高效環境友善製程回收鋰離子電池正極材料製備 析氧反應之催化劑

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蔡武雄(WU-XIONG CAI) 查詢紙本館藏

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化學工程與材料工程學系

論文名稱

高效環境友善製程回收鋰離子電池正極材料製備析氧反應之催化劑
(Efficient and environmentally friendly process for recycling lithium-ion battery cathode materials into Oxygen Evolution Reaction catalysts)

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至系統瀏覽論文 (2027-9-1以後開放)

摘要(中)

鋰離子電池(Lithium Ion Battery, LIB)作為一種新興的二次能源系統，因其高能量密度、長循環壽命和優異的安全性能而被廣泛應用。這些電池在電子產品如智能手機、筆記本電腦和其他便攜設備中占有重要地位。此外，隨著電動車市場的快速增長，鋰離子電池已成為電動車的主要動力來源。隨著時間的推移，老舊的鋰離子電池逐漸達到其循環壽命的終點，隨之而來的是大量的鋰離子電池廢棄物產生，隨著電子產品和電動車的不斷普及，鋰離子電池的需求只會持續增長，這也導致了報廢電池數量的增加。這些廢棄電池含有大量有價值的金屬，如鋰、鈷、鎳等，如果不加以回收再利用，不僅會造成資源浪費，還會對環境造成潛在危害，因此鋰離子電池廢棄物的處理和回收，成為一個迫切解決的重要環保問題。
本研究致力於開發同時具有高效率及環保性的濕式冶金方法來進行鋰離子電池正極材料之回收，以亞臨界醋酸浸出對鋰鎳鈷鋁氧化物(NCA)進行回收，透過實驗確定了最佳反應條件為溫度180℃、6M醋酸、固液比30g/L、反應時間4小時，可得到96%以上的Al、Co、Li、Ni浸出效率，後續將回收後所得到之金屬分別以水熱法及真空雷射鹽類還原法兩種方法，再利用於合成水電解產氫製程中所使用之三元鐵鎳鈷催化劑泡沫鎳電極，在循環伏安法測定中獲得最佳起始電位1.359V，且在固定電流密度100mA/cm2的計時電位法測定500小時後電壓只上升了0.07V，顯示了優異的電化學性能及穩定性，也顯示了回收的廢棄鋰離子電池正極材料金屬在循環利用上有非常高的未來發展性與應用潛力。

摘要(英)

Lithium-ion batteries (LIBs) are an emerging secondary energy system widely used due to their high energy density, long cycle life, and excellent safety performance. These batteries play a crucial role in electronic products such as smartphones, laptops, and other portable devices. Furthermore, with the rapid growth of the electric vehicle (EV) market, LIBs have become the primary power source for EVs. Over time, as old lithium-ion batteries reach the end of their cycle life, a significant amount of LIB waste is generated. With the continued proliferation of electronic products and EVs, the demand for lithium-ion batteries will only increase, leading to a corresponding rise in the number of discarded batteries. These waste batteries contain valuable metals such as lithium, cobalt, and nickel. If not properly recycled, it will result in resource wastage and pose potential environmental hazards. Therefore, the treatment and recycling of lithium-ion battery waste have become urgent and critical environmental issues.
This study aims to develop an efficient and environmentally friendly hydrometallurgical method for the recovery of cathode materials from LIBs. Subcritical acetic acid leaching was used to recover lithium nickel cobalt aluminum oxide (NCA). Through experiments, the optimal reaction conditions were determined to be a temperature of 180°C, 6M acetic acid, a solid-liquid ratio of 30g/L, and a reaction time of 4 hours, achieving leaching efficiencies of over 96% for Al, Co, Li, and Ni. The recovered metals were then used to synthesize ternary iron-nickel-cobalt catalysts on nickel foam electrodes for hydrogen production via water electrolysis, using hydrothermal and vacuum laser salt reduction methods. Cyclic voltammetry measurements showed an optimal onset potential of 1.359V, and chronoamperometry at a fixed current density of 100mA/cm² demonstrated that the voltage increased by only 0.07V after 500 hours, indicating excellent electrochemical performance and stability. This also highlights the significant future development potential and application prospects for recycled metals from spent lithium-ion battery cathode materials.

關鍵字(中)

★ 鋰離子電池回收
★ 濕式冶金
★ 亞臨界流
★ 循環經濟
★ 析氧反應

關鍵字(英)

論文目次

摘要 i
Abstract ii
誌謝 iv
目錄 v
圖目錄 viii
表目錄 x
一、前言與ESG指標 1
二、文獻回顧 3
2.1鋰離子電池介紹 3
2.2.1鋰離子電池正極活性材料介紹 4
2.2鋰離子電池正極材料之回收 4
2.2.1火法冶金 5
2.2.2濕式冶金 5
2.2.3直接回收法 7
2.2.4機械化學法 8
2.2.5電化學法 8
2.3水電解 9
2.3.1再生能源之發展 9
2.3.2析氧反應與電催化劑發展 10
2.3.3電催化劑之合成方法 11
2.3.4鎳、鈷和鐵基電催化劑 13
2.4回收材料循環利用於製備析氧反應催化劑 14
三、實驗步驟 15
3.1實驗藥品 15
3.2實驗材料 16
3.3亞臨界流醋酸回收NCA活性材料 16
3.3 NCA回收液於三元金屬催化劑之合成應用 16
3.3.1水熱法進行三元金屬催化劑合成 16
3.3.2真空雷射鹽類製程(PLMS)進行三元金屬催化劑合成 17
3.4分析儀器 19
3.4.1場發射掃描式電子顯微鏡(Field Emission-Scanning Electron Microscopy, FE-SEM) 19
3.4.2感應耦合電漿光學發射光譜儀(Inductively coupled plasma optical emission spectrometry, ICP-OES) 19
3.4.3 X射線繞射儀(X-ray diffractometer, XRD) 20
3.4.4 X射線光電子能譜儀(X-ray photoelectron spectroscopy, XPS) 21
3.4.5電化學量測系統(CH Instruments electrochemical analyzer, CHI) 22
四、結果與討論 23
4.1亞臨界流醋酸對NCA活性材料浸出程序 23
4.1.1 NCA活性材料 23
4.1.2酸浸出程序 24
4.1.3不同實驗參數下之浸出效率 28
4.2 NCA浸出溶液前驅物合成三元金屬催化劑 32
4.2.1 FeNiCo催化劑 32
4.2.2 電化學特性分析 37
4.3循環回收程序之成本 39
五、結論 42
六、參考文獻 43

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指導教授

洪緯璿

審核日期

2024-7-29

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