開發簡化合成步驟的四醯胺基大環配體含鐵催化劑及其對廢水中染料的分解效率

Development of the FeIII-TAML (tetra-amido macrocyclic ligand) catalysts with simplified synthetic procedures and their activity for dye degradation in wastewater.

許志弘(Zhi-Hong Xu)

指導教授 ： 陳志欣

淡江大學/理學院/化學學系碩士班/碩士(2022年)

https://doi.org/10.6846/TKU.2022.00617

摘要

在此研究中我們設計並合成了三種不同的新型FeIII-TAML催化劑，這三個分子的代號分別為Zhc、Zhd、Zhe。我們將這三個分子設計成只需要一個步驟就可以合成出該FeIII-TAML催化劑的配體分子，並使用兩種不同的步驟合成Zhe的配體分子Zhe-1，兩方法的總產率分別為15%和13%，證明一步合成法可行。將Zhc、Zhd、Zhe和第一代原型FeIII-TAML催化雙氧水降解甲基橙，以紫外-可見吸收光譜觀察甲基橙最大吸收波長463 nm的吸收度變化來比較四種不同FeIII-TAML催化劑的催化效率，最後在特定條件下，原型FeIII-TAML、Zhc、Zhd和Zhe四種FeIII-TAML催化劑在30分鐘內分別降解了66%、4%、78%、100%的甲基橙。

關鍵字

高階氧化工藝 ； 芬頓試劑 ； 鐵-四醯胺基大環配體催化劑

並列摘要

In this study, we designed and synthesized three different FeIII-TAML catalysts, i.e., Zhc, Zhd, and Zhe, respectively. We designed these three molecules to synthesize the ligand of the FeIII-TAML catalyst in only one step, and used two different steps to synthesize the ligand molecule Zhe-1 of Zhe. The total yields of these two methods were 15% and 13%, proving that the one-step synthesis method is acceptable. Zhc, Zhd, Zhe and the first-generation prototype FeIII-TAML were used to catalyze the hydrogen peroxide to degrade the methyl orange, and the absorbance change of methyl orange at the maximum absorption wavelength of 463 nm was observed by UV-Vis spectroscopy to compare the catalytic efficiency of four different FeIII-TAML catalysts, finally, under specific conditions, the prototype FeIII-TAML, Zhc, Zhd and Zhe four FeIII-TAML catalysts degraded 66%, 4%, 78%, 100% methyl orange.

並列關鍵字

Advanced oxidation process ； Feton reagent ； FeIII-TAML

參考文獻

1. Regan H. Asian rivers are turning black. And our colorful closets are to blame. CNN, 2020, https://edition.cnn.com/style/article/dyeing-pollution-fashion-intl-hnk-dst-sept/index.html

2. Andreozzi, R.; Caprio, V.; Insola, A.; Marotta, R. Advanced oxidation processes (AOP) for water purification and recovery. Catal. Today 1999, 53, 51-59.

3. Yang, Z.; Shan, C.; Pan, B.; Pignatello, J. J. The Fenton Reaction in Water Assisted by Picolinic Acid: Accelerated Iron Cycling and Co-generation of a Selective Fe-Based Oxidant. Environ. Sci. Technol. 2021, 55, 8299-8308.

4. Choi, J.; Park, H.; Hoffmann, M. R. Effects of Single Metal-Ion Doping on the Visible-Light Photoreactivity of TiO2. J. Phys. Chem. C 2010, 114, 783-792.

5. Collins, T. J.; Ryabov, A. D. Targeting of High-Valent Iron-TAML Activators at Hydrocarbons and Beyond. Chem. Rev. 2017, 117, 9140-9162.