預測固體溶質於超臨界二氧化碳添加共溶劑系統之溶解度

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丁翊修(Yi-Hsiu Ting) 查詢紙本館藏

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化學工程與材料工程學系

論文名稱

預測固體溶質於超臨界二氧化碳添加共溶劑系統之溶解度
(Predict the solubility of solid compounds in SCCO2 with cosolvents)

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摘要(中)

本研究利用Peng-Robinson + COSMOSAC 狀態方程式 ( PR + COSMOSAC EOS) 預測藥物固體在超臨界二氧化碳添加共溶劑的系統之溶解度，收集近年相關文獻中23種藥物於雙成分超臨界二氧化碳溶液中的溶解度數據，利用此模型進行計算並探討其結果。同時也採用了Wang and Lin [1] 等人提出的環狀結構修正參數加入此模型進行優化並預測固體溶解度。本研究計算了23種固體溶質共60個系統，總共約1132個實驗數據點，計算的溫度範圍從298.15 K至353 K，壓力最高達40 MPa，整體的平均對數誤差從優化前的0.77降至優化後的0.64，此結果與Wang and Lin [1] 差異不大，這也代表PR+COSMOSAC EOS不僅能夠預測藥物固體在雙成份超臨界二氧化碳中的溶解度，也適用於三成分超臨界二氧化碳系統。
不僅如此，某些物質的熔點與熔化熱，來自各個文獻提供之數據頗有差異，經研究發現，改變物質熔點及熔化熱會影響其預測結果，且這些誤差不可忽視。所以，若取得適當的熔點及熔化熱，即能更進一步增加預測之精確度，故PR+COSMOSAC EOS 在超臨界流體技術工業上是一種方便且有用的計算工具，而相關的參數優化仍持續研究中。

摘要(英)

In the study, we use Peng-Robinson + COSMOSAC equation of state (EOS) to predict the solubility of solid solutes in supercritical carbon dioxide (SCCO2) with cosolvent. We collected solubility data including 23 solid solutes from literatures published in recent years and we used the model to calculate solubility and discussed results. We also added optimized parameter which was proposed by Wang and Lin [1] to improve prediction accuracy for solids with ring structure. In the study, 23 solid solutes including 60 systems were calculated. ( T = 298.15－353 K, P = 0.1－40 MPa, and about 1126 solubility data.) The ALD-x (average logarithmic deviation in solubility) is 0.77 and decreased to 0.64 when adding the optimized parameter in program. This result is similar to the Wang and Lin ‘s, that is, PR + COSMOSAC EOS can predict the solubility of solid solutes not only in SCCO2, but also in SCCO2 with cosolvents.
Moreover, melting temperature (Tm) and heat of fusion (Hm) of a solid compound are required in the method. It is found that experimental results of Tm and Hm from different research groups are different. These errors cannot be neglected. Therefore, choosing suitable Tm andHm of solid compounds can increase prediction accuracy. We think our prediction result is acceptable and we still devote to optimizing the parameter of the method. Furthermore, PR+COSMOSAC EOS is also a useful tool in the future, especially for solid compounds whose experimental data are difficult to obtain.

關鍵字(中)

★ 超臨界二氧化碳
★ 固體溶解度
★ 共溶劑
★ 純預測模型

關鍵字(英)

★ Supercritical carbon dioxide
★ solid solubility
★ cosolvent
★ PR+COSMOSAC EOS

論文目次

中文摘要 i
英文摘要 ii
誌謝 iii
目錄 iv
表目錄 v
圖目錄 vii
符號說明 ix
第一章緒論 1
1-1 超臨界流體性質及相關發展 1
1-2 添加共溶劑之影響 4
1-3 熱力學理論模型及文獻回顧 4
第二章預測固體溶質於超臨界二氧化碳添加共溶劑系統之溶解度 8
2-1 研究背景及動機 8
2-2 理論模式 8
2-2-1 Peng-Robinson + COSMOSAC 狀態方程式 9
2-2-2分子表面電荷密度 10
2-3 計算細節 15
第三章結果與討論 20
3-1 添加不同共溶劑對預測結果之影響 21
3-2 物質熔點(Tm)及熔化熱(∆Hm)選擇之重要性 22
3-3 多重根的影響 23
第四章結論 25
參考文獻 64

參考文獻

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指導教授

謝介銘(Chieh-Ming Hsieh)

審核日期

2016-7-27

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