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1、河北工業(yè)大學(xué)碩士學(xué)位論文膠束催化丙烯環(huán)氧化摘要在實(shí)驗(yàn)室內(nèi)利用管式固定床對(duì)丙烷脫氫催化反應(yīng)進(jìn)行了研究。分別以丙烷脫氫生成的C3H8-C3H6-H2混合氣體和純丙烯為原料，采用300mL不銹鋼氣液攪拌釜式反應(yīng)器對(duì)丙烯環(huán)氧化反應(yīng)在卟啉錳膠束催化體系中進(jìn)行了研究，通過紫外-可見分光光度計(jì)對(duì)膠束催化劑結(jié)構(gòu)進(jìn)行了表征。用氣相色譜儀對(duì)反應(yīng)產(chǎn)物進(jìn)行了分析。丙烷脫氫制丙烯過程的研究結(jié)果表明，在Pt/γ-Al2O3,Pt-Na/γ-Al2O3和Pt-Sn-Na/γ-Al2O3三種催化劑中，Pt-Sn-Na/γ-Al2O3催化效果最佳。還原條
2、件為450℃H2中還原2h。實(shí)驗(yàn)優(yōu)化了Pt-Sn-Na/γ-Al2O3催化丙烷脫氫工藝條件，當(dāng)溫度為580℃，丙烷流量40mL/min和催化劑2g時(shí)，丙烷轉(zhuǎn)化率為33.2%，丙烯選擇性可達(dá)84.6%，丙烯收率28.1%。卟啉錳在表面活性劑水溶液中的增溶實(shí)驗(yàn)結(jié)果表明，TX-100對(duì)卟啉錳的增溶效果較好。紫外-可見光譜對(duì)卟啉錳在膠束中的增溶位置研究結(jié)果表明，卟啉錳增溶于膠束的柵欄層。丙烯為原料的膠束催化丙烯環(huán)氧化結(jié)果表明，反應(yīng)體系中H2O2濃度過高反而不利于PO的生成，原因是H2O2與丙烯在卟啉錳催化劑表面競爭吸附。篩選出丙
3、烯環(huán)氧化比較好的膠束催化工藝條件為卟啉錳濃度1mmol/L，H2O2濃度20mmol/L，咪唑與卟啉錳摩爾比12:1，TX-100濃度60mmol/L。在丙烯流量50mmol/L和溫度30℃的條件下，H2O2利用率可達(dá)11.8%，PO收率4.9%。在C3H8-C3H6-H2混合氣體為原料的條件下，膠束催化丙烯環(huán)氧化實(shí)驗(yàn)，未檢測到PO。關(guān)鍵詞：環(huán)氧丙烷，膠束催化，丙烯，丙烷脫氫iMICELLARCATALYSISFORPROPENEEPoXIDATIoNABSTRACTThepropanedehydrogenationwa
4、sstudiedintubularfixedreactorsystemThemicellarcatalysisforpropeneepoxidationwasstudiedin300mLstainlesssteelgas—liquildstirredreactor,bothC3H8一C3H6一H2andpropenebeingusedasfeedstocks．ThemicellarcatalysisstructurewascharacterizedbyUV-visspectrophotometer．Theproducts
5、wereanalyzedbygaschromatographyExperimentalresultsofpropanedehydrogenationindicatedthatamongPt／7一A1203，Pt—Na一一A1203andPt—Sn—NaJ7一A1203exhibitedtheoptimumcatalysisperformanceunderthereductiontemperature450。Candreductiontime2hours．Thereactionconditionsinpropanedehy
6、drogenationbyPt—Sn—Na／7一A1203catalysiswereoptimizedWhentemperaturewas580。C，theflowofpropanewas40mL／min，theamountofcatalystwas29andtheconversionofpropanewas33．25％，theselectivityofpropenereached84．62％andtheyieldofpropenewas28．14％．Thesolubilizationexperimentofmangan
7、eneporphyrininsurfactantssolutionindicatedthatTX—．100exhibitedbettersolubilitytomanganeneporphyrin．Thelocationexperimentofmicelle—incorporatedmanganeseporphyrinbyUV-vismethodindicatedthatmanganeseporphyrinwassolubilizedinthepalisadelayerofmicelle．Experimentalresu
8、ltsofmicellarcatalysissystemindicatedthattoohighH202concentrationwasunfavorabletoformationofPOresultingfromcompetiveadsorptionofH202andC3H6onthemanganeneporphy
