鋁離子電池具有成本低、鋁元素豐度高、無毒、安全（金屬鋁負極反應過程中不會產生支狀晶）等優勢，已成為替代鋰離子電池的下一代可充電電池的有希望的候選者。目前眾多研究者主要以石墨體系陰極為研究對象，石墨優點為價格便宜且倍率性能。但石墨電極的電容量和能量密度不足。另一種體系為使用轉化型材料作為陰極，轉化型材料具有高理論容量和能量密度，但其容量衰減快、循環性能差等問題。因此，轉化型電池正極材料需要近一步研究探索與改善。
在本論文中，透過三種策略來改善轉化型電極材料問題，包含: (1)結構設計: 利用傾斜角沉積技術和低溫等離子體輔助硒化工藝開發三維螺旋棒陣列結構的二硒化鉬正極，該製程避免使用粘結劑可有效避免電池中的副反應對整體性能影響，此外該電池優異性能表現可歸因於螺旋棒陣列結構，有利於增加電化學活性位點並加快電子傳輸；(2) 電解液設計: 鋁硒電池中硒正極與離子液體搭配使用會引發容量快速衰減，循環性能差問題，透過引入新型的深共晶溶劑作為電解液，該電解液不會產生副反應，可有效穩定電池反應進而提升循環性能；(3) 電極設計: 在有機鹵素鈣鈦礦-鋁電池體系中，正極材料中的碘在電池充放電過程中會產生大量多碘化物，引發嚴重的穿梭效應造成電池容量急速衰退，透過在有機鹵素鈣鈦礦正極中引入長鏈烷基胺，可有效錨定多碘化物抑制穿梭效應，進而提升電池壽命。總之，本論文從三個方向來改善轉化型材料缺點包含結構設計、電解液設計與電極設計，提高電池正極電化學反應效率，有效利用活性物質，減少副反應與穩定反應過程，進而提升電池性能，為新型儲能電池的下一步發展提供重要參考。

Rechargeable aluminum-ion batteries (AIBs) have developed rapidly as a promising candidate for next-generation rechargeable batteries to replace Li-ion batteries (LIBs) due to the very low cost and high abundance of aluminum (1.5 wt % in the Earth’s crust), nontoxic, a high specific capacity (Al 2980 mAh g–1, 8063 mAh cm–3), and safety (reversible dendrite-free deposition). Until now, researchers have focused on graphite-based cathode materials with the advantage of low cost and high-rate ability. However, the specific capacity and energy density of graphite-based cathode is insufficient. On the other hand, the conversion-type cathode materials have been reported in AIBs, which be expected to achieve high theoretical capacity and energy density. Nevertheless, the conversion-type materials have some critical issues still need to be resolve, including fast cycle fading and unstable long term cycling ability. Therefore, it is necessary to explore new strategies to overcome cycle fading and enhance long-term stability for conversion-type cathode materials.
In this thesis, three kinds of strategies are used to overcome the critical issue of conversion- type materials, including: (1) Structure design: A three-dimensional helical rod array structure of molybdenum diselenide was developed by using glancing angle deposition technology and low-temperature plasma-assisted selenization process. The process avoids the side reaction owing to binders-free, and helical nanorod arrays can increase the specific surface area and shorten the diffusion channel of the electric charges; (2) Electrolyte design: the rechargeable aluminum selenium battery with the ionic liquid demonstrates rapid capacity fading and poor cycle performance. Through introducing a new type of deep eutectic solvent as the electrolyte, which can effectively stabilize the battery reaction and improve the cycle performance; (3) Electrode design: the rechargeable aluminum-organic-inorganic halide perovskite battery with the ionic liquid exhibit serve capacity fading, owing to shuttle effect of polyiodides. The introduction of long-chain alkylamines in cathode can anchor polyiodides, leading to enhance battery cycling life. We propose these three strategies to improve the shortcomings of conversion materials, improve the electrochemical reaction efficiency of battery cathodes, effectively utilize active materials, and improve battery performance, providing important references for the next development of new energy storage batteries.

