JP2022507895A - 光起電力装置用の増強されたペロブスカイト材料 - Google Patents
光起電力装置用の増強されたペロブスカイト材料 Download PDFInfo
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- JP2022507895A JP2022507895A JP2021528880A JP2021528880A JP2022507895A JP 2022507895 A JP2022507895 A JP 2022507895A JP 2021528880 A JP2021528880 A JP 2021528880A JP 2021528880 A JP2021528880 A JP 2021528880A JP 2022507895 A JP2022507895 A JP 2022507895A
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- perovskite material
- lead
- certain embodiments
- perovskite
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- 239000005020 polyethylene terephthalate Substances 0.000 description 1
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- 238000010248 power generation Methods 0.000 description 1
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- 239000002109 single walled nanotube Substances 0.000 description 1
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- 229910052715 tantalum Inorganic materials 0.000 description 1
- 125000000999 tert-butyl group Chemical group [H]C([H])([H])C(*)(C([H])([H])[H])C([H])([H])[H] 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
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- 125000005580 triphenylene group Chemical group 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 1
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- 230000001755 vocal effect Effects 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
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- 229910052984 zinc sulfide Inorganic materials 0.000 description 1
- DRDVZXDWVBGGMH-UHFFFAOYSA-N zinc;sulfide Chemical compound [S-2].[Zn+2] DRDVZXDWVBGGMH-UHFFFAOYSA-N 0.000 description 1
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Abstract
Description
