石油炼制与化工 ›› 2014, Vol. 45 ›› Issue (5): 29-33.

• 催化剂 • 上一篇    下一篇

MeAPO-5型分子筛的合成及其催化环己烷氧化性能研究

赵俊琦,施胜斌,程时标   

  1. 中国石化石油化工科学研究院
  • 收稿日期:2013-11-27 修回日期:2013-12-24 出版日期:2014-05-12 发布日期:2014-04-22
  • 通讯作者: 程时标 E-mail:sbcheng.ripp@sinopec.com

SYNTHESIS OF MeAPO-5 MOLECULAR SIEVES AND THEIR CATALYTIC PERFORMANCE FOR CYCLOHEXANE OXIDATION

  • Received:2013-11-27 Revised:2013-12-24 Online:2014-05-12 Published:2014-04-22

摘要: 在不添加HF的基础上,使用水热法合成分别含有Ce,Fe,Cr,Ti,Sn的5种MeAPO-5分子筛。采用X射线荧光、N2吸附-脱附、X射线衍射、傅里叶变换红外光谱、31P和27Al的核磁共振对MeAPO-5分子筛进行表征。以环己烷空气氧化为探针反应,考察这5种MeAPO-5分子筛对环己烷氧化反应的催化性能。结果表明,以CeAPO-5分子筛为催化剂时,在1.25 MPa、165 ℃条件下反应0.5 h,环己烷转化率为10.9%,环己醇、环己酮、环己基过氧化氢的选择性分别为40.0%,29.3%,10.2%,这3种产物的总收率达到8.7%,明显高于其它4种分子筛,因此,CeAPO-5分子筛是较为适宜的环己烷空气氧化催化剂。

Abstract: Five kinds of MeAPO-5 molecular sieves containing Ce, Fe, Cr, Ti, and Sn, respectively were synthesized by hydrothermal method in the absence of HF. The successful synthesis of the MeAPO-5 molecular sieves was verified by the characterization of X-ray fluorescence spectrometry, N2 adsorption-desorption isotherm, XRD, FT-IR, and NMR of 31P and 27Al. The catalytic performance of the five MeAPO-5 molecular sieves in the cyclohexane oxidization reaction with air was investigated. Using the CeAPO-5molecular sieve, at the reaction conditions: 1.25 MPa and 165 ℃ for 0.5 h, the cyclohexane conversion is 10.9%, and the selectivity for cyclohexanol, cyclohexanone, and cyclohexylhydroperoxide is 40.0%, 29.3%, and 10.2%, respectively, and the total yield of the three products is up to 8.7%, which is evidently the highest among all MeAPO-5 molecular sieves tested, showing the CeAPO-5 molecular sieve is a more proper catalyst for the oxidizing reaction of cyclohexane with air.