compounds, e.g. Cu In Se2, Cu Ga Se2, Cu In Ga Se2
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Abstract
【解決手段】裏面電極層200及び光吸収層300を含むCIGSまたはCZTS系薄膜型太陽電池において、光吸収層の組成が、CuξInΨGa1−Ψ(SξSe1−ξ)2(0.85≦x<1、0<y<1、0<z<1、x、y及びzは、実数)またはCu(2−π)Zn(2−θ)Snθ(SPSe(1−P))4(1.4≦p<2、0<q<2、0<r<1、p、q及びrは、実数)であることを特徴とする。
【選択図】図1
Description
1)モリブデン裏面電極層の形成
ガラス基板(soda−lime glass)を有機溶媒と蒸溜水とで洗浄した後、60℃で12時間乾燥する。乾燥したガラス基板にモリブデンターゲット(target)(純度99.999%)を使って、DCスパッタリング法で5mTorrアルゴン雰囲気下でDC150Wで50分間金属モリブデン裏面電極層を蒸着する。該蒸着されたモリブデン厚膜の厚さは、約1μmであり、図4に例示されたように、約100nm程度の結晶粒サイズを有し、約0.18Ω/squの面抵抗を有する。
蒸着されたモリブデン電極上に銅ターゲット(純度99.999%)を使って、DCスパッタリング法で5mTorrアルゴン雰囲気下でDC100Wで3分40秒間蒸着して、100nmの厚さを有する銅薄膜をコーティングする(図5)。
製造されたCu/Mo/ガラス基板上にCIGS粉末が均一に分散されたコーティング液(ペースト)を用いて、スクリーン印刷工程でCIGS薄膜を塗布して、図6に例示されたように、6〜8μmの厚さを有するCIGS層(光吸収粉末層)を形成する。該形成されたCIGS層を水素が4%含まれたアルゴンガス雰囲気下でセレニウムソースと共に550℃で1時間熱処理する。この際、光吸収粉末層は、焼結されて光吸収層に変化し、同時に、銅薄膜は、光吸収層に吸収され、モリブデン電極層は、焼結されたCIGS光吸収層と直接接触を成す(図3及び図7)。セレン化条件によって銅薄膜が吸収され、追加的なセレン化が進行する場合、一部のモリブデン薄膜が二セレン化モリブデン層を成して、光吸収層とモリブデン薄膜との間に存在し、銅薄膜の厚さと密度とを調節して、二セレン化モリブデン層の厚さを必要なほどに決定することもできる。
CIGS薄膜上にCBD法(化学槽蒸着法)で厚さ50nmのCdS層を形成し、引き続きCdS層の表面にZnOターゲットを使って、RFスパッタリング法でi型ZnO透明電極を50nm厚さに蒸着し、同じスパッタリング法でアルミニウムがドーピングされたZnO(AZO)ターゲットを使って、AZO透明電極を500nm厚さに蒸着して太陽電池を製造する。この電池の表面に電流を収集するために、グリッドマスクパターンを利用した熱蒸発法でNi50nm及びAl 1μmのグリッド電極を形成する。
銅薄膜の形成段階を省略したことを除いては、実施例と同じ工程でCIGS系薄膜型太陽電池を製造した。このように生成された太陽電池の光吸収層薄膜のSEM写真は、図8のようであり、1.1μmのモリブデン電極層の56%に該当する0.62μmがセレン化されて、約4倍の体積膨張によって2.6μmの二セレン化モリブデン層が形成された。
実施例と比較例とのモリブデン裏面電極層のセレン化程度を比較するために、各方法で生成された薄膜(図7及び図8)のXRDパターン(実施例=上、比較例の=下)を図9から説明した(XRD、X−ray diffraction method(Bruker D8 Advance))。実施例の薄膜の場合、CIGS光吸収層以外のモリブデンパターンが主に観察されて、モリブデンピーク(Mo、2θ=40.5゜±0.5゜)強度が、二セレン化モリブデンピーク(MoSe2、2θ=32゜±0.5゜または57゜±0.5゜)強度の約20倍に表われることを観察することができる。比較例の薄膜では、モリブデン(Mo)パターンは減る一方、二酸化モリブデン(MoSe2)パターンが大きく表われる(モリブデンパターンピークが、二セレン化モリブデンパターンピークの約1.2倍)。
200:モリブデン裏面電極層
210:二セレン化モリブデン層
300:光吸収層
310:光吸収粉末層
400:バッファ層
500:透明電極層
800:銅薄膜
Claims (12)
- 基板と、
モリブデン裏面電極層と、
銅薄膜と、
光吸収粉末層と、
を含むことを特徴とする銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池製造用の中間体薄膜。 - 前記光吸収粉末層の組成は、CuξInΨGa1−Ψ(SξSe1−ξ)2(0<x<1、0<y<1、0<z<1、x、y及びzは、実数)またはCu(2−π)Zn(2−θ)Snθ(SPSe(1−P))4(0<p<2、0<q<2、0<r<1、p、q及びrは、実数)であり、
ドクターブレード法、スクリーン印刷法、スピンコーティング法、スプレーコーティング法、及びペインティング法を含む非真空型工程を通じて塗布されたことを特徴とする請求項1に記載の銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池製造用の中間体薄膜。 - 前記モリブデン裏面電極層の厚さは、0.5ないし5μmであり、
前記銅薄膜の厚さは、前記光吸収粉末層の厚さの1ないし10%であることを特徴とする請求項1に記載の銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池製造用の中間体薄膜。 - 基板の一面にモリブデン裏面電極層を形成する段階と、
