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1、湖南大學(xué)碩士學(xué)位論文氯丙烯環(huán)氧化法制環(huán)氧氯丙烷催化劑性能研究姓名:陳康莊申請(qǐng)學(xué)位級(jí)別:碩士專(zhuān)業(yè):化學(xué)工程指導(dǎo)教師:徐偉箭;王槐玉20060524碩士學(xué)位論文摘要目前,世界上環(huán)氧氯丙烷的生產(chǎn)方法有兩種:氧丙烯高溫氯化法和烯丙醇法。但這兩種方法都存在副產(chǎn)大量廢水和廢渣的環(huán)保問(wèn)題。利用Ts.1催化氯丙烯和雙氧水的環(huán)氧化反應(yīng),具有反應(yīng)條件溫和,反應(yīng)速度快,過(guò)程無(wú)污染等優(yōu)點(diǎn),開(kāi)發(fā)高效、清潔的新:[藝具有重要意義。本文設(shè)計(jì)了一種“蒸餾一失活”的方法,考察了氯丙烯、雙氧水中雜質(zhì),反應(yīng)助劑等因素對(duì)TS.1穩(wěn)定性的影響。采用N2物理吸附、熱失重(TGA)、X射線(xiàn)
2、衍射(XRD)、紅外光譜(IR)、元素分析(ICP)、熒光分析法(CRP)等方法,對(duì)新鮮、失活和再生催化劑進(jìn)行了表征和分析,并采用酸處理、烘干和高溫焙燒等方法,對(duì)失活的催化劑進(jìn)行了再生研究。結(jié)果表明:l、過(guò)多的溶劑可促進(jìn)副反應(yīng)的發(fā)生,副反應(yīng)生成的大分子影響催化劑的穩(wěn)定性:2、鐵離子沉積到‘rS—l上,影響TS一1的穩(wěn)定性;3、在氯丙烯直接環(huán)氧化體系,大分子吸附于催化劑上,是造成催化劑失活的原岡:4、采用酸處理、烘干和高溫焙燒的方法,可使經(jīng)蒸發(fā)法失活的催化劑活性恢復(fù)到新鮮催化劑的水平。5、氯丙烯環(huán)氧化法膜分離實(shí)驗(yàn)表明催化劑的ECH廣:能較為理想,
3、且能滿(mǎn)足過(guò)氧化氫的轉(zhuǎn)化率、ECH的收率和選擇性。關(guān)鍵詞:鈦硅分子篩:失活;再生:表征:環(huán)氧化法里璺絲至塞些童皇!竺圣墨里堡竺些型篁璧竺壘AbstractTherearetWOwaysfortheproductionofepoxychloropropane:hightemperaturechlorinationofchloropropeneandallylalcoholmethod.Butallthesetwomethodshaveenvironmentalharassmentthatlargenumbersofwastewaterandwast
4、eresidueareproduced.Theexploitationofnewcleanlytechnicswithhighefficiencyismuchimportant.However’theepoxidationofchloropropenewithhydrogenperoxidecatalyzedbyTS.1possessthemeritsasmildreactionconditions,rapidreactionrateandnopollution.Inthispaper,adistillation—deactivationmet
5、hodwasused.Theeffectsofchloropropene,impuritiesinhydrogenperoxide,andreactionpromoterontheTS一1stabilitywerealsostudied.Thenewly,deactivedandreactivatedcatalystswerecharacterizedandanalyzedbymethodsofphysicaladsorptionofnitrogengas,thermogravimetricanalyses,X-rayresonancediff
6、ractionmethod,infraredanalyses,elementanalyzerandfluorescentanalyzedmethod.Thereactivationsofdeactivatedcatalystsweredonebyacidtreatments,stovingmethodandhightemperatureroasting.1.Superabundantsolventwouldacceleratethesidereactiotl,andthebyproductmacromoleculeaffectedthecata
7、lyststability;2.TheironionwouldaffectthestabilityofTS一1whenitwasdepositedonTS一1;3.Theadsorptionofmacromoleculesoncatalystswasthemajorreasonfordeactivationofthecatalystsinepoxidationofchloropropcne;4.Themethodasacidtreatments,storingmethodandhightemperatureroastingcouldmaketh
8、edeactivatedcatalystsindistillationreachthecatalysislevelasnewlycatalyst;5.