高能量密度、環境友善以及價格低廉電極材料被視為決定下一世代鋰離子的關鍵參數。鋰離子電池被廣泛的用於儲能系統、可攜式電子裝置、自動化機械和電動工具中。除此之外，鋰離子電池也被應用在電動汽車上來減少石化燃料以及溫室氣體的排放，進而降低對自然環境的衝擊。以石墨作為鋰離子電池的負極材料，可以有較低的花費，穩定的平台以及提供許多層狀結構供鋰離子嵌入。然而其較低的理論電容量，以及容易長出鋰枝晶的問題，增加了以石墨作為負極材料的鋰離子電池許多安全上以及性能上的疑慮。目前，有許多的方法正在被開發用來取代石墨扮演的負極角色，如使用硫、矽、石墨烯、鍺、過渡金屬氧化物或是有機材料來構築鋰離子電池的負極。其中，為了滿足高能量密度、循環壽命、製備容易以及價格低廉的要求，有機材料被認為是最佳的選項來建構鋰離子電池的負極。在設計上，有機材料為主的電池可以不只是和大多數鹼金屬、鹼土金屬如 Li+, Na+, K+, Mg2+, and Ca2+，也可以減少排放到大氣中的二氧化碳。然而，較差的導電子能力以及容易溶解在電解液的問題，仍然困擾著有機鋰離子電池的發展，也成為有機離子電池開發的首要問題。
導電高分子”PITN” 在所有共軛高分子能隙最小，並具有高導電性，已被研究為具有和鋰離子以及電解液離子作用能力（Li+和PF6-）的氧化還原活性雙極電極材料，其中 n型摻雜/去摻雜反應電位在 0.0 -3.0 V之間(和Li+有關)，p-型摻雜/去摻雜的反應電位在1.5-4.5 V之間，而b-型（全有機電池）同時對Li+ 和PF6-離子進行摻雜的電位範圍為0.0-4.0 V的/去摻雜反應。該PITN在n摻雜和p摻雜過程中分別在其環狀C–S–C鍵和苯環上接受鋰和PF6-離子。研究發現，在第一次電化學反應過程中形成了多硫化鋰和硫化鋰。但是，PITN電池的阻抗，速率性能和能量密度不受這些產物所影響。與陽極材料（例如石墨，矽和其他共軛聚合物）相比，此機制呈現了更優異的表現。通過原位X射線吸收光譜，臨場傅立葉變換紅外光譜，場發射電子顯微鏡和X射線光電子能譜研究PITN電極的表面特性。此外，本研究也繼續討論在PITN上進行n摻雜和p摻雜的反應機制。 PITN電極接受的鋰離子在第二個循環中的比容量為730 mAhg-1，與PF6-反應時的比容量為106 mAhg-1。在雙極模式下，電池性能表現出約92 mAhg-1的容量。低帶隙共軛PITN在雙極電化學反應方面顯示出高可逆性，凸顯出此材料在有機鋰離子電池的應用性。
在第二部分的研究中，低分子量有機羰基化合物，馬來酰胺酸和馬來酸鋰，由於其易於合成，低成本和高理論容量而被認為是LIB中有益的儲能材料。馬來酸鋰是通過簡單的濕化學合成方法，以馬來酰胺酸為前驅物合成的。馬來酰胺酸電極具有出色的倍率容量（932 mAg-1時為156 mAhg-1）和循環壽命，經過50次循環後可逆容量為46.6 mAg-1時為455 mAhg-1，平均庫侖效率約為98 ％。 MA陽極電極在第一個循環中提供了約685 mAh g-1的可逆容量，並且比馬來酸鋰電極具有更高的倍率容量。有機馬來酰胺酸電極的出色性能和高可逆容量可歸因於其化學結構重整為新的基於氮的高離子擴散化合物。
在最後研究的部分中，我們開發了兩種新的基於雙馬來酸酯的有機陽極材料，即二鋰N，N-（對-亞苯基）雙馬來酸酯（Li2-p-PBM）和二鋰N，N-（2-氟-對-亞苯基）雙馬來酸（Li2-F-p-PBM），包括其通過簡單的濕化學方法合成以及對LIB的電化學研究。使用Brunauer-Emmett-Teller（BET）和Barrett-Joyner-Halenda（BJH）方法測量了這些化合物的比表面積和孔徑分佈，結果表明，氟取代（Li2-F-p-PBM）樣品相較非取代電極（Li2-p-PBM）表現出較大的表面積和孔徑分佈。這表明Li2-F-p-PBM樣品的較高表面積和孔隙率可有助於增強電極界面處的電荷轉移，從而實現更好的電化學性能。 Li2-F-p-PBM的電化學性能顯示出更高的可逆容量（0.1 C時為557 mAhg-1），更好的倍率性能（10 C時為185 mAhg-1）和出色的循環壽命表現。Li2-F-p-PBM電極的優異電化學性能可歸因於氟效應，該效應改善了鋰離子擴散和電子電導率。但是，氟的作用尚未得到充分研究，因此，還需要進一步搭配其他臨場分析技術徹底分析該機制。

