開發一種新的系統和電池設計，是當今非常迫切需要的，以使其具有更高的容量及能量密度、成本效益、環境友好和安全性。本研究設計了一種電池，以硫複合材料為陽極，及尖晶石型陰極的新型電池系統，使具有高能量密度、低成本和安全性，同時克服了鋰金屬陽極相關的安全問題，及石墨陽極的低理論電容量的問題。
與目前用於提高鋰離子電池能量密度的材料相比，鋰金屬被認為是具有潛力的陽極材料。 然而，鋰金屬陽極受限於會產生破壞性枝晶構造，其會導致安全上的隱患，因此亟需具有高電容量和高安全性的陽極。由聚丙烯腈（S-C（PAN））合成出的硫化碳陽極已被用作於鋰硫電池的陰極。 在本研究的第一部分中，相反地，將S-C（PAN)當作陽極並與LMO組成電池時，在C-rate為1，工作電位在1到3.2V範圍內時，其全電池的能量密度為185 Wh kg-1（SC（PAN）+ LMO）。全電池（S-C（PAN）|| LMO）的特色在於充放電速率為0.1 C和2 C時，其可逆放電電容量分別為1378 mAh g-1s和868 mAh g-1s。 速率為1 C時，電池循環400圈後，電容量乃然保有807 mAh g-1s，平均衰減率為 0.7 mAh g-1s* cycle-1，平均庫侖效率為99.5％。 S-C（PAN）陽極的界面化學被特別地研究，並證明了S-C（PAN）是一種有趣的陽極材料，可以是鋰金屬的安全替代材料，因為硫具有很高的理論電容量（1675 mAh g-1）、對環境友好、低成本及能量密度高。
鋰錳氧（LMO）是鋰離子電池中最具潛力的正極材料之一。 然而，錳的溶解及其在陽極表面上的沉積導致較差的循環穩定性。為了緩解這些問題，本論文的第二部份，以電紡織方式將聚偏二氟乙烯（PVDF）和石榴石狀之Li5.6Ga0.26La2.9Zr1.87Nb0.05O12組成的纖維膜（PVDF @ LGLZNO）直接塗覆在LMO電極上，作為有潛力的人造陰極/電解質界面層（CEI），其膜厚度可藉由電紡織處理時間來優化。為了實現在惡劣條件下（如高溫或高速率），我們將覆膜的LMO陰極與新型S-C（PAN)陽極結合，電池可具有良好的電容量保持能力、出色的速率能力。與普通的電極相比，塗有PVDF @ LGLZNO複合材料的電極（LMO-30min），在室溫（25°C）和高溫（55°C）下，都具有出色的循環穩定性、速率性能以及電容量保持能力。在XPS的輔助下，展示出在高C-rates和55°C時，PVDF @ LGLZNO纖維膜成功抑制了錳的溶解，而單只有PVDF塗層及普通的LMO陰極無法防止其自身劣化。纖維膜顯著抑制了陰極/電解質界面處的不良副反應，並降低了電荷轉移阻力。具有PVDF @ LGLZNO（LMO-30min）修飾陰極和S-C（PAN）陽極的電池在1 C下經過1000次循環後，仍有77％的電容量保持率，相當於每次循環僅有0.023％的容量衰減。
在本論文的最後部分，通過將（S-C（PAN））陽極與LiNi0.5Mn1.5O4（LNMO）陰極的結合，設計出了一種新型高壓鋰離子電池。然而，一般由1M之六氟磷酸鋰（LiPF6）溶於碳酸亞乙酯（ethylene carbonate）和碳酸二乙酯（diethyl carbonate）（1：1）做為電池之電解液時，會因電解液的氧化分解而引起高容量衰退。為了減緩這種容量衰減，開發出1,1,2,2-四氟乙基-2,2,3,3-四氟丙基醚（1, 1, 2, 2-Tetrafluoroethyl-2, 2, 3, 3-tetrafluoropropyl ether），碳酸氟亞乙酯（fluoroethylene carbonate）和碳酸甲乙酯(ethyl methyl carbonate)（體積比例3：2：5)，作為新型高電壓鋰離子電池的最佳電解質。所開發出的電解質相對於對照的電解質，提升了半電池（Li || S-C（PAN）和 Li || LiNi0.5Mn1.5O4）和全電池（S-C（PAN）|| LiNi0.5Mn1.5O4）的循環穩定性和速率性能。用1 M LiPF6於FEC / EMC / TTE（3：2：5）電解質所製備的全電池，在速率為2C下，放電電容量為688 mAh g-1 s，相較於對照電解液僅有 19 mAh g-1 s 的放電電容量。XPS結果證實，所採用的電解質有效地穩定了全電池中（S-C（PAN））陽極和LiNi0.5Mn1.5O4陰極的表面。

Developing a new battery design to enable rechargeable lithium batteries with higher capacity, energy density as well as cost efficiency, environmental friendliness, and safety is quite urgent. Designed a cell that overcomes the safety problems associated with lithium metal anode and the low theoretical capacity of graphite anode. The new battery system designed by using sulfur composite as anode and spinel-type as cathode provides high energy density, low cost, and no safety concern.

