合成具供體-受體架構的混合配體Zr(IV)-MOFs以提升光催化染料降解性能;Synthesis of Mixed-Ligand Zr(IV)-MOFs with Donor-Acceptor Architectures for Enhanced Photocatalytic Dye Degradation

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Title:	合成具供體-受體架構的混合配體Zr(IV)-MOFs以提升光催化染料降解性能;Synthesis of Mixed-Ligand Zr(IV)-MOFs with Donor-Acceptor Architectures for Enhanced Photocatalytic Dye Degradation
Authors:	黃修瑋;Huang, Hsiu-Wei
Contributors:	化學工程與材料工程學系
Keywords:	金屬有機框架;光催化;雅甲基藍;亞甲基藍;MOFs;Photocatalysis
Date:	2025-07-14
Issue Date:	2025-10-17 11:13:51 (UTC+8)
Publisher:	國立中央大學
Abstract:	本研究利用一鍋法（ One-pot synthesis）合成一系列具有供體-受體（ Donor-Acceptor, D-A）架構的混合配體鋯金屬有機框架（ Zr(IV)-MOFs），並探討其在染料吸附與光催化降解中的性能。 MOFs 的金屬中心選 Zr(IV)，並以四(4-羧基苯基)卟啉（ Tetra(4- carboxyphenyl)porphyrin, TCPP）作為供體配體， 4,4′-(1,3,6,8-四氧代苯並[M][3,8]菲咯啉 -2,7(1H,3H,6H,8H)- 二基 ) 二苯甲酸 (4,4′-(1,3,6,8- Tetraoxobenzo[Lmn][3,8]phenanthroline-2,7(1H,3H,6H,8H)-diyl)dibenzoic acid, NDIDB) 作為受體配體，藉此構建具有拓展電子傳遞通道的 MOFs 結構。為改善材料性能，本研究比較了不同金屬前驅物（ ZrCl4 與 ZrOCl2·8H2O）與調節劑（ Formic acid 與 Acetic acid）對 MOFs 形貌、孔結構及光催化活性的影響。材料表徵包含 FTIR、、 XRD、、 SEM、、 XPS 與 TGA 分析，以確認 MOFs 的結構與化學組成；吸附實驗方面，針對陽離子型染料亞甲基藍（ Methylene Blue, MB）與陰離子型染料甲基橙（ Methyl Orange, MO）進行有效性探討，其中僅進行 MO 的吸附試驗。結果顯示，所合成之混合配體 MOFs 在吸附 MB 時表現出明顯的表面電荷調控能力，純度較高的 TCPP 衍生物更能調控 MOF 表面電性，進而影響對帶電染料的選擇性吸附。在可見光與藍光光源下進行的亞甲基藍光催化降解實驗中，不同 MOFs 材料表現出不同的降解速率與動力學行為、，其中以 DA-OCl-ML-A-N 在可見光條件下展現最佳光催化性能。此外， pH 值亦顯著影響吸附行為，在酸性與鹼性條件下均觀察到吸附效率優於中性，推測與 Zr 中心表面位點的質子化/去質子化特性相關。綜上，本研究提出一種高效率的 D-A 結構混合配體 MOFs 合成策略，證明其在選擇性吸附與可見光光催化降解陽離子染料方面具高度應用潛力，為水污染處理材料設計提供新方向。;This study reports the one-pot synthesis of a series of donor–acceptor (D-A) structured mixed-ligand Zr(IV)-based metal–organic frameworks (MOFs) for dye adsorption and photocatalytic degradation. Tetra(4-carboxyphenyl)porphyrin (TCPP) and NDIDB were used as donor and acceptor ligands, respectively, to construct MOFs with enhanced electron transfer pathways. The influence of different metal precursors (ZrCl4, ZrOCl2·8H2O) and modulators (formic acid, acetic acid) on the morphology, porosity, and photocatalytic activity was investigated. Characterization by FTIR, XRD, SEM, XPS, and TGA confirmed the structure, morphology, and thermal stability of the materials. Adsorption tests using methylene blue (MB) and methyl orange (MO) revealed that MOFs synthesized with high-purity TCPP showed better surface charge control and selective adsorption toward charged dyes. Photocatalytic tests under visible and blue light showed that DA-OCl-ML-A-N exhibited the best performance. Additionally, pH had a notable impact, with higher degradation observed under basic conditions. Overall, this work demonstrates an effective D-A MOF synthesis strategy with strong potential for applications in dye removal and water treatment.
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