Please use this identifier to cite or link to this item: http://hdl.handle.net/11455/3339
標題: Supercritical Fluid Extraction of 3,5-Diprenyl-4-Hydroxycinnamic Acid (DHCA) from Brazilian Propolis and Purification of DHCA
超臨界流體萃取巴西蜂膠中的3,5-雙異戊烯基-4-羥基肉桂酸與其純化製程
作者: 李蔭濃
Lee, Ying-Nong
關鍵字: DHCA
DHCA
propolis
hot pressurized
ultra-sonic
supercritical fluid
RSM
column purification
anti-oxidative
DPPH
LDL
蜂膠
熱壓萃取
超音波萃取
超臨界
RSM
管柱純化
抗氧化
DPPH
低密度脂蛋白
出版社: 化學工程學系
摘要: 本研究分別以熱壓攪拌、超音波震盪與添加乙酸乙酯的超臨界二氧化碳三種方法,萃取蜂膠原塊中的3,5-Diprenyl-4-Hydroxycinnamic Acid(DHCA),並利用應答曲面法(RSM),探討各萃取製程,獲得DHCA最大回收率與純度值的預測條件。120毫升乙酸乙酯索式萃取1克蜂膠16小時,可得到91.9(mg/g)DHCA,即DHCA占蜂膠原塊中的9.19wt%。 在熱壓攪拌與超音波震盪兩種乙酸乙酯的萃取製程方面,吾人分別以95℃與2.5小時以及55℃與2.5小時為RSM之設計中心點。實驗結果顯示,熱壓攪拌的設計中心點與RSM模擬最大值之條件相近,DHCA回收率與純度分別為88.79wt%和16.26wt%。而超音波震盪RSM的設計條件內,回收率隨著萃取溫度仍持續上升。75.03wt%的最大回收率出現在75℃、2.5小時。16.26wt%的純度最大值則在中心點(55℃、2.5小時)上。經由萃取條件的敏感度測試後,顯示超臨界流體溫度與添加共溶劑比例為主要影響回收率與純度之變因,因此選定50℃與4wt%的添加比例為RSM之設計中心點。實驗結果顯示,當添加6wt%乙酸乙酯時,DHCA回收率由3.68%,大幅提昇至13.88wt%。且回收率呈現持續上升的趨勢。而對於純度而言,在50℃與添加2wt%乙酸乙酯條件下,純度預測值達43.38wt%,但隨著乙酸乙酯添加比例的上升而緩慢下降。然而在RSM設計範圍內,純度皆保持在40wt%以上。 接著,三種溶劑萃出液,分別經正相樹脂silica gel-60的管柱分離程序。上管柱前,如經正己烷與甲醇的異液萃取的預處理程序,DHCA純度皆可達95wt%以上,熱壓攪拌萃出液的上柱純化物DHCA的總回收率4.05wt%是最高值。如不經溶劑預處理,僅超臨界萃出純化物之DHCA的純度達95wt%,且總回收率為最高,可達9.41wt%。最後,經本研究純化的95%DHCA甲醇溶液與三種製程萃出液的DPPH自由基清除與抑制低密度脂蛋白(LDL)氧化的數據,均顯示萃出液中DHCA的含量與二種抗氧化指標能力有一定的相關連性。
This study investigated hot pressurized ethyl acetate (EA), ultra-sonic EA, and supercritical carbon dioxide (SC-CO2) added with EA extractions to recover 3,5-Diprenyl-4-Hydroxycinnamic Acid (DHCA) from Brazilian propolis. Response Surface Methodology (RSM) was applied to find operation conditions in obtaining the highest recovery and purity of DHCA for these extractions. The maximum content of DHCA in propolis is 91.9 (mg/g), obtained by 16-hour Soxhlet extraction of one gram solid with 120mL EA. Center composite RSM schemes designed at 95 ◦C, 2.5-hour and 55 ◦C, 2.5-hour were individually employed for hot pressurized and ultra-sonic extractions. For hot pressurized extraction, predicted maximum recovery and purity of DHCA are 88.79 wt% and 16.26 wt%, which is corresponding to experimental data at the design point. However, for ultra-sonic extraction, the DHCA recovery is only up to 75.03 wt% and is still increasing with temperature in the range investigated, but the DHCA purity also attains 16.26 wt% close to that of the design point. Our experimental results further indicated that temperature and addition ratio of EA are two major factors to influence the recovery and purity of DHCA for SC-CO2 extraction. The 50 ◦C and 4 wt% EA addition was selected as the RSM design point. Then, the DHCA recovery substantially increased from 3.68% (no adding) to 13.88wt% (6 wt% EA adding) and was still increasing, while the maximum DHCA purity reached 43.38 wt% at 50 ◦C and 2 wt% EA addition, slowly decreased in the ranges investigated. Nevertheless, the DHCA purities in the SC-CO2 extracts are all over 40wt%. Normal phase Sil-60 resin column purification coupled with liquid-liquid n-hexane and methanol extractions of these three extracts produced 95 wt% purity of DHCA. The largest total DHCA recovery in this column purification was 4.05 wt% only for the purified extract of hot pressurized EA treated with L-L extractions. Without pre-treated L-L extractions, only the purified SC-CO2 extract attained the 95 wt% purity and obtained 9.41wt% of the largest total DHCA recovery. Finally, anti-oxidative abilities of scavenging DPPH free radical and the inhibition of low density lipid (LDL), treated by the 95wt% purity DHCA and those extracts, revealed a positive correlation between the quantity of DHCA and anti-oxidative ability.
URI: http://hdl.handle.net/11455/3339
Appears in Collections:化學工程學系所

文件中的檔案:

取得全文請前往華藝線上圖書館



Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.