臺灣博碩士論文加值系統

過量的二氧化碳排放是當今全球暖化主要原因，因此發展再生能源是近年來最受矚目的研究領域。二氧化碳的光催化還原反應不僅可減少二氧化碳的排放量、妥善將太陽能以化學鍵方式貯存，還可將二氧化碳轉化為加值化產物，促進人類經濟活動的豐富度。其中有機高分子材料的組成元素在地球含量相對其他貴金屬觸媒更豐沛，因此用於光催化二氧化碳還原的研究近幾年開始受到重視。我們使用萘雙亞醯胺與芴兩類型的單體合成聚合物與小分子，討論高分子上不同官能基結構、予體受體交互作用、以及分子共軛長度對於光催化二氧化碳還原反應的影響。在不添加犧牲試劑與金屬元素的條件下，將各項材料進行光催化二氧化碳還原的異相催化。其中PF-Br展現最佳的一氧化碳產率8.422 μmol g-1 h-1，且擁有接近100%對氫氣與甲烷的選擇性。本研究亦透過理論計算，探討光催化二氧化碳還原可能的反應機制，期望能找出影響光催化效率的關鍵因素。

Excess emission of CO2 is considered the main reason for global warming; As a result, renewable energy has attracted much research attention in recent years. Photocatalytic CO2 reduction could potentially decrease CO2 concentration on earth. Moreover, the solar energy might be stored through transforming CO2 into other energy sources. Among all the photocatalysts used in CO2 reduction, organic polymers, which are mostly composed of abundant light elements, emerge as a highly promising material in recent years. In this study, we use naphthalene diimide and fluorene units to synthesize a variety of compounds, and discuss the relation among the photocatalytic efficiency, the physical properties, and chemical structures. Experiments of heterogeneous photocatalytic CO2 reduction with water were carried out, in the absent of sacrificial agents and metal cocatalysts. The results reveal that PF-Br showed the highest CO production rate of 8.422 μmol g-1 h-1 and the selectivity was close to 100%. Last but not least, the mechanisms with regard to the photocatalytic reduction of CO2 to CO are investigated by with DFT calculation, providing rationale for the experimental observation.

摘要 i
Abstract ii
目錄 iii
圖目錄 v
圖表目錄 x
表目錄 xi
第一章 緒論 1
1-1 光催化二氧化碳還原 1
1-1-1 光催化二氧化碳還原之背景 1
1-1-2 光催化二氧化碳還原之條件 3
1-2 有機高分子於光催化二氧化碳還原 7
1-2-1 多孔有機聚合物(Porous organic polymers, POPs) 7
1-3 研究動機 22
第二章 結果與討論 24
2-1 材料合成與結構鑑定 24
2-1-1 線性高分子 24
2-1-2 COFs材料 28
2-2 材料的光物理性質和電化學性質 32
2-2-1紫外光–可見光光譜 32
2-2-2循環伏安法 34
2-2-3螢光光譜與時間解析螢光光譜 36
2-3 材料的表面性質分析 39
2-3-1 掠角入射廣角X光散射分析 39
2-3-2 接觸角量測 45
2-3-3 比表面積量測與粗糙度量測 46
2-4 材料的光催化效率比較 48
2-5 光催化二氧化碳還原之機制探討 53
第三章 結論 57
第四章 實驗方法 58
4-1試藥 58
4-2 實驗儀器 58
4-3 光催化實驗方法 60
4-3-1 樣品製備 60
4-3-2 實驗架設 61
4-3-3 氣體定量 61
4-4 DFT理論計算 62
4-5合成步驟 62
第五章 文獻 74
第六章 附錄 80

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