Please use this identifier to cite or link to this item: http://hdl.handle.net/11455/59103
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dc.contributor.author楊鴻銘zh_TW
dc.contributor.other行政院國家科學委員會zh_TW
dc.contributor.other國立中興大學化學工程學系(所)zh_TW
dc.date2010zh_TW
dc.date.accessioned2014-06-06T13:19:54Z-
dc.date.available2014-06-06T13:19:54Z-
dc.identifierNSC98-2221-E005-055zh_TW
dc.identifier.urihttp://hdl.handle.net/11455/59103-
dc.description.abstract醚酯類化學品是重要醫藥品,可應用於抗膽固醇、抗血脂等醫藥用途。以往合成醚酯類的主要方法須應用醇鈉來進行反應,有反應時間長與產率低的缺點,利用相間轉移觸媒則可改進上述缺點。合成醚酯化合物可經由多種路徑,例如由鹵酯類進行醚化反應、由醚酸類進行酯化反應、由醇酸之醚化與酯化同時進行等。一般相間轉移觸媒僅具有單一活性基位,一次僅能攜帶一分子的水相反應物進行反應,若使相間轉移觸媒具有多個活性基位,則可大幅促進催化反應速率。第三液相是相間轉移觸媒在特定條件下,高濃度的活性觸媒中間體析出自成一相介於水油兩相間,其性質介於親水疏水之間,水相和有機相反應物均可進入此液相內進行反應,因此可在溫和條件下大幅提高反應速率。第三液相相間轉移催化反應不需使用昂貴的無水或非質子溶劑及危害環境的含鹵素溶劑,是對環境親和的綠色化學技術。超音波化學為合成化學品極有效的技術,當高頻超音波在液體溶液中傳送時,造成溶液中漸歇式的壓縮與釋壓而形成局部空穴,空穴中之氣體溫度及壓力瞬間可達5000K 與數百大氣壓,有利於反應進行。因此若將多活性基相間轉移觸媒技術與超音波結合則有利於在環境親和條件下來合成高價值化學品。本計畫之研究目的即在發展以超音波輔助多活性基相間轉移觸媒在液-液相及三液相由醚酸經酯化反應來合成醚酯類特用化學品。本計畫分兩年完成,第一年:合成各式多活性基相間轉移觸媒,探討不同官能基之催化特性,在液-液相由超音波輔助進行相間轉移觸媒催化醚酸酯化反應,第二年則以第一年結果為基礎,將多活性基相間轉移觸媒形成第三液相,並以超音波來促進多活性基第三液相觸媒來催化醚酸之酯化反應。本計畫預定之工作項目:第一年,探討中心分子結構對多活性基觸媒之合成條件、多活性基觸媒中間體之合成與純化,觸媒中間體在兩液相之分佈,取代反應之多活性基觸媒中間體之動態變化,有機相本質反應及超音波與攪拌之聯合效應,分散系統之質量傳送與界面反應現象,並建立反應動力學模式等;第二年,以超音波輔助多活性基觸媒形成第三液相,水相反應物、鹽類、多活性基觸媒官能基對第三液相形成之影響,第三液相中多活性基觸媒中間體之動態變化,超音波促進之第三液相本質反應速率,三液相界面特性及反應機構,及超音波操作變數對總體反應速率之影響等,探討第三液相觸媒之回收再利用程序及其催化效率,並建立液-液-液相催化反應系統模式。本計畫研究結果可提供以多活性基相間轉移觸媒進行製程設計以合成醚酯類特用化學品。zh_TW
dc.description.abstractEther-esters are important pharmaceuticals used as anticholesteremics and antilipemics.In the past, ether-esters were synthesized from sodium metal and alcohols, but having thedrawbacks of longer reaction time and low yield. Such disadvantages can be overcome byphase transfer catalysis (PTC) technique. Ether-esters can be synthesized from several routes,such as etherification of halo-esters, esterification of ether-acids, or sequential etherificationand esterification of alcoholic acids.In general, PT catalyst offers only one active site to transfer one molecule of reactantonce. If one molecule of PTC provides more than one site at a time, the reaction rate can begreatly enhanced. The third-liquid phase is formed from the phase-transfer catalyst underspecific conditions at which the catalytic intermediate is highly concentrated in a thin layerbetween the aqueous and organic phases. This thin layer is called the third-liquid phase withintervenient property of hydrophilic and hydrophobic types. Both the aqueous and organicreactants can transfer into this phase to react with each other, thus resulting in a faster reactionrate. Third-liquid phase-transfer catalysis (TLPTC) is an environmentally benign technologyin organic synthesis due to non-usage of aprotic or halide-containing solvents. Sonochemistryis also effective in synthesizing chemicals. When the ultrasound propagates in a liquidsolution, the alternate compression and depression are produced to form cavities within whichtemperature and pressure can reach 5000 K and several hundred bars. The reaction rate is thusenhanced. The combination of multi-site PTC technique and ultrasound shows a benefit forsynthesizing high-value chemicals under environmentally friendly conditions.The purpose of this