あるPV実施形態は、図1に示すような太陽電池の例示的な図を参照して説明することができる。ある実施形態による例示的なPVアーキテクチャは、実質的に基板-アノード-IFL-活性層-IFL-カソードの形態であってもよい。ある実施形態の活性層は、光活性であってもよく、および/または光活性材料を含んでもよい。従来から知られるように、他の層および材料を電池内で利用してもよい。さらに、用語「活性層」の使用は、いかなる他の層の特性をも、明示的にまたは暗示的に、制限または他の方法で定義することを意味しないことに留意する必要がある。例えば、ある実施形態では、IFLのいずれかまたは両方が、それらが半導体である場合、活性であってもよい。特に、図1を参照すると、様式化された一般的なPVセル1000が示されており、PV内のいくつかの層の高い界面特性が示されている。PV1000は、ペロブスカイト材料PV実施形態など、いくつかのPVデバイスに適用可能な、一般的なアーキテクチャを表す。PVセル1000は、透明基板層1010を有し、この透明基板層1010は、ガラス(または太陽放射線に対して同様に透明な材料)であってもよく、これにより、太陽放射線は、層を通って透過できる。ある実施形態の透明層は、スーパーストレートまたは基板(例えば、図2の基板層3901と同様)とも称され、ガラス、ポリエチレン、ポリプロピレン、ポリカーボネート、ポリイミド、PMMA、PET、PEN、カプトン、または石英のような、各種硬質または可撓性材料の1または2以上を有してもよい。一般に、基板という用語は、製造中にデバイスが堆積される材料を参照するために使用される。光活性層1040は、電子ドナーまたはp型材料、および/または電子アクセプタまたはn型材料、および/またはp型およびn型の両方の材料特性を示す両極性半導体、および/またはn型またはp型の特性を示さない真性半導体から構成されてもよい。ある実施形態では、光活性層1040は、本明細書に記載されるようなペロブスカイト材料であってもよい。図1に示されるように、活性層または光活性層1040は、2つの導電性電極層1020および1060の間に挟まれる。図1において、電極層1020は、スズドープ酸化インジウム(ITO材料)、または本願に記載された他の材料のような透明導電体であってもよい。他の実施形態では、第2の基板1070および第2の電極1060は、透明であってもよい。前述のように、ある実施形態の活性層は、必ずしも光活性である必要はない。ただし、図1に示すデバイスでは、光活性である。電極層1060は、アルミニウム材料または他の金属、または炭素のような他の導電性材料であってもよい。従来から知られる他の材料を使用してもよい。また、セル1010は、図1の例に示されるような界面層(IFL)1030を有する。IFLは、電荷分離を支援し得る。他の実施形態では、IFL1030は、多層IFLを有してもよく、これは、以降詳細に議論される。また、電極1060に隣接するIFL1050があってもよい。ある実施形態では、電極1060に隣接するIFL1050は、さらに多層IFLを有し、または代わりに、多層IFLを有してもよい(再度、以降詳細に説明される)。ある実施形態によるIFLは、性質が半導体であってもよく、固有、両極性、p型、またはn型のいずれであってもよく、あるいは性質が誘電体であってもよい。ある実施形態では、デバイスのカソード側のIFL(例えば、図1に示すようなIFL1050)は、p型であってもよく、デバイスのアノード側のIFL(例えば、図1に示すようなIFL1030)は、n型であってもよい。しかしながら、他の実施形態では、カソード側IFLは、n型であり、アノード側IFLは、p型であってもよい。セル1010は、電極1060および1020により、ならびにバッテリ、モータ、キャパシタ、電力グリッド、または他の電気負荷のような放電ユニットにより、電気リードに取り付けられてもよい。
ある実施態様において、本開示では、薄膜コートIFLを含む、PV内の1または2以上の界面層の有利な材料および設計が提供される。薄膜コートIFLは、本願で議論される各種実施形態により、PVの1または2以上のIFLで使用されてもよい。
ペロブスカイト材料は、PVまたは他のデバイスの1または2以上の態様に組み込まれてもよい。ある実施形態によるペロブスカイト材料は、一般式CwMyXzで表されてもよく、ここでCは、1または2以上のカチオン(例えば、アミン、アンモニウム、ホスホニウム、第1族金属、第2族金属、および/または他のカチオンまたはカチオン的化合物)を含み、Mは、1または2以上の金属(例えば、Be、Mg、Ca、Sr、Ba、Fe、Cd、Co、Ni、Cu、Ag、Au、Au、Hg、Sn、Ge、Ga、Pb、In、Tl、Sb、Bi、Ti、Zn、Cd、Hg、およびZrを有する)を含み、Xは、1または2以上のアニオンを含み、w、y、およびzは、1~20の実数を表す。ある実施形態では、Cは、1または2以上の有機カチオンを有してもよい。ある実施形態では、各有機カチオンCは、各金属Mよりも大きくてもよく、各アニオンXは、カチオンCおよび金属Mの両方と結合可能であってもよい。特定の実施形態において、ペロブスカイト材料は、一般式がCMX3であってもよい。