Abstract in Chinese i
Abstract ii
Acknowledgements iv
Chapter 1 Introduction 1
1.1 Introduction to aluminum ion batteries 1
1.2 Energy Storage Mechanism 3
1.2.1 Intercalation of AlCl4- Anions Mechanism 3
1.2.2 Intercalation of Al3+ Cations Mechanism 6
1.2.3 Conversion Mechanism 9
1.3 Novel Conversion-Type Electrode 11
1.3.1 Chalcogen Materials 11
1.3.2 Halogen Materials 17
1.3.3 Halide Perovskite Materials 21
1.4 Nonaqueous Electrolyte 25
1.4.1 Ionic liquid 25
1.4.2 Deep Eutectic Solvents 27
1.5 Material analysis method and technology 32
1.5.1 Raman Spectroscopy 32
1.5.2 X-ray Photoelectron Spectroscopy (XPS) 33
1.5.3 X-ray Diffraction (XRD) 34
1.5.4 Scanning Electron Spectroscopy (SEM) 35
1.5.5 Transmission Electron Microscopy (HR-TEM) 36
1.5.6 Coin cell testing system (LANHE CT2001A) 37
1.5.7 Potentiostat and Electrochemical Impedance Spectroscopy 38
1.6 Motivation 39
1.6 Overview of the Dissertation 40
Chapter 2 Three-Dimensional Molybdenum Diselenide Helical Nanorod Arrays for High-Performance Aluminum-Ion Batteries 43
2.1 Methods 43
2.1.1 Glancing Angle Deposition 43
2.1.2 Low-Temperature Plasma-Assisted Selenization 43
2.1.3 Material Characterization 44
2.1.4 Cell Fabrication and Electrochemical Tests 44
2.1.5 Ex Situ Characterization 45
2.2 Results and Discussion 46
2.2.1 Schematic illustration of the MoSe2 HNRAs toward AIBs. 46
2.2.2 Characterizations of the as-grown MoSe2 HNRAs 49
2.2.3 Electrochemical performance of MoSe2 HNRA-based AIBs 54
2.2.4 Ex situ characterization of MoSe2 HNRAs in AIBs at different discharge and charge status. 61
2.3 Summary 69
Chapter 3 High-Performance Rechargeable Aluminum–Selenium Battery with a New Deep Eutectic Solvent Electrolyte: Thiourea-AlCl3 70
3.1 Methods 70
3.1.1 Materials 70
3.1.2 Growth of Se Nanowires by Selenization 70
3.1.3 Preparation of Thiourea-AlCl3 Electrolyte 71
3.1.4 Preparation of EMIC-AlCl3 Electrolyte 71
3.1.5 Electrolyte Characterization 71
3.1.6 Electrochemical Measurements 71
3.1.7 Ex Situ Battery Measurements 72
3.2 Results and Discussion 73
3.2.1 Characterizations of Se NWs@CC 73
3.2.2 Electrolyte speciation studies of Thiourea-AlCl3 Electrolyte 78
3.2.3 Electrochemical performance of Al-Se batteries 80
3.2.4 Al–Se batteries using the EMIC- and thiourea-based electrolyte. 87
3.2.5 Ex situ measurements of Al–Se batteries 91
3.3 Summary 98
Chapter 4 Long-Chain Alkylammonium Organic–Inorganic Hybrid Perovskite for High Performance Rechargeable Aluminon-ion Battery 99
4.1 Methods 99
4.1.1 Materials 99
4.1.2 Synthesis of perovskites 99
4.1.3 Preparation of EMIC(1-ethyl-3-methylimidazolium chloride)-AlCl3 electrolyte 100
4.1.4 Material characterization 100
4.1.5 Electrochemical measurements 101
4.1.6 Ex-situ battery measurements 101
4.1.7 Computational details 101
4.2 Results and Discussion 103
4.2.1 Characterization of LCA perovskite/Al battery 103
4.2.2 Electrochemical performance of LCA perovskite/Al battery 109
4.2.3 Kinetic studies of the LCA perovskite/Al battery. 122
4.2.4 Ex-situ measurements of the LCA perovskite/Al battery. 125
4.2.5 DFT calculation I3- absorption energy 138
4.3 Summary 143
Chapter 5 Conclusion 144
Chapter 6 Future Prospective 145
Chapter 7 Reference 147

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