project is to develop the technique of ultrasound assisted multi-sitephase-transfer catalysis in liquid-liquid and tri-liquid phases for the esterification ofether-acids to synthesize ether-esters specialty chemicals. This project would be completedwithin two years. For the first year, different kinds of multi-site phase-transfer catalysts(abbreviated as MSPTCs) are synthesized, and the characteristics of functional groups inMSPTCs for catalyzing esterification of ether-acids in liquid-liquid phases under ultrasoundirradiation will be explored. For the second year, based on the results in the first year, theformation of third-liquid phase for MSPTCs, and the esterification of ether-acids overthird-liquid MSPTCs under ultrasound irradiation will be investigated.The research items are (1) for the first year, exploring the effect of central molecularstructure on preparing MSPTCs, synthesis and purification of catalytic intermediate ofMSPTCs, distribution of catalytic intermediate between two-liquid phases, dynamic variationof catalytic intermediate of MSPTCs under substitution reaction, intrinsic reaction, effect ofcombination of ultrasound and stirring, mass-transfer and interfacial phenomena in dispersedsystem, setting up the kinetic model, and (2) for the second year, ultrasound irradiation onforming the third-liquid phase of MSPTCs, effects of aqueous reactant, functional groups ofMSPTCs, and salts on the formation of third-liquid phase, dynamic variation of catalyticintermediate of MSPTCs in the third-liquid phase, ultrasound assisted intrinsic reaction,interfacial characteristics of third-liquid phase, reaction mechanism, effects of operatingparameters and ultrasound on the overall reaction, recovery process and activity of reusedMSPTCs, and setting up the liquid-liquid-liquid kinetic model. The research results can beused to design the TLPTC process with MSPTCs for synthesizing ether-esters specialtychemicals in the future.en_US
dc.language.isozh_TWzh_TW
dc.relation.urihttp://grbsearch.stpi.narl.org.tw/GRB/result.jsp?id=1906431&plan_no=NSC98-2221-E005-055&plan_year=98&projkey=PB9808-0436&target=plan&highStr=*&check=0&pnchDesc=%E8%B6%85%E9%9F%B3%E6%B3%A2%E8%BC%94%E5%8A%A9%E5%A4%9A%E6%B4%BB%E6%80%A7%E5%9F%BA%E7%9B%B8%E9%96%93%E8%BD%89%E7%A7%BB%E8%A7%B8%E5%AA%92%E5%9C%A8%E5%A4%9A%E6%B6%B2%E7%9B%B8%E5%82%AC%E5%8C%96%E9%85%AF%E5%8C%96%E5%90%88%E6%88%90%E9%86%9A%E9%85%AF%E5%8C%96%E5%AD%B8%E5%93%81%E4%B9%8B%E7%A0%94%E7%A9%B6en_US
dc.subject基礎研究zh_TW
dc.subjectMulti-site Phase-Transfer Catalysten_US
dc.subject化學工程類zh_TW
dc.subject多活性基相間轉移觸媒zh_TW
dc.subject第三液相zh_TW
dc.subject超音波zh_TW
dc.subject醚酯化學品zh_TW
dc.subject綠色化學技術zh_TW
dc.subjectThird-Liquid Phaseen_US
dc.subjectUltrasounden_US
dc.subjectEther-Estersen_US
dc.subjectGreen Chemistry Technologyen_US
dc.title超音波輔助多活性基相間轉移觸媒在多液相催化酯化合成醚酯化學品之研究zh_TW
dc.titleUltrasound Assisted Multi-Sites Phase-Transfer Catalyzed Esterification in Multi-Liquid Phases for Synthesizing Ether-Ester Chemicalsen_US
dc.typeResearch Reportszh_TW
item.openairecristypehttp://purl.org/coar/resource_type/c_18cf-
item.cerifentitytypePublications-
item.languageiso639-1zh_TW-
item.openairetypeResearch Reports-
item.fulltextno fulltext-
item.grantfulltextnone-
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