本研究旨在利用常壓電漿產生裝置對鋰離子電池負極ZnCo2O4材料進行改質，藉由氮摻雜及碳沉積的方式以期提升其電性表現。通過水熱法對合成的ZnCo2O4粉末進行氮摻雜，並利用常壓電漿束對極片進行表面改質。為探討氮摻雜對負極材料的影響，由表面特征分析發現，氮摻雜部分填補材料中的氧空缺，並與材料表面的懸空半鍵結結合形成新的含氮鍵結，促使負極材料電化學性能提升，循環穩定性得到改善。經過水熱法和電漿處理後，該負極材料具有均勻的氮摻雜，且表現出最佳的電化學性能。
另外，通過對原有常壓電漿束的裝置進行改造，使之可以在室溫、常壓的狀況下沉積碳在電池極片表面。藉由電漿診斷技術對產生的電漿中被激發或被游離的粒子。通過激發光譜分析發現，在電漿中明顯出現碳簇粒子，且在加入氮氣後，氮化碳粒子也出現在電漿中。經由掃描電子顯微鏡分析，發現經過常壓電漿表面處理，碳保護層可沉積在負極材料表面，有效改變表面化學鍵結。由於保護碳層的沉積和氮摻雜， ZnCo2O4負極材料的循環穩定性獲得有效提升。根據此研究成果，常壓電漿束具有在室溫、常壓條件下，同時進行快速碳沉積和表面氮摻雜的應用價值，並可具次世代高效率鋰電池開發之潛力。

The main objective of this dissertation is to improve the electrochemical performances of ZnCo2O4 (ZCO) Li-ion anode material by nitrogen-doping and carbon deposition. As for nitrogen doping, two rapid methods, including hydrothermal to treat powder and atmospheric pressure plasma jet (APPJ) to modify the electrode, were used to dope nitrogen in the ZCO anode material. Via hydrothermal method, nitrogen was doped in the ZCO spinel lattice, while APPJ mainly activated and modified the electrode surface binding with the dangling bond. N-doped compounds were formed on the electrodes by hydrothermal and APP methods. The uniformity, chemical composition, and diffraction patterns were examined by electron probe microanalyzer (EPMA), X-ray photoelectron spectroscopy (XPS) and X-ray diffractometer (XRD). Nitrogen doping effectively improved electrochemical performance in cycling retention and the capacity at a current density of 1C. This study provides a rapid and inexpensive nitrogen doping processes to efficiently promote the electrochemical performance in ZCO anode.
In addition, a special set-up of atmospheric pressure plasma jet generator was applied to deposit carbon on the electrode. Significant amounts of C(I) and C2 clusters were discovered using optical emission spectroscopy. After adding N2, the CN species appeared in the plasma, owing to C and N2 reaction during the plasma generation. The results from the field emission scanning electron microscope (FESEM) and X-ray photoelectron microscopy (XPS) reveal the change in surface morphology and chemical bonding by plasma treatment. After 20 times of Ar+N2 plasma treatment, a significant increment in cycling stability under 1000 mA/g was evident.

List of Table III
Figure Caption IV
Abstract VIII
Chapter 1. Introduction 1
1.1 Background 1
1.2 Motivation and Objectives 3
1.3 Thesis Overview 4
Chapter 2. Literature Review 6
2.1 Development of LIB Anodes 6
2.2 Development of ZnCo2O4 Anode 9
2.3 Overview of Nitrogen Doped Methods in LIB Anodes 11
2.4 Overview of Carbon Deposition Methods in LIB Anodes 15
2.5 Overview of Atmospheric Pressure Plasma Jet 19
Chapter 3. Experiment Procedure 31
3.1 Sample Preparation 31
3.2 Electrochemical Analysis Preparation 32
3.3 Nitrogen Doping Processes 32
3.3.1 Hydrothermal Process 32
3.3.2 Plasma Treatment 33
3.4 Carbon Deposition Process 33
3.5 Plasma Diagnosis 34
3.6 Surface Characterization 34
3.6.1 Scanning Electron Microscope (SEM) 34
3.6.2 X-ray Photoelectron Spectroscopy (XPS) 34
3.6.3 X-ray Diffractometer (XRD) 35
3.6.4 Electron Probe Microanalyzer (EPMA) 35
3.6.5 Brunauer-Emmett-Teller (BET) 35
3.6.6 Electrochemical Analysis 35
Chapter 4. Results and Discussions 38
4.1 Nitrogen Doping of ZnCo2O4 38
4.1.1 Nitrogen Doping of ZnCo2O4 Electrode via Atmospheric Pressure Plasma Jet (APPJ) 41
4.1.2 Nitrogen Doping of ZnCo2O4 Electrode by Hydrothermal Process for Enhanced Electrochemical Performances 51
4.1.3 Nitrogen Doping of ZnCo2O4 Electrode by Hydrothermal Process and Atmospheric Pressure Plasma Jet (APPJ) 61
4.2 Carbon Deposition and Nitrogen Doping of ZnCo2O4 via Atmospheric Pressure Plasma Jet (APPJ) 70
Chapter 5. Conclusions 90
References: 92

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