JP2023506683A - 再充電可能な金属ハロゲン化物電池のための多孔質シリコンアノード - Google Patents
再充電可能な金属ハロゲン化物電池のための多孔質シリコンアノード Download PDFInfo
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- JP2023506683A JP2023506683A JP2022525961A JP2022525961A JP2023506683A JP 2023506683 A JP2023506683 A JP 2023506683A JP 2022525961 A JP2022525961 A JP 2022525961A JP 2022525961 A JP2022525961 A JP 2022525961A JP 2023506683 A JP2023506683 A JP 2023506683A
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- battery
- anode
- metal
- electrolyte
- porous
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Links
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Images
Classifications
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- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/134—Electrodes based on metals, Si or alloys
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0569—Liquid materials characterised by the solvents
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- H—ELECTRICITY
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
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- H01M4/0492—Chemical attack of the support material
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
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- H—ELECTRICITY
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Abstract
Description
次に、本発明を以下の非限定的な実施例に関して記載する。
陽極酸化法を、約700ミクロンの厚さのホウ素ドープ(p型)結晶シリコン基板を濃縮HF(49%)の溶液に浸漬することにより行った。次いで、電気バイアスを、同様に溶液中に置かれたPt電極に対する基板に印加する。p型ドープIV族半導体材料層は正極として機能し、Pt電極は負極として作用した。
(実施例2)
直接溶融合金法を利用して、実施例1の多孔質シリコンアノードをプレリチウム化および金属化した。リチウム金属をホットプレート上で160℃~190℃で加熱し、リチウム金属を溶融状態に到達させた。次いで、多孔質シリコンの表面を、溶融されたリチウム金属と約30秒間密接に接触させた。その後、未反応のLi金属を多孔質シリコンの表面から除去した。
(実施例3)
ヨウ化リチウム(LiI)をバイアルに置き、アルゴンを満たしたグローブボックス(<0.1ppmのH2OおよびO2)内のホットプレート上で120℃で1時間乾燥した。3-メトキシプロピオニトリル(MPN)を分子篩(3Å)で一晩精製した。1Mの乾燥LiIをMPNに添加および溶解し、一晩軽く撹拌した。
(実施例4)
(エッチング時間:500秒)
図5は、5mA/cm2の電流密度での比容量に対する、多孔質シリコンアノードを有する再充電可能なヨウ化リチウム電池のサイクル数のプロットである。エッチング時間は500秒と記録され、これは上述したように、結晶シリコンアノードで形成された多孔質領域の深さを決定し、エッチング時間の増加は、多孔質領域においてより深い細孔を提供する。比放電容量は、第1のサイクルでは約0.7mAh/cm2から開始し、次のサイクルでは約1.0mAh/cm2まで増加し、約50回目のサイクルまで続いた。
(実施例5)
(エッチング時間:1200秒)
図6は、5mA/cm2の電流密度での比容量に対する、多孔質シリコンアノードを有する再充電可能なヨウ化リチウム電池のサイクル数のプロットである。エッチング時間は1200秒と記録された。比放電容量は、第1のサイクルで約0.5mAh/cm2から開始し、次のサイクルでは約1.0mAh/cm2まで増加し、約250回目のサイクルまで続いた。
