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《zn-cr催化劑上甲醇氧化重整制氫研究》由會(huì)員上傳分享,免費(fèi)在線閱讀,更多相關(guān)內(nèi)容在學(xué)術(shù)論文-天天文庫(kù)。
1、摘要本論文采用不銹鋼微通道反應(yīng)器,首先考察TCr203/ZnO固溶體催化劑對(duì)甲醇水汽重整反應(yīng)的催化性能。結(jié)果表明ZnO是其中的活性組分,cr的加入有助于催化劑活性和穩(wěn)定性的提高,這可歸因于ZnCr204固溶體的形成。但Cr的加入導(dǎo)致CO選擇性增加。在浸漬法制備了Zn.Cr催化劑上,考察了甲醇水汽重整、甲醇部分氧化、甲醇氧化重整以及水氣變換等反應(yīng)過程,探討了甲醇水汽重整和氧化重整兩個(gè)過程的獨(dú)立反應(yīng)網(wǎng)絡(luò)。研究表明,甲醇水汽重整過程可以簡(jiǎn)單地用甲醇水汽重整和分解兩個(gè)平行反應(yīng)來描述:‰乩100×l0nex,鴿產(chǎn))喘0.8毗66-0。A0lm。l/gcaIhr‰_119l×1
2、0¨exp(蘭鼉$編moJ/gcat.hr甲醇氧化重整包含了甲醇氧化和水汽重整兩個(gè)獨(dú)立過程。低溫下主要是甲醇氧化過程,可用甲醇部分氧化、完全氧化和甲醇分解三個(gè)反應(yīng)簡(jiǎn)單描述:POMCOMDMrt=1.135×109xgxp(蘭鼉筍磁-。.439龜O.216m01/刪r一.230×106XCXp(二等)磷妒mol柵hr%_2042×109×exp(毫掣以0./1H6m。I/gcat.IIr“』而高溫下上述三個(gè)反應(yīng)可以按快速反應(yīng)處理,而且還伴有水汽重整過程SRM嘲鄖ox1015exp(專蘆躲礎(chǔ)3m。1/gcat.nr。M糾勱4×10”exp(二等馬嘿m。J/gear.hr
3、關(guān)鍵詞:甲酵,重整,動(dòng)力學(xué),zn.cr催化劑,微反應(yīng)器Abs訂actAbstractWeiqiangCao(ChemicalEngineering)DirectedbyProfessorGuangwenChenThecombinedreformingofmethanol(CRM)isoneofthemostpromisingroutesforonboardhydrogenproductionfrommethanolduetoitshighefficiency.Thecurrentinvestigationofhydrogenproductionfrommethano
4、lmainlyfocusesonCu—basedandPal-basedcatalysts.However,theyfilenotsuitable南rhydrogenproductionbecauseCu—basedcatalystsdeactivatequicklyandPd·Zncatalystsaretooexpensive.OurstudiesshowedthattheZn—CrcatalystwasapotentialcatalystforhydrogengenerationbyCRMduetoitshighstabilityandselectivity.
5、ThecatalyticperformanceofasolidsolutionCr20s/ZnOforsteamreformingofmethanol(SRM)wasstudiedinthisthesis,usingamicrochannelreactor.TheresultsshowedthatZnOistheactivesiteandtheadditionofCrpromotedtheactivityandselectivityofthecatalyst,whichcouldbeattributedtotheformationofZnCr204spinel.Ho
6、wever,increasingCrcontentresultedinincreasingCOselectivity.ThereactionnetworksoftheSRMandCRMprocessesOVertheZn—Crcatalystwerefirstascertainedbyinvestigatingpartialoxidationofmethanol(POM),SRM,CRMandwatergasshift(wGs)andsoon.ThereactionkineticsofSRMandCRMwerethenstudiedusingastainlessst
7、eelmicrochannelreactor,basedonthereactionnetwork.TheresultsindicatedthattheSRMprocessshouldincludetwoindependentoverallreactions,Decompositionofmethanol(DM)andSRM.TheWGSandreverseWGSreactionscouldbeignoredinthereactionnetworkAbstract‰=1,100x10Hexp(i篙竽)聰唰“m01/gcat.hr‰:1.191×1011exp(—-