在本實驗中我們採用化學氧化法使CuO自生長在泡沫銅(Cu-Foam)上。以苯-1,4-二羧酸(Benzene-1,4-dicarboxylic acid)作為有機配體，利用水熱法合成贋電容複合超級電容器之電極材料，成功使片狀的鎳金屬有機框架(Ni-MOF)生長在CuO/Cu-Foam上。形成分層結構的Cu-Foam/CuO/Ni-MOF三元複合電極。接下來以簡單的回流法來合成片狀的鎳金屬有機框架(Metal-Organic-framework)結構的(Ni-MOF、PANI/Ni-MOF、PANI/g-C3N4/Ni-MOF、PANI/g-C3N4/NiO/Ni-MOF)，藉由進一步添加導電聚合物聚苯胺(Polyaniline)、導電碳材石墨相氮化碳(g-C3N4)和金屬氧化物(NiO)，來強化純材料的各種電化學性質，像是比電容、電子擴散係數和循環穩定性等等。
通過X-ray粉末繞射、傅立葉變換紅外光譜、拉曼光譜和X射線光電子能譜儀等儀器進行材料的特徵分析。通過掃描和穿透式電子顯微鏡獲得顯微圖像來研究分析材料的形貌。最後開發的電極運用於超級電容器中。
其中PANI/g-C3N4/NiO/Ni-MOF四元複合材料電極在5 A/g的輸入電流密度下顯示出較高的比電容為2420 F/g，並且在20 A/g的高輸入電流密度下仍保有初始比電容數值的75.2%約為1820 F/g的比電容保持能力。最後將四元複合材料用於開發固態不對稱超級電容器，並通過Swagelok cell裝置進行製造分析。負極和正極分別為活性碳(AC)電極和四元複合電極的不對稱超級電容器表現出高功率和能量密度。所製造的超級電容器在長達3000次循環後表現出優異的穩定性，與初始5個循環相比仍保留99.5%的比電容值，表明它具有進一步的工作潛力。

In this experiment, we used the chemical oxidation method to make CuO self-grown on copper foam (Cu-Foam). Using benzene-1,4-dicarboxylic acid as an organic ligand, a pseudocapacitor electrode materials was synthesized by a hydrothermal method, and a sheet-like nickel metal organic framework (Ni-MOF) was successfully grown on CuO/Cu-Foam. Formation of a layered Cu-Foam/CuO/Ni-MOF ternary composite electrode. Next, we used a simple reflow method to synthesize sheet-like nickel metal-organic-framework structures (Ni-MOF, PANI/Ni-MOF, PANI/g-C3N4/Ni-MOF, PANI/g-C3N4/NiO/Ni-MOF), by further adding conductive polymer polyaniline, conductive carbon material graphitic carbon nitride (g-C3N4) and metal oxide (NiO), to enhance the electrochemical performance of pure materials properties, such as specific capacitance, electron diffusion coefficient, and cycling stability, among others.
The obtained materials were confirmed with characterization tools such as X-ray powder diffraction, Fourier transform infrared, Raman spectroscopy and X-ray photoelectron spectroscopy. The morphology was studied by obtaining microscopic images from scanning electron microscopy and transmission electron microscopy. Finally, developed electrodes were used in applications of supercapacitors.
The quaternary composite material of PANI/g-C3N4/NiO/Ni-MOF shows a higher specific capacitance of 2420 F/g at a current density output of 5 A/g, and at a current density of 20 A/g, the specific capacitance is 1820 F/g and still retains 75.2% of the initial specific capacitance. This result is higher than other electrodes. Finally, the quaternary composite material was used to develop solid state asymmetric supercapacitors and the fabrication analysis was done via Swagelok cell setup. The asymmetric supercapacitor with activated carbon (AC) electrode and quaternary composite electrode in negative and positive side respectively, showed high energy and power density. In addition, the fabricated supercapacitor showed excellent stability after up to 3000 cycles, and still retained 99.5% of the specific capacitance value compared with the initial 5 cycles and showed that it has further working potentials.

第一章　緒論　　 1
1.1　前言　　1
1.2　研究動機　　4
1.3　研究目的　　7
第二章　文獻回顧　　 13
2.1　超級電容器簡介　　13
2.2　超級電容器的種類　　17
2.3 電雙層超級電容器(EDLCs)　　20
2.3-1　活性碳(Acitvated Carbon)　　21
2.3-2　碳黑(Carbon Black, (CB))　　22
2.3-3　活化和改質碳基材料　　23
2.4　贋電容超級電容器(pseudocapacitor)　　24
2.4-1　金屬有機框架電極(MOF)　　25
2.4-2　MOF的結構　　25
2.4-3　MOF結構相對於構建的多樣性　　27
2.4-4　MOF結構在尺寸的多樣性　　27
2.4-5　如何強化MOF的性質　　29
第三章　實驗流程與分析　　 31
3.1　實驗儀器　　31
3.2　實驗藥品　　33
3.3　實驗流程　　35
3.3-1　合成g-C3N4材料　　35
3.3-2　合成氧化物NiO材料　　35
3.3-3　合成PANI, PANI/g-C3N4和PANI/g-C3N4/NiO複合材料　　37
3.3-4　複合電極材料PANI/g-C3N4/NiO/Ni-MOF合成和製作　　39
3.3-5　複合電極材料Ni-MOF/CuO/Cu foam合成和製作　　41
3.3-6　固液態電解質製作流程　　43
3.3-7　超級電容器製作組裝流程　　44
3.4　材料特性分析　　46
3.4-1　X-光繞射分析(X-ray diffraction, XRD)　　46
3.4-2　拉曼光譜分析(Raman spectra)　　47
3.4-3　傅立葉轉變紅外光譜分析(FT-IR spectra)　　48
3.4-4　N2吸附/脫附等溫曲線　　50
3.4-5　X-ray光電子能譜分析(XPS)　　52
3.4-6　表面微觀分析(SEM、EDS、FE-SEM、TEM)　　52
第四章　實驗結果與討論　　 54
4.1　PANI/g-C3N4/NiO/Ni-MOF四元複合材料之結果與討論　　54
4.1-1　X-ray繞射分析　　54
4.1-2　拉曼光譜Raman spectra分析　　56
4.1-3　傅立葉變換紅外光譜FT-IR分析　　58
4.1-4　熱重熱差TGA分析　　60
4.1-5　比表面積與孔隙度分析儀BET分析　　61
4.1-6　X-ray 光電子能譜XPS分析　　63
4.1-7　形貌和顯微結構研究　　65
4.1-8　合成材料的電化學性質　　69
4.1-9　不對稱超級電容器組件(Swagelok cell)的性能　　88
4.1-10　超級電容器的實際應用　　93
4.2　Ni-MOF/CuO/Cu foam三元複合材料之結果與討論　　95
4.2-1　X-ray 繞射分析　　95
4.2-2　拉曼光譜Raman spectra分析　　97
4.2-3　傅立葉變換紅外光譜FT-IR分析　　99
4.2-4　氫氣程序升溫還原(H2-TPR)分析　　100
4.2-5　X-ray 光電子能譜XPS分析　　101
4.2-6　形貌和顯微結構研究　　103
4.2-7　合成材料的電化學性質　　106
4.2-8　不對稱超級電容器組件(Swagelok cell)的性能　　122
4.2-9　超級電容器的實際應用　　125
第五章　結論　　 127
參考文獻　　129

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