隨著科技的不斷地進步和人們對於用電量的需求上升，儲能系統的重視度持續攀升。與其他種類的電池相比較，鋰離子電池擁有較高的能量密度、循環壽命長等優點，現今已被普遍應用在儲能設備系統上，它被視為成功的能源儲存科技之一。
常用的傳統鋰離子電池中陽極其電容量受到限制，而有機材料結構可調整，它所形成的電極毒性低、質量輕，但它易溶於電解液中使得電池循環穩定性不佳。所以我們將有機單體與金屬離子合成一維配位聚合物，它可擁有多個氧化還原活性中心，可以讓理論電容量發揮到更高。
本研究以新合成的錳金屬有機材料，線性[MnL(DMF)2]n (MLD)和非線性[MnL(Py)3] n (MPy)，應用在鋰離子電池的正極材料。它們是由1,4-二氰基-2,3,5,6-四羥基苯(LH4)作為有機單體與錳離子進行反應形成的聚合物。它們具有苯醌結構，在電池反覆地充放電過程中，共軛羥基會得失兩個電子，同時與錳金屬能發生協同氧化還原反應，創造多個電荷轉移反應。MLD是由錳在軸向位置與二甲基甲醯胺分子 (DMF)進行配位；MPy是利用吡啶分子(pyridine)置換掉軸向的二甲基甲醯胺分子。MLD 在500 mA g‒1 的電流密度下可得初始電容量296 mAh g‒1 經過160次循環充放電過程，電容量保有率為81.0 %，在5 A g‒1下可得 203 mAh g‒1 經過1000次循環充放電過程後，電容量保有率為54.9 %；MPy在500 mA g‒1 的電流密度下可得出使電容量279 mAh g‒1，經過160次循環充放電過程，電容量保有率則為81.3 %，在20 A g‒1下可得 140 mAh g‒1 經過1000次循環充放電過程，電容量保有率仍可保有83.7 %。從電化學反應可得知，MPy在更高的電流密度下，仍然可以進行充放電反應，並且擁有更高的保有率。這是因為MPy中吡啶分子不僅提供C≡N⋯H, C≡N⋯π，還有 π⋯π, C−H⋯π 作用力，使結構之間更穩定，同時可供應更多的電荷傳輸途徑，因此擁有更佳的倍率性能。藉由非原位(ex-situ)之掃描電子顯微鏡、X光繞射、X射線光電子能譜儀以及傅立葉轉換紅外光譜等技術，進一步探討其循環充放電的過程中它們的反應機制與化學變化。透過此研究於錳系金屬有機材料的了解，能為下一代可充式電池發展奠定基礎。

Compared with other types of batteries, lithium-ion batteries (LIBs) possess relatively high energy density and longer life span, they have already been widely used in energy storage systems and are considered to be one of the most successful energy storage technologies. Traditional inorganic-based LIBs typically have a limited capacity and therefore organic-based compounds are promising as active materials. Organic-based electrodes have several advantages, such as structure tunability, nontoxicity, and light weight. However, they display poor cycling stability owing to the dissolution issues in organic electrolytes. One strategy to solve the problem is to combine redox-active organic bridging ligand with metallic nodes to form coordination polymers (CPs). This type of materials could have a variety of redox-active centers leading to higher theoretical capacity.
In this study, by reacting redox-active bridging ligand 1,4-dicyano-2,3,5,6-tetrahydroxybenzene (LH4) with manganese ions from manganese nitrate, two novel 1D manganese-based CPs, namely, linear [MnL(DMF)2]n or MLD and non-linear [MnL(Py)3]n or MPy, have been synthesized as cathode materials for LIBs. In MLD, the manganese is coordinated to dimethylformamide (DMF) molecules in the axial positions, while for MPy, the DMF is replaced by pyridine (Py) molecules. During discharge and charge, the quinone groups of LH4 gain and lose two electrons due to lithiation/delithiation process. Simultaneously, the manganese metal centers have been confirmed to undergo synergistic redox reactions, resulting in multiple-electron transfer reactions leading to high practical capacities. The initial capacity of MLD at a rate of 500 mA g‒1 is 296 mAh g‒1, with a capacity retention maintained at 81.0 % after 160 cycles, whereas at 5 A g‒1, the compound initially delivers 203 mAh g‒1 and maintains 54.9 % after 1000 cycles. When tested in LIBs, MPy initially gives 279 mAh g‒1 at 500 mA g‒1, and delivers 81.3 % after 160 cycles. Interestingly, at 5 A g‒1, MPy can give a capacity of 140 mAh g‒1 with a capacity retention as high as 83.7 % after 1000 cycles. It can be included from the electrochemical investigations that MPy can operate at higher current density and can provide a better capacity retention. This is because Py in MPy not only offers C≡N⋯H, C≡N⋯π, but also π⋯π, and C−H⋯π weak interactions, therefore stabilizing structures and providing more pathways for electron transfer along the 1D CP chains. Ex-situ scanning electron microscopy (SEM), powder X-ray diffraction (PXRD), X-ray photoelectron spectroscopy (XPS), and Fourier-transform infrared spectroscopy (FT-IR) are used to elucidate the reaction mechanism and the changes of electrochemical reactions in the cyclic process. Without a doubt, the insights into MLD and MPy can lay a foundation for Mn-based materials of CPs for evolution of next-era rechargeable batteries.

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