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钛硅分子筛的改性对环己烷氧化反应的影响

Effect of titanium silicalite modification on cyclohexane oxidation

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【作者】 宋厚杰齐骏鑫郭舒隽方嘉辉陈晓晖黄清明

【Author】 Song Houjie;Qi Junxin;Guo Shujuan;Fang Jiahui;Chen Xiaohui;Huang Qingming;National Engineering Research Center for Chemical Fertilizer Catalyst,Fuzhou University;Zhicheng College,Fuzhou University;

【机构】 福州大学化肥催化剂国家工程研究中心福州大学至诚学院

【摘要】 使用不同改性液H2SO4-H2O2、(NH42CO3-H2O2、(NH4)HF2-H2O2和(NH42CO3+(NH4)HF2-H2O2混合溶液对中空钛硅分子筛进行改性。采用XRD、UV-Vis和拉曼光谱进行表征分析,考察改性前后钛硅分子筛在环己烷氧化反应的催化性能。结果表明,改性过程没有破坏钛硅分子筛的MFI拓扑结构,但提高了钛硅分子筛相对结晶度,并脱除了部分锐钛矿相TiO2;与未改性钛硅分子筛相比,环己醇和环己酮选择性及H2O2有效利用率明显提高,以改性液(NH42CO3+(NH4)HF2-H2O2改性钛硅分子筛效果最佳,醇酮选择性提高12.78个百分点,H2O2有效利用率提高17.33个百分点;(NH42CO3+(NH4)HF2-H2O2混合溶液改性钛硅分子筛显著降低H2O2用量,在己内酰胺生产过程中有很好的应用前景。

【Abstract】 Hollow titanium silicalite( HTS) was modified by different solutions of H2SO4-H2O2,( NH42CO3-H2O2,( NH4) HF2-H2O2and( NH42CO3+( NH4) HF2-H2O2. The modified HTS samples were characterized by XRD,UV-Vis and Raman. The catalytic performance of HTS before and after modification for cyclohexane selective oxidation were investigated. The results showed that the modification of HTS did notdestroy its topological structure of MFI,improved the relative crystallinity of HTS,and partial anatase Ti O2 was removed. Compared with the HTS,the selectivity to cyclohexanol and cyclohexanone,and the utilization rate of H2O2 over modified HTS were improved obviously. HTS modified by the solution of( NH42CO3+( NH4) HF2- H2O2 for cyclohexane selective oxidation exhibited optimal catalytic performance,and the selectivity to cyclohexanol and cyclohexanone was increased by 12. 78 percentage point,the utilization rate of H2O2 was improved by 17. 33 percentage point; HTS modified by the solution of( NH42CO3+( NH4) HF2-H2O2 remarkably decreased H2O2 dosage,which had good application prospect in the process of caprolactam production.

【基金】 国家自然科学基金(20976030)资助项目
  • 【文献出处】 工业催化 ,Industrial Catalysis , 编辑部邮箱 ,2016年02期
  • 【分类号】TQ426
  • 【被引频次】2
  • 【下载频次】205
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