本實驗合成兩種新型多孔性碳材，第一類是藉由含有羥基官能基的分子(雙酚A，1,1'-聯-2-萘酚和酚醛樹脂)與溴化氰反應合成新的氰酸酯化合物，藉由其氰酸酯熱固化作用形成具由三嗪環的聚氰酯網狀結構，第二類是通過傅-克烷基化反應成功合成了一種以雙酚A為基本結構單元的超交聯多孔聚合物，再將兩者與KOH進行化學活化反應製備出多孔性碳材料，用作固體吸附劑，有效地除去二氧化碳、溶劑中污染物和柔性超級電容器的電極材料。
在高溫下，氰酸酯化合物的氰酸酯官能基進行熱固化作用得到聚氰酯網狀結構，其具有良好的熱穩定性，而雙酚A則透過傅-克烷基化反應形成高度的交聯結構使其熱穩定性得到提升，使兩者都可以在高溫下接受氫氧化鉀活化以提升孔洞性質。
進一步利用比表面積分析儀 (BET) 探討多孔性碳材，a-BPAC，a-BNC和a-PFC，分別顯示比表面積為1136,1080和1645 m2 g-1，HBPA-700則具有最高的比表面積為2340.7 m2g-1，因為其經過700℃的高溫鍛燒提升其孔洞含量。得到的多孔碳材皆可以有效捕捉二氧化碳以及吸附溶液中的污染物。我們還使用HBPA-700作為電極材料來製造柔性電容器。電容器可以在沒有外部刺激的作用下進行10次斷開和癒合並快速恢復其電容性能。有趣的是，電容器可以承受各種物理變形仍保持其電容性能。

In this experiment, two types of porous carbon materials were synthesized. The first type was to synthesize new cyanate ester compounds (bisphenol A, 1,1-bi-2-naphthol and phenolic novolac resin) by reacting a hydroxyl group with cyanogen bromide, and then via thermal cyclotrimerization form polycyanurate networks, the second type is the synthesis of a hypercrosslinked porous polymer with bisphenol A as the basic structural unit through the Friedel-Crafts alkylation reaction, and then the samples with the KOH chemical activation reaction was performed to prepare a porous carbon material. The porous carbon materials are used as a solid adsorbent to effectively remove carbon dioxide, solvent contaminants and as electrode materials of flexible supercapacitors.
At high temperature, the thermal cyclotrimerization of the cyanate esters functional group form polycyanurate with good thermal stability. Bisphenol A through the Friedel-Crafts alkylation reaction form hypercrosslinked porous polymer, the crosslinked structure enhances its thermal stability. Both can be activated by potassium hydroxide at high temperatures to enhance pore properties.
Further investigation of porous carbon materials using a specific surface area analyzer (BET). a-BPAC, a-BNC and a-PFC showed specific surface areas 1136, 1080 and 1645 m2 g-1, respectively. The HBPA-700 had the highest specific surface areas is 2340.7 m2g-1 because its high-temperature calcination at 700°C to increase its pore content. The obtained porous carbon materials can effectively capture carbon dioxide and adsorb pollutants in the solution. We also use HBPA-700 as an electrode material to manufacture flexible capacitors. Capacitors can be cut and healed 10 times without external stimuli and quickly restore their capacitive performance. Interestingly, capacitors can withstand various physical deformations while still maintaining their capacitive performance.

論文審定書 i
致謝 ii
摘要 iii
Abstract iv
Outline of contents vi
List of Figure ix
List of Scheme ix
List of Table xiv
1.1. Introduction xvi
1.1.1.Nitrogen-doped porous carbon material (NPCs) xvi
1.1.2.Polycyanurate 2
1.1.3. Hydrothermal carbonization (HTC) 6
1.2. Experimental Section 8
1.2.1. Materials 8
1.2.2. Synthesis 8
1.2.3 Instrumentations 12
1.3. Result and discussion 14
1.3.1 Synthesis and characterization of cyanate monomers 14
1.3.2. Cyclotrimerization of cyanate monomers 15
1.3.3. TGA thermograms of polycyanurate porous carbon material 18
1.3.4. The Powder X-ray diffraction and Raman spectra of polycyanurate porous carbon material 20
1.3.5. The X-ray photoelectron spectroscopy of polycyanurate porous carbon material 21
1.3.6. Porous structures of polycyanurate porous carbon material 24
1.3.7. CO2 capture of polycyanurate porous carbon material 27
1.3.8. Contaminants Sorption of polycyanurate porous carbon material 29
1.4. Conclusion 34
1.5. References 36
2.1. Introduction 52
2.1.1.Hypercrosslinked porous polymers (HCPs) 52
2.1.2.KOH-activated carbons for supercapacitor electrodes 57
2.1.3.Flexible Supercapacitors 59
2.2. Experimental Section 63
2.2.1. Materials 63
2.2.2. Synthesis 63
2.2.3. Instrumentations 66
2.3. Results and discussion 68
2.3.1.Synthesis and characterization of hypercrosslinked porous carbon material 68
2.3.2.TGA thermograms of hypercrosslinked porous carbon material 70
2.3.3.The Powder X-ray diffraction and Raman spectra of hypercrosslinked porous carbon material 72
2.3.4.The X-ray photoelectron spectroscopy of hypercrosslinked porous carbon material 73
2.3.5.Porous structures of hypercrosslinked porous carbon material 76
2.3.6.CO2 capture of hypercrosslinked porous carbon material 78
2.3.7.Contaminants Sorption of hypercrosslinked porous carbon material 79
2.3.8.Hypercrosslinked porous carbon material for supercapacitor 84
2.4. Conclusion 90
2.5. References 92
Supporting information 103

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