探討Donor-Acceptor聚醯乙胺共價有機框架之有機染劑光降解性質;Investigation of Photocatalytic Properties of Donor-Acceptor PI-COFs through the Degradation of Organic Dye

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題名:	探討Donor-Acceptor聚醯乙胺共價有機框架之有機染劑光降解性質;Investigation of Photocatalytic Properties of Donor-Acceptor PI-COFs through the Degradation of Organic Dye
作者:	陳彥昶;Chen, Yen-Chang
貢獻者:	化學工程與材料工程學系
關鍵詞:	共價有機框架;光觸媒;covalent organic framework;photocatalyst
日期:	2025-07-14
上傳時間:	2025-10-17 11:14:08 (UTC+8)
出版者:	國立中央大學
摘要:	在工業快速發展下，伴隨而來的工業汙染也正危害著環境，紡織、皮革、印刷業中則使用了大量的有機染劑，這些含有染劑的工業廢水也是全球水汙染來源之一，其中有部分染劑具有毒性、致突變性或難以被生物降解，並且會阻擋陽光及降低水中的溶氧，因此當汙水排放將會嚴重影響人體健康與自然環境，也會阻礙水資源處理。本研究使用共價有機框架（Covalent Organic Frameworks, COFs）作為有機光觸媒，以含氨基之三聚氰胺作為單體並與對苯二甲醛或二酸酐合成出SNW-1與具有D-A系統的醯乙胺結構之PI-COF201與PI-COF202，其中PI-COFs所使用的直接加熱合成法與常見的溶劑熱合成法相比，可以合成出結晶度更高的產物以及擁有更高的產率，而且合成過程不需加入有機溶劑，因此是更簡單也更符合綠色化學的合成法。而本實驗使用亞甲基藍（Methylene Blue, MB）作為染劑，並在MB水溶液中加入COFs搖晃吸附24小時後取出做吸光度測試，探討COF材料對染劑的吸附效果，之後再將溶液以450 nm之藍光照射以探討材料對於染劑的光降解能力，其中SNW-1擁有高達323.342 m²/g的比表面積，並且對MB有85.36 %的吸附，因此是適合作為染劑吸附的材料，而PI-COF201、PI-COF202則分別對於MB有39.44及20.86 %的光降解效果，因此可作為染劑的光降解觸媒，而PI-COFs則透過在光催化實驗中加入自由基清除劑，探討光降解MB可能降解機制，實驗結果顯示兩種PI-COF因其能隙大小差異以及HOMO（Highest Occupied Molecular Orbital）、LUMO（Lowest Unoccupied Molecular Orbital）位置不同，分別以⸱HO2與⸱O2-做為主要降解途徑。研究結果顯示了這些新興的COF材料對於水中的染劑確實能達到移除效果，並且可依其不同的材料性質做為染劑吸附劑或光降解觸媒，雖然目前COF材料的研究及應用不及傳統觸媒廣泛，但其獨特的材料性質仍充滿發展性及研究價值。 ;The rapid development of industry has led to significant industrial pollution, posing substantial threats to the environment. Industries such as textile, leather, and printing which extensively utilize organic dyes and dispose of industrial waste water containing these dyes are major sources of global water pollution. Some of the dyes exhibit toxicity, mutagenicity, or resistance to biodegradation. Furthermore, their presence obstructs sunlight penetration and reducing dissolved oxygen levels in water bodies. Consequently, the disposal of such waste water severely jeopardizes human health and the natural environment, impeding water resource treatment as well. This study investigates covalent organic frameworks (COFs) as organic photocatalysts. Using amine-containing melamine as a monomer, SNW-1 was synthesized by combining it with terephthalaldehyde. Additionally, PI-COF201 and PI-COF202, featuring imide structures with a D-A (donor-acceptor) system, were synthesized from melamine and dianhydrides. The synthesized PI-COFs using direct heating method offers several advantages compared to traditional solvothermal method, including higher crystallinity and improved yields of the products. Furthermore, this method requires no organic solvents, which makes it simpler and more environmentally friendly. Methylene blue (MB) was used as the model organic dye in this study. To investigate the adsorption capabilities of the materials, the COFs were added into MB aqueous solution and agitated on an orbital shaker for 24 hours, subsequently, the samples were analyzed via absorbance tests. For photocatalytic studies, the samples underwent blue light irradiation with the wavelength of 450 nm. Results showed that SNW-1 ,with a high surface area of 323.342 m²/g , demonstrated 85.36% adsorption of MB, making it a suitable dye adsorbent. In contrast, PI-COF201 and PI-COF202 exhibited photodegradation efficiencies of 39.4 and 20.86 % for MB, respectively, thus indicating their potential as photocatalysts. To elucidate the possible mechanisms of MB photodegradation, radical scavenger were introduced to the photocatalytic reaction experiment involving PI-COFs. Experimental results revealed that, due to the variations in their bandgap energies as well as the positions of HOMO (Highest Occupied Molecular Orbital) and LUMO (Lowest Unoccupied Molecular Orbital) of the PI-COFs, the dominant degradation pathways were identified as ⸱HO2 and ⸱O2- for PI-COF201 and PI-COF202, respectively. Research findings indicate that these emerging COF materials are indeed effective in removing dyes from water. Depending on their distinct material properties, they can function either as dye adsorbents or as photocatalytic degradation catalysts. While research and application of COF materials are currently less widespread than traditional catalysts, their unique material properties still present significant developmental and research value.
顯示於類別:	[化學工程與材料工程研究所] 博碩士論文

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