(実施例6)
(エッチング時間:2400秒)
図7は、5mA/cm2の電流密度での比容量に対する、多孔質シリコンアノードを有する再充電可能なヨウ化リチウム電池のサイクル数のプロットである。エッチング時間は2400秒と記録された。比放電容量は、第1のサイクルで約0.5mAh/cm2から開始し、次のサイクルでは約1.0mAh/cm2まで増加し、約500回目のサイクルまで続いた。
非多孔質シリコンアノードを有する再充電可能なヨウ化リチウム電池
図8は、5mA/cm2の電流密度での比容量に対する、裸の(非多孔質)シリコンアノードを有する再充電可能なヨウ化リチウム電池のサイクル数のプロットである。エッチング時間は、アノードが多孔質領域を含んでいないこと示す0秒と記録された。裸の(非多孔質)シリコンアノードを上の実施例4~6に記載したのと同じ方法でプレリチウム化した。比放電容量は、第1のサイクルで約0.6mAh/cm2から開始し、次のサイクルでは約0.9mAh/cm2まで増加し、約20回目のサイクルまで続いた。
Claims (18)
- 電池であって、
金属ハロゲン化物および導電性材料を含み、前記金属ハロゲン化物が活性カソード材料として作用する、カソードと;
約0.5ミクロン~約500ミクロンの深さの細孔を有する表面を具備し、前記表面におよび前記細孔の少なくとも一部に金属を含む、多孔質シリコンアノードと;
前記アノードおよび前記カソードに接触し、ニトリル部分を含む、電解質と
を含む、電池。 - 前記金属が、Li、Na、Mg、Zn、Al、ならびにこれらの混合物および組合せからなる群から選択される、請求項1に記載の電池。
- 前記金属が、約5オングストローム未満のRMS表面粗さを有する層を含む、請求項2に記載の電池。
- 前記アノードが結晶Siを含む、請求項1に記載の電池。
- 前記アノードが、B、Al、In、Ga、ならびにこれらの混合物および組合せからなる群から選択される金属でドープされている、請求項1に記載の電池。
- 活性カソード材料としてハロゲン分子を含む、請求項1に記載の電池。
- 前記アノードと前記カソードの間にセパレータを含む、請求項1に記載の電池。
- 前記電解質がイオン伝導性材料を含む、請求項1に記載の電池。
- 前記電池が、酸素、空気、一酸化窒素、二酸化窒素、ならびにこれらの混合物および組合せからなる群から選択される酸化性ガスを含む、請求項1に記載の電池。
- 前記電解質が、エーテル、グリム、カーボネート、アミド、アミン、有機硫黄溶媒、有機リン溶媒、有機シリコン溶媒、フッ化溶媒、複素環溶媒、ならびにこれらの混合物および組合せからなる群から選択される溶媒を含む、請求項1に記載の電池。
- 前記金属ハロゲン化物が、溶媒中で各ハロゲン化物イオンおよび各金属イオンに解離する電解質塩を含み、前記ハロゲン化物イオンがI、Br、ClおよびFのうちの少なくとも1つのイオンを含み、前記金属イオンが、Li、MgおよびNaのうちの少なくとも1つのイオンを含む、請求項1に記載の電池。
- 各金属イオンおよび各対アニオンに解離する追加の塩をさらに含み、前記金属イオンが、Li、MgおよびNa、ならびにこれらの混合物および組合せからなる群から選択され、前記アニオンが硝酸アニオン(NO3 -)、ヘキサフルオロリン酸アニオン(PF6 -)、テトラフルオロホウ酸アニオン(BF4 -)、ビスオキサラトホウ酸アニオン(BOB-)、ジフルオロオキサラトホウ酸アニオン(DFOB-)、トリフルオロメタンスルホン酸アニオン(TF-)、トリフルオロスルホニルイミドアニオン(TFSI-)、ならびにこれらの混合物および組合せからなる群から選択される、請求項11に記載の電池。
- 前記金属ハロゲン化物を含む前記活性カソード材料に加えて専用のカソード材料をさらに含み、前記専用のカソード材料が、前記電池が接続される外部電気回路への導電路を提供する、請求項1に記載の電池。
- 電池を形成する方法であって、
結晶Si基板を陽極酸化して、少なくとも500nmの深さの細孔を有する多孔質Siアノードを形成することと;
前記多孔質Siアノードを、Li、Na、Mg、Zn、Al、ならびにこれらの混合物および組合せからなる群から選択される金属で金属化することと;
セパレータを、金属ハロゲン化物を含む活性カソード材料およびニトリル化合物を含む非水溶媒を含む電解質溶液に浸すことと;
前記電解質溶液に浸した前記セパレータを前記アノードと集電体の間に置くことと;
酸化性ガスを前記積層されたアノード、前記溶液に浸した前記セパレータ、および前記集電体に導入して前記電池を形成することと
を含む、方法。 - 前記多孔質Siアノードが、Li金属層を含む、請求項14に記載の方法。
- 前記層が、約5オングストローム未満のRMS表面粗さを有する、請求項15に記載の方法。
- 前記多孔質Siアノードが、B、Al、In、Ga、ならびにこれらの混合物および組合せからなる群から選択される金属でドープされる、請求項14に記載の方法。
- 充電/放電サイクル数における前記電池の平均サイクル寿命と陽極酸化時間との比が、約2以上である、請求項14に記載の方法。
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