3を有してもよい。
ある実施形態では、本開示により、1または2以上のペロブスカイト材料を有する、PVおよび他の同様のデバイス(例えば、電池、ハイブリッドPV電池、FET、LED、非線形光学系(NLO)、導波路など)の複合設計が提供されてもよい。例えば、1または2以上のペロブスカイト材料は、ある実施形態の第1および第2の活性材料(例えば、図3の活性材料3906aおよび3908a)のいずれかまたは両方として機能してもよい。より一般的には、本開示のある実施形態では、1または2以上のペロブスカイト材料を含む活性層を有するPVまたは他のデバイスが提供される。そのような実施形態では、ペロブスカイト材料(すなわち、任意の1または2以上のペロブスカイト材料を有する材料)は、各種アーキテクチャの活性層に使用されてもよい。また、ペロブスカイト材料は、活性層の任意の1または2以上の部材(例えば、電荷輸送材料、メソポーラス材料、光活性材料、および/または界面材料、これらの各々は、以下により詳細に議論される)の機能を果たすことができる。ある実施形態では、同じペロブスカイト材料が、複数のそのような機能に寄与することができる。ただし、他の実施形態では、複数のペロブスカイト材料がデバイスに含有され、各ペロブスカイト材料が、1または2以上のそのような機能を果してもよい。特定の実施形態では、ペロブスカイト材料がどのような役割を果たす場合でも、それは、各種状態でデバイス中に調製されおよび/または提供されてもよい。例えば、ある実施形態では、これは実質的に固体であってもよい。デバイス内(例えば、メソポーラス層、界面層、電荷輸送層、光活性層、または他の層、および/または電極のような、デバイスの別の部材上)に、溶液または懸濁液がコーティングされ、またはその他の方法で堆積されてもよい。ある実施形態では、ペロブスカイト材料は、デバイスの別の構成要素の表面上に、in-situで形成されてもよい(例えば、薄膜固体としての気相成膜により)。ペロブスカイト材料を有する層を形成する、任意の他の適切な手段が使用されてもよい。
前述のように、ある実施形態では、活性層中のペロブスカイト材料は、一般式CMX3-yX’y(0≧y≧3)を有し、ここで、Cは、1または2以上のカチオン(例えば、アミン、アンモニウム、第1族金属、第2族金属、ホルムアミジニウム、グアニジニウム、エテンテトラミン、ホスホニウム、イミダゾリウム、および/または他のカチオンまたはカチオン状化合物)を有し、Mは、1または2以上の金属(例えば、Be、Mg、Ca、Sr、Ba、Fe、Cd、Co、Ni、Cu、Ag、Au、Hg、Sn、Ge、Ga、Pb、In、Tl、Sb、Bi、Ti、Zn、Cd、Hg、およびZr)を有し、XおよびX’は、1または2以上のアニオンを有する。ある実施形態では、ペロブスカイト材料は、CPbI3-yClyを有してもよい。ある実施形態では、ペロブスカイト材料は、以降に記載の工程を用いて、例えば、ドロップキャスティング、スピンキャスティング、スロット-ダイ印刷、スクリーン印刷、またはインクジェット印刷により、基板層上にPVデバイスの活性層として堆積されてもよい。
0g H2O/m3以上のガス、および20g H2O/m3以下のガスを有する制御された湿度環境で行われてもよい。
いわゆる「層状」2Dペロブスカイトは、ペロブスカイトが、前述のメチルアンモニウムカチオンおよびホルムアミジニウムカチオンよりも長いアルキル鎖を有する有機カチオンで形成される場合に、形成されることが知られている。層状2Dペロブスカイトは、ルドルスデン-ポッパー相、ディオン-ヤコブソン(Dion-Jacobson)相、およびオーリビリウス(Aurivillius)相等の構造を有する。例えば、メチルアンモニウムまたは前述の他のカチオンの代わりに、1-ブチルアンモニウムを置換することにより、「1ステップ」法(本願には記載されていない)において、ペロブスカイトの形成中に、ルドルスデン-ポッパー2Dペロブスカイトが生じる。そのようなペロブスカイトでは、1-ブチルアンモニウムは、ペロブスカイトが完全な結晶格子を形成することを妨げ、代わりに、ペロブスカイトは、単結晶構造の厚さを有するペロブスカイトの「シート」中に形成される。図5には、ルドルスデン-ポッパーの構造5500を示す。これは、1-ブチルアンモニウムカチオン5510を有する。図5からわかるように、ブチルアンモニウムカチオンの「尾部」により、ペロブスカイト材料の鉛およびヨウ化物の部分、他の鉛とヨウ化物構造の間に、分離が生じ、2Dペロブスカイトの「シート」が得られる。従って、ペロブスカイト材料の形成中の1-ブチルアンモニウムまたはベンジルアンモニウムのような、「バルキー」な有機カチオンの導入は、ペロブスカイトのルドルスデン-ポッパー形態が望まれない場合、好ましくない。