High energy density, eco-friendly and low-cost electrode materials are the crucial parameters for the next-generation rechargeable batteries. Lithium-ion batteries (LIBs) are widely used as energy storage systems in portable electronics, automatic machines, and power tools. It also used in electric vehicles to eliminate environmental pollution caused by using fossil fuel and avoid global warming. Graphite is the anode material in commercial LIBs owing to its low working potential, flat plateau, low cost and reversibly insert lithium-ion between its many layer structures. However, graphite only provides low theoretical capacity (372 mAh g−1) and presents a high risk of lithium dendrites growth that prevents increasing energy demand. Recently, several methods are ongoing to replace the graphite anode with new battery architecture such as sulfur, silicon, graphene, germanium, transition metal oxide, and organic-based materials (OEMs). To satisfy the criteria of high energy density, long cycle life, easy fabrication, and the low cost for energy storage, organic materials are the best option. This organic battery design not only because they accept most of the alkali- or alkali-earth metal ions such as Li+, Na+, K+, Mg2+, and Ca2+ for energy storage but also eradicating the carbon-dioxide released to the atmosphere. Organic-based LIBs are among the future promising energy storage rechargeable batteries owing to their easy synthesis, often renewable, cheap, environmentally friendly and deliver much higher theoretical capacities with structural flexibility. However, their poor electronic conductivity and highly soluble in liquid electrolyte still impede their practical application. Hence, the development of organic batteries with high conductivity, high theoretical capacity, and natural abundance can solve the obstacles of the current inorganic batteries.

Conductive polymer, polyisothianaphthene (PITN) has the smallest bandgap among all conjugated polymers and delivers high electrical conductivity, investigated as a redox-active bipolar electrode material with electrolyte ions (Li+ and PF6−): n-type doping/dedoping reaction associated with Li+ binding in a potential range 0.0-3.0 V, p-type doping/dedoping mechanism involved with PF6- binding in a potential range 1.5-4.5 V and b-type (all-organic battery) where both the Li+ and PF6– ions undergo doping/dedoping reaction in a potential range 0.0-4.0 V versus Li/ Li+ is reported in our first approach. This PITN accepts both lithium and PF6- ions on its cyclic C–S–C bond and benzene ring during the processes of n-doping and p-doping respectively. This study discovers that lithium polysulfide and lithium sulfide are formed during the first electrochemical reaction; however, the impedance, rate performance, and energy density of PITN cells are not affected by those side products. By contrast, an increment of superior rate (10 C) testing is significantly improved by those new sulfur-based solid electrolyte interphase formations compared with transitional anode materials, such as graphite, silicon, and other conjugated polymers. The surface characteristics of the PITN electrode are investigated through in situ X-ray absorption spectroscopy, in operando Fourier transform infrared spectroscopy, scanning electron microscopy, and X-ray photoelectron spectroscopy. Furthermore, the reaction mechanisms of n-doping and p-doping on PITN are discussed. The PITN electrode’s acceptance of lithium ions exhibits a specific capacity of 730 mAhg-1 at the second cycle as well as of 106 mAhg-1 when it reacts with PF6-. The battery performance exhibits a capacity of approximately 92 mAhg-1 in the bipolar mode. The low-bandgap conjugated PITN is shown to have high reversibility in terms of bipolar electrochemical reactions, which indicates that it can be a promising bipolar organic material for use in lithium-ion batteries.

In the second work, low-molecular-weight organic carbonyl compounds, maleamic acid, and lithium maleamate are considered beneficial energy storage materials in LIBs owing to the ease of their synthesis, low cost, and high theoretical capacity. Lithium maleamate is synthesized by a simple wet chemistry method adopting maleamic acid as a precursor. The maleamic acid electrode delivers a superior rate capability (156 mAhg-1 at 932 mAg-1) and long-term cyclability with a reversible capacity of 455 mAhg-1 at 46.6 mAg-1 after 50 cycles with an average coulombic efficiency of about 98%. The MA anode electrode delivered a high reversible capacity of about 685 mAh g−1 in the first cycle and a higher rate capability than that of the lithium maleamate electrode. The outstanding performance and high reversible capacity of the organic maleamic acid electrode can be attributed to the reforming of its chemical structure into new nitrogen-based highly ionic diffusion compounds.
In the final work, we develop two new bismaleamate-based organic anode materials namely dilithium N, N- (p-phenylene) bismaleamate (Li2-p-PBM), and dilithium N, N-(2-Fluoro-p-phenylene) bismaleamate (Li2-F-p-PBM) including their synthesis via simple wet chemistry method and their electrochemical investigations for LIBs. They have carbonyl groups with carboxylic acid and amide as redox-active centers for lithium-ion insertions. Specific surface area and pore size distribution of these compounds were measured using the Brunauer- Emmett-Teller (BET) and Barrett-Joyner-Halenda (BJH) methods revealed that the fluorine substituted (Li2-F-p-PBM) sample exhibits a large BET specific surface area and pore size distribution compared to the non-substituted electrode (Li2-p-PBM) sample. This indicates that the higher surface area and porosity for the Li2-F-p-PBM sample can contribute to enhancing charge transfer at the interface of the electrode ensuing better electrochemical performance. The electrochemical performance for the Li2-F-p-PBM showed a higher reversible capacity (557 mAhg-1 at 0.1 C), better rate performance (185 mAhg-1 at 10 C), and superior cyclability (425 mAhg-1 after 350 cycles at 1 C) in comparison with the unsubstituted electrode. The excellent electrochemical performance of the Li2-F-p-PBM electrode could be attributed to the fluorine effects which improves the lithium-ion diffusion and electronic conductivity. However, the fluorine effect is not fully investigated, therefore, further in-operando techniques are required to figure out thorough.

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