摘要: | 在目前的電解液型二次電池系統中,可充式鋁電池(RAB)因其優異的特性,如高體積能量密度、高速率充放電穩定性、環保、地球蘊含豐富和低成本(基於陰極和陽極材料)。 此外,可充式鋁電池所使用的電解液系統具有不易燃、低毒性和低環境衝擊等諸多優點。 但是直到目前為止鋁電池還存在一些問題需要被克服,如低放電電壓平台、高腐蝕性電解質、嚴重的自放電現像以及謎團般的氯鋁酸鹽陰離子 - 石墨插層反應。 在本研究中,我們著重在鋁電池的自放電現象。 針對充放電速率、石墨正極材料的影響、鋁負極的純度和離子液體陽離子的類型進行系統性的研究。 通過上述努力,我們將推測鋁電池的自放電機制。 此外我們研究了摻混石墨正極材料(如氮摻雜,硼摻雜)中的自放電現象。 幸運的是,摻雜石墨不僅增強了電容值表現,同時增強了高速性能表現。 不幸的是,由於摻混後的高能量插層狀態(Stage-3 GIC),使得自放電問題變得更嚴重。 並通過NSRRC中的In-situ XRD分析,我們追踪了充電和放電過程中石墨正極材料的相變化,做為該機制的有力證據。 最後,本研究首次對鋁電池的自放電機制及其影響因素進行了詳盡研究。 期待這些結果將有助於未來鋁電池商業化的發展。 ;Among current electrolyte-based rechargeable battery systems, the rechargeable aluminum battery (RAB) stands out for its predominating advantages, such as high-volumetric energy density, high-rate charge-discharge stability, eco-friendliness, earth abundance, and low-cost (based on cathode and anode material). Moreover, the electrolyte systems of the rechargeable aluminum battery have many advantages such as nonflammable, low toxicity and environmental impact. However, there still some problem need be overcome like low discharge voltage plateau, the highly corrosive electrolyte, serious self-discharge phenomenon and the puzzle for chloroaluminate anion–graphite intercalation reactions. In this study, we focused on the self-discharge phenomenon. Systematical research on effect of cathode materials, purity of aluminum anode, charge/discharge rate and the type of ionic liquid cation will be carried out. With the aforementioned efforts, we will examine the self-discharge mechanism of aluminum batteries. Furthermore, we investigated the self-discharge phenomenon in doped graphite cathode materials (using N-doped, B-doped). Fortunately, doped graphite enhanced not only the capacitance but also the high-rate performance like our prediction. Unfortunately, the self-discharge problem became more serious due to the high energy state intercalation (Stage-3 GIC). With the In-situ XRD analysis in NSRRC, we traced the phase transformation in cathode materials from charge to self-discharge than discharge. The results were a powerful evidence for the mechanism in this study. Finally, this study is the first research about the self-discharge mechanism for RAB and its impact factor. Perhaps the results will have contributed to the development of commercialization of aluminum batteries in the future. |