低碳化学与化工2024，Vol.49Issue(4)：51-57,7.DOI:10.12434/j.issn.2097-2547.20230239
乙撑胺改性纯硅分子筛用于环己酮肟气相重排制已内酰胺
Ethylenediamine-modified pure silicalite molecular sieves applied in preparation of caprolactam via cyclohexanone oxime gas-phase rearrangement
丁克鸿 1王根林 1王刚 1王铖 1郭昊天 1梅学赓1
作者信息
- 1. 江苏扬农化工集团有限公司,江苏 扬州 225001
- 折叠
摘要
Abstract
The preparation of caprolactam(CPL)by cyclohexanone oxime(CHO)gas-phase Beckmann rearrangement is a green and environmentally friendly production process,but the performance of gas-phase rearrangement catalysts has always restricted the industrial application of this process.In order to enhance the reaction performance of gas-phase Beckmann rearrangement,ethyleneamine with different molecular sizes were used to modify pure silicalite molecular sieves.Characterization of the modified pure silicalite molecular sieves was carried out by scanning electron microscopy(SEM),transmission electron microscopy(TEM),X-ray diffraction(XRD)and N2 adsorption/desorption tests,and the catalytic performance of the catalysts for CHO gas-phase Beckmann rearrangement was evaluated.The results indicate that the pure silicalite molecular sieves maintain their original MFI topology after ethyleneamine-modification,and the Brunner-Emmet-Teller(BET)specific surface area decreases to 354.1 m2/g,and the CPL selectivity increases to 97.00%.The effects of reaction temperature,weight hourly space velocity and mass fraction of CHO on gas-phase Beckmann rearrangement were investigated.The optimal reaction processes are as follows:reaction temperature 370℃,weight hourly space velocity of CHO 1.0 h-1 and mass fraction of CHO 30%.Under the optimal reaction processes,the CHO conversion rate of S-1-B catalysts is≥99.90%,and the CPL selectivity of S-1-B catalyst is≥97.00%.The S-1-B catalyst has single-pass life of 1200 hours and stable regeneration performance,which has good industrial application prospect.关键词
己内酰胺/气相重排/分子筛改性/环己酮肟Key words
caprolactam/gas-phase rearrangement/molecular sieve modification/cyclohexanone oxime分类
化学化工引用本文复制引用
丁克鸿,王根林,王刚,王铖,郭昊天,梅学赓..乙撑胺改性纯硅分子筛用于环己酮肟气相重排制已内酰胺[J].低碳化学与化工,2024,49(4):51-57,7.
