【作者】 曹卫强；

【导师】 陈光文；

【作者基本信息】 中国科学院研究生院（大连化学物理研究所） ， 化学工程， 2006， 硕士

【摘要】 本论文采用不锈钢微通道反应器,首先考察了Cr2O3/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ZnCr2O4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: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: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:更多还原

【Abstract】 The combined reforming of methanol (CRM) is one of the most promising routes for onboard hydrogen production from methanol due to its high efficiency. The current investigation of hydrogen production from methanol mainly focuses on Cu-based and Pd-based catalysts. However, they are not suitable for hydrogen production because Cu-based catalysts deactivate quickly and Pd-Zn catalysts are too expensive. Our studies showed that the Zn-Cr catalyst was a potential catalyst for hydrogen generation by CRM due to its high stability and selectivity.The catalytic performance of a solid solution Cr2O3/ZnO for steam reforming of methanol (SRM) was studied in this thesis, using a microchannel reactor. The results showed that ZnO is the active site and the addition of Cr promoted the activity and selectivity of the catalyst, which could be attributed to the formation of ZnCr2O4 spinel. However, increasing Cr content resulted in increasing CO selectivity.The reaction networks of the SRM and CRM processes over the Zn-Cr catalyst were first ascertained by investigating partial oxidation of methanol (POM), SRM, CRM and water gas shift (WGS) and so on. The reaction kinetics of SRM and CRM were then studied using a stainless steel microchannel reactor, based on the reaction network. The results indicated that the SRM process should include two independent overall reactions, Decomposition of methanol (DM) and SRM. The WGS and reverse WGS reactions could be ignored in the reaction network.更多还原