ペロブスカイト材料の結晶構造への1,4-ジアンモニウムブタン、または後述する他のポリアンモニウム有機化合物の導入により、その材料の特性が改善されてもよい。ある実施形態では、以下に記載するような、1,4-ジアンモニウムブタンのFAPbI3ペロブスカイトへの添加により、有利な特性を有するペロブスカイト材料が提供されてもよい。ある実施形態では、1,4-ジアンモニウムブタンは、前述のプロセスにおいて、バルキーな有機カチオン塩の代わりに、1,4-ジアンモニウムブタン塩を用いて、ペロブスカイト材料に導入されてもよく、1,4-ジアンモニウムブタン塩(または本願に記載の他の有機ポリアンモニウム塩)の添加は、前述のバルキーな有機カチオン塩の添加が行われるペロブスカイトの製造方法の任意の段階で行われてもよい。1,4-ジアンモニウムブタンのような有機カチオンをペロブスカイト材料の結晶構造に含有させることにより、本願に開示のペロブスカイト材料の「理想的な」化学量論比から逸脱した、ペロブスカイト材料の一般式が得られる。例えば、そのような有機カチオンの含有により、ペロブスカイト材料は、一般式FAPbI3で表される、化学量論的または超化学量論的な一般式を有してもよい。この場合、ペロブスカイト材料の一般式は、CxMyXzで表されてもよい。ここで、x、yおよびzは、実数である。
Claims (30)
- ペロブスカイト材料であって、
CxMyXzの一般式を有するペロブスカイト結晶格子と、
前記ペロブスカイト結晶格子の表面または粒界の近傍にあるバルキーな有機カチオンと、
を有し、
ここで、x、y、zは実数であり、
Cは、第1族金属、第2族金属、メチルアンモニウム、ホルムアミジニウム、グアニジニウム、およびエテンテトラミンからなる群から選択された、1または2以上のカチオンを有し、
Mは、Be、Mg、Ca、Sr、Ba、Fe、Cd、Co、Ni、Cu、Ag、Au、Hg、Sn、Ge、Ga、Pb、In、Tl、Sb、Bi、Ti、Zn、Cd、Hg、Zr、およびこれらの組み合わせからなる群から各々選択された、1または2以上の金属を有し、
Xは、ハロゲン化物、擬ハロゲン化物、カルコゲニド、およびこれらの組み合わせからなる群から各々選択された、1または2以上のアニオンを有する、ペロブスカイト材料。 - 前記バルキーな有機カチオンの少なくとも一つの尾部基は、当該ペロブスカイト材料の前記表面または粒界と化学的に接続されていない、請求項1に記載のペロブスカイト材料。
- 前記バルキーな有機カチオンは、前記ペロブスカイト材料結晶格子の前記表面または粒界から、前記ペロブスカイト材料結晶格子内に50nm未満の位置に存在する、請求項1に記載のペロブスカイト材料。
- 前記バルキーな有機カチオンは、n-ブチルアンモニウム、ベンジルアンモニウム、ブタン-1,4-ジアンモニウム、ペンチルアンモニウム、ヘキシルアンモニウム、ポリ(ビニルアンモニウム)、フェニルエチルアンモニウム、3-フェニル-1-プロピルアンモニウム、4-フェニル-1-ブチルアンモニウム、1,3-ジメチルブチルアンモニウム、3,3-ジメチルブチルアンモニウム、1-オクチルアンモニウム、およびこれらの組み合わせからなる群から選定される、請求項1に記載のペロブスカイト材料。
- 前記バルキーな有機カチオンは、1-ブチルアンモニウムを有する、請求項1に記載のペロブスカイト材料。
- 前記バルキーな有機カチオンは、1-ヘキシルアンモニウムを有する、請求項1に記載のペロブスカイト材料。
- 前記バルキーな有機カチオンは、1-オクチルアンモニウムを有する、請求項1に記載のペロブスカイト材料。
- 前記バルキーな有機カチオンは、ベンジルアンモニウムを有する、請求項1に記載のペロブスカイト材料。
- 前記ペロブスカイト材料結晶格子は、立方晶構造を有する、請求項1に記載のペロブスカイト材料。
- ホルムアミジニウムヨウ化鉛ペロブスカイト材料と、
