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陶瓷膜反應(yīng)器中環(huán)己酮氨肟化的催化劑失活機(jī)制與再生

發(fā)布時(shí)間:2018-04-30 19:52

  本文選題:環(huán)己酮肟 + TS-分子篩 ; 參考:《化工學(xué)報(bào)》2017年05期


【摘要】:基于陶瓷膜反應(yīng)器開發(fā)出無有機(jī)溶劑的環(huán)己酮氨肟化新工藝,探討TS-1催化劑失活機(jī)制。采用XRD及Rietveld全譜擬合、FT-IR、N_2吸附-脫附、TGA/DSC、GC-MS等手段對TS-1分子篩的骨架結(jié)構(gòu)、晶胞參數(shù)、比表面積和有機(jī)物種類進(jìn)行了表征分析。結(jié)果表明,無有機(jī)溶劑的環(huán)己酮氨肟化反應(yīng)過程中,存在硅流失的現(xiàn)象,但TS-1骨架完整,晶胞參數(shù)未明顯變化;環(huán)己酮、環(huán)己酮肟及反應(yīng)副產(chǎn)物等吸附在TS-1催化劑的表面及孔道內(nèi),使比表面積下降52.6%、孔體積減少了41.6%,是造成TS-1失活的主要原因,空氣氛圍中于600℃煅燒3 h,可以恢復(fù)催化劑的活性。
[Abstract]:Based on ceramic membrane reactor, a new process of ammoximation of cyclohexanone without organic solvent was developed, and the deactivation mechanism of TS-1 catalyst was discussed. The skeleton structure, unit cell parameters, specific surface area and organic species of TS-1 molecular sieve were characterized by means of XRD and Rietveld full-spectrum fitting, such as FT-IRN _ 2 adsorption-desorption and TGA / DSC-GC-MS. The results showed that there was silicon loss in the ammoximation of cyclohexanone without organic solvent, but the TS-1 skeleton was intact and the unit cell parameters did not change obviously, cyclohexanone, cyclohexanone, cyclohexanone, cyclohexanone, cyclohexanone, Cyclohexanone oxime and by-products were adsorbed on the surface and pore channels of TS-1 catalyst, which reduced the specific surface area and pore volume by 52.6 and 41.6 respectively, which were the main causes of TS-1 deactivation. The activity of the catalyst could be restored after calcined at 600 鈩,

本文編號(hào):1825960

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