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High-performance thin-felt [email protected] catalysts synthesized via seed-assisted vapor phase transport for methanol-to-propylene reaction: Effects of crystal size, mesoporosity and aluminum uniformity
Journal of Catalysis ( IF 7.3 ) Pub Date : 2018-02-12 , DOI: 10.1016/j.jcat.2018.01.025
Jia Ding , Pengjing Chen , Guofeng Zhao , Ye Liu , Yong Lu

A series of thin-felt [email protected] catalysts are fabricated via the seed-assisted vapor-phase transport (VPT) method. The crystal size and mesoporosity of zeolite shell are controllably tuned toward enhanced diffusion by increasing the silicalite-1 seeding gel (SG) amount used. The microstructured catalyst obtained with a high SG amount of 50% contains a smaller crystal size of ∼70 nm and higher mesopore volume of 0.21 cm3 gzeolite−1, which markedly prolonged single-run lifetime with a remarkable decrease in the coking rate in the MTP process. The adverse effect of non-uniform aluminum in the zeolite shell on the MTP stability is revealed. The use of aluminum-containing SG to replace the pure-silica one makes the acid sites of as-obtained ZSM-5 mounted on SS-fiber distributed homogeneously thereby leading to a marked suppression of hydrogen transfer, and as a result, the catalyst single-run lifetime is further increased by ∼40%. This promising [email protected] catalyst is stable for at least 1600 h (>94% conv.) with a high propylene selectivity of ∼36% at 450 °C using a WHSV of 1 h−1 for a feed of MeOH/H2O molar ratio of 1:1, by taking advantage of improved diffusion from mesoporosity development and uniform aluminum distribution as well as our distinctive microfibrous-engineered design.



中文翻译:

通过种子辅助气相传输合成的用于甲醇到丙烯反应的高性能稀毡[电子邮件保护]催化剂:晶体尺寸,介孔率和铝均匀性的影响

通过种子辅助气相传输(VPT)方法制造了一系列薄毡[电子邮件保护的]催化剂。通过增加使用的silicalite-1晶种凝胶(SG)的量,可控制地调节沸石壳的晶体尺寸和介孔性,以增强扩散。SG含量高达50%的微结构催化剂的晶体尺寸较小,约为70 nm,中孔体积较高,为0.21 cm 3  g沸石-1,显着延长了单次运行寿命,并且MTP工艺中的焦化率显着降低。揭示了沸石壳中铝的不均匀对MTP稳定性的不利影响。用含铝的SG代替纯二氧化硅使安装在SS纤维上的ZSM-5的酸位均匀分布,从而显着抑制了氢的转移,结果使催化剂单一运行寿命进一步增加了约40%。这种有前途的[受电子邮件保护的]催化剂在450°C下使用1 h -1的WHSV进行MeOH / H 2进料,可在至少1600 h(> 94%换算)下稳定,并具有约36%的高丙烯选择性。O摩尔比为1:1,这是由于利用了中孔形成过程中改善的扩散和均匀的铝分布以及我们独特的微纤维工程设计而获得的。

更新日期:2018-02-12
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