In the first part of this study, we designed a new cell by coupling S-C(PAN) as anode and paired with lithium manganese oxide ( LiMn2O4, LMO) cathode for the first time. The full cell delivers an energy density of 185 Wh kg-1(S-C(PAN)+LMO) at 1 C within the voltage range from 1 to 3.2 V. The full cell (S-C(PAN)||LMO) is characterized by a reversible discharge capacity of 1378 mAh g-1S and 868 mAh g-1S at 0.1 C and 2 C, respectively. At 1 C, a retention capacity of 807 mAh g-1S is achieved at the 400th cycle with an average decay rate of 0.7 mAh g-1S*cycle-1 and an average Coulombic efficiency of 99.5%. Interfacial chemistry of S-C(PAN) anode is particularly investigated and S-C(PAN) is demonstrated as one interesting anode material, an alternative to lithium metal, due to its high theoretical capacity of sulfur (1675 mAh g-1), environmental friendliness, low cost, and high energy density.

Secondly, the dissolution of manganese and its deposition on the anode surface cause poor for the high capacity fading special at 55 oC and 1 C-rate. To alleviate these issues, a fibrous film composed of polyvinylidene difluoride (PVDF) and Li5.6Ga0.26La2.9Zr1.87Nb0.05O12 type garnet (PVDF@LGLZNO) is coated directly on the LiMn2O4 (LMO) electrode and it functions as a promising artificial cathode-electrolyte interphase (CEI). To realize a cell with good capacity retention, excellent rate capability and resilience under harsher conditions (e.g. elevated temperature or high rates), the coated LMO cathode is coupled with the new anode which consists of sulfurized carbon derived from polyacrylonitrile (S-C(PAN)). The electrode (LMO-30min) coated with PVDF@LGLZNO composite material shows outstanding cycling stability and rate capability, as well as capacity retention when compared to bare electrode both at room temperature (25 °C) and elevated temperature (55 °C). The PVDF@LGLZNO fibrous coating suppresses the dissolution of manganese both at high C-rates and 55 °C, as supported by XPS, whereas PVDF coated and bare LMO cathodes are not able to prevent themselves from further deterioration. The fibrous film significantly inhibits undesirable side reactions at the cathode-electrolyte interface and reduces charger transfer resistance. The cell with PVDF@LGLZNO (LMO-30min) modified cathode and S-C(PAN) anode delivers capacity retention of 77% after 1000 cycles at 1 C-rate, corresponding to the average capacity decay of 0.023% per cycle.

In the final part of this dissertation, a new high voltage lithium-ion battery is designed by coupling sulfurized carbon anode from polyacrylonitrile (S-C(PAN)) and LiNi0.5Mn1.5O4 (LNMO) cathode. However, a high capacity fading was originated when the cell made with 1M lithium hexafluorophosphate (LiPF6) in ethylene carbonate (EC) and diethyl carbonate (DEC) (1:1) due to oxidative decomposition of solvents. To mitigate this capacity fading, 1, 1, 2, 2-Tetrafluoroethyl-2, 2, 3, 3-tetrafluoropropyl ether (TTE), fluoroethylene carbonate (FEC), and ethyl methyl carbonate (EMC) (3:2:5) was introduced as the best electrolyte for new developed high voltage lithium-ion battery. The best electrolyte developed enhanced the cyclic stability and rate capability of both half-cells (Li||S-C(PAN and Li||LiNi0.5Mn1.5O4) and S-C(PAN)||LiNi0.5Mn1.5O4 full-cells relative to control electrolyte. The discharge capacity of full-cell made with 1M lithium hexafluorophosphate (LiPF6) in FEC/EMC/TTE (3:2:5) electrolyte reaches 688 mAh g-1 S a rate of 2 C, while 19 mAh g-1 S for the control electrolyte. The adopted electrolyte can effectively stabilize the surfaces of both sulfurized carbon anodes from polyacrylonitrile (S-C(PAN)) and LiNi0.5Mn1.5O4 cathode within the full cell as the X-ray photoelectron spectroscopy (XPS) results confirmed.

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