電動車與再生能源的發展帶動對於儲能裝置的需求，具有高能量密度的鋰離子電池因此被視為最具潛力的電池系統。在鋰離子電池中，正極材料除了在電壓與電容上扮演重要角色，也會大幅影響其製作成本，故如何在低成本的條件下開發出具有高能量密度的正極材料，是研究正極材料中十分重要的一環。無鈷富鋰層狀正極材料具有低成本、環境友善等特性，且能量密度可高達1000 Wh/kg，遠超越目前所有商用正極材料。然而，此種材料需倚賴高電壓下Li2MnO3的活化來提升其電容值，易引發不可逆的相轉變而使可用電容與平均電壓隨充放電循環迅速衰減，較差的導電性也使無鈷富鋰正極材料無法應用於高速充放電循環中。高鎳材料雖為目前層狀材料的發展趨勢，但相較於錳元素，鎳元素的價格高、地表含量低，故若能在富鋰正極材料中以較高含量的錳來取代鎳的使用，將可進一步降低成本並大幅提升可用電容量。此外，過去雖已有許多以離子摻雜改善無鈷富鋰層狀正極材料之結構穩定性的研究，但尚未有使用鋅離子進行摻雜。在本篇研究中，我們使用鋅離子摻雜於具有不同鎳錳比例的無鈷富鋰層狀正極材料中，低鎳/錳比例的無鈷富鋰層狀正極材料雖具有較高的放電比電容與能量密度，但維持率不如高鎳/錳比例的材料，會隨著充放電循環而快速衰減。透過系統性的研究，我們發現當使用適量鋅離子摻雜於低鎳/錳比例的無鈷富鋰層狀正極材料時，將可有效減緩不可逆相變化生成，使其在充放電循環中保有良好的電化學表現。具有高能量密度、高電化學穩定性，且低成本的高錳低鎳的無鈷富鋰正極材料，將可透過鋅離子摻雜而實現。

Due to the increasing demand on high energy density, more research is drawn to lithium-ion batteries (LIBs) in recent decades. Among all the cathodes used in LIBs, cobalt-free lithium-rich layered oxides (LLOs) not only have the highest energy density (over 1000 Wh/kg) but are cost-effective and eco-friendly. However, LLOs suffer from the layered-to-spinel phase transformation, which lead to severe voltage fading and capacity decay during cycling, inhibiting from the practical usage. In this research, cobalt-free LLOs were successfully synthesized by carbonate co-precipitation method. We systematically studied the effect of zinc doping in cobalt-free LLOs with different Ni/Mn ratios for the first time. We demonstrated that Zn2+ ions, used as pillar ions, effectively alleviated the capacity decay and voltage fading in cobalt-free LLOs with low Ni/Mn ratio. The energy density could be greatly improved from 750 Wh/kg to 870 Wh/kg, and the corresponding retention could be highly maintained within 50 cycles as well. A promising cathode material with high energy density, good stability, and low cost could thus be obtained by zinc doping in cobalt-free LLOs with low Ni/Mn ratio.

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