JP2017069206A - 負極活物質、それを採用した負極、及びリチウム電池 - Google Patents
負極活物質、それを採用した負極、及びリチウム電池 Download PDFInfo
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- JP2017069206A JP2017069206A JP2016192955A JP2016192955A JP2017069206A JP 2017069206 A JP2017069206 A JP 2017069206A JP 2016192955 A JP2016192955 A JP 2016192955A JP 2016192955 A JP2016192955 A JP 2016192955A JP 2017069206 A JP2017069206 A JP 2017069206A
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- Prior art keywords
- negative electrode
- active material
- electrode active
- silicon
- fesi
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Abstract
Description
本発明が解決しようとする他の課題は、上記負極活物質を採用した負極を提供することである。
本発明が解決しようとするさらに他の課題は、上記負極を採用して寿命特性が向上したリチウム電池を提供することである。
本発明のさらに他の側面では、上記リチウム電池用負極を含む、リチウム電池が提供される。
ここで、用語「非活性」は、電池の充放電時、リチウムイオンの吸蔵/放出に関与しないことを意味し、用語「活性」は、電池の充放電時、リチウムイオンの吸蔵/放出に関与することを意味する。
ところで、活性シリコン粒子は、充放電時に体積変化が大きく、何回も充放電した後には、シリコン系合金を含む活物質が壊れたり、活物質間の導電経路が断絶されたりするような問題点が発生する。また、かような問題点によって、電池のサイクル寿命特性が低下することがある。
本実施形態によるリチウム電池は、上記した負極を含む。例えば、一実施形態によるリチウム電池は、上記した負極活物質を含む負極と、この負極に対向して配置される正極と、負極及び正極の間に配置される電解質と、を含んでもよい。
それら電池の製造方法は、当該分野に周知されているので、詳細な説明は省略する。
図5を参照すれば、リチウム電池200は、正極130、負極120、及び正極130と負極120との間に配置されたセパレータ140を含む。前述の正極130、負極120及びセパレータ140が巻き取られたり折り畳まれて電池容器150に収容される。次に、電池容器150に電解質が注入され、封入部材160によって密封され、リチウム電池200が完成される。電池容器150は、円筒型、角型、薄膜型などでもある。リチウム電池は、リチウムイオン電池でもある。
[リチウム二次電池の製造]
(負極の製造)
まず、Si 80.2原子%、Fe 17.9原子%及びMn 1.9原子%を混合した後、それらを真空誘導溶解炉(Yein Tech.、韓国)に投入し、大気による酸化を最大限抑制するために、真空雰囲気下で溶解させ、親合金を作製した。
Si 81.2原子%、Fe 18.6原子%及びMn 0.2原子%を混合して親合金を製造したシリコン系合金を、負極活物質として使用したことを除いては、実施例1と同一の方法を使用してリチウム二次電池を製造した。
Si 80.9原子%、Fe 17.0原子%及びAl 2.1原子%を混合して親合金を製造したシリコン系合金を、負極活物質として使用したことを除いては、実施例1と同一の方法を使用してリチウム二次電池を製造した。
Si 78.3原子%、Fe 15.6原子%及びMn 6.1原子%を混合して親合金を製造したシリコン系合金を、負極活物質として使用したことを除いては、実施例1と同一の方法を使用してリチウム二次電池を製造した。
