An integrated approach to the key parameters in methanol‐to‐olefins reaction catalyzed by MFI/MEL zeolite materials  

MFI/MEL分子筛催化甲醇制烯烃反应关键参数的集成方法

作　　者：Chuncheng Liu Evgeny A.Uslamin Sophie H.van Vreeswijk Irina Yarulina Swapna Ganapathy Bert M.Weckhuysen Freek Kapteijn Evgeny A.Pidko Chuncheng Liu;Evgeny A.Uslamin;Sophie H.van Vreeswijk;Irina Yarulina;Swapna Ganapathy;Bert M.Weckhuysen;Freek Kapteijn;Evgeny A.Pidko(代尔夫特理工大学化学工程系,无机系统工程,代尔夫特,荷兰;巴斯夫股份公司,工艺研究和化学工程,路德维希港,德国;乌特勒克大学德拜纳米材料科学研究所,无机化学与催化,乌特勒克,荷兰;代尔夫特理工大学化工系,催化工程系,代尔夫特,荷兰)

机构地区：[1]Inorganic Systems Engineering,Department of Chemical Engineering,Delft University of Technology,Van der Maasweg 9,2629 HZ Delft,the Netherlands [2]BASF SE,Process Research and Chemical Engineering,Ludwigshafen 67056,Germany [3]Inorganic Chemistry and Catalysis,Debye Institute for Nanomaterials Science,Utrecht University,Universiteitsweg 99,3854 CG Utrecht,the Netherlands [4]Catalysis Engineering,Department of Chemical Engineering,Delft University of Technology,Van der Maasweg 9,2629 HZ Delft,the Netherlands

出　　处：《Chinese Journal of Catalysis》2022年第7期1879-1893,共15页催化学报（英文）

基　　金：supported by the BASF and the Advanced Research Center Chemical Building Blocks Consortium (ARC CBBC) for Funding under Project (2016.007.TUD)

摘　　要：Identification of the catalyst characteristics correlating with the key performance parameters including selectivity and stability is key to the rational catalyst design. Herein we focused on the identification of property-performance relationships in the methanol-to-olefin(MTO) process by studying in detail the catalytic behaviour of MFI, MEL and their respective intergrowth zeolites. The detailed material characterization reveals that both the high production of propylene and butylenes and the large Me OH conversion capacity correlate with the enrichment of lattice Al sites in the channels of the pentasil structure as identified by 27 Al MAS NMR and 3-methylpentane cracking results. The lack of correlation between MTO performance and other catalyst characteristics, such as crystal size, presence of external Brønsted acid sites and Al pairing suggests their less pronounced role in defining the propylene selectivity. Our analysis reveals that catalyst deactivation is rather complex and is strongly affected by the enrichment of lattice Al in the intersections, the overall Al-content, and crystal size. The intergrowth of MFI and MEL phases accelerates the catalyst deactivation rate.了解与关键催化性能参数(如选择性和稳定性)相关的催化剂特性对于合理设计催化剂是非常重要的.本文重点考察了甲醇制烯烃(MTO)过程中MFI、MEL及其共生沸石分子筛的催化行为和构效关系.表征结果表明,丙烯和丁烯的高产率和MeOH的高转化率均与Pentasil分子筛结构中晶格Al位的富集相关,这也被27Al MAS NMR结果和3-甲基戊烷裂解结果证实.催化剂对MTO反应的催化性能与其晶体尺寸、外部B酸中心和铝配对等性质之间缺乏相关性,表明它们对提高丙烯选择性的作用不大.本文分析表明,催化剂失活非常复杂,受交叉点处晶格铝富集、总铝含量和晶体尺寸影响较大,且MFI和MEL相共生加速了催化剂失活.

关 键 词：Structure‐performance relationship Zeolite catalysis Methanol‐to‐olefin conversion Al‐distribution ACIDITY Intergrowth MFI/MEL Pentasil 

分 类 号：TQ221.2[化学工程—有机化工] TQ426