zn-cr催化剂上甲醇氧化重整制氢研究

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1、摘要本论文采用不锈钢微通道反应器，首先考察TCr203／ZnO固溶体催化剂对甲醇水汽重整反应的催化性能。结果表明ZnO是其中的活性组分，cr的加入有助于催化剂活性和稳定性的提高，这可归因于ZnCr204固溶体的形成。但Cr的加入导致CO选择性增加。在浸渍法制备了Zn．Cr催化剂上，考察了甲醇水汽重整、甲醇部分氧化、甲醇氧化重整以及水气变换等反应过程，探讨了甲醇水汽重整和氧化重整两个过程的独立反应网络。研究表明，甲醇水汽重整过程可以简单地用甲醇水汽重整和分解两个平行反应来描述：‰乩100×l0nex，鸽产)喘0．8毗66-0。A0lm。l／gcaIhr‰_119l×1

2、0¨exp(兰鼍$编moJ／gcat．hr甲醇氧化重整包含了甲醇氧化和水汽重整两个独立过程。低温下主要是甲醇氧化过程，可用甲醇部分氧化、完全氧化和甲醇分解三个反应简单描述：POMCOMDMrt=1．135×109xgxp(兰鼍笋磁-。．439龟O．216m01／删r一．230×106XCXp(二等)磷妒mol栅hr％_2042×109×exp(毫掣以0．／1H6m。I／gcat．IIr“』而高温下上述三个反应可以按快速反应处理，而且还伴有水汽重整过程SRM嘲郧ox1015exp(专芦躲础3m。1／gcat．nr。M纠劢4×10”exp(二等马嘿m。J／gear．hr

3、关键词：甲酵，重整，动力学，zn．cr催化剂，微反应器Abs订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)聪唰“m01／gcat．hr‰：1．191×1011exp(—-