金屬有機骨架於藥物輸送與醋酸吸附之應用、非晶態向結晶態金屬有機骨架的轉變

Sustainable Synthesis of MOFs for Drug Delivery and Acetic Acid Capture and Insights on the Crystallization from Amorphous Nucleation Cluster to Crystalline MOF

蘇穎穎(Pamela Berilyn So)

指導教授 ： 陳欣聰

共同指導教授 ： 林嘉和(Chia-Her Lin)

中原大學/理學院/化學研究所/博士(2021年)

https://doi.org/10.6840/cycu202100342

摘要

本論文由三個部分組成，皆是探討金屬有機骨架(MOF)的各種合成方法和應用。第
一部分探討了生物相容 MOF(MIL-100(Fe))作為載體，用於有效遞送 diclofenac(DCF)。
MIL-100 (Fe)用作活性藥物的載體，可保護其免受惡劣的胃部環境和藥物過早代謝的弊病，
同時包含 MOF 合成和載藥量的直接合成方式證明可以成功將 DCF 付載進 MOF 的，同時，DCF
可以用作活性藥物，接頭和大小調節劑。
研究的第二部分著眼於以放大劑量的鋁金屬 MOF (MIL-68(Al))合成。其中，原始合成
配方內的 N，N-二甲基甲酰胺(DMF)由異丙醇(IPA)成功地替代，這是一種綠色環保且更具
成本效益的溶劑。此外還探索了溶劑的重複使用，IPA 經回收後，能用於三個連續的合成
過程，從而產生質量更穩定的產品。隨後證明了合成的 MIL-68(Al)對乙酸(AA)的吸附，即
使在 100 ppm 的低起始濃度下也顯示出對 AA 的良好移除效率(100％去除率)，表現出比市
售品(活性碳與 zeolite 13x)更好的性能。
第三部分探討了非晶態金屬有機向結晶態 MOF 的轉化的初步研究。由於材料中存在缺
陷，因此可以將 MOF 進行轉換和重新排列。與原始的 MOF 合成相比，無序的無定形狀態通
過適當的去溶劑化步驟，可以在更短的時間內獲得高度結晶的 MOF。這種通過加熱和真空
的去溶劑化合成方法實現了高速化的 MOF 結晶。

關鍵字

金屬有機骨架 ； 藥物輸送 ； 結構轉相 ； 吸附 ； 永續化學

並列摘要

This three-part study explores various synthesis methods and applications of metal-organic
frameworks (MOF). The first part explores the use of the biocompatible MOF MIL-100(Fe) for the
efficient delivery of diclofenac (DCF). MIL-100(Fe) served as the carrier of the active drug
enabling protection from harsh gastric environment and premature drug metabolism. De novo
synthesis combining MOF synthesis and drug loading proved successful with DCF serving as the
active drug, the linker, and size modulator at the same time.
The second part of this study focuses on the sustainable scale-up synthesis of an aluminum
MOF, MIL-68(Al). Successful replacement of N,N-dimethylformamide (DMF), the organic
solvent used for synthesis, by isopropyl alcohol (IPA), a greener and more cost efficient solvent
was achieved. In addition, solvent reusability was also explored where in IPA was used for three
consecutive synthesis yielding consistent quality products. This was followed by the demonstration
of the acetic acid (AA) adsorption of the synthesized MIL-68(Al) showing good removal for AA
(100% removal rate) even at low starting concentrations of 100 ppm, exhibiting better capability
than commercially available activated carbon and zeolite 13x.
Lastly, the third part comprises the preliminary study on the crystallization of amorphous
nucleation clusters to crystalline MOF. With the defect present in the material, transformation and
rearrangement to MOFs is possible. From a disordered amorphous state, with proper desolvation
procedure, highly crystalline MOFs may be achieved at a shorter time as compared with pristine
MOF synthesis. This synthesis approach by desolvation combined with heating and vacuum lays
out an expressway towards MOF crystallization.

並列關鍵字

metal-organic framework ； drug delivery ； transformation ； adsorption ； sustainable chemistry

參考文獻

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