S-1分子筛羟基窝锚定钴用于丙烷脱氢制丙烯
收稿日期: 2022-12-05
网络出版日期: 2023-05-15
基金资助
国家重点研发计划项目(2022YFE0116000);国家自然科学基金(22202193);中国博士后基金(2019M661147);中国科学院青年创新促进会(2021182);大连化物所创新基金(DICP I202217)
Co anchored on silanol nests of S-1 zeolite for propane dehydrogenation to propylene
Received date: 2022-12-05
Online published: 2023-05-15
以全硅MFI分子筛（S-1）为载体，采用简单的浸渍法制备了不同钴（Co）含量的Co/S-1催化剂并应用于丙烷脱氢反应。利用X射线衍射（XRD）、氮气吸附-脱附、傅里叶变换红外光谱（FT-IR）等技术对Co/S-1进行表征。结果表明，Co负载在S-1载体上并与S-1的Si—OH反应生成单位点Co物种和超小的Co纳米团簇，这些物种是丙烷脱氢的主要活性中心。Co的负载量对丙烷脱氢影响很大，当负载量较低时，活性Co物种较少，丙烷脱氢性能较差；当负载量较高时，Co物种会团聚成大颗粒不利于丙烷脱氢反应。通过优化制备条件，发现当Co负载量为1%（质量分数）时，Co/S-1的丙烷脱氢性能最优，循环使用5次后丙烷转化率、丙烯选择性和丙烯产率均未出现明显的下降。
贾育红 , 胡忠攀 , 王坤院 , 韩晶峰 , 魏迎旭 , 刘中民 . S-1分子筛羟基窝锚定钴用于丙烷脱氢制丙烯[J]. 无机盐工业, 2023 , 55(5) : 121 -127 . DOI: 10.19964/j.issn.1006-4990.2022-0714
Co/S-1 catalysts with different cobalt（Co） contents were prepared by a simple impregnation method using pure silica MFI zeolite（S-1） as carrier and applied to the dehydrogenation of propane.Co/S-1 was characterized by X-ray diffraction（XRD），nitrogen adsorption desorption，and Fourier transform infrared spectroscopy（FT-IR）.The results showed that Co was loaded on the S-1 carrier and reacted with the Si—OH of S-1 to form unit point Co species and ultra small Co nanoclusters，which were the main active centers for propane dehydrogenation.The loading amount of Co had a significant impact on propane dehydrogenation.When the loading amount was low，there were fewer active Co species and propane dehydrogenation performance was poor.When the loading amount was high，the Co species would agglomerate into large particles，which was not conducive to the propane dehydrogenation reaction.By optimizing the preparation conditions，it was found that when the Co loading amount was 1%（mass fraction），the propane dehydrogenation performance of Co/S-1 was optimal.After 5 cycles of recycling，there was no significant decrease in propane conversion，propylene selectivity，and propylene yield.
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