10478.1,2二氯丙烷催化脫氯性能的研究

1、12二氯丙烷催化脫氯性能的研究摘要本文制備了FeCl3AICl3TiCl√AC催化劑，將其應(yīng)用于1，2二氯丙烷催化脫氯制丙烯的反應(yīng)中。采用固定床反應(yīng)器，考察了不同反應(yīng)工藝條件對(duì)催化劑活性的影響，通過(guò)XRD、BET和SEM等方法對(duì)催化劑進(jìn)行了表征。本文還考察了1，2二氯丙烷分別在NaOH水溶液、NaOH醇溶液中發(fā)生消除反應(yīng)制得1氯丙烯。采用高壓釜反應(yīng)器，考察了不同反應(yīng)工藝條件對(duì)消除反應(yīng)的影響。一、1，2二氯丙烷催化脫氯反應(yīng)本文以FeCl3

2、、AICl3、TICl4為活性組分，活性炭為載體，采用浸漬負(fù)載法制備了FeCl3AICl3TiCl4／AC催化劑，并通過(guò)XRD、SEM、BET等手段對(duì)其進(jìn)行表征。從XRD和SEM譜圖中得出，活性炭負(fù)載金屬氯化物后，石墨特征衍射峰仍然明顯存在，說(shuō)明金屬氯化物均勻負(fù)載在活性炭表面，并未對(duì)活性炭的石墨結(jié)構(gòu)造成破壞。BET結(jié)果表明：FeCl3AICl3一TiCl4／AC催化劑的比表面積為10814m2／g，孔體積023cm3／g，催化劑的孔結(jié)構(gòu)

3、以微孔為主，含有部分中孑L。從NH3TPD譜圖中可以看出該催化劑存在較多的弱酸位以及少量的中酸位。實(shí)驗(yàn)考察了FeCl3A1C13TiCl4／AC催化劑對(duì)12二氯丙烷脫氯反應(yīng)的影響。結(jié)果表明：當(dāng)溫度處于250300。C時(shí)，F(xiàn)eCl3AICl3TiCl4／AC催化劑主要催化1，2二氯丙烷脫氯化氫生成1氯丙烯。當(dāng)溫度高于350℃時(shí)，催化劑主要催化l，2二氯丙烷脫氯氣生成丙烯。兩者的變化趨勢(shì)相反，總選擇性在91％左右。在低空速下，F(xiàn)eCl3AI

4、Cl3TiCl4／AC催化劑主要催化12二氯丙烷脫氯氣生成丙烯，隨著空速的增加丙烯的選擇性隨之降低。當(dāng)反應(yīng)溫度為460。C，質(zhì)量空速為06h。時(shí)，F(xiàn)eCl3A1C13TiCl4／AC催化劑對(duì)l，2一二氯丙烷的催化活性最高，1，2一二氯丙烷的轉(zhuǎn)化率大于99％，丙烯的選擇性為87，9％。二、1，2二氯丙烷堿性消除反應(yīng)本文以1，2二氯丙烷堿性消除脫氯化氫制備1氯丙烯為探針，采用高壓釜反應(yīng)裝置，考察了不同溶劑、反應(yīng)溫度、原料摩爾比等因素對(duì)消除反

5、應(yīng)的影響。1、以1，2一二氯丙烷為原料，將其與NaOH水溶液混合，在表面活性劑的作用下發(fā)生消除反應(yīng)制備了1氯丙烯。最佳反應(yīng)條件為：反應(yīng)溫度為150℃，NaOH和1，2。二氯丙烷摩爾比為11：1，NaOH摩爾濃度為12mol／L、以十六烷基三甲基溴化銨為表面活性劑，其用12二氯丙烷催化脫氯性能的研究AbstractlIllIqllIllIIIIllIllIlUIIIIIIIY3130475Inthethesis，theFeCl3一AICl

6、3一TiCl4／ACcatalystwasprepared，whichwasappliedtothereactionof12一dichloropropanetopropyleneincatalyticdechlorinationTheeffectsofdifferentreactionconditionsoncatalystactivitywereinvestigatedinfixedbedreactorThecatalystwasch

7、aracterizedbyXRD，BETSEMandsomeothermethodsItwasalsoinvestigatedthat12一dichloropropaneoccurredeliminationreactionwithNaOHsolutionorNaOHalcoholsolutiontoprepare1allylchloride，andtheeffectsofdifferentreactionconditionsoneli

8、minatereactioninautoclavereactorswereinvestigated112dichloropropanecatalyticdechlorinationTheFeCl3AICl3一TiCVACcatalystWaspreparedbyimpregnationsupportingmethodwithFeCl3，AICl3andTiCl4astheactivecomponentandactivatedcarbon

9、asthecarrierThecatalystwascharacterizedbyXRD，SEM，BETandothermeansTheXRDandSEMresultsshowedthatafterthemetalchlorideswereloadedtothesurfaceofactivatedcarbon，graphitecharacteristicdiffractionpeakswerestillevidentItindicate

10、dthatthemetalchlorideswereloadedtothesurfaceofactivatedcarbonequablyandtheydidnotdamagetothegraphitestructuresofactivatedcarbonTheBETresultsshowedthatthespecificsurfaceareawas10814m2／g，porevolumeWas023cm’／gandthereexiste

11、dmesoporesandthemajorpartofmicroporesItcanbeseenfromtheNH3TPDspectrathattherearemanyweakacidsitesandasmallamountofacidsitesinthecatalystTheeffectofFeCl3AICl3—TiCla／ACcatalyston12dichloropropanedechlorinationwasinvestigat

12、edTheresultsshowedthatwhenthetemperaturewas250℃to300℃，F(xiàn)eCl3一A1C13一TiCldACcatalystmainlycatalyzed12一dichloropropanedehydrochlorinationgenerate1allylchlorideWhenthetemperaturewashigherthan350℃catalystmainlycatalyzed12dichl

13、oropropaneoffchlorinetopropyleneThechangetrendofthebothisincontrastAndthetotalselectivityisabout91％AtlowspacevelocityFeCl3一AICl3TiCl4／ACcatalystwasmainlyappliedto12一dichloropropaneoffchlorinetopropyleneAsairspeedincreasi

14、ng，theselectivityofpropylenedecreasedWhenthereactiontemperaturewas460℃andthequalityofthespacevelocitywas06h一thecatalyticactivityofFeCl3一AICl3TiCh／ACcatalystfor1，2dichloropropanewasthehighest，theconversionof12dichloroprop

15、anewasmorethan99％andtheselectivityofpropylenewas879％212一dichloropropaneeliminationreactionofchlorinatedhydrocarbonsTheinfluencesofdifferentsolvents，reactiontemperature，moleratioandotherfactorsontheeliminationreactionwith