リチウム二次電池用正極活物質とその製造方法及びその用途

Anodic active material for lithium secondary battery and its production and use

Abstract

(57)【要約】 【課題】 高温下でも充放電サイクル特性や保存安定 性が良好でかつ高容量、高出力のリチウム二次電池を構 成できるリチウム電池正極用のリチウム−遷移金属系ハ ロゲン化酸化物を提供する。 【解決手段】 一般式Li 1+a Mg b M c Mn 2-a-b-c O 4-d X e (式中、MはV、Cr、Fe、Co、Niから選ば れた少なくとも1種類以上の置換金属元素、Xは少なく とも1種類以上のハロゲン元素。)で表されるリチウム −マグネシウム−マンガン含有遷移金属ハロゲン化酸化 物を主成分とするリチウム二次電池用正極活物質におい て、該正極活物質の粒子の表層側から内部に向かって酸 素原子を置換したハロゲンの濃度が減少してゆく濃度傾 斜層が存在し、粒子内部とのハロゲン濃度の差が、表層 部のハロゲン濃度と粒子内部のハロゲン濃度との差の1 0%に減衰するまでの深さが、最表面から0.3〜50 nmであるような傾斜構造を有し、かつ正極活物質中の 全ハロゲン含有量とリチウム以外の全金属元素の含有量 との原子比X/(Mn+Mg+M)が0.002〜0. 15であるリチウム二次電池用正極活物質。
PROBLEM TO BE SOLVED: To obtain a lithium-transition metal-based oxyhalide for lithium battery anode capable of constructing high-capacity, high-output lithium secondary batteries good in charge-discharge cycle characteristics and preservation stability even at high temperatures. SOLUTION: The subject anodic active material for lithium secondary batteries is such one as to consist mainly of a lithium-magnesium-manganese-contg. transition metal oxyhalide of the formula Li1+aMgbMcMn2-a-b-cO4-dXc (M is at least one of V, Cr, Fe, Co and Ni; X is at least one halogen element); wherein there exists a concentration-gradient layer where the concentration of the halogen(s) substituted for the oxygen atom(s) is decreased from the surface layer of the particle of the anodic active material toward the inside thereof, and there is a gradient structure where such a depth that the halogen concentration difference relative to the inside of the particle is diminished to 10% of the halogen concentration difference between the surface layer and the inside of the particle is 0.3-50 nm under the uppermost surface, and the ratio of the total halogen content to the content of all of the metal elements except lithium is 0.002-0.15 in terms of the atom ratio: X/(Mn+Mg+M).

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