前記モリブデン裏面電極層上に銅薄膜を形成する段階と、
前記銅薄膜上に銅・インジウム・ガリウム・セレニウムまたは銅・亜鉛・錫・硫黄の光吸収粉末層を形成して、銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池製造用の中間体薄膜を製造する段階と、
前記銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池製造用の中間体薄膜を熱処理して光吸収層を形成する段階と、
を含む銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池の製造方法。 - 前記基板は、
ガラス質、金属、セラミック、及び高分子からなる群から選択されたことを特徴とする請求項4に記載の銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池の製造方法。 - 前記モリブデン裏面電極層を形成する段階は、
モリブデンを基板上に電子ビームコーティング法(electron beam coating)、スパッタリング法(sputtering)、化学蒸着法(chemical vapor deposition)、または有機金属化学蒸着法(metal−organic chemical vapor deposition)でコーティングすることを特徴とする請求項4に記載の銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池の製造方法。 - 前記銅薄膜を形成する段階は、
真空蒸発法((thermal) vacuum evaporation)、電子ビームコーティング法、スパッタリング法、化学蒸着法(chemical vapor deposition;CVD)、有機金属化学蒸着法(metal−organic chemical vapor deposition;MOCVD)、または電気化学的メッキ法(electro−chemical deposition)を通じて前記モリブデン裏面電極層上に銅薄膜を形成することを特徴とする請求項4に記載の銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池の製造方法。 - 前記光吸収粉末層を形成して、銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池製造用の中間体薄膜を製造する段階は、
非真空環境で、CuξInΨGa1−Ψ(SξSe1−ξ)2(0<x<1、0<y<1、0<z<1、x、y及びzは、実数)またはCu(2−π)Zn(2−θ)(SPSe(1−P))4(0<p<2、0<q<2、0<r<1、p、q及びrは、実数)の組成比を有する粉末またはペーストを、ドクターブレード法、スクリーン印刷法、スピンコーティング法、スプレーコーティング法、及びペインティング法を含む非真空型工程を通じて塗布する段階を含むことを特徴とする請求項4に記載の銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池の製造方法。 - 前記銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池製造用の中間体薄膜を熱処理して光吸収層を形成する段階は、
250ないし900℃の不活性または還元性のセレニウムガスで熱処理する段階を含み、
熱処理中に、前記銅薄膜が前記光吸収層に吸収または拡散されて、光吸収層の組成が、CuξInΨGa1−Ψ(SξSe1−ξ)2(0.85≦x<1、0<y<1、0<z<1、x、y及びzは、実数)またはCu(2−π)Zn(2−θ)Snθ(SPSe(1−P))4(1.4≦p<2、0<q<2、0<r<1、p、q及びrは、実数)で決定されることを特徴とする請求項4に記載の銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池の製造方法。 - CdS、ZnS(O,OH)、ZnSe、InS(O,OH)、In2S3、ZnInξSeΨ、Zn1−ξMgξO(0<x<1、0<y<1、x及びyは、実数)、またはその混合物をCBD法(chemical bath deposition、化学槽蒸着法)、電子ビームコーティング法、スパッタリング法、または化学蒸着法(CVD)を通じて蒸着させることによって、前記光吸収層の上部にバッファ層を形成する段階をさらに含むことを特徴とする請求項4に記載の銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池の製造方法。
- ZnO、AZO(aluminuim−doped zinc oxide)、BZO(boron−doped zinc oxide)、ITO(indium tin oxide)、FTO(fluorine−doped tin oxide)、またはその混合物を電子ビームコーティング法、またはスパッタリング法を通じて蒸着させることによって、前記光吸収層の上部に透明電極層を形成する段階をさらに含むことを特徴とする請求項4に記載の銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池の製造方法。
- 請求項4ないし請求項11のうち何れか一項によって製造されたことを特徴とする銅・インジウム・ガリウム・セレニウム(CIGS)または銅・亜鉛・錫・硫黄(CZTS)系太陽電池。
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