前記ホルムアミジニウムヨウ化鉛ペロブスカイト材料の表面または粒界の近傍にあるベンジルアンモニウムカチオンと、
を有する、ペロブスカイト材料。 - 前記ベンジルアンモニウムカチオンの少なくとも一つのベンジル基は、前記ホルムアミジニウムヨウ化鉛ペロブスカイト材料内の前記表面または粒界と化学的に接続されていない、請求項10に記載のペロブスカイト材料。
- 前記ベンジルアンモニウムカチオンは、前記ホルムアミジニウムヨウ化鉛ペロブスカイト材料の前記表面または粒界から、前記ホルムアミジニウムヨウ化鉛ペロブスカイト材料内に50nm未満の位置に存在する、請求項10に記載のペロブスカイト材料。
- 前記ホルムアミジニウムヨウ化鉛ペロブスカイト材料は、立方晶構造を有する、請求項10に記載のペロブスカイト材料。
- ペロブスカイト材料を堆積する方法であって、
基板上に鉛塩前駆体を堆積して、鉛塩薄膜を形成する工程と、
前記鉛塩薄膜上にバルキーな有機カチオン溶液を堆積する工程と、
前記鉛塩薄膜上に第2の塩前駆体を堆積して、ペロブスカイト前駆体薄膜を形成する工程と、
前記基板をアニールして、ペロブスカイト材料を形成する工程と、
を有する、方法。 - 前記バルキーな有機カチオン溶液は、n-ブチルアンモニウム、ベンジルアンモニウム、ブタン-1,4-ジアンモニウム、ペンチルアンモニウム、ヘキシルアンモニウム、ポリ(ビニルアンモニウム)、フェニルエチルアンモニウム、3-フェニル-1-プロピルアンモニウム、4-フェニル-1-ブチルアンモニウム、1,3-ジメチルブチルアンモニウム、3,3-ジメチルブチルアンモニウム、1-オクチルアンモニウム、アンモニウム官能化ペリレン、およびこれらの組み合わせからなる群から選定された、バルキーな有機カチオンを有する、請求項14に記載の方法。
- 前記バルキーな有機カチオン溶液は、1-ブチルアンモニウムを有する、請求項14に記載の方法。
- 前記バルキーな有機カチオン溶液は、ベンジルアンモニウムを有する、請求項14に記載の方法。
- 前記バルキーな有機カチオン溶液は、0.01から0.1Mの間のバルキーな有機カチオン濃度を有する、請求項14に記載の方法。
- 前記バルキーな有機カチオン溶液は、0.03から0.05Mの間のバルキーな有機カチオン濃度を有する、請求項14に記載の方法。
- 前記鉛塩前駆体、前記第2の塩前駆体、および前記バルキーな有機カチオン溶液は、スピンコーティング、スロットダイ印刷、ブレードコーティング、スパッタリング、PE-CVD、熱蒸着、またはスプレーコーティングにより、堆積される、請求項14に記載の方法。
- 前記鉛塩前駆体は、ヨウ化鉛(II)、チオシアン酸鉛(II)、塩化鉛(II)、臭化鉛(II)、およびこれらの組み合わせからなる群から選定された、1または2以上の鉛塩を有する、請求項14に記載の方法。
- 前記鉛塩前駆体は、ヨウ化鉛(II)を有する、請求項14に記載の方法。
- 前記第2の塩前駆体は、ヨウ化ホルムアミジニウム、チオシアン酸ホルムアミジニウム、またはチオシアン酸グアニジニウムを有する、請求項14に記載の方法。
- 前記第2の塩前駆体は、ヨウ化ホルムアミジニウムを有する、請求項14に記載の方法。
- 前記鉛塩前駆体は、アミノ酸、5-アミノ吉草酸ヨウ化水素酸塩、1,8-ジヨードオクタン、1,8-ジチオオクタン、ハロゲン化ホルムアミジニウム、酢酸、トリフルオロ酢酸、ハロゲン化メチルアンモニウム、水、およびこれらの組み合わせからなる群から選択された、1または2以上の添加剤を有する、請求項14に記載の方法。
- 前記鉛塩前駆体は、無水ジメチルホルムアミドに溶解した、90:10のmol比のPbI2:PbCl2を有する、請求項14に記載の方法。
- アニールするステップは、周囲空気、制御された湿度環境、純アルゴン、純窒素、純酸素、純水素、純ヘリウム、純ネオン、純クリプトン、純CO2、およびこれらの組み合わせからなる群から選定された雰囲気において行われる、請求項14に記載の方法。
- アニールするステップは、50℃以上、300℃以下の温度で実施される、請求項14に記載の方法。
- 制御された湿度環境においてアニールするステップは、0g以上のH2O/m3空気、20g以下のH2O/m3空気の絶対湿度で行われる、請求項27に記載の方法。
- 制御された湿度環境においてアニールするステップは、約4から7gのH2O/m3空気の間の絶対湿度で行われる、請求項27に記載の方法。
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