近年，リチウムイオン二次電池の高エネルギー密度の向上が望まれている．高エネルギー 密度の向上の研究として正極・負極材料の元素選定，結晶構造の選定および粒子径の改良が 挙げられる．正極材料では，正極材料の高電圧化，Li過剰系材料および活物質のナノ粒子合 成に関する研究が多数報告されている．しかしながら，その多くは液相法や固相法による合 成例である．一般的に液相法および固相法は，組成の制御が容易であるという利点を持って いるが，Fe，Cr，Mo，Mn，Cuの不純物の混入が避けられず高純度でのナノ粒子合成には不 向きである．また，合成においては室温から高温への反応機構により，物質の駆動力として 活性化エネルギー，反応動力学に基づいた合成法となり，10時間以上の長時間の合成と14 工程数を必要とするため，コストと時間に課題がある．負極材料に関しても同様にSiを用 いた多くの研究報告がされている．負極材料の多くは，液相法と固相法による合成法で行わ れている．しかしながら，正極同様に合成途中での不純物の混入およびSiの酸化の影響が 避けられないため，電池容量が変動する課題がある．そこで本研究では，数ミリ秒の短時間
55
合成および純度の高いナノ粒子の合成プロセスである高周波熱プラズマを用い，リチウム イオン二次電池の正極・負極材料ナノ粒子の合成を一段階合成で行い，その特性および生成 機構について解明することを目的とした．本論文の構成概略図をFig. 1-11に概略を下記に 示した．
第1章
第1章では，熱プラズマ，ナノ粒子，電池の特徴，リチウムイオン二次電池のナノ粒子応 用例について記述した．さらに，高周波熱プラズマを用いたナノ粒子合成に関する既往の研 究とその動向を記した．最後に本研究の目的を示した．
第2章
第 2 章では，高周波熱プラズマを用いた合成の実験装置，実験条件，分析方法を記載し た．
第3章
第3章では，Li-Mn系の二元系複合酸化物ナノ粒子合成に関する実験結果と考察について
記述した．熱プラズマ処理におけるガス流量，酸素分圧および原料供給を変化させ生成物へ の影響を検討した．また核生成温度および熱力学的検討から生成機構を考察した．さらに，
合成したLi-Mn酸化物の電池特性について考察した．
第4章
第4章では，Li-Ni系の二元系複合酸化物ナノ粒子合成に関する実験結果と考察について 記述した．熱プラズマ処理におけるガス流量，酸素分圧や原料供給を変化させ生成物への影 響を検討した．また核生成温度および熱力学的検討から生成機構を考察した．さらに，合成
したLi-Ni酸化物の電池特性について考察を行った．
第5章
第5章では，高電圧の正極電池材料として期待されるLi-Ni-Mn系の三元系複合酸化物ナ ノ粒子合成に関する実験結果と考察について記述した．第3章および第4章で合成した Li-Mn酸化物および Li-Ni 酸化物に Niおよび Mnを置換し高電圧材料化させることを目的と し，核生成温度および熱力学的な検討から生成機構を考察した．さらに，合成したLi-Ni-Mn 酸化物の電池特性について考察を行った．
第6章
第6章では，高容量の正極電池材料として期待されるLi-Nb-Mn系の三元系複合酸化物ナ ノ粒子合成に関する実験結果と考察について記述した．第3章で合成した Li-Mn 酸化物に Nb を置換および Li過剰化では Li3NbO4に Mnを置換し高容量材料化させることを目的と
56
し，核生成温度および熱力学的検討から生成機構を考察した．さらに，電池特性について考 察を行った．
第7章
第7章では，高容量の負極電池材料として期待されるSi-Ti系のSi複合酸化物ナノ粒子合 成に関する実験結果と考察について記述した．SiおよびTiのモル分率を変化させ生成物へ の影響を検討した．また核生成温度および熱力学的検討から生成機構を考察した．さらに，
電池特性について考察を行った．
第8章
第8章では，本研究のまとめと今後の課題・展望について述べた．
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