臺灣博碩士論文加值系統

在本論文中，我們報導了第一個共價苯並惡嗪骨架（CBF-1）製成新的雙孔和單孔共價有機骨架應用於CO2吸收和超級電容器中。首先，三官能氨基苯基三嗪（TAPT）、三官能羥基苯基三嗪（THPT）和多聚甲醛產生曼尼希反應，再藉由溶劑熱法製成共價苯並惡嗪骨架（CBF-1）。新的CBF-1經歷熱交聯固化後產生高度交聯的CBF（CCBF-1），碳化後進行KOH活化，使其轉化為氮摻雜的微孔碳（N-DMC）。經熱固化、碳化和活化後的CBF-1明顯的提高了熱性質和BET表面積。有趣的是，N-DMC表現出球形形態，具有優異的熱穩定性（高達Td5為663ºC，焦炭產率為85％），高BET表面積（高達1469 m2 g-1），孔徑為2.07 nm 。從CBF-1到CCBF-1再到N-DMC的熱轉化直接增強了CO2捕獲和電化學電容。 N-DMC分別在298和273 K時顯示出優異的CO2捕獲能力，分別為3.85和7.46 mmol / g。此外，N-DMC在電流密度為1.0 Ag-1時顯示出185 Fg-1的高電化學電容，並且在4000次循環後在20 Ag-1下具有優異的86％平均保留穩定性能。
此外，我們報告了一種方法，來研究超分子相互作用對2D COF拓撲調節的影響，作為管理其性質的新技術。我們是通過引入原始和取代的二胺單體來實現:聯苯胺（BD）和1,4-二羥基聯苯胺（DHBD）進入雙咔唑單體的骨架中。使用[C2 + C2]拓撲圖設計新的具有1D開放微孔的微孔二咔唑COF（Cz-BD和Cz-DHBD），藉由希夫鹼縮合反應成功合成四甲酰基-二咔唑作為C2節和C2鏈接基的二胺芳香族， 得到的COF具有兩種不同的拓撲結構，Cz-BD具有四孔結構的單孔，而Cz-DHBD具有帶有兩種不同孔的kagome結構;一個是六邊形，另一個是三角形。這些COF具有高結晶度，水溶性和有機溶劑穩定性，大表面積和高孔隙率，具有開放的一維（1D）微孔通道和密集排列的π-陣列結晶層。這些COF表現出協同的結構效應並實現了超高性能的CO2吸收。

In this thesis, we report the first covalent benzoxazine framework (CBF-1) in addition to new dual-pore and single-pore Covalent organic frameworks and their application for CO2 uptake and supercapacitor. First, Covalent benzoxazine framework (CBF-1) was synthesized via a solvothermal method using trifunctional aminophenyl triazine (TAPT), and trifunctional hydroxyphenyl triazine (THPT) paraformaldehyde through Mannich condensation reaction. This new CBF-1 underwent thermal cross-linked curing to generate a highly cross-linked CBF (CCBF-1), which, with carbonization followed by KOH activation, was converted into nitrogen-doped microporous carbon (N-DMC). The thermal curing, carbonization, and activation for CBF-1 have dramatically enhanced the thermal properties and BET surface area. Interestingly, the formed N-DMC exhibited a spherical morphology with excellent thermal stability (up to Td5 of 663 ºC and char yield of 85%), high BET surface areas (up to 1469 m2 g-1), and pore size of 2.07 nm. The thermal transformation from CBF-1 to CCBF-1, then to N-DMC directly enhanced the CO2 capture and electrochemical capacitance. N-DMC showed excellent CO2 capture capacities of 3.85 and 7.46 mmol/g at 298 and 273 K, respectively. Moreover, N-DMC showed high electrochemical capacitance of 185 Fg-1 at current density 1.0 Ag-1, and excellent stability performance of 86% average retention at 20 Ag-1 after 4000 cycles.
In addition, we report a conceptual strategy to study the effect of supramolecular interactions on the topological regulating of 2D COFs as a new technique to manage their properties. Our strategy was achieved by introducing pristine and substituted diamines monomers; Benzidine (BD) and 1,4-dihydroxybenzidine (DHBD) into the skeleton of bicarbazole monomer. The newly designed microporous bicarbazole COFs (Cz-BD and Cz-DHBD) with 1D open micropores were designed using a [C2 + C2] topology diagram and successfully synthesized via a Schiff-base condensation reaction of tetraformyl-bicarbazole as C2 knot and aromatic diamines as C2 linker. The resulting COFs have two different topologies, Cz-BD bears a single-pore with tetragonal structure, while Cz-DHBD has a kagome structure bearing two different kinds of pores; one is hexagonal and the other is triangular. These COFs feature high crystallinity, aqueous and organic and solvents stability, large surface area and high porosity with open one-dimensional (1D) microporous channels and densely aligned π-arrays of crystalline sheets. These COFs exhibited synergistic structural effects and achieved ultrahigh-performance of CO2 uptake.

Chapter I
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Chapter II

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Chapter III

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