上記実施例1、及び比較例1ないし比較例3で製造された負極活物質に対して、1.5406ÅのCu−Kαを使用して、XRD分析(D8 focus、Bruker社製)を実施した。その結果を図6に示す。
容量維持率[%]=[各サイクルでの放電容量/最初のサイクルでの放電容量]×100 (数式1)
130 正極
140 セパレータ
150 電池容器
160 封入部材
200 リチウム電池
Claims (15)
- シリコン系合金を含む負極活物質であって、
前記シリコン系合金は、Si−Fe−M1で表示され、
前記M1は、リチウム(Li)、マグネシウム(Mg)、カルシウム(Ca)、チタン(Ti)、バナジウム(V)、クロム(Cr)、マンガン(Mn)、コバルト(Co)、ニッケル(Ni)、銅(Cu)、亜鉛(Zn)、イットリウム(Y)、ジルコニウム(Zr)、モリブデン(Mo)、インジウム(In)、スズ(Sn)、ホウ素(B)、炭素(C)、酸素(O)及びリン(P)のうちから1種以上選択され、
前記シリコン系合金は、Si単一相、FeSi2アルファ相及びFeSi2ベータ相を含み、
前記負極活物質は、Cu−Kαを使用したX線回折分析スペクトルにおいて、前記FeSi2アルファ相による回折角度(2θ)17.0+/−0.5゜での回折ピーク、及び前記FeSi2ベータ相による回折角度(2θ)28.7+/−0.5゜での回折ピークを示し、
前記FeSi2アルファ相による回折ピークの回折強度に対する、前記FeSi2ベータ相による回折ピークの回折強度の比が、0.1以上である、負極活物質。 - 前記FeSi2アルファ相による回折ピークの回折強度に対する、前記FeSi2ベータ相による回折ピークの回折強度の比が、0.2ないし3.0である、請求項1に記載の負極活物質。
- 前記M1は、チタン(Ti)、バナジウム(V)、クロム(Cr)、マンガン(Mn)、コバルト(Co)、ニッケル(Ni)、銅(Cu)及び亜鉛(Zn)のうちから1種以上選択された、請求項1に記載の負極活物質。
- 前記シリコン系合金において、Si,Fe及びM1原子の総個数を基準に、Siの含量は、67ないし92原子%であり、Feの含量は、4ないし32原子%であり、M1の含量は、0.3ないし6.0原子%である、請求項1に記載の負極活物質。
- 前記シリコン系合金において、Si,Fe及びM1原子の総個数を基準に、Siの含量は、75ないし90原子%であり、Feの含量は、9ないし22原子%であり、M1の含量は、0.3ないし6.0原子%である、請求項1に記載の負極活物質。
- 前記FeSi2アルファ相及び前記FeSi2ベータ相は、前記Si単一相と界面をなし、前記Si単一相を取り囲むマトリックスの役割を行う、請求項1に記載の負極活物質。
- 前記シリコン系合金において、前記M1は、前記Si単一相、前記FeSi2アルファ相及び前記FeSi2ベータ相の結晶格子のうち、少なくとも一つに、ドーピングされている、請求項1に記載の負極活物質。
- 前記シリコン系合金は、M1含有ケイ化物を含まない、請求項1に記載の負極活物質。
- 前記シリコン系合金は、Si−Fe−Mnで表示され、
前記シリコン系合金において、Si、Fe及びMn原子の総個数を基準に、Siの含量は、75ないし90原子%であり、Feの含量は、9ないし22原子%であり、Mnの含量は、0.3ないし6.0原子%である、請求項1に記載の負極活物質。 - 前記シリコン系合金は、Si80Fe18Mn2、Si80.2Fe17.9Mn1.9、Si83.9Fe13.2Mn2.9、Si87.5Fe10.9Mn1.6またはSi78.3Fe21.1Mn0.6である、請求項9に記載の負極活物質。
- 前記シリコン系合金は、Mn含有ケイ化物を含まない、請求項10に記載の負極活物質。
- 前記Mn含有ケイ化物が、MnSi1.7である、請求項11に記載の負極活物質。
- 前記シリコン系合金の平均粒径(D50)は、1μmないし5μmである、請求項1ないし12のうちいずれか1項に記載の負極活物質。
- 請求項1ないし13のうちいずれか1項に記載の負極活物質を含む、リチウム電池用負極。
- 請求項14に記載のリチウム電池用負極を含む、